ALBERT

Description: 〈p〉Publication date: 15 November 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 257〈/p〉 〈p〉Author(s): Dan Yang, Liyun Cao, Liangliang Feng, Jianfeng Huang, Koji Kajiyoshi, Yongqiang Feng, Qianqian Liu, Wenbin Li, Li Feng, Guojuan Hai〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉The synergistic achievement of geometric optimization and surface/interfacial modulation of electrocatalysts for booting the overall efficiency of water splitting is highly desirable yet challenging. Herein, a novel hierarchical Ni〈sub〉3〈/sub〉S〈sub〉2〈/sub〉/VS〈sub〉4〈/sub〉 nanohorn array grown on nickel foam (NS-horn/NF) is prepared by a self-driven synthesis strategy. We demonstrate that 〈em〉in-situ〈/em〉 generation of VS〈sub〉4〈/sub〉 in the NS-horn/NF not only triggers the formation of such unique hierarchical architecture, but favors the graft of enriched active bridging S〈sub〉2〈/sub〉〈sup〉2−〈/sup〉 on the strong coupling interface between Ni〈sub〉3〈/sub〉S〈sub〉2〈/sub〉 and VS〈sub〉4〈/sub〉, and thus the enhanced HER kinetics. More importantly, the abundant active nickel oxides for the OER availably form on the interface benefiting from the surface reconstruction of NS-horn/NF due to the partial leaching of vanadium (IV) of VS〈sub〉4〈/sub〉, which promotes the adsorption of OH〈sup〉−〈/sup〉 and leads to the fast OER rate-determining step in alkaline media. When employed to assemble an alkaline electrolyzer as both anode and cathode, NS-horn/NF electrode only needs a small voltage of 1.57 V to yield 10 mA cm〈sup〉−2〈/sup〉 and retains this activity for at least 70 h. Our findings put forward fresh insights into the rational design of highly efficient bifunctional electrocatalysts toward water spitting for next-generation energy conversion and storage devices.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319306575-ga1.jpg" width="433" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 November 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 257〈/p〉 〈p〉Author(s): Tao Zeng, Shuqi Li, Yi Shen, Haiyan Zhang, Hongru Feng, Xiaole Zhang, Lingxiangyu Li, Zongwei Cai, Shuang Song〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Herein, we designed a novel sodium-doped covalent triazine-based framework with a 3D honeycomb nanoarchitecture (H-CTF-Na) as visible-light-responsive organocatalyst to efficiently drive advanced oxidation processes (AOPs). Experimental and theoretical findings reveal that Na doping narrows the band gap by elevating the band edges and the 3D hierarchical nanocellular morphology improves light harvesting and electron transfer. With these merits, H-CTF-Na showed a photoactivity enhancement of 4.9–6.0-fold for the degradation of carbamazepine (CBZ) compared to those of pristine CTFs and g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 through peroxymonosulfate (PMS) activation under visible-light irradiation. The quenching and EPR results indicate that a synergistic effect between photooxidation (〈em〉h〈sup〉+〈/sup〉〈/em〉) and PMS activation (〈sup〉•〈/sup〉OH and SO〈sub〉4〈/sub〉〈sup〉•−〈/sup〉) derived from the vigorous capture of photogenerated e〈sup〉−〈/sup〉 by PMS is responsible for the marked efficacy of H-CTF-Na/vis/PMS system. Moreover, this system exhibited excellent versatility in degrading other organics (such as various phenols and dyes) and good reusability in terms of five high-efficiency recycled uses.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319306617-ga1.jpg" width="265" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 November 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 257〈/p〉 〈p〉Author(s): Zhihong Ye, Enric Brillas, Francesc Centellas, Pere Lluís Cabot, Ignasi Sirés〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉The feasibility of destruction of organic pollutants in water at near-neutral pH by homogeneous electro-Fenton (EF) process employing a soluble Fe(III)–EDDS complex as catalyst is demonstrated for the first time. The performance of the Fe(III)–EDDS-assisted EF process with carbon-felt or air-diffusion cathodes was evaluated from the degradation of butylated hydroxyanisole (BHA) in sulfate medium. The influence of applied current, pH and Fe(III):EDDS ratio and dosage on BHA decay and mineralization was related to the evolution of H〈sub〉2〈/sub〉O〈sub〉2〈/sub〉 and iron concentrations. Using Fe(III)–EDDS, up to 50% Fe(II) regeneration was achieved in 10 min, whereas only 23% was transformed using hydrated Fe〈sup〉3+〈/sup〉. Almost total removal of BHA was achieved thanks to homogenous Fenton, heterogeneous Fenton with cathodically adsorbed Fe(III), and electrocatalysis. The mineralization partly corresponded to the gradual destruction of EDDS by hydroxyl radical (〈em〉k〈/em〉〈sub〉abs〈/sub〉 = 5.22 × 10〈sup〉9〈/sup〉 M〈sup〉−1〈/sup〉 s〈sup〉−1〈/sup〉), and involved the formation of 5 oxidation and 6 dimerization or cyclization by-products.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319306538-ga1.jpg" width="327" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 November 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 257〈/p〉 〈p〉Author(s): Jiangyao Chen, Zhigui He, Yuemeng Ji, Guiying Li, Taicheng An, Wonyong Choi〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉The photocatalytic transformation mechanisms of styrene, were compared in TiO〈sub〉2〈/sub〉 system under ultraviolet (UV) and vacuum ultraviolet (VUV) irradiations. TiO〈sub〉2〈/sub〉/VUV displayed higher photocatalytic degradation and mineralization efficiencies (100% and 51% within 8 min) than TiO〈sub〉2〈/sub〉/UV (86% and 21% within 60 min), and the increased efficiencies were contributed from enhanced production of 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉OH through VUV photolysis of H〈sub〉2〈/sub〉O and O〈sub〉2〈/sub〉. The addition reactions of these enhanced 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉OH converted styrene to benzaldehyde and other small molecular carbonyl compounds in TiO〈sub〉2〈/sub〉/VUV gas system. Due to absence of atmospheric 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉OH in TiO〈sub〉2〈/sub〉/UV system, styrene underwent cycloisomerisation to form a bicyclic byproduct, benzocyclobutene, which further transformed to benzocyclobutenone, benzocyclobutenol, phthalan, phthalide and phthalic anhydride on photocatalyst TiO〈sub〉2〈/sub〉. Meanwhile, both systems shared same pathways from styrene to monoaromatic alcohols, ketones, aldehydes on TiO〈sub〉2〈/sub〉 through 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉OH addition. Our results provide a deep insight into 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉OH-determined photocatalytic transformation mechanism of AHs and their final fate in atmospheric environment.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319306587-ga1.jpg" width="247" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 November 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 257〈/p〉 〈p〉Author(s): Wei Gao, Bin Tian, Wenyan Zhang, Xuqiang Zhang, Yuqi Wu, Gongxuan Lu〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Solar irradiation spectrum on the earth consists of about 50% infrared energy, which has not used effectively in chemical storage and conversion into hydrogen via photocatalytic route. In this work, we reported the catalytic hydrogen generation over a photocatalyst consisting of semiconductor CdS and an up-conversion component NaYF〈sub〉4〈/sub〉-Yb〈sup〉3+〈/sup〉-Er〈sup〉3+〈/sup〉(NYF) under infrared light irradiation. Under 980 nm laser irradiation, the input infrared light was up-converted into visible light, which was used to excite CdS to produce hydrogen and oxygen. The isotope experiments confirmed both of hydrogen and oxygen were produced from water. The highest hydrogen evolution rate of 3.38 μmol g〈sup〉−1〈/sup〉 h〈sup〉−1〈/sup〉 has been achieved. 0.008% of AQE under NIR light irradiation has been approached.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉The NIR/visible-light driven over-all water splitting was achieved over Pt/CdS/NaYF〈sub〉4〈/sub〉-Yb〈sup〉3+〈/sup〉-Er〈sup〉3+〈/sup〉 catalyst by taking advantages of the NIR-to-visible upconversion and the inhibition of the reverse H〈sub〉2〈/sub〉-O〈sub〉2〈/sub〉 recombination reaction via transferring the photo-generated oxygen molecules away from the photocatalyst surface by PFDL. This method makes the most visible light-responsive semiconductor photocatalysts capable utilizing in overall split water by NIR/visible light irradiation.〈/p〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S092633731930654X-ga1.jpg" width="275" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Haiyuan Zou, Ge Li, Lele Duan, Zongkui Kou, John Wang〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Herein, we report a new type of efficient trifunctional electrocatalyst by in situ coupling amorphous cobalt nitride (CoN〈em〉〈sub〉x〈/sub〉〈/em〉) nanoparticles within three-dimensional (3D) nitrogen-doped graphene aerogel (NGA). The CoN〈em〉〈sub〉x〈/sub〉〈/em〉/NGA nanohybrid with hierarchical porous strucuture guarantees the superior activities toward ORR, OER and HER, due to abundant dual active CoN〈em〉〈sub〉x〈/sub〉〈/em〉 and N〈em〉〈sub〉x〈/sub〉〈/em〉C sites. Impressively, it also exhibits a long lifetime and exceptionally high electrochemical performances as a cathode and an anode in a two-electrode overall water splitting electrolyzer, and also as an air-cathode in a rechargeable Zn-air battery. In addition, the CoN〈em〉〈sub〉x〈/sub〉〈/em〉/NGA-based water splitting electrolyzer and two Zn-air batteries can be integrated together to effectively self-drive electrochemical water splitting device with high gas evolution rates of 186 and 372 μmol h〈sup〉−1〈/sup〉 for O〈sub〉2〈/sub〉 and H〈sub〉2〈/sub〉, respectively. This work paves a way for designing advanced non-noble multifunctional catalysts, aiming for the real application of energy storage and conversion devices.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉A trifunctional catalyst, denoted as CoN〈em〉〈sub〉x〈/sub〉〈/em〉/NGA, is sucessufully constructed based on MOF derived amorphous CoN〈em〉〈sub〉x〈/sub〉〈/em〉 on nitrogen-doped graphene aerogel. This CoN〈em〉〈sub〉x〈/sub〉〈/em〉/NGA nanohybrid effectively catalyzes water oxidation, proton reduction and oxygen reduction reactions, and thereby promises the real application of integrated rechargable zinc-air battery to self-drive water splitting device.〈/p〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308471-ga1.jpg" width="219" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Jiří Henych, Štěpán Stehlík, Karel Mazanec, Jakub Tolasz, Jan Čermák, Bohuslav Rezek, Andreas Mattsson, Lars Österlund〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉We report on the synthesis and characterization of TiO〈sub〉2〈/sub〉/Nanodiamond (ND) nanocomposites for rapid decontamination of chemical warfare agents (CWA) and toxic industrial compounds prepared by a simple water-based, low-temperature method using urea as a homogeneous precipitating agent. The excellent water-compatibility of NDs promoted their good dispersion within the TiO〈sub〉2〈/sub〉 matrix resulting in intergrown TiO〈sub〉2〈/sub〉/ND nanostructures. NDs with an abundance of oxygen-containing surface moieties increased the porosity of the composites resulting in their three times more efficient spontaneous degradation of the CWA soman in solution compared to pure TiO〈sub〉2〈/sub〉. In situ DRIFT spectroscopy revealed the enhanced reactive adsorption and solar light photodecomposition of dimethyl methyl phosphonate vapor on TiO〈sub〉2〈/sub〉/ND. The charge transfer across TiO〈sub〉2〈/sub〉/ND interfaces that hinder recombination of photo-excited electron-hole pairs was inferred from surface potential measurements. The results indicate that well-dispersed NDs forming heterojunctions together with their high porosity contribute to the reactive properties of the nanocomposites.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308446-ga1.jpg" width="369" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: Available online 28 August 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental〈/p〉 〈p〉Author(s): Guangbo Liu, Zhonghua Li, Jianjian Shi, Kun Sun, Yujin Ji, Zhiguo Wang, Yunfeng Qiu, Yuanyue Liu, Zhijiang Wang, PingAn Hu〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉The great bottleneck that lies in CO〈sub〉2〈/sub〉 reduction reaction (CO〈sub〉2〈/sub〉RR) electrocatalysts is to simultaneously enhance their conductivity and density of active sites. Herein, we developed a black reduced porous SnO〈sub〉2〈/sub〉 nanosheets electrocatalyst that enabled possessing both metallic conductivity and high density of active sites via vacancy engineering. The black reduced porous SnO〈sub〉2〈/sub〉 nanosheets showed high activity and selectivity for CO〈sub〉2〈/sub〉RR to formate, with maximum Faradaic efficiency (FE) of 92.4% at the low overpotential of 0.51 V and stable FE of 90 ± 2% in the large potential range from -0.6 to -1.1 V vs. reversible hydrogen electrode (RHE). Density functional theory (DFT) calculations indicated that the introduction of oxygen vacancy increased carrier density and lowered the adsorption of 〈math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="si1.svg"〉〈msup〉〈mtext〉 HCOO〈/mtext〉〈mo〉-〈/mo〉〈/msup〉〈/math〉 * and HCOOH by 0.29 and 0.17 eV, respectively, accounting for the improved CO〈sub〉2〈/sub〉RR to formate performance.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308811-ga1.jpg" width="301" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈p〉Vertically aligned black reduced porous SnO〈sub〉2〈/sub〉 nanosheets were succesfully developed via vacancy engineering for the first time, which simultaneously realized the promoted conductivity and active sites, hence leading to the efficient and durable CO〈sub〉2〈/sub〉RR to formate.〈/p〉 〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Shengbo Zhang, Mei Li, Wenjun Qiu, Jinyu Han, Hua Wang, Xiao Liu〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉The effective molecular-catalyst-based device that converts CO〈sub〉2〈/sub〉 to value-added products is of significance but challenging. Herein, utilizing organosilica nanotubes as the solid chelating ligands, we successfully construct heterogeneous molecular rhenium catalysts for efficient CO〈sub〉2〈/sub〉 photoreduction to CO. The nanotube framework compositions and the microenvironment of the rhenium catalysts are finely regulated, aiming to enhance the catalytic selectivity and activity in water-containing systems. By adjusting bipyridine amounts and capping the surface silanols, the preferential adsorption for CO〈sub〉2〈/sub〉 over H〈sub〉2〈/sub〉O around the active sites is realized. Relative to that of the unmodified catalyst, the CO selectivity increased greatly from 53% to 94% in water/acetonitrile. Furthermore, the heterogeneous molecular catalysts exhibit a total turnover number that is nine times higher than the corresponding homogeneous one (134 〈em〉versus〈/em〉 15). Using 〈em〉in situ〈/em〉 infrared spectroscopy and density functional theory calculations, a reasonable mechanism for high CO selectivity in the presence of H〈sub〉2〈/sub〉O is demonstrated.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉The heterogeneous molecular rhenium catalysts were constructed based on porous organosilica nanotubes for the photoreduction of CO〈sub〉2〈/sub〉 to CO. The microenvironment around the active sites was modulated to realize the preferential adsorption of CO〈sub〉2〈/sub〉 over H〈sub〉2〈/sub〉O in water containing systems, resulting in the high CO selectivity of 94%.〈/p〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308604-ga1.jpg" width="339" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): A. Chunduri, S. Gupta, O. Bapat, A. Bhide, R. Fernandes, M.K. Patel, V. Bambole, A. Miotello, N. Patel〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉A unique cobalt-phosphide-boride (Co-P-B) catalyst was synthesized via simple chemical-reduction route. The obtained catalyst was amorphous in nature, resembling the spherical morphology of Co-B nanoparticles. X-ray photoelectron spectroscopy revealed that B loses electrons to Co while P gains electrons from Co. This unique electron transfer mechanism in Co-P-B is a combination of the characteristics showcased by Co-B and Co-P catalysts individually. The optimized catalyst (Co-P-B-5) showed overpotentials of 145 mV and 290 mV to achieve the benchmark current density of 10 mA/cm〈sup〉2〈/sup〉 for HER and OER, respectively, in 1 M NaOH. From theoretical calculations, it was observed that addition of P modulates the electron density at Co sites, thereby optimizing the H-adsorption capability, leading to higher HER rate. During anodic polarization, Co-P-B-5 shows formation of large number of CoOOH species on its surface, facilitating OER. Finally, stability, recyclability and wide-pH suitability of Co-P-B-5 was established to demonstrate its industrial viability.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307970-ga1.jpg" width="294" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Bin Chen, Zhuo Zhang, Sangkuk Kim, Minki Baek, Dokyoung Kim, Kijung Yong〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Oxygen evolution reaction (OER) is a key process in various advanced technologies for renewable energy conversion, such as water splitting and metal-air batteries. However, as a four-electron coupled reaction, the OER is kinetically sluggish and limited by its high overpotential and low efficiency. The design of novel nanostructured electrocatalysts is highly desirable to promote OER kinetics. Herein, a bio-inspired nanoleaf electrocatalyst has been successfully achieved for the first time by 〈em〉in situ〈/em〉 growing ultrathin NiCo layered double hydroxide (LDH) nanosheets on CuO nanowires. Attributed to the mechanical support of CuO nanowire veins, the NiCo LDH lamina presents a large lateral size (more than 10 μm) and unique hierarchical structure that consisted of ultrathin nanosheets with numerous exposed edges. The CuO veins distributed across the LDH lamina can serve as the fast path for charge transfer and significantly promote the LDH conductivity. Compared to the conventional NiCo LDH nanosheets, the novel nanoleaves with enlarged electrochemical surface area, edge-rich active sites, and improved conductivity exhibit greatly enhanced OER performances with an impressive 9.3 fold enhanced activity, much lower overpotential of 262 mV at 10 mA cm〈sup〉−2〈/sup〉, as well as good stability and flexibility. The biomimetic nanoleaf structures and the corresponding design strategy can be broadly applied to other functional 2D materials for advanced applications.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉〈strong〉A biomimetic nanoleaf electrocatalyst〈/strong〉 is achieved for the first time by combining ultrathin NiCo layered double hydroxide (LDH) lamina with CuO nanowire veins. The CuO veins support the LDH lamina and serve as fast path for charge transfer. The hierarchical nanoleaves with large surface area, edge-rich active sites, and improved conductivity exhibit superior electrochemical performances for oxygen evolution reaction.〈/p〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307635-ga1.jpg" width="387" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Lei Qin, Zhuotong Zeng, Guangming Zeng, Cui Lai, Abing Duan, Rong Xiao, Danlian Huang, Yukui Fu, Huan Yi, Bisheng Li, Xigui Liu, Shiyu Liu, Mingming Zhang, Danni Jiang〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉HNO〈sub〉3〈/sub〉-modified carbon black supported Ni-Au bimetallic nanocatalysts (HCB-Ni-Au) with different Ni/Au molar ratio were synthesized for hydrogenation of nitroaromatics. The synergistic effect between bimetallic nanoparticles and HCB, Ni and Au nanoparticles improved the catalytic efficiency. The reaction mechanism and pathway investigation exhibited that nitroaromatics were reduced by cleavage of 〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/sbnd"〉N〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/dbnd"〉O bond and azo linkage (〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/sbnd"〉N〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/dbnd"〉N〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/sbnd"〉) and uptake of H from Ni〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/sbnd"〉H and Au〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/sbnd"〉H bonds. Density functional theory theoretical calculation showed 4-nitrophenol (4-NP) with higher free energy was easier to be catalyzed. The activation of enthalpy for MO was 65.7 kcal mol〈sup〉−1〈/sup〉, which displayed the highest catalytic rate of 2.1055 min〈sup〉−1〈/sup〉. Meanwhile, the reaction rate of 4-NP hydrogenation catalyzed by HCB-Ni〈sub〉6〈/sub〉-Au〈sub〉1〈/sub〉 reached 1.9617 min〈sup〉−1〈/sup〉, which was 15 and 38 times higher than that of Ni and Au monometallic nanocatalyst, respectively. HCB-Ni〈sub〉6〈/sub〉-Au〈sub〉1〈/sub〉 with good structural stability could be well reused and applied in tap, distilled, river, and lake water samples.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307817-ga1.jpg" width="212" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Wei Ni, Congxin Li, Xiaogang Zang, Min Xu, Silu Huo, Mingquan Liu, Zhiyu Yang, Yi-Ming Yan〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Copper oxides have been used as efficient electrocatalysts for electrocatalytic reduction of carbon dioxide (CO〈sub〉2〈/sub〉). However, understanding the catalytic mechanism of copper oxides electrocatalysts based on identifying their active species is difficult due to the presence of multivalent Cu, such as Cu(0), Cu(I) and Cu(II) species, during the reaction. Also, developing copper oxides electrocatalysts with high selectivity and long durability for carbon dioxide reduction reaction (CO〈sub〉2〈/sub〉RR) is highly desired. Herein, we report the preparation of Cu〈sub〉x〈/sub〉O decorated graphene oxides (G-Cu〈sub〉x〈/sub〉O-T) electrocatalyst by a controllable chemical reduction method. The G-Cu〈sub〉x〈/sub〉O-2 h electrocatalyst exhibits high selectivity towards HCOOH (81%) with a current density of 19.3 mA cm〈sup〉-2〈/sup〉 at -0.8 V vs RHE, as well as good durability (retaining 87.2% of initial activity after 9 hours continuous operation). Our study reveals that the observed high performance of G-Cu〈sub〉x〈/sub〉O-2 h electrocatalyst should not only benefit from the stabilized 〈math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="si1.gif" overflow="scroll"〉〈msubsup〉〈mtext〉CO〈/mtext〉〈mn〉2〈/mn〉〈mrow〉〈mo〉•〈/mo〉〈mo〉-〈/mo〉〈/mrow〉〈/msubsup〉〈/math〉 intermediate, but also contribute from the facilitated rate-limiting step of 〈math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="si2.gif" overflow="scroll"〉〈msup〉〈mtext〉HCOO〈/mtext〉〈mo〉-〈/mo〉〈/msup〉〈/math〉 desorption, which are both closely related to an optimized Cu(I) content in the electrocatalyst. Moreover, a 〈em〉“buffering effect”〈/em〉 is proposed to explain the promising durability of G-Cu〈sub〉x〈/sub〉O-2 h, where Cu(II) species should serve as sacrificial sources to supply Cu(I) from the thick subsurface layers, thereby balancing the content of Cu(I) at the surface and maintaining the activity of the electrocatalyst during the reaction. Our work provides crucial insights into the role of multivalent Cu in CO〈sub〉2〈/sub〉 reduction reaction, which are important for designing and preparing copper oxides based electrocatalysts with high selectivity and durability for electrochemical reduction of CO〈sub〉2〈/sub〉 into liquid fuels.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307908-ga1.jpg" width="352" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Can Ma, Shuo Feng, Jinming Zhou, Rufen Chen, Yu Wei, Hui Liu, Sen Wang〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉The greatest problem in the homogeneous Fenton reaction is the low production of HO〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉 owing to the slow Fe〈sup〉III〈/sup〉/Fe〈sup〉II〈/sup〉 cycle. In this study, we demonstrate a new co-catalyst of FeP and trace Fe〈sup〉2+〈/sup〉 that can greatly enhance the decomposition efficiency of H〈sub〉2〈/sub〉O〈sub〉2〈/sub〉 and accelerate the degradation of methylene blue (MB). This co-catalyst is applicable in a broad pH range (pH = 3.0−9.0) and capable of degrading 95.74% and 89.01% of MB with 100 ppm in concentration within 30 s at pH 3 and 5, and 99.65% and 90.06% within 3 min at pH 7 and 9. The coexistence of FeP with Fe〈sup〉II〈/sup〉 accelerates the Fe〈sup〉III〈/sup〉/Fe〈sup〉II〈/sup〉 cycle by electron transfer between Fe〈sup〉δ+〈/sup〉 in FeP and Fe〈sup〉III〈/sup〉. Mössbauer spectra and density functional theory calculations indicate that the unique structure of FeP plays an important role in accelerating the Fe〈sup〉III〈/sup〉/Fe〈sup〉II〈/sup〉 cycle.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉The Fe〈sup〉III〈/sup〉/Fe〈sup〉II〈/sup〉 cycle in Fenton-like reaction was accelerated by the electron transfer within FeP. Mossbauer spectra and DFT calculation confirmed the existence of electron transfer.〈/p〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307611-ga1.jpg" width="348" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): D. Ishutenko, Yu. Anashkin, P. Nikulshin〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉K-CoMo/〈em〉Sup〈/em〉 (where 〈em〉Sup〈/em〉 = Al〈sub〉2〈/sub〉O〈sub〉3〈/sub〉, SiO〈sub〉2〈/sub〉, TiO〈sub〉2〈/sub〉 and ZrO〈sub〉2〈/sub〉) catalysts were synthesized using H〈sub〉3〈/sub〉PMo〈sub〉12〈/sub〉O〈sub〉40〈/sub〉, CoCO〈sub〉3〈/sub〉, KOH and citric acid. The catalysts were characterized by temperature-programmed reduction (TPR), temperature-programmed desorption of NH〈sub〉3〈/sub〉, X-ray photoelectron spectroscopy, transmission electron microscopy. Samples were tested in hydrotreating of model fluid catalytic cracking gasoline and in selective hydrogenation of 1,5-hexadiene and 〈em〉n〈/em〉-heptene-1. The type of used carrier significantly affected the morphology of active phase and catalytic properties. Active sites productivity of K-CoMo/〈em〉Sup〈/em〉 catalysts in hydrodesulfurization (HDS) and olefin hydrogenation (HYDO) reactions as well as HDS/HYDO selectivity correlated with active phase morphology excepting TiO〈sub〉2〈/sub〉-supported sample. Productivity of active sites in reactions of selective hydrogenation of diolefin depended on maximum peak reduction obtained from TPR, which in turn was a function of acidity of using supports. The highest HDS/HYDO selectivity was obtained at catalyst which possessed the lowest selectivity towards partial hydrogenation of diolefine compared to complete hydrogenation.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307878-ga1.jpg" width="500" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Yunxiang Li, Jian Ren, Shuxin Ouyang, Weishu Hou, Tristan Petit, Hui Song, Huayu Chen, Davin Philo, Tetsuya Kako, Jinhua Ye〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Atomic structure tailoring towards high electron mobility is an essential approach to maximizing the solar energy-conversion efficiency of polymeric carbon nitride (CN) but still presents a significant challenge. Here we construct a smooth carrier channel in the basal plane of CN by filling the rich defects in layer with various kinds of short carbon chains, whereby the light-induced carriers transfer kinetics is boosted distinctly. Consequently, the optimal carbon chains-planted CN delivers a remarkably enhanced photocatalytic performance, achieving a 13.2 and 29.2-fold improvement in H〈sub〉2〈/sub〉 evolution and CO〈sub〉2〈/sub〉 reduction, respectively. This study provides an in-depth insight into the modulation of in-plane electrical conductivity at molecular scale over CN and offers new opportunities for reinforcing the reaction kinetics of organic-based photocatalysts.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉This study demonstrates a novel approach to tailor electronical conductivity of polymeric carbon nitride (CN) by constructing molecule-level carbon chains in the defect-rich layers of CN, whereby the light-induced carriers transfer kinetics is boosted dramatically.〈/p〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307738-ga1.jpg" width="299" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Yu-Xuan Xiao, Jie Ying, Ge Tian, Yong Tao, Hao Wei, Si-Yu Fan, Ze-Hao Sun, Wan-Juan Zou, Jie Hu, Gang-Gang Chang, Weihua Li, Xiao-Yu Yang, Christoph Janiak〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉The strong Pt-carbon interaction is a very promising way to high-performance design of electrocatalysts. However, the heavy d-π overlap, a high strength of Pt-C bonding, in sp〈sup〉2〈/sup〉 bonded graphitic carbons with low level of defects is rarely reported. Herein, PtPd nanoparticles and graphitic carbon nanofibers (PtPd/CNF) have been integrated via heavy d-π overlap by an interfacial wettability approach and their formation mechanism has also been fully elucidated. The features of strong d-π overlap and high dispersion of metals offer PtPd/CNF with enhanced ORR activity (5.8 folds of specific activity than commercial Pt/C), and excellent structural stability and electrocatalytic durability. A new “heavy d-π overlap” concept, characteristics, and mechanism are proposed at an atomic-/nanoscale to clarify the generation of the predictive interaction as well as the interface charge transfer. It is believed that the study on heavy d-π overlap sheds new light on the fundamental aspects of the nature of Pt-C interaction.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308276-ga1.jpg" width="264" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Shihui Xing, Zhao Liu, Qi Xue, Shiwei Yin, Fumin Li, Weiwei Cai, Shuni Li, Pei Chen, Pujun Jin, Hongchang Yao, Yu Chen〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Reducing the overpotential of alcohol oxidation reactions is highly desirable for alkaline direct alcohol fuel cells, but there is still no substantial progress. In this study, unique three-dimensional free-standing Rh nanoroses are synthesized and applied to the isopropanol oxidation reaction. Compared to traditional Pt black electrocatalyst, as-prepared Rh nanoroses exhibit a significant negative shift both in the onset oxidation potential (Δ = 0.223 V) and peak potential (Δ = 0.435 V) as well as 7.5-fold mass activity at 0.3 V for the isopropanol oxidation reaction (IOR) in alkaline electrolyte. The density functional theory calculation indicates the enhanced IOR activity originates form the higher adsorption energy of isopropanol on Rh surface than Pt surface. Since Rh nanoroses have unparalleled activity, this research may bring a new broad of perspective on the isopropanol oxidation reaction.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉Rh nanoroses assembled from ultrathin nanosheets are applied to the isopropanol oxidation reaction, which exhibit significant negative shift both in the onset oxidation/peak potentials and enhanced mass activity compared with Pt black.〈/p〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S092633731930829X-ga1.jpg" width="246" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Ran Li, Xitao Li, Jiaojiao Wu, Xinding Lv, Yan-Zhen Zheng, Zhijie Zhao, Xiaoqing Ding, Xia Tao, Jian-Feng Chen〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Organic-inorganic perovskites like MAPbI〈sub〉3〈/sub〉 with excellent optoelectric properties have recently gained concerns in photocatalytic HI splitting. However, their achieved hydrogen evolution reaction (HER) rates are still insufficient. Herein, a 2D few-layer black phosphorus (BP) as cocatalyst was anchored on MAPbI〈sub〉3〈/sub〉 via electrostatic coupling. The resultant BP/MAPbI〈sub〉3〈/sub〉 is rather stable in HI solution during the whole photoreaction, yielding a superb HER rate of 3742 μmol h〈sup〉−1〈/sup〉 g〈sup〉−1〈/sup〉 under visible irradiation, which is two orders of magnitude higher than that of MAPbI〈sub〉3〈/sub〉-only, far higher than that of MAPbI〈sub〉3〈/sub〉/Pt and also shows the advanced HER performance among MAPbI〈sub〉3〈/sub〉 based systems. The remarkably boosted HER activity is thoroughly explored by optical/optoelectrochemical measurements, showing that BP can act as an electron promoter to trap electrons derived from MAPbI〈sub〉3〈/sub〉 through a type I heterojunction in the interface. This contributes to a new paradigm for high-efficiency photocatalysts by anchoring non-metal cocatalyst onto MAPbI〈sub〉3〈/sub〉 for solar energy conversion.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308227-ga1.jpg" width="500" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): M. Abidi, A.A. Assadi, A. Bouzaza, A. Hajjaji, B. Bessais, S. Rtimi〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉In this study, photoactive Cu〈sub〉x〈/sub〉O/TiO〈sub〉2〈/sub〉 coatings were prepared using magnetron sputtering operated at different powers and modes (Direct-current magnetron sputtering and High Power Impulse magnetron sputtering). Indoor/outdoor air pollutions (Volatile Organic Compounds, VOCs) degradation have been dramatically reduced on sputtered Cu〈sub〉x〈/sub〉O/TiO〈sub〉2〈/sub〉 on polyester (PES) cloth under low intensity visible light. The Low intensity visible light was used to irradiate the sputtered photocatalysts, which degraded various VOC molecules concomitant with a bacterial inactivation ability. The VOC removal kinetics were studied in the dark and under visible light as a function of the deposition time and applied peak currents during the coating by HiPIMS. High concentrations of chloroform and butyraldehyde were shown to be degraded (90% and 85%, respectively) on Cu〈sub〉x〈/sub〉O/TiO〈sub〉2〈/sub〉-PES fabrics under daylight irradiation. The repetitive reuse of the sputtered coatings was also investigated showing the long operational lifetime of the prepared fabrics. The deposition rates of Ti and Cu atoms and their atomic distribution along the sputtered film have been investigated by Transmission Electronic Microscopy (TEM). Redox catalysis was shown to happen within the VOC degradation time as detected by X-ray Photoelectron Spectroscopy (XPS). Deconvolution of the Cu2p3/2 peak in the Cu〈sub〉x〈/sub〉O/TiO〈sub〉2〈/sub〉 on PES samples showed changes in the Cu〈sub〉2〈/sub〉O and CuO within the VOCs degradation and the bacterial inactivation. The interfacial charge transfer (IFCT) between Cu〈sub〉x〈/sub〉O induced under light leading to VOCs oxidation path seemed to require a low photons energy and were able to oxidize the pollutants even at high concentrations. The mechanisms involving the VOCs degradation on Cu〈sub〉x〈/sub〉O/TiO〈sub〉2〈/sub〉 catalysts are suggested in which the holes generated by Cu〈sub〉2〈/sub〉O transfer to TiO〈sub〉2〈/sub〉 in the TiO〈sub〉2〈/sub〉(n)/Cu〈sub〉x〈/sub〉O(p) in the hetero-junction. This transfer is favored by the electrostatic interaction between both semiconductors. The photo-generated ROS, mainly 〈sup〉⦁〈/sup〉OH-radicals were determined by fluorescence method. The possible contribution of the 〈sup〉⦁〈/sup〉OH-radicals in the bacterial inactivation on the sputtered Cu〈sub〉x〈/sub〉O/TiO〈sub〉2〈/sub〉 catalysts was discussed. DRS, TEM, contact angle (CA) and XPS were used to characterize the catalyst optical and structural properties.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308215-ga1.jpg" width="365" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Lijun Yang, Lei Zhang〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Cost-effective transition metal-carbon-based hybrids have been widely dedicated to water splitting. Herein, a new three dimensional N-enriched holey carbon layers encapsulated bimetallic phosphides (CoNiP@CN) was synthesized by 〈em〉in situ〈/em〉 growth, pyrolysis and phosphorization of CoNi mixed zeolite imidazole frameworks (ZIFs)@ZIF-8 films on Ni foam. CoNiP@CN/NF exhibited smaller overpotentials, lower charge transfer resistance and considerable stability for electrocatalysis. The better performance was attributed to the high conductivity of bimetallic phosphides and N-doped porous carbon, the maximum utilization of active sites on 3D conductive substrate and the protection of bimetallic phosphides by N-doped carbon layers. As an integrated high-performance non-noble electrocatalyst for overall water splitting, the CoNiP@CN/NF requires only 1.59 V@30 mA cm〈sup〉-〈/sup〉 in alkaline solution, which is comparable to many other non-noble metal catalysts. This work highlights the construction highly efficient transition metal-carbon-based electrocatalyst derived from well-defined ZIF precursor, promoting the development of low-cost non-noble metal hybrids in energy chemistry.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307994-ga1.jpg" width="283" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Sotiris Lycourghiotis, Eleana Kordouli, Labrini Sygellou, Kyriakos Bourikas, Christos Kordulis〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉 〈p〉Nickel catalysts supported on palygorskite of varying Ni content were synthesized following the deposition–precipitation method. The catalysts were characterized using various techniques and evaluated in a semi-batch reactor for the transformation of 〈em〉waste cooking oils〈/em〉 (WCO) into 〈em〉green diesel〈/em〉 at 310 °C and hydrogen pressure 40 bar.〈/p〉 〈p〉The nickel nanoparticles supported on palygorskite were proved to be very active. The conversion of the WCO was about 100%. The green diesel content of the liquid product depends mainly on the nickel surface exposed per gram of catalyst, following a volcano like trend and maximized (81.9 wt %) over the sample with 30 wt % Ni. Taking into account the very high ratio of WCO volume to catalyst mass (100 mL/g) and that the evaluation of the catalysts was performed under solvent free conditions, these results demonstrate the successful use of mineral palygorskite for developing promising “natural catalysts” for green diesel production.〈/p〉 〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308057-ga1.jpg" width="377" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: Available online 10 August 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental〈/p〉 〈p〉Author(s): Han Zheng, Jianguo Bao, Ying Huang, Luojing Xiang, Faheem, Bangxing Ren, Jiangkun Du, Mallikarjuna N. Nadagouda, Dionysios D. Dionysiou〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉In this study, magnetic porous sulfurized Fe〈sub〉2〈/sub〉O〈sub〉3〈/sub〉 (PS-Fe〈sub〉2〈/sub〉O〈sub〉3〈/sub〉) composites were prepared through the co-precipitation method and were applied to activate peroxymonosulfate (PMS) for the degradation of emerging contaminants. Characterization results indicated that PS-Fe〈sub〉2〈/sub〉O〈sub〉3〈/sub〉 catalyst with uniform elemental distribution possessed a large number of micro- and meso- pores. When the molar ratio of FeSO〈sub〉4〈/sub〉:S〈sub〉2〈/sub〉O〈sub〉3〈/sub〉〈sup〉2−〈/sup〉 was 2:1 during the synthesis process, the PS-Fe〈sub〉2〈/sub〉O〈sub〉3〈/sub〉-2 exhibited the best performance on PMS activation for atrazine (ATZ) removal. The catalytic activity of PS-Fe〈sub〉2〈/sub〉O〈sub〉3〈/sub〉 catalysts was enhanced with increased sulfurization extent. The effects of catalyst dosage, PMS concentration, pH, and water impurities (i.e. Cl〈sup〉−〈/sup〉, HCO〈sub〉3〈/sub〉〈sup〉−〈/sup〉, NO〈sub〉3〈/sub〉〈sup〉−〈/sup〉 and humic acid) on ATZ degradation were investigated. Both sulfate radicals and hydroxyl radicals were detected in the PS-Fe〈sub〉2〈/sub〉O〈sub〉3〈/sub〉-2/PMS system, and sulfate radicals played the predominant role for the degradation of ATZ. The cycle of 〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/tbnd"〉Fe(II)/〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/tbnd"〉Fe(III) and surface-bonded hydroxyl group both contributed to the PMS activation, and the reduction of Fe〈sup〉3+〈/sup〉 to Fe〈sup〉2+〈/sup〉 was significantly accelerated by the low-valent sulfur species (such as 〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/tbnd"〉sulfite) on the catalyst surface. The transformation products of ATZ in PS-Fe〈sub〉2〈/sub〉O〈sub〉3〈/sub〉-2/PMS system were monitored on LC/MS, which were probably generated through lateral chain oxidation and dechlorination-hydroxylation. Overall, PS-Fe〈sub〉2〈/sub〉O〈sub〉3〈/sub〉 has potential to be a feasible catalyst for the removal of organic pollutants from water.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308021-ga1.jpg" width="294" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Sung Min Lee, Hyunju Lee, Junhyeong Kim, Sang Hyun Ahn, Suk Tai Chang〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Electrochemical reduction for conversion of CO〈sub〉2〈/sub〉 to value-added chemicals is considered a promising method to relieve global warming. To develop a highly active and selective electrocatalyst for efficient CO〈sub〉2〈/sub〉 conversion, it is essential to overcome the large overpotential and to suppress the competitive hydrogen evolution reaction (HER). Herein, we report a simple and controllable fabrication method for Ag electrocatalytic films using all-water-based solution processes via a seed-meditated metal growth technique. Varying the deposition conditions allows the N/S doping ratio in Ag films with high coverage and good adhesion to be easily controlled in the range of 1.14–8.23. The doping ratio has a significant effect on the CO Faradaic efficiency (FE), as the S content modulates the binding energy of reaction intermediates, whereas the N content is effective for suppressing the HER on the Ag film surface.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S092633731930791X-ga1.jpg" width="498" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Weifang Zhang, Feng Liu, Yonggang Sun, Jing Zhang, Zhengping Hao〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Multiple heavy-metal ions (e.g. Cr(VI) and As(III)) normally co-exist in acid wastewater, making the wastewater treatment complicated. Herein, the synergistic redox conversion and removal of Cr(VI)/As(III) were effectively achieved by applying iron(III) cross-linking alginate hydrogel beads (Fe-SA) as photocatalyst under simulated sunlight. Results show that not only 100% of the Cr(VI)/As(III) redox conversion was obtained in 150 min at pH 3.0, but also the removal efficiency of the transformed products (Cr(III) and As(V)) was greatly enhanced to above 80% in a wide pH range of 3–7. The 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉CO〈sub〉2〈/sub〉〈sup〉−〈/sup〉 radicals, produced by the ligand to metal charge transfer (LMCT) excitations on Fe-SA, together with the phtocatalysis-generated Fe(II), was responsible for the Cr(VI) reduction. Meanwhile, 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉OH originating from 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉CO〈sub〉2〈/sub〉〈sup〉−〈/sup〉 mainly contributed to the As(III) oxidation, as confirmed by electron paramagnetic resonance and the by-product of CO〈sub〉2〈/sub〉. Moreover, Fe-SA composite presented excellent reusability and performance in treatment of Cr(VI)/As(III) in real waters.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307921-ga1.jpg" width="250" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Teng-Fei Chen, Shu-Yan Han, Zhi-Peng Wang, Hui Gao, Lin-Yang Wang, Yu-Heng Deng, Chong-Qing Wan, Yang Tian, Qiang Wang, Guo Wang, Gui-Sheng Li〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Isostructural 〈strong〉UiO-66-(SO〈sub〉3〈/sub〉H)〈sub〉2〈/sub〉〈/strong〉, 〈strong〉UiO-66-(SH)〈sub〉2〈/sub〉〈/strong〉 and 〈strong〉UiO-66-(SCH〈sub〉3〈/sub〉)〈sub〉2〈/sub〉〈/strong〉 were obtained through systemic synthesis by decorating the sulfur-containing groups (X = –SCH〈sub〉3〈/sub〉, –SH, –SO〈sub〉3〈/sub〉H) on the terephthalate linkers of UiO-66 (a metal-organic framework constructed with terephthalate linkers and Zr(IV)-oxo clusters). These UiO-66-X〈sub〉2〈/sub〉 derivates exhibited as n-type semiconductors, wherein the electronic properties and molecule dimensions of the function groups –X played key roles in determining their band gap (E〈sub〉g〈/sub〉) and photoactive properties. The –SCH〈sub〉3〈/sub〉 is shown as the most efficient functional group and is responsible for that dramatically narrowed E〈sub〉g〈/sub〉 of the 〈strong〉UiO-66-(SCH〈sub〉3〈/sub〉)〈sub〉2〈/sub〉〈/strong〉 and photocatalytic property. In sharp contrast to that state-of-the-art UiO-66-NH〈sub〉2〈/sub〉 (constructed with 2-aminoterephthalate linkers) having no visible-light induced photocatalytic activity to split water into H〈sub〉2〈/sub〉 even with Pt as co-catalyst, Pt/〈strong〉UiO-66-(SCH〈sub〉3〈/sub〉)〈sub〉2〈/sub〉〈/strong〉 showed a high efficient H〈sub〉2〈/sub〉 generation (3871 μmol/g) from water with sacrificial ascorbic acid (0.2 M) under λ 〉 400 nm irradiation. The structure-property relationship of UiO-66-X〈sub〉2〈/sub〉 was studied through experimental and theoretical methods.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉Isostructural 〈strong〉UiO-66-(SO〈sub〉3〈/sub〉H)〈sub〉2〈/sub〉〈/strong〉, 〈strong〉UiO-66-(SH)〈sub〉2〈/sub〉〈/strong〉 and 〈strong〉UiO-66-(SCH〈sub〉3〈/sub〉)〈sub〉2〈/sub〉〈/strong〉 were obtained through systemic synthesis by decorating the functional groups (X = –SCH〈sub〉3〈/sub〉, –SH, –SO〈sub〉3〈/sub〉H) on the terephthalate linkers of UiO-66. Effect of electronic nature, molecular dimension and geometry of the function groups that display on the photocatalytic property of the MOF’s material is studied.〈/p〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307933-ga1.jpg" width="255" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: Available online 7 August 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental〈/p〉 〈p〉Author(s): Yiseul Park, Chuhyung Kim, Minsun Kim, Soonhyun Kim, Wonyong Choi〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Fe〈sub〉2〈/sub〉O〈sub〉3〈/sub〉 nanorods loaded on carbon nanofiber sheet (Fe〈sub〉2〈/sub〉O〈sub〉3〈/sub〉/CNF) was found to be active in degrading aromatic pollutants spontaneously under the dark and ambient condition without using any chemical reagent or external energy to assist the degradation reaction. The removal of aromatic pollutants was not caused by adsorption but by oxidative degradation since the generation of degradation intermediates and products was observed. The Fe〈sub〉2〈/sub〉O〈sub〉3〈/sub〉/CNF exhibited selective degradation activities for aromatic-compounds. Degradation was induced by Fe〈sub〉2〈/sub〉O〈sub〉3〈/sub〉/CNF only, whereas neither iron oxide nor bare CNF alone exhibited any degradation activity. The degradation on the Fe〈sub〉2〈/sub〉O〈sub〉3〈/sub〉/CNF was enabled only in the presence of dissolved O〈sub〉2〈/sub〉 of which reduction led to the generation of reactive oxygen species (ROS). It is proposed that electrons spontaneously transfer from aromatic-compound to O〈sub〉2〈/sub〉 via Fe〈sub〉2〈/sub〉O〈sub〉3〈/sub〉/CNF with initiating the oxidative degradation and the concurrent ROS generation. The direct electron transfer from organic compound to Fe〈sub〉2〈/sub〉O〈sub〉3〈/sub〉/CNF, which lead to oxidative degradation.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308124-ga1.jpg" width="301" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈p〉〈strong〉Park et al., “Ambient-Temperature Catalytic Degradation of Aromatic Compounds on Iron Oxide Nanorods Supported on Carbon Nanofiber Sheets”〈/strong〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Meixuan Cai, Ruobai Li, Zhijie Xie, Jiaxing Huang, Yongqin Zeng, Qianxin Zhang, Haijin Liu, Wenying Lv, Guoguang Liu〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉The development of novel noble metal-free semiconductor catalysts with high photocatalytic efficiency is of great importance toward the degradation of organic compounds. In this work, a core-shell heterojunction MoS〈sub〉2〈/sub〉/Cd〈sub〉0.9〈/sub〉Zn〈sub〉0.1〈/sub〉S photocatalytic material was successfully synthesized via a simple one-step hydrothermal method. The introduction of MoS〈sub〉2〈/sub〉 led to a significant improvement in the photocatalytic degradation of diclofenac (DCF). It was confirmed that 0.1% loading content of MoS〈sub〉2〈/sub〉 achieved an optimal photocatalytic efficiency of 86% in the degradation of DCF under visible light irradiation, which was 1.8 times higher than that of Cd〈sub〉0.9〈/sub〉Zn〈sub〉0.1〈/sub〉S. The MoS〈sub〉2〈/sub〉/Cd〈sub〉0.9〈/sub〉Zn〈sub〉0.1〈/sub〉S heterostructured composites possessed improved photocatalytic properties, which implied that the combination of Cd〈sub〉0.9〈/sub〉Zn〈sub〉0.1〈/sub〉S and MoS〈sub〉2〈/sub〉 shortened the carrier transport pathway and facilitated the separation efficiency of electrons and holes. Reactive species (RS) scavenging experiments and electron spin resonance (ESR) demonstrated that superoxide radicals (O〈sub〉2〈/sub〉〈sup〉•−〈/sup〉) and electron holes (h〈sup〉+〈/sup〉) played predominant roles throughout the DCF degradation process. The primary intermediates were explored through HRAM LC/MS/MS, and a transformation pathway was tentatively proposed. This study promoted the application of an economical, highly efficient and visible light driven MoS〈sub〉2〈/sub〉 co-catalyst for the degradation of organic contaminants.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307799-ga1.jpg" width="280" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: Available online 16 August 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental〈/p〉 〈p〉Author(s): Jabbar Gardy, Ehsan Nourafkan, Amin Osatiashtiani, Adam F. Lee, Karen Wilson, Ali Hassanpour, Xiaojun Lai〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Catalytic transesterification of triglycerides and esterification of free fatty acids underpins sustainable biodiesel production, wherein efficient heterogeneous catalysts are sought to replace mineral acids. A robust, magnetic core-shell SO〈sub〉4〈/sub〉/Mg-Al-Fe〈sub〉3〈/sub〉O〈sub〉4〈/sub〉 catalyst was synthesised by stepwise co-precipitation, encapsulation, and surface functionalisation. The resulting magnetically-separable catalyst has a surface area of 123 m〈sup〉2〈/sup〉 g〈sup〉-1〈/sup〉, uniform 6.5 nm mesopores, and a high total acid site loading of 2.35 mmol g〈sup〉-1〈/sup〉. Optimum conditions for the (trans)esterification of waste cooking oil (WCO) over the sulfated solid acid catalyst were 95 °C, a methanol:WCO molar ratio of 9:1, and 300 min reaction to achieve 98.5 % FAME yield. Esterification of oleic acid to methyl oleate resulted in an 88 % yield after 150 min under the same reaction conditions. The magnetic solid acid catalyst exhibited good thermal and chemical stability and enabled facile catalyst separation post-reaction and the production of high quality biodiesel.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308409-ga1.jpg" width="301" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Kaihang Ye, Ya Li, Hao Yang, Mingyang Li, Yongchao Huang, Shanqing Zhang, Hongbing Ji〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Designing and constructing effective and stable photocatalysts is the major challenge in the development of photocatalysis. Herein, we demonstrate a conceptual strategy to effectively improve the charge separation in a ternary material system (CeO〈sub〉2〈/sub〉/C/SnS〈sub〉2〈/sub〉), by introducing ultrathin carbon layer between CeO〈sub〉2〈/sub〉 nanorods and SnS〈sub〉2〈/sub〉 particles as a conductive electron transport “highway”. Such ternary CeO〈sub〉2〈/sub〉/C/SnS〈sub〉2〈/sub〉 gives rise to a largely enhanced photocatalytic removal performance of phenol (100%, 60 min), comparing with CeO〈sub〉2〈/sub〉/SnS〈sub〉2〈/sub〉 (50%) and CeO〈sub〉2〈/sub〉 (20%). Experimental results reveal that carbon layer acts as a high work function, superior electron mobility accepts and enables a fast transportation, accelerating the photocatalytic degradation performance of phenol. Our design introduces material components to provide a dedicated charge-transport pathway, conquering the materials’ intrinsic properties, providing a new perspective for water purity.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S092633731930832X-ga1.jpg" width="407" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Xinlong Xu, Zhangxun Xia, Xiaoming Zhang, Ruili Sun, Xuejing Sun, Huanqiao Li, Chuchu Wu, Junhu Wang, Suli Wang, Gongquan Sun〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉The rational design of highly efficient, low-cost and methanol-tolerant catalysts toward the oxygen reduction reaction (ORR) is urgently desired for the commercialization of direct methanol fuel cells (DMFCs). Herein, a novel Fe-N-C catalyst (ZIF/MIL-10-900) is derived from a mixture of ZIF-8 and MIL-101(Fe) and atomically dispersed FeN〈sub〉4〈/sub〉 structures are confirmed by Mössbauer spectra and X-ray absorption spectroscopy. Study on the pyrolysis procedure reveals that Fe atoms in FeN〈sub〉4〈/sub〉 are from MIL-101(Fe), while ZIF-8 acts as structural support and nitrogen sources. The as-prepared catalyst demonstrates a comparable ORR activity with the commercial Pt/C possessing a half-wave potential (E〈sub〉1/2〈/sub〉) of 0.78 V in acids, in combination with excellent methanol tolerance and stability. One of the highest peak power density of 83 mW cm〈sup〉−2〈/sup〉 in DMFC (3 M CH〈sub〉3〈/sub〉OH) by adopting ZIF/MIL-10-900 as cathode catalyst is obtained, which is 2.8-fold higher than that of the commercial Pt/C in the same operating condition.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉Atomically dispersed Fe-N-C catalyst is fabricated by a rational designed dual-MOFs strategy for efficient and low-cost DMFC application.〈/p〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S092633731930788X-ga1.jpg" width="500" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Wei Zhou, Tao Jia, Dongqiao Zhang, Zhikun Zheng, Wei Hong, Xudong Chen〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Due to the longer conjugation length and higher rigidity of the indofluorene, poly(indenofluorene) (PIF) demonstrates better optical absorption capability and faster carriers mobility than the corresponding polyfluorene (PF). In this study, a donor-acceptor (D〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/sbnd"〉A) type PIF (PIFDTBT) is synthesized and coupled with g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 nanosheets to construct conjugated polymer dots/g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 nanosheets (Pdots/CNNS). Ascribed to the enhanced light absorption, suitable band positions, and outstanding carriers mobility resulted by the introduction of indenofluorene units, the HER of PIFDTBT Pdot/CNNS is 7.6 times higher than that of F8DTBT Pdots/CNNS at the 1〈sup〉st〈/sup〉 run without metallic co-catalyst. Interestingly, the HER enhancement of PIFDTBT Pdots/CNNS compared to F8DTBT Pdots/CNNS correspondingly increases from 7.6 times at the 1〈sup〉st〈/sup〉 run to 14.3 times at the 4〈sup〉th〈/sup〉 run. This research can provide an insight for constructing organic nanocomposites with improved optical response and enhanced stability by electron donor units adjustment of the conjugated polymer.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308136-ga1.jpg" width="300" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Chengzhang Zhu, Yuting Wang, Zhifeng Jiang, Fanchao Xu, Qiming Xian, Cheng Sun, Qing Tong, Weixin Zou, Xiaoguang Duan, Shaobin Wang〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Developing low-cost and high-performance catalysts is significant to solar-to-fuel conversion. Here, the synthesis of zero-dimensional (0D) CeO〈sub〉2〈/sub〉 nanocrystal-decorated two-dimensional (2D) layered hybrids of MoS〈sub〉2〈/sub〉/g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 was reported for the first time. In the absence of noble-metal cocatalyst, the optimized ternary CeO〈sub〉2〈/sub〉@MoS〈sub〉2〈/sub〉/g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 still manifested high photocatalytic activity toward H〈sub〉2〈/sub〉 generation, with a rate of 65.4 μmol/h, which is approximately 8.3 and 17.5-fold greater than g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 and CeO〈sub〉2〈/sub〉, respectively. The corresponding apparent external quantum efficiency reached 10.35% at a wavelength of 420 nm. The superior photocatalytic behavior of CeO〈sub〉2〈/sub〉@MoS〈sub〉2〈/sub〉/g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 heterojunction could be ascribed to the positive synergetic effects of well-matched energy-level positions and effective charge separation arose from the multi-step electron transfer processes between Ce〈sup〉4+〈/sup〉/Ce〈sup〉3+〈/sup〉 reversibility pairs and heterostructures. Furthermore, the adsorption ability of reactant H〈sub〉2〈/sub〉O molecules on CeO〈sub〉2〈/sub〉@MoS〈sub〉2〈/sub〉/g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 was investigated. Due to the interfacial electronic interaction and Ce〈sup〉3+〈/sup〉 species, CeO〈sub〉2〈/sub〉@MoS〈sub〉2〈/sub〉/g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 presented more reaction active sites with enhanced adsorption capacity and decreased energy barrier for reactant H〈sub〉2〈/sub〉O molecules adsorption, which collaboratively promoted photocatalytic water splitting. This study provides new insights into the rational design of inexpensive ternary photocatalyst with multilevel electron transfer for efficiently converting solar energy into hydrogen without noble metals.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308197-ga1.jpg" width="494" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Xiaoqing Gao, Shanhui Zhu, Mei Dong, Jianguo Wang, Weibin Fan〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Highly efficient synthesis of valuable γ-valerolactone (GVL) by levulinic acid (LA) hydrogenation is still a challenge for Ru-based catalysts under mild condition. In this work, we have reported that ultrathin TiO〈sub〉2〈/sub〉 nanosheets supported Ru nanoparticles showed extraordinarily high catalytic activity, GVL yield (99.1%) and reusability owing to the formation of Ru〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/sbnd"〉O〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/sbnd"〉Ti interfacial structure. The turnover frequency (TOF) reached as high as 19,045 h〈sup〉−1〈/sup〉 at 100 °C, much higher than those of Ru/SiO〈sub〉2〈/sub〉, Ru/GO, Ru/MoS〈sub〉2〈/sub〉, and commercial Ru/C. DFT calculation elucidates that the dominant reaction pathway of LA hydrogenation to GVL is preferentially hydrogenated to CH〈sub〉3〈/sub〉CHOCH〈sub〉2〈/sub〉CH〈sub〉2〈/sub〉COOH*, followed by cyclization to CH〈sub〉3〈/sub〉(OH)C〈sub〉4〈/sub〉OH〈sub〉4〈/sub〉OH* (GVL − OH) and final dehydroxylation, irrespective of surface structure. Compared to Ru (0 0 2) facet, Ru/TiO〈sub〉2〈/sub〉 interfacial structure changes the rate-determining step from initial hydrogenation to cyclization, which greatly declines the activation barrier from 0.81 eV to 0.48 eV.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308239-ga1.jpg" width="339" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Jiangli Wang, Xueqiu You, Chi Xiao, Xiaoping Zhang, Shuhui Cai, Wenlong Jiang, Shengshi Guo, Shuohui Cao, Zhong Chen〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉In this work, highly active MoS〈sub〉2〈/sub〉 nanoflowers/graphene nanosheets (GNS) composites are successfully prepared through a simple hydrothermal method and are employed as Pt supports to prepare Pt/MoS〈sub〉2〈/sub〉/GNS for ethanol oxidation. The catalyst is characterized both physically and electrochemically to investigate the effect of MoS〈sub〉2〈/sub〉/GNS on Pt. Moreover, in situ electrochemistry - nuclear magnetic resonance, with the strength in structural characterization, quantitative analysis, and real-time measurement, is carried out to monitor molecular changes of reaction products and elucidate reaction mechanism of ethanol oxidation reaction, providing sampling resolution of 4s. Significantly, a small size of 5.4 nm Pt decorated Pt/MoS〈sub〉2〈/sub〉/GNS is achieved. Pt/MoS〈sub〉2〈/sub〉/GNS exhibits 2.1-fold increase in electrochemical active surface area, 2.2-fold increase in catalytic activity, and 2.0-fold increase in durability compared to commercial Pt/C during ethanol oxidation, which can be attributed to the synergistic effect of the interconnected nanoflower-on-nanosheet structure of MoS〈sub〉2〈/sub〉/GNS, the better dispersion of Pt nanoparticles, and the interactions between substrate materials and Pt. The results suggest that Pt/MoS〈sub〉2〈/sub〉/GNS could be an alternative electrocatalyst for efficient ethanol oxidation reaction. This work provides a promising strategy in the synthesis and monitoring of composite materials as high-performance ethanol oxidation catalysts.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308069-ga1.jpg" width="331" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 5 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 258〈/p〉 〈p〉Author(s): Hao-Wei Lin, Duraisamy Senthil Raja, Xui-Fang Chuah, Cheng-Ting Hsieh, Yu-An Chen, Shih-Yuan Lu〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Bi-metallic metal organic framework (MOF) compounds, FeNi(BDC)(DMF,F), adequately modulated through alloying of Ni and Fe, were demonstrated outstanding electrocatalysts for overall water splitting. It was composed of two well mixed bi-metallic MOF phases, Fe-rich FeNi(BDC)(DMF,F) and Ni-rich FeNi(BDC)(F), each containing two molecularly well mixed metallic clusters, to give pronounced hierarchical synergistic effects toward overall water splitting, delivering current densities of 10 and 400 mA cm〈sup〉−2〈/sup〉 at ultralow cell voltages of 1.58 and 1.90 V, respectively, outperforming the pairing of benchmark electrodes, Pt-C//IrO〈sub〉2〈/sub〉. The stability of the electrodes was also excellent, experiencing only minor chronoamperometric decay after a continuous operation at 400 mA cm〈sup〉−2〈/sup〉 for 30 h. The success may be attributed to the MOF/substrate synergistic effects between the FeNi(BDC)(DMF,F) and the conductive macroporous nickel foam, the inter-molecular synergistic effects between the two constituent MOF phases, and the intra-molecular synergistic effects between the FeO〈sub〉6〈/sub〉 and NiO〈sub〉6〈/sub〉 clusters of the Fe-rich FeNi(BDC)(DMF,F).〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉Hierarchical synergistic effects of bi-metallic MOFs boost electrolytic water splitting performances.〈/p〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307696-ga1.jpg" width="200" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Shangcong Sun, Yibin Feng, Lun Pan, Xiangwen Zhang, Ji-Jun Zou〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Overall water splitting is vital in solar-hydrogen conversion. In addition to charge separation, the regulation of surface kinetics and suppression of backward reaction become particularly crucial. Herein, an all-in-one Pt·Ni(OH)〈sub〉2〈/sub〉/C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 photocatalyst is proposed by integrating Pt@Ni(OH)〈sub〉2〈/sub〉 composited nanowires and isolated Pt clusters on C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉. In this heterostructure, Pt@Ni(OH)〈sub〉2〈/sub〉 with rich coordinatively unsaturated sites effectively boost O〈sub〉2〈/sub〉 evolution, and Pt-O-Ni interaction retards O〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/sbnd"〉O bond cleavage thus inhibiting backward H〈sub〉2〈/sub〉O regeneration. Meanwhile isolated Pt forms an Schottky junction with C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 for electron transfer and proton reduction. Consequently, Pt·Ni(OH)〈sub〉2〈/sub〉/C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 achieves stoichiometric water splitting with H〈sub〉2〈/sub〉/O〈sub〉2〈/sub〉 evolution of 1330/632 μmol g〈sup〉−1〈/sup〉 h〈sup〉−1〈/sup〉, and an outperforming AQE of 4.2% at 420 nm. Our work manifests that accelerating charge migration, inhibiting backward reaction and tuning surface kinetics are dominant in water splitting, for which a rational design of robust redox pathways is necessary.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S092633731930774X-ga1.jpg" width="239" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Huimin Hao, Xia Li, Xianjun Lang〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Anthraquinones (AQs) are well-known for their excellent redox properties. In this contribution, AQs were designated as a photoredox active ligand of TiO〈sub〉2〈/sub〉 for selective aerobic oxidation of organic sulfides. Importantly, we have found that there is an interrelation between the structural nuances of AQs and the conversions of sulfides. Particularly, with 2 mol% of (2,2,6,6-tetramethylpiperidin-1-yl)oxyl (TEMPO) as the redox mediator, organic sulfides can be selectively oxidized into sulfoxides with aerial O〈sub〉2〈/sub〉 by 1,2-dihydroxyanthraquinone (1,2-DHA) acting a photoredox active ligand of anatase TiO〈sub〉2〈/sub〉 under visible light illumination. This work highlights the potential of designing photoredox active ligand of metal oxide semiconductors to construct visible-light-induced selective aerobic oxidation reactions.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307842-ga1.jpg" width="267" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 5 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 258〈/p〉 〈p〉Author(s): Yao Chen, Xiaoming Deng, Jieya Wen, Jian Zhu, Zhenfeng Bian〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Composite of porphyrins and piezoelectric materials is a promising method to overcome the limitation of photocatalytic response of composite catalysts, inhibit photogenerated electron-hole recombination and enhance photocatalytic degradation performance. Here, the Fe-S electronic channel is formed by the combination of MoS〈sub〉2〈/sub〉 and iron porphyrin, which enhances the electron transfer performance of iron porphyrin to MoS〈sub〉2〈/sub〉 semiconductor. At the same time, two-dimensional MoS〈sub〉2〈/sub〉 surface with piezoelectric properties forms an electric field, which further enhances charge separation and piezoelectric catalytic performance. The photoexcitation of porphyrin and the piezoelectric excitation of molybdenum sulfide cooperate with each other under the simultaneous action of light and ultrasound. Oxygen radicals and hydroxyl radicals are enhanced, and the catalytic degradation performance is further enhanced. By strengthening the interaction between porphyrins and piezoelectric materials, especially bonding, a good and stable catalyst for pollutant degradation and purification was prepared.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307702-ga1.jpg" width="334" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Yang Yu, Shijie You, Jiannan Du, Zipeng Xing, Ying Dai, Hun Chen, Zhuang Cai, Nanqi Ren, Jinlong Zou〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Fabrication of efficient catalyst/co-catalyst for enhancing methanol oxidation and oxygen reduction reactions (MOR/ORR) is the key to make direct methanol fuel cells more economical. Here, hierarchical CoO@nitrogen-doped porous carbon@SnO〈sub〉2〈/sub〉 (CoO@NPC@SnO〈sub〉2〈/sub〉) polyhedrons are prepared as active catalysts for ORR and Pt supports/co-catalysts for MOR using zeolitic imidazolate frameworks-67 (ZIF-67). For ORR, CoO@NPC@SnO〈sub〉2〈/sub〉-1 (Co@NPC-to-SnCl〈sub〉2〈/sub〉·2H〈sub〉2〈/sub〉O mass ratio of 1: 1) exhibits a more positive peak potential (0.82 V vs. RHE) than that of commercial Pt/C (10 wt.%). Outer SnO〈sub〉2〈/sub〉 shells can prevent CoO cores (active tetrahedral Co〈sup〉2+〈/sup〉) from corrosion during ORR. For MOR, Pt-CoO@NPC@SnO〈sub〉2〈/sub〉-1 (5 wt.%) shows a much higher mass activity (1518 mA mg〈sub〉Pt〈/sub〉〈sup〉−1〈/sup〉) than that of Pt/C (496.8 mA mg〈sub〉Pt〈/sub〉〈sup〉−1〈/sup〉). High CO tolerance of Pt-CoO@NPC@SnO〈sub〉2〈/sub〉-1 is attributed to strong metal (Pt)-metal oxides (SnO〈sub〉2〈/sub〉) interactions, which facilitate adsorption of OH〈sup〉−〈/sup〉 on SnO〈sub〉2〈/sub〉 to remove CO〈sub〉ads〈/sub〉. Therefore, this study provides a strategy to enhance ORR/MOR performance by using hierarchically-structured catalysts/co-catalysts from ZIF templates.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307891-ga1.jpg" width="299" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Lei Tian, Shixiong Min, Fang Wang〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Developing highly active and stable cocatalysts at lower costs is greatly crucial for high-performance semiconductor-based photocatalytic H〈sub〉2〈/sub〉 evolution from water splitting. Herein, we report that noble-metal-free metallic vanadium carbide (VC) can function as a superior cocatalyst when integrated with CdS for efficient photocatalytic H〈sub〉2〈/sub〉 evolution under visible light irradiation (≥420 nm). The most efficient CdS/VC (15 wt.%) composite photocatalyst exhibits an exceptionally high photocatalytic H〈sub〉2〈/sub〉 evolution rate of 14.2 mmol h〈sup〉−1 〈/sup〉g〈sup〉−1〈/sup〉, up to 12 times higher than that of pristine CdS. The apparent quantum efficiency (AQE) of H〈sub〉2〈/sub〉 evolution reaches up to 8.7% at 420 nm. Moreover, the CdS/VC (15 wt.%) shows good stability for H〈sub〉2〈/sub〉 evolution after eight consecutive cycles of continuous light irradiation of 40 h. Most notably, the H〈sub〉2〈/sub〉 evolution activity of CdS/VC is even higher than or comparable to that of platinized CdS (CdS/Pt) prepared by photoreduction or chemical reduction at the same cocatalyst loading (1 wt.%). Furthermore, VC can also serve as an efficient H〈sub〉2〈/sub〉 evolution cocatalyst on various semiconductor photocatalysts (TiO〈sub〉2〈/sub〉 and g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉) and in a dye-sensitized photocatalytic system. Electrochemical and photoelectrochemical measurements reveal that VC can function as an efficient electrocatalyst not only to reduce the overpotential of H〈sup〉+〈/sup〉/H〈sub〉2〈/sub〉O reduction to H〈sub〉2〈/sub〉 but also to effectively capture the photogenerated electrons of CdS for enhancing the separation efficiency of photogenerated carriers thanks to its outstanding metallic conduction, thus substantially improving the photocatalytic H〈sub〉2〈/sub〉 evolution activity of CdS/VC photocatalyst. This work demonstrates that noble-metal-free VC is a promising alternative to Pt as an efficient H〈sub〉2〈/sub〉 evolution catalyst for electrocatalytic and photocatalytic energy conversion.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉Metallic vanadium carbide (VC) as a noble-metal-free cocatalyst demonstrates high activity and stability in catalyzing photocatalytic H〈sub〉2〈/sub〉 evolution when integrated with CdS nanoparticles under visible light irradiation, achieving up to 12 times higher activity than pristine CdS and an apparent quantum efficiency (AQE) of 8.7% at 420 nm.〈/p〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307751-ga1.jpg" width="293" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Shujun Qiu, Yongli Shen, Guijuan Wei, Shuang Yao, Wei Xi, Miao Shu, Rui Si, Min Zhang, Junfa Zhu, Changhua An〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Maximizing the usage of cocatalyst to provide fruitful proton reduction sites and suppress charge carrier recombination is an effective stratagy to dramatically improve the photocatalytic performance. Herein, anchoring single atoms (SAs) of Pt onto the ultrathin porous CdS@carbon dots (CDs) nanosheets has been achieved through 〈em〉in-situ〈/em〉 reduction of Pt precursor. X-ray absorption fine structure spectra identify that the single Pt atoms are bonded as Pt-S with a coordination number 4, due to the scattering between platinum center and the sulfur atoms. The Pt single atoms exhibit strong capacity to trap photo-generated electrons, rendering CdS@CDs/Pt-SAs as a class of efficient solar-driven photocatalyst. It shows an outstanding activity towards H〈sub〉2〈/sub〉 generation at rate of 45.5 mmol h〈sup〉−1〈/sup〉 g〈sup〉−1〈/sup〉, which is 133 times of that for bare CdS@CDs. The novel method can be extended to the preparation of various functional nanocatalysts owing to its versatility and facileness.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307829-ga1.jpg" width="222" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Yingguang Zhang, Muyan Wu, Y.H. Kwok, Yifei Wang, Wei Zhao, Xiaolong Zhao, Haibao Huang, Dennis Y.C. Leung〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉A series of TiO〈sub〉2〈/sub〉/MnO〈sub〉2〈/sub〉 heterojunction catalysts were fabricated through an in-situ hydrothermal method, and for the first time, catalysts with this heterojunction structure were used for VUV-PCO toluene degradation. After the MnO〈sub〉2〈/sub〉 coating, the TiO〈sub〉2〈/sub〉/MnO〈sub〉2〈/sub〉 catalysts performed excellently for both VOCs degradation and residual ozone decomposition with removal efficiency reaching 96.0% and 99.9%, respectively. The enhanced photocatalytic activity towards toluene degradation could be attributed to the heterojunction structure of TiO〈sub〉2〈/sub〉/MnO〈sub〉2〈/sub〉, which provides excellent contact between MnO〈sub〉2〈/sub〉 and TiO〈sub〉2〈/sub〉, and suppresses the recombination of photogenerated electron-hole pairs. Moreover, benefiting from the MnO〈sub〉2〈/sub〉, the ozone generated in the system could be efficiently utilized and eliminated during the VUV-PCO process. The photocatalytic mechanism of TiO〈sub〉2〈/sub〉/MnO〈sub〉2〈/sub〉 for the toluene degradation and ozone decomposition was proposed.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉TiO〈sub〉2〈/sub〉/MnO〈sub〉2〈/sub〉 heterojunction catalysts are fabricated by in situ method, which exhibit excellent performance in degrading toluene through VUV-PCO process as well as O〈sub〉3〈/sub〉 elimination.〈/p〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307805-ga1.jpg" width="306" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: Available online 2 August 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental〈/p〉 〈p〉Author(s): Sara Madadi, Luc Charbonneau, Jean-Yves Bergeron, Serge Kaliaguine〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Cobalt substituted mesoporous SBA-16 catalysts, made by post grafting technique using directly cobalt acetylacetonate as the precursor was prepared. High loading of cobalt finely dispersed on SBA-16 silica was obtained. The Co/SBA-16 catalysts exhibited high conversion and selectivity in epoxidation of limonene towards limonene epoxides with molecular oxygen as the most desirable oxidant and isobutyraldehyde as co-reagent under very mild conditions in the presence of green solvent ethylacetate. A variety of characterization techniques such as nitrogen physisorption, XRD, DR-UV-vis, XPS, TEM indicates that the proposed impregnation procedure is a highly tunable and reproducible strategy to disperse transition metals in mesoporous silica materials. The unique pore structure of Co/SBA-16 catalyst could be beneficial for the epoxidation of bulky alkene molecules. The reaction conditions were systematically investigated using a statistical experimental design. Repeated catalytic tests showed no remarkable difference in the activity of fresh and recycled catalysts over three process cycles.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307957-ga1.jpg" width="301" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Yan Lin, Yuan Pan, Shoujie Liu, Kaian Sun, Yuansheng Cheng, Ming Liu, Zhaojie Wang, Xiyou Li, Jun Zhang〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Tuning structure, morphology and electronic state of electrocatalysts is essential to achieve highly efficient water splitting. Herein, we report synthesis of snap bean-like multi-dimensional core/shell Ni/NiCoP nano-heterojunctions (NHs) by adopting a solid phase transformation strategy. In the special structure, Ni nanoparticles are enclosed and strung by single phased NiCoP, forming strings of Ni/NiCoP core/shell heterojunctions, which showed improved stability and activity for both hydrogen evolution (HER) and oxygen evolution reactions (OER). X-ray photoelectron spectroscopy and synchrotron-radiation-based X-ray absorption spectroscopy reveal that interactions at the interface of Ni/NiCoP greatly changed electronic structures, which is a key intrinsic factor to underpin the enhanced electrocatalytic performance. Density functional theory calculations demonstrate Ni/NiCoP interface provide more optimal binding strength for H adatom and H〈sub〉2〈/sub〉O molecule for HER, strong capture of hydroxyl, high valence Ni/Co species for OER. All these peculiarities facilitate the electrocatalytic process: only 1.57 V was needed to reach the current density of 10 mA·cm〈sup〉−2〈/sup〉 for the overall water splitting using Ni/NiCoP NHs as both electrodes. This work demonstrates a facile strategy for synthesis of sophisticated catalytic interface at nano level and endows nano-heterojunction catalysts with enhanced performance for catalytic applications.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉Highlights〈/p〉 〈p〉〈/p〉 〈dl〉 〈dt〉•〈/dt〉 〈dd〉〈p〉A novel multi-dimensional Ni/NiCoP core/shell NHs was constructed.〈/p〉〈/dd〉 〈dt〉•〈/dt〉 〈dd〉〈p〉The Ni/NiCoP NHs exhibits enhanced bifunctional HER and OER performances.〈/p〉〈/dd〉 〈dt〉•〈/dt〉 〈dd〉〈p〉The interactions at the interface of Ni/NiCoP changed the electronic structures.〈/p〉〈/dd〉 〈dt〉•〈/dt〉 〈dd〉〈p〉The Ni/NiCoP NHs reveal more optimal binding strength for H adatom and H〈sub〉2〈/sub〉O molecule.〈/p〉〈/dd〉 〈dt〉•〈/dt〉 〈dd〉〈p〉Only 1.57 V was needed for water splitting using Ni/NiCoP NHs at 10 mA·cm〈sup〉−2〈/sup〉.〈/p〉〈/dd〉 〈/dl〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307854-ga1.jpg" width="336" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Chengwu Zhang, Tianyi Li, Jingyi Zhang, Song Yan, Chuanyu Qin〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉It has been recognized that a ferrous–polyphosphate complex can activate oxygen to produce reactive oxygen species (ROS) capable of degrading organic compounds. 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉OH has been confirmed as the predominant ROS. However, the role of O〈sub〉2〈/sub〉〈sup〉•–〈/sup〉 during the degradation of these contaminants has not been clearly explained. In this study, we demonstrate that, in addition to producing H〈sub〉2〈/sub〉O〈sub〉2〈/sub〉 and 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉OH, O〈sub〉2〈/sub〉–〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉can directly participate in the degradation of 〈em〉p-〈/em〉nitrophenol (PNP). EPR analysis and probe tests showed that O〈sub〉2〈/sub〉〈sup〉•–〈/sup〉 was largely produced in the first 15 min of the reaction, during which PNP was rapidly degraded. Masking experiments indicated that O〈sub〉2〈/sub〉〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉–, rather than O〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉H, was the main ROS for the direct degradation of PNP. GC〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/sbnd"〉MS and LC-MS〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/sbnd"〉 confirmed that O〈sub〉2〈/sub〉〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉– reduced PNP to p-aminophenol. The PNP degradation pathway was proposed accordingly. Another two monocyclic aromatics with different functional groups were also investigated to further confirm the impact of O〈sub〉2〈/sub〉〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉– on contaminant degradation. It was found that the degree of O〈sub〉2〈/sub〉〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉– participation during direct degradation mainly depends on the molecular structures of the contaminants. In addition, STPP always maintains the ability of promoting Fe〈sup〉2+〈/sup〉 to activate O〈sub〉2〈/sub〉 after adding Fe〈sup〉2+〈/sup〉 four times in the system. The aforementioned results indicate that STPP can be reused in the reaction system.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307763-ga1.jpg" width="478" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Nan Zhang, Quan Quan, Ming-Yu Qi, Zi-Rong Tang, Yi-Jun Xu〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉The basic mantra of “structure-dictates-function” in chemistry has inspired tremendous interests in designing various architectures toward specific applications. In this work, hierarchically tailorable double-array structures composed of TiO〈sub〉2〈/sub〉 nanotube arrays (TNTAs) and axially grown ZnO nanorod arrays (ZNRAs) have been constructed through a two-step anodization method combined with a heteroepitaxial growth process regulated by electrodeposited reduced graphene oxide (RGO). The obtained TNTAs/RGO/ZNRAs film hybrids exhibit enhanced photocatalytic and photoelectrochemical performances along with favorable photostability as compared to the single component and binary counterparts. This is ascribed to the synergistic effect of the matchable band alignment of the components, the 1D-on-1D double-array architecture with vectorial pathways for charge carriers transport, and the electrically conductive RGO for bridging the directional electron flow to further promote the separation and transfer of charge carriers. This work is anticipated to provide instructive recipe for rational design and construction of composite films with optimized photo(electro)catalytic performances.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉Hierarchically tailorable double-array hybrids consisting of TiO〈sub〉2〈/sub〉 nanotube arrays (TNTAs) and axially grown ZnO nanorod arrays (ZNRAs) regulated by electrodeposited reduced graphene oxide (RGO) onto TNTAs have been constructed, which exhibit enhanced photocatalytic and photoelectrochemical performances along with favorable photostability as compared to the single component and binary counterparts.〈/p〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308331-ga1.jpg" width="250" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Fang Luo, Ruizhi Xu, Shuangxiu Ma, Quan Zhang, Hao Hu, Kongang Qu, Shenglin Xiao, Zehui Yang, Weiwei Cai〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Development of earth-abundant, efficient and stable electrocatalysts for water splitting is of crucial importance for environmentally friendly energy conversion and storage. Here, we report an oxygen deficient cobalt tungstate nanoparticles with diameter of 8 nm (CoWO〈sub〉4-x〈/sub〉@C) as efficient bifunctional electrocatalyst for hydrogen evolution reaction (HER) and oxygen reduction reaction (OER), which exhibits comparable HER activity to commercial Pt/C with overpotentials of 32.5 mV and 46.8 mV vs. RHE to deliver current density of 10 mA cm〈sup〉−2〈/sup〉 in acidic and alkaline mediums, respectively, ascribed to the rich oxygen vacancies facilitating the hydrogen adsorption and its relative recombination, respectively. Additionally, undetectable degradation is observed for CoWO〈sub〉4-x〈/sub〉@C after 10,000 potential cycles indicating high durability. Meanwhile, CoWO〈sub〉4-x〈/sub〉@C requires only 295 mV overpotential to deliver 10 mA cm〈sup〉−2〈/sup〉 in the OER test, which is better than the benchmarking IrO〈sub〉2〈/sub〉 (313 mV). 1.57 V comparably lower than Pt/C-IrO〈sub〉2〈/sub〉 (1.59 V) is required for achieving the water splitting current density of 10 mA cm〈sup〉−2〈/sup〉 without any degradation for 12 h.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308379-ga1.jpg" width="245" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Chengwu Yang, Zhe Xue, Jiaqian Qin, Montree Sawangphruk, Xinyu Zhang, Riping Liu〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Structural defect engineering toward g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 plane usually has great benefit on modulating electron structure and photocatalytic performance. Here, we report a porous g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 material with heterogeneous structural defects, oxygen atom replacing edge nitrogen and cyano group, obtained via a facile treatment method. The reconstructed material shows narrowing band gap, high light absorption and fast charge separation. Theoretical calculation discloses that the doped oxygen atom and the nearby atoms accept electrons as reduction site to produce hydrogen, while the undoped fraction and cyano group take the duty to oxidize water. The delocalization of reactive sites drives charge shuttle on the plane, limiting recombination of charge carriers. Consequently, the modified g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 shows excellent photocatalytic activity with apparent quantum efficiency of 8.41% under 420 nm wavelength, surpassing pure g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 and other reported materials with defect compilation. We think that this work provides a new avenue to understand the function of structural defect on prompt charge separation.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308410-ga1.jpg" width="209" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Yujia Yang, Lejin Xu, Wuyang Li, Weijie Fan, Shuang Song, Jun Yang〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Fe-based heterogeneous Fenton-like catalysts has shown tremendous potential for wastewater treatment, but the investigation of adsorption, reduction and oxidation mechanism remains challenging. In this study, nanoscale zero-valent iron encapsulated in three-dimensional graphene network (3D-GN@nZVI) was synthesized and characterized as a heterogeneous Fenton-like catalyst via the activation of dissolved oxygen (DO) for adsorption and degradation of sulfadiazine (SDZ). 3D-GN@nZVI had the synergistic effect of catalytic reactivity for sulfadiazine removal, which was evaluated in view of the effects of operational factors. The role of adsorption, reduction and oxidation was determined; in 3D-GN@nZVI/DO system, sulfadiazine was removed mainly by the attack of hydroxyl radicals (〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉OH). The possible degradation pathway of sulfadiazine was inferred by identifying reactive oxidizing species and degradation intermediates. According to the X-ray photoelectron spectroscopy (XPS) analysis, Fourier Transform infrared spectroscopy (FTIR) analysis and density functional theory (DFT) calculations, the distribution and transfer of electrons on the surface of 3D-GN@nZVI were illustrated, and the adsorption and oxidation mechanisms of sulfadiazine through DO-driven and micro-electrolysis-enhanced heterogeneous Fenton-like reaction were proposed. The comprehensive mechanism was elucidated to provide new insights to advance the DO-driven Fenton-like process and to inspire the development of nZVI and relevant composites.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308033-ga1.jpg" width="306" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Lulu Zhang, Hongwen Zhang, Cankun Jiang, Jie Yuan, Xueyan Huang, Ping Liu, Wenhui Feng〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉A novel ternary Z-scheme system of WO〈sub〉3〈/sub〉@MoS〈sub〉2〈/sub〉/CdS is successfully constructed using a three-step wet-chemical route, where MoS〈sub〉2〈/sub〉 locates between the rod-shaped WO〈sub〉3〈/sub〉 and CdS nanoparticles and simultaneously plays multiple roles of the charge transfer mode switcher, electron-hole mediator and cocatalyst. As a charge transfer mode switcher, MoS〈sub〉2〈/sub〉 can transform the conventional type-Ⅱ charge transfer mode to Z-scheme. In such a Z-scheme system, as an electron-hole mediator, MoS〈sub〉2〈/sub〉 is applied to quench the energy of the electrons from WO〈sub〉3〈/sub〉 and the holes from CdS in shorten length, and thus the more left electrons from CdS can transfer to MoS〈sub〉2〈/sub〉, which can be further applied to photocatalytic evolution H〈sub〉2〈/sub〉 owing to the cocatalyst role of MoS〈sub〉2〈/sub〉. Benefitting from the multifunctional roles of MoS〈sub〉2〈/sub〉, such a Z-scheme system of WO〈sub〉3〈/sub〉@MoS〈sub〉2〈/sub〉/CdS shows an enhanced photocatalytic performance.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308203-ga1.jpg" width="433" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Lijie Xu, Yang Sun, Lu Gan, Jiangang Han, Ping Wang, Lei Yu, Xiang Mei, Wei Li, Baoling Lyu, Chun Pei, Wei Chu〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Photoconversion of NO〈sub〉3〈/sub〉〈sup〉−〈/sup〉/NO〈sub〉2〈/sub〉〈sup〉−〈/sup〉 at wastewater relevant concentrations as an advanced oxidation approach to degrade dimethyl pthalate (DMP), a relatively photoinert endocrine disruptor, were examined. Three different wavelengths (350 nm, 300 nm, 254 nm) were involved. The influence of NO〈sub〉3〈/sub〉〈sup〉−〈/sup〉 or NO〈sub〉2〈/sub〉〈sup〉−〈/sup〉 was found to be wavelength-dependent. The 254 nm UV light could decompose DMP efficiently, but photolysis of DMP was slow at λ =300 nm and noneffective at λ =350 nm, which could be catalyzed by the presence of NO〈sub〉3〈/sub〉〈sup〉−〈/sup〉 or NO〈sub〉2〈/sub〉〈sup〉−〈/sup〉. Both 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉OH and O〈sub〉2〈/sub〉〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉〈sup〉−〈/sup〉 were detected, while 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉OH was identified as the primary contributor to DMP decomposition. NO〈sub〉2〈/sub〉〈sup〉−〈/sup〉 plays a dual role as both a source and sink of 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉OH, depending on the relative abundance between NO〈sub〉2〈/sub〉〈sup〉−〈/sup〉 and DMP. NO〈sub〉3〈/sub〉〈sup〉−〈/sup〉 was more efficient than NO〈sub〉2〈/sub〉〈sup〉−〈/sup〉 for treating low-level DMP. However, higher organic content could effectively inhibit the quenching role of NO〈sub〉2〈/sub〉〈sup〉−〈/sup〉, making NO〈sub〉2〈/sub〉〈sup〉−〈/sup〉 more efficient for catalyzing DMP decomposition. For irradiation at λ =350 nm, NO〈sub〉3〈/sub〉〈sup〉−〈/sup〉 was completely ineffective, while self regeneration of NO〈sub〉2〈/sub〉〈sup〉−〈/sup〉 enabled Δ[NO〈sub〉2〈/sub〉〈sup〉−〈/sup〉]:Δ[〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉OH] 〈〈1. For irradiation at λ =300 nm, cycling between NO〈sub〉2〈/sub〉〈sup〉−〈/sup〉 and NO〈sub〉3〈/sub〉〈sup〉−〈/sup〉 occurred, and the transformation from NO〈sub〉2〈/sub〉〈sup〉−〈/sup〉 to NO〈sub〉3〈/sub〉〈sup〉−〈/sup〉 proceeded much faster. Complete decomposition of DMP at concentrations higher than those of NO〈sub〉2〈/sub〉〈sup〉−〈/sup〉 or NO〈sub〉3〈/sub〉〈sup〉−〈/sup〉 was observed, and mineralization was also achieved. Based on the identification of the intermediates, 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉OH addition to the aromatic ring and hydrogen atom abstraction by 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉OH were the dominant pathways, while nitration products were detected at low levels.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307040-ga1.jpg" width="496" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Hong Xia, Zhen Zhang, Jia Liu, Yang Deng, Dongxu Zhang, Peiyao Du, Shouting Zhang, Xiaoquan Lu〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Cost-effective, highly efficient and conveniently recycled heterogeneous catalyst is urgently desirable for wastewater treatment. Wood-derived monolith offers new opportunity because of its toilless functionalization and flexible processing. Herein, ferrum manganese oxide nanosheets (Fe-Mn-O NSs) were successfully grown on the microchannels of carbonized wood to construct a novel 3D wood-derived block for efficient wastewater treatment. The wood carbon not only acts as a 3D substrate to support Fe-Mn-O NSs, but also contributes to unimpeded mass diffusion benefiting from the numerous open channels and hierarchical pores on channel walls. More importantly, except for the exposure of sufficient active sites, several important surface properties (i.e. surface defects, surface charge, low-valence metal concentration and charge transfer) were improved by doping alien-metal element, resulting in greatly improved Fenton activity and stability. Notably, due to flexible processing of wood carbon, this block catalyst can be extended to filter membrane for removing pollutants in flow wastewater.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308045-ga1.jpg" width="210" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Zizheng Ai, Yongliang Shao, Bin Chang, Lei Zhang, Jianxing Shen, Yongzhong Wu, Baibiao Huang, Xiaopeng Hao〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉As a metal-free polymeric semiconductor, graphitic carbon nitride (g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉) is a promising candidate for photocatalytic water splitting but suffers from the insufficient optical absorption and sluggish utilization of photocarriers. Herein, based on the energy band engineering theory, a new design philosophy of tunable p-n homojunction is proposed and realized in a novel P-doped g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 (PCN) material. Through regulating the tendency of transformation in p-n homojunction, a strong internal electric field is built and integrated with two secondary internal electric fields by further decorating with Ti〈sub〉3〈/sub〉C〈sub〉2〈/sub〉, leading to the formation of a triple-internal electric field system. Thus the spatial separation efficiency of photocarriers is improved and their lifetime is prolonged. The specific photocatalyst exhibits excellent overall water splitting performance in pure water with a notable quantum yield. This work presents a peculiar concept of adjustable p-n homojunction and holds great significance for the rational design of advanced photocatalyst in water splitting.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308240-ga1.jpg" width="349" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Feiyang Chen, Ligang Xia, Yan Zhang, Jing Bai, Jiachen Wang, Jinhua Li, Mohammadi Rahim, Qunjie Xu, Xinyuan Zhu, Baoxue Zhou〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Carbonate widely exist in wastewater and natural water. Here we proposed an efficient refractory organics degradation method for carbonate-containing wastewater via generating carbonate radical based on a photoelectrocatalytic TNA-MCF system. In the system, TiO〈sub〉2〈/sub〉 nanotube arrays (TNA) and modified carbon felt (MCF) were used as photoanode and cathode, respectively. HCO〈sub〉3〈/sub〉〈sup〉−〈/sup〉 was used as electrolyte. The results show that the system achieved 85.78% removal rate after 120 min in rhodamine B degradation, which is 30% higher than that using SO〈sub〉4〈/sub〉〈sup〉2−〈/sup〉 as electrolyte. The excellent performance is attributed to the strong oxidation of 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉CO〈sub〉3〈/sub〉〈sup〉−〈/sup〉 to organics, which originates from the reactions between HCO〈sub〉3〈/sub〉〈sup〉−〈/sup〉 and h〈sub〉vb〈/sub〉〈sup〉+〈/sup〉 on TNA photoanode. It was also generated from the activation of HCO〈sub〉3〈/sub〉〈sup〉−〈/sup〉 with H〈sub〉2〈/sub〉O〈sub〉2〈/sub〉 or O〈sub〉2〈/sub〉〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉〈sup〉−〈/sup〉 on MCF cathode. Moreover, the mechanism of 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉CO〈sub〉3〈/sub〉〈sup〉−〈/sup〉 formation and its efficient degradation of organics were investigated. These results demonstrate that this system has a potential application in refractory organics degradation.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308185-ga1.jpg" width="318" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: Available online 10 August 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental〈/p〉 〈p〉Author(s): Jinge Du, Shuanglong Ma, Haiping Liu, Haichao Fu, Li Li, Zhuoqian Li, Yi Li, Jianguo Zhou〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉In this work, a novel AgInS〈sub〉2〈/sub〉 nanosheets/TiO〈sub〉2〈/sub〉 nanobelts photocatalyst was prepared by a facile hydrothermal method. The AgInS〈sub〉2〈/sub〉/TiO〈sub〉2〈/sub〉 with the optimal ration showed excellent photocatalytic performance in simultaneous 〈em〉Escherichia coli〈/em〉 (〈em〉E. coli〈/em〉) disinfection and Cr(VI) reduction or 〈em〉E. coli〈/em〉 disinfection and bisphenol A (BPA) degradation. The superior photocatalytic effect were possibly attributed to formation of heterojunction between AgInS〈sub〉2〈/sub〉 nanosheets and TiO〈sub〉2〈/sub〉 nanobelts, which could increase the absorption of visible light, facilitate the separation of photo-induced carrier and held the redox of photo-generated e– and h〈sup〉+〈/sup〉. The production of reactive species during the disinfection process was also investigated by employing chemical scavengers, electron spin resonance, and spectroscopy technique, revealing the paramount role of h〈sup〉+〈/sup〉 and •O〈sub〉2〈/sub〉–. This study paves a new way to rationally design the novel TiO〈sub〉2〈/sub〉 nanobelts or AgInS〈sub〉2〈/sub〉 nanosheets based photocatalysts for combined pollution remediation in water environment.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308082-ga1.jpg" width="301" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Sunkyu Kim, Bradie S. Crandall, Michael J. Lance, Nicole Cordonnier, Jochen Lauterbach, Erdem Sasmaz〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Tri-reforming of methane (TRM) produces syngas by directly utilizing flue gas from a fossil fuel-fired power plant without requiring post-combustion CO〈sub〉2〈/sub〉 separation. In this work, different yolk sizes of a NiCe@SiO〈sub〉2〈/sub〉 multi–yolk–shell nanotube catalyst were prepared and their catalytic properties were evaluated at different oxidizer (CO〈sub〉2〈/sub〉 + H〈sub〉2〈/sub〉O + O〈sub〉2〈/sub〉) to methane (O/M) feed ratios for TRM. The NiCe@SiO〈sub〉2〈/sub〉 multi–yolk–shell nanotube catalyst can exhibit longer stability than the conventional NiCe/SiO〈sub〉2〈/sub〉〈sup〉Imp〈/sup〉 catalyst synthesized by impregnation method due to its controlled morphology and synergetic interactions of Ni–Ce and Ni–Si species. At a low O/M feed ratio of 1.0, NiCe@SiO〈sub〉2〈/sub〉 with smaller yolks (〈 20 nm) shows higher resistance to carbon deposition than NiCe@SiO〈sub〉2〈/sub〉 with larger yolks due to the facile oxidation of carbon. On the other hand, NiCe@SiO〈sub〉2〈/sub〉 with larger yolks (〉 30 nm) presents stable TRM activity at a high O/M feed ratio of 1.1, whereas NiCe@SiO〈sub〉2〈/sub〉 consisting of smaller yolks deactivates. Deactivation of NiCe@SiO〈sub〉2〈/sub〉 with smaller yolks can be explained by the re-oxidation of active Ni species, in which carbon formation and oxidation rates, and Ce〈sup〉3+〈/sup〉/Ce〈sup〉4+〈/sup〉 redox properties play a crucial role. Our results indicate that the NiCe@SiO〈sub〉2〈/sub〉 multi–yolk–shell nanotube structures can provide high TRM activity, yet their structure should be tuned for stable performance by considering the yolk sizes and interaction of Ni–Ce species.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307830-ga1.jpg" width="373" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Félix Urbain, Ruifeng Du, Pengyi Tang, Vladimir Smirnov, Teresa Andreu, Friedhelm Finger, Nuria Jimenez Divins, Jordi Llorca, Jordi Arbiol, Andreu Cabot, Joan Ramon Morante〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉We investigate cobalt ferrite nanoparticles (NPs) supported on large-scale electrodes as oxygen evolution reaction (OER) catalysts. Colloidal CoFe〈sub〉2〈/sub〉O〈sub〉4〈/sub〉 NPs were loaded on low-cost and high surface area nickel foam (NF) scaffolds. The coating process was optimized for large electrode areas, ensuring a proper distribution of the NPs on the NF that allowed overcoming the electrical conductivity limitations of oxide NPs. We were able to produce CoFe〈sub〉2〈/sub〉O〈sub〉4〈/sub〉-coated NFs having 10 cm〈sup〉2〈/sup〉 geometric surface areas with overpotentials below 300 mV for the OER at a current density of 50 mA/cm〈sup〉2〈/sup〉. Such impressively low overpotentials suggested using CoFe〈sub〉2〈/sub〉O〈sub〉4〈/sub〉 NP-based electrodes within a water electrolysis device. In this prototype device, stable operating currents up to 500 mA at remarkably low cell-voltages of 1.62 and 1.53 V, at ambient and 50 °C electrolyte temperatures, respectively, were reached during operation periods of up to 50 h. The high electrochemical energy efficiencies reached at 50 mA/cm〈sup〉2〈/sup〉, 75% and 81% respectively, rendered these devices particularly appealing to be combined with low-cost photovoltaic systems for bias-free hydrogen production. Therefore, CoFe〈sub〉2〈/sub〉O〈sub〉4〈/sub〉 NP-based electrolysers were coupled to low-cost thin-film silicon solar cells with 13% efficiency to complete a system that afforded solar-to-fuel efficiencies above 10%.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉a) Sketch of the experimental prototype reactor used to assess the overall electrolysis performance. b) Linear sweep measurements of the CoFe〈sub〉2〈/sub〉O〈sub〉4〈/sub〉@NF electrodes (10 cm〈sup〉2〈/sup〉 geometric area) combined with the Ti/Pt cathode (10 cm〈sup〉2〈/sup〉 geometric area) for a configuration containing Nafion and BPM membrane, respectively.〈/p〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S092633731930801X-ga1.jpg" width="422" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Subhajyoti Samanta, Rajkumar Yadav, Abhinav Kumar, Anil Kumar Sinha, Rajendra Srivastava〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Mimicking the artificial photosynthesis utilizing solar energy for the production of hydrocarbon fuel is a sustainable strategy to tackle the fossil fuel-based energy crisis. Herein, a surface-modified g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 was synthesized by the co-condensation of urea + thiourea and 2-methyl imidazole. Physicochemical characterizations reveal that O and C are co-doped, as evident by the XPS and solid-state NMR spectroscopy. The light absorption edge is red shifted, lifetimes of the charge carriers, and electron injection efficiencies are ameliorated appropriately. Photocatalysts are employed in the CO〈sub〉2〈/sub〉 reduction (from TEOA dissolved water + CO〈sub〉2〈/sub〉 gas mixture) and H〈sub〉2〈/sub〉O〈sub〉2〈/sub〉 production (from pure H〈sub〉2〈/sub〉O and O〈sub〉2〈/sub〉 in absence of any organic electron/proton donor) without involving any co-catalyst. CO〈sub〉2〈/sub〉-adsorption/TPD measurements support the higher CO〈sub〉2〈/sub〉 uptake and lower adsorption energy after the surface modification as confirmed from DFT calculation. Mott-Schottky and VBXPS confirm that C, O co-doping bring required thermodynamic potential that facilitates the CO〈sub〉2〈/sub〉/CH〈sub〉3〈/sub〉OH and O〈sub〉2〈/sub〉/H〈sub〉2〈/sub〉O〈sub〉2〈/sub〉 reactions.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308008-ga1.jpg" width="353" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Hao Yan, Shuang Yao, Bin Yin, Wei Liang, Xin Jin, Xiang Feng, Yibin Liu, Xiaobo Chen, Chaohe Yang〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Bimetallic PtRu catalyst was first reported for oxidation of glycerol to glyceric acid in base-free medium using O〈sub〉2〈/sub〉 as the oxidant. A combination of density functional theory (DFT) calculations and multi-characterizations (e.g., H〈sub〉2〈/sub〉-TPR, HAADF-STEM and XPS) revealed that the strong interaction between Pt and Ru could promote the dispersion of PtRu alloy nanoparticles and enhance the electronic coupling effect on the metal surface. Meanwhile, compared to the monometallic Pt catalyst, the introduction of Ru contributes to the direct dissociation of molecular oxygen and water to hydroxyl group, leading to the excellent catalytic activity. A volcanic-shaped relationship between Ru/Pt ratio, catalytic performance, structure-sensitivity and electronic coupling effect was systematically established. Furthermore, the role of structure-sensitivity and electronic coupling effect for the enhanced catalytic activity of PtRu catalysts with different Ru/Pt ratios are distinguished in detail. Finally, the Pt〈sub〉0.8〈/sub〉Ru〈sub〉0.8〈/sub〉/MCM-41 catalyst showed excellent catalytic activity (TOF: 823.9 h〈sup〉−1〈/sup〉), glyceric acid selectivity (80.1%) and stability (recycling for 5th) under the optimized conditions (80 °C, 1 MPa O〈sub〉2〈/sub〉 and 12 h). The insights and methodology reported here may pave the way to the rational design of bimetallic catalysts for efficient conversion of bio-derived substrates under mild conditions.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉Bimetallic PtRu/MCM-41 catalyst were prepared for facile oxidation of glycerol to glyceric acid by the co-impregnation method. PtRu nanoparticles were uniformly dispersed on the MCM-41, resulting in the more accessible alloy sites for the glycerol oxidation to glyceric acid.〈/p〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308173-ga1.jpg" width="500" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): J. Soto-Hernández, C.R. Santiago-Ramirez, E. Ramirez-Meneses, M. Luna-Trujillo, Jin-An Wang, L. Lartundo-Rojas, A. Manzo-Robledo〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Electrochemical reduction of NO〈sub〉x〈/sub〉 species such as nitrates (NO〈sub〉3〈/sub〉〈sup〉−), nitrites (NO〈sub〉2−)〈/sub〉〈/sup〉, nitric oxide (NO), nitrogen dioxide (NO〈sub〉2〈/sub〉) and their mixtures, was studied at the interface of palladium (Pd) and palladium-copper (PdCu) nanoparticles supported on carbon Vulcan (C). The electro-catalysts were synthesized by impregnation route with a low noble metal content of 5% wt. Pd and 2.5% wt. Pd for the mono and bi-metallic electrocatalyst, respectively. It was found by XRD analysis the formation of a solid solution in the bi-metallic catalyst and the TEM analysis suggest that the incorporation of copper decreases the particle size from 12 to 3 nm in comparison with its counterpart free of copper. Also, XPS technique verify the presence of Pd and Cu species in their metallic-oxidation states. Linear sweep and cyclic voltammetry techniques were used for the evaluation of the electrochemical NO〈sub〉x〈/sub〉 reduction, using alkaline solutions of NO〈sub〉2〈/sub〉〈sup〉−〈/sup〉 or NO〈sub〉3〈/sub〉〈sup〉−〈/sup〉 saturated with NO〈sub〉2〈/sub〉 (synthesized in-situ) and NO (from commercial source). The results showed that the catalytic-activity at the current versus potential (i-E) characteristics improves significantly due to the presence of copper (as also demonstrated by CO-stripping-electrochemical active surface area calculations), inhibiting the process associated with the hydrogen evolution reaction. It is also noted in this work that the reduction faradic-current is c.a. 6 times higher at saturated solutions with NO and NO〈sub〉2〈/sub〉. The NO〈sub〉x〈/sub〉 species were reduced mainly to nitrogen, ammonia and hydrazine as confirmed using on-line differential electrochemical mass spectrometry (DEMS) during steady-state experiments.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307945-ga1.jpg" width="385" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Eirini Zagoraiou, Maria K. Daletou, Labrini Sygellou, Stella Ballomenou, Stylianos G. Neophytides〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉This work addresses scientific issues regarding the most challenging component of PEM fuel cells, the electrocatalyst, and explores a new approach to exploit the differentiations induced to the metal by the surface chemistry of the support. The study focuses on the development of Pt based electrocatalysts supported on pyridine modified carbon nanotubes with different Pt loadings, their thorough characterization and parallel comparison with non-modified or conventional carbon supports. The aim is the interpretation of the catalyst electrochemical behavior through a structural and physicochemical characterization study. The introduction of pyridines can differentiate the metal deposition, in terms of dispersion, nanoparticle properties, platinum oxidation state and metal-support interactions. Moreover, the substrate can play a decisive role on the size and functionality of the electrochemical interface. This approach constitutes a promising route for developing materials with innovative features aiming to a serious reduction in the Pt loads through increased activity and metal utilization.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307969-ga1.jpg" width="467" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Sourav Das, Ananyo Jyoti Misra, A.P. Habeeb Rahman, Bhaskar Das, R. Jayabalan, Ashok J. Tamhankar, Amrita Mishra, Cecilia Stålsby Lundborg, Suraj K. Tripathy〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉In the present study, we report the solar-photocatalytic disinfection (SPCD) of a multidrug resistant (MDR) bacterium, 〈em〉Bacillus〈/em〉 sp. CBEL-1 using Ag@SnO〈sub〉2〈/sub〉@ZnO core-shell nanocomposites (NCs) as catalyst. Complete disinfection was observed within 210 min with a catalyst concentration of 500 mg/L when subjected to NCs mediated PCD under solar irradiation. H〈sub〉2〈/sub〉O〈sub〉2〈/sub〉 was found to be the key reactive oxygen species (ROS) involved in SPCD of targeted bacteria. Increase in production of 4-HNE along with change in fatty acid profile of bacteria after SPCD induced oxidative stress indicates the compromisation of bacterial cell membrane. Irreversible change in antibiotic resistance profile of the target bacteria was notice after SPCD, without recovery even after 96 h post disinfection experiments. Traditional disinfectants and UV-250 nm were found to have marginal impact on the resistance profile of the bacteria compared to that of SPCD. Disinfection achieved using the NCs were also validated for real water samples.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308112-ga1.jpg" width="500" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Kinga Gołąbek, Antonio E. Palomares, Joaquin Martínez-Triguero, Karolina A. Tarach, Krzysztof Kruczała, Vladimir Girman, Kinga Góra-Marek〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉This paper reports the activity of different Ce-BEA zeolites for the catalytic oxidation of trichloroethylene and it is focused on determining the nature of the catalyst active sites. The study was made by using a microporous zeolite BEA, two types of desilicated BEA zeolites and mildly steamed desilicated BEA zeolites. The catalysts were prepared by introducing Ce to the zeolites with incipient wetness impregnation and their structural, textural, and acidic properties were established. The evolution of TCE conversion was correlated with the physicochemical properties of the zeolites. It is shown that highly developed mesopore surface area, well-dispersed cerium species and a high number of Brønsted sites results in the highest activity. The activity and selectivity of the Ce-loaded zeolites were found to be dependent on the number of high strength Brønsted acid centres. The hierarchical materials with a higher density of hydroxyls showed higher yields to HCl while the formation of chlorine was prevented.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307684-ga1.jpg" width="277" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Xingxing Jiang, Xikui Wang, Zhenjie Liu, Qinglong Wang, Xin Xiao, Haiping Pan, Man Li, Jiawei Wang, Yong Shao, Zhangquan Peng, Yan Shen, Mingkui Wang〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Electrochemical reduction of CO〈sub〉2〈/sub〉 is promising for mitigating the excessive CO〈sub〉2〈/sub〉 emission. However, the low efficiency and poor selectivity for targeted products block the practical application of most conventional electrocatalysts. Here, we developed an electronic regulation Cu embedded into Sn nanoparticles heterogeneous bimetallic catalyst, with high catalytic activity and selectivity for electrochemical reduction of CO〈sub〉2〈/sub〉. The excellent performance of high activity is mainly due to the appearance of abundant Sn-Cu interfaces after Cu embedded into Sn nanoparticles. XPS characterization indicates that the atomic Sn electronic structure of the bimetallic catalyst was significantly regulated by deposited Cu atoms. DFT calculations in combination with In-situ Raman spectroscopy characterization on CO〈sub〉2〈/sub〉 reduction process further indicates that the electronic regulation of bimetallic catalyst facilitates the formation of key intermediate HCOO 〈sup〉•〈/sup〉 followed by the generation of formate with high selectivity. The present design provides a method for prepare bimetallic catalyst with high catalytic performance.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307866-ga1.jpg" width="285" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 December 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 259〈/p〉 〈p〉Author(s): Huimin Liu, Ping Wu, Haitao Li, Zibin Chen, Lizhuo Wang, Xin Zeng, Yuxiang Zhu, Yijiao Jiang, Xiaozhou Liao, Brian S. Haynes, Jinhua Ye, Catherine Stampfl, Jun Huang〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Harnessing the vast supply of solar energy as the driving force to produce ammonia from abundant nitrogen gas and water is beneficial for both relieving energy demands and developing sustainable chemical industry. Bulk carbon nitride (B-g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉), exfoliated carbon nitride (E-g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉) and graphite (g-C) supported Ru-K catalysts, denoted as Ru-K/B-g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉, Ru-K/E-g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 and Ru-K/g-C, respectively, with the layered materials serving both as supports and light harvesters, were designed for photocatalytic ammonia synthesis. It was discovered that, besides the light harvesting properties of the catalysts which played roles in photocatalytic reactions, the structure of the supports influenced greatly the preferential locations of Ru species, which further exerted effects on the N〈sub〉2〈/sub〉 activation process and ultimately impacted the ammonia production rate. The fine Ru nanoparticles uniformly and randomly dispersed on the monolayered E-g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 did not provide outstanding activity in ammonia photosynthesis; in contrast, Ru nanoparticles at the step edges of bulk g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 exhibited lower overall barriers for N〈sub〉2〈/sub〉 activation and a much enhanced photocatalytic ammonia synthesis rate due to the synergy effects between metal and support as confirmed by density functional theory (DFT) calculations. The discovery of the relationship between reactivity and support geometry in this study will be important in guiding the rational predesign of efficient photocatalysts.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319307726-ga1.jpg" width="266" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: Available online 30 March 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental〈/p〉 〈p〉Author(s): Seung Yo Choi, Seonghun Kim, Kyung Jin Lee, Jin Young Kim, Dong Suk Han, Hyunwoong Park〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉We present an off-grid, standalone electrocatalytic H〈sub〉2〈/sub〉O〈sub〉2〈/sub〉 production reaction (HPR) using carbon nanotubes (CNT) wired to hydrogen-treated TiO〈sub〉2〈/sub〉 nanorod (h-TNR) arrays catalyzing the oxidation of As(III) to As(V) under simulated solar light (AM 1.5; 100 mW⋅ cm〈sup〉―2〈/sup〉). Loading CNT onto acid-treated carbon paper (a-CP) significantly enhances the catalytic 2-electron transfer to O〈sub〉2〈/sub〉, leading to a Faradaic efficiency (FE) of ˜100% for the HPR. To drive the HPR, the 2-electron oxidation of toxic As(III) to less toxic As(V) that accompanies the production of the proton/electron couples is achieved at an FE of 〉80% using the h-TNR arrays. The high FEs of the anodic and cathodic reactions are maintained over 10 h when a direct-current voltage of 0.7 V is applied to the h-TNR photoanode and CNT/a-CP cathode pair. The coupling of a mono-Si photovoltaic array that is one-tenth the size of h-TNR photoanode to the pair of h-TNR and CNT/a-CP successfully drives the standalone operation of both reactions at the high FEs (〉90%). The surface characterization of the as-synthesized materials and the reaction mechanism are discussed in detail.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319302826-ga1.jpg" width="301" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: Available online 29 March 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental〈/p〉 〈p〉Author(s): Yongming Zhong, Siyuan Yang, Xin Cai, Shengsen Zhang, Qiongzhi Gao, Yingju Liu, Zhuohong Yang, Shihe Yang, Yueping Fang〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Highly efficient and easily recyclable monolithic photocatalysts with elaborate hierarchical heterostructure and functional components are desirable to tap solar energy and produce green hydrogen fuels for the sustainable future. Inspired by the natural leaves, here we have rationally designed and fabricated an efficient artificial leaf photocatalyst, i.e., the first monolithic photomembrane of CdS/ZnO nanocage arrays grown into the interspaces of multilayered reduced graphene oxide (rGO) nanosheets (denoted as CdS/ZnO/rGO). The CdS/ZnO/rGO have elaborate hierarchical porous heterostructure and multifunctional components, such as multilayer rGO nanosheets for visible light absorption/harvesting, rapid charge transport and collection, hollowed CdS/ZnO nanocage arrays for light harvesting and charge utilization, and multiple heterojunction interfaces for efficient charge separation. It can been used not only as a monolithic photocatalyst, but also directly as a freestanding photoanode in the photoelectrochemical (PEC) cell system, exhibits an enhanced performance of photocatalytic (PC) or PEC hydrogen generation under different monochrome light irradiation in full-visible light region. Moreover, the CdS/ZnO/rGO photo-membrane can macroscopically realize the separation of photogenerated hole elimination and hydrogen generation by adjusting co-catalysts loading position. Impressively, it still delivered a PC H〈sub〉2〈/sub〉 generation activity (0.79 µmol cm〈sup〉-2〈/sup〉  h〈sup〉-1〈/sup〉) and a photocurrent response of 250 µA cm〈sup〉-2〈/sup〉 even under near-infrared light (λ =700 nm) irradiation, a striking feature rarely achieved in prior arts.〈/p〉〈/div〉 〈h5〉Graphic Abstract〈/h5〉 〈div〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319302966-ga1.jpg" width="301" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈p〉Highly efficient and easily recyclable CdS/ZnO/rGO photomembrane with full-visible light response and efficient charge separation has achieved the excellent photocatalytic and photoelectrochemical hydrogen generations.〈/p〉 〈p〉Graphical Abstract〈/p〉 〈/div〉

Description: 〈p〉Publication date: 15 August 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 251〈/p〉 〈p〉Author(s): Jiajun Wang, Kuan Chang, Zeyu Sun, Ji Hoon Lee, Brian M. Tackett, Cheng Zhang, Jingguang G. Chen, Chang-Jun Liu〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Modifying the nanostructures and chemical compositions provides an opportunity of developing the effective and inexpensive hydrogen evolution reaction (HER) electrocatalysts. Herein, porous transition metal doped tungsten phosphide (M-WP, M=Mo, Co) catalysts have been developed as enhanced HER electrocatalysts in comparison with pristine WP. Owing to the incorporated transition metals, the as-prepared M-WP nanomaterials exhibit porous nanostructures, abundant active sites and reduced charge transfer resistances. Density functional theory (DFT) calculations further demonstrate that the Co dopant simultaneously facilitates the water dissociation step and optimizes the hydrogen adsorption free energy during the entire HER process. Consequently, the Co-WP catalyst shows efficient and stable HER performance over wide pH range. This work demonstrates how metal dopants promote the HER kinetics and develops the strategy for further designing non-precious metal based nanomaterials for energy conversion and electrocatalysis.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319302875-ga1.jpg" width="497" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 August 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 251〈/p〉 〈p〉Author(s): Raana Mahmoodi, Mir Ghasem Hosseini, Haleh Rasouli〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉In this research work, Ni-Pd nanoparticles with core-shell structure (C〈sub〉Ni〈/sub〉-S〈sub〉Pd〈/sub〉) were synthesized on different catalyst supports such as reduced graphene oxide (rGO), pure polyaniline (PANI) and polymeric composites of rGO with PANI (rGO-PANI) for the first time. In polymeric composite supports, the ratio of rGO to PANI was altered (0.36, 0.14 and 0.11). That way, after chemical reduction of graphene oxide to rGO with sodium borohydride, different polymeric composite supports of rGO-PANI were prepared by chemical oxidation of different amounts of aniline monomer with ammonium persulfate (APS) in rGO dispersions and named as rGO-PANI1 (rGP1), rGO-PANI2 (rGP2) and rGO-PANI3 (rGP3). X-ray diffraction (XRD), field emission scanning electron microscopy (FE-SEM), energy-dispersive X-ray spectroscopy (EDX), transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HR-TEM), fourier transform infrared (FT-IR) spectra, inductively coupled plasma mass spectrometry (ICP-MS) analysis and X-ray photoelectron spectrometer (XPS) were employed to study the morphology and crystal structure of the novel nanostructures. Catalytic behavior of the catalysts respect to NaBH〈sub〉4〈/sub〉 oxidation was evaluated in half-cell configuration and in direct borohydride-hydrogen peroxide fuel cell. The cyclic voltammetry results showed that C〈sub〉Ni〈/sub〉-S〈sub〉Pd〈/sub〉/rGP1 has the highest borohydride oxidation current density (42678 A. g〈sup〉−1〈/sup〉) respect to C〈sub〉Ni〈/sub〉-S〈sub〉Pd〈/sub〉/PANI (17072 A. g〈sup〉−1〈/sup〉), C〈sub〉Ni〈/sub〉-S〈sub〉Pd〈/sub〉/rGO (39085 A. g〈sup〉−1〈/sup〉), C〈sub〉Ni〈/sub〉-S〈sub〉Pd〈/sub〉/rGP2 (32260 A. g〈sup〉−1〈/sup〉) and C〈sub〉Ni〈/sub〉-S〈sub〉Pd〈/sub〉/rGP3 (24954 A. g〈sup〉−1〈/sup〉). As well as, the single fuel cell studies indicated that with C〈sub〉Ni〈/sub〉-S〈sub〉Pd〈/sub〉/rGP1 as anodic electrocatalyst, power density (339.10 mW.cm〈sup〉-2〈/sup〉) was enhanced as 64.54% and 8.52% in comparison with C〈sub〉Ni〈/sub〉-S〈sub〉Pd〈/sub〉/PANI (120.23 mW.cm〈sup〉-2〈/sup〉) and C〈sub〉Ni〈/sub〉-S〈sub〉Pd〈/sub〉/rGO (310.20 mW.cm〈sup〉-2〈/sup〉), respectively. Theses consequences imply that the rGP1 polymeric composite with the ratio of rGO/PANI = 0.36 is a suitable support substance that can improves the electroactivity for borohydride oxidation considerably.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319302863-ga1.jpg" width="266" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 5 August 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 250〈/p〉 〈p〉Author(s): 〈/p〉

Description: 〈p〉Publication date: 15 August 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 251〈/p〉 〈p〉Author(s): Huoshuai Huang, Yun Song, Najun Li, Dongyun Chen, Qingfeng Xu, Hua Li, Jinghui He, Jianmei Lu〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉As the most promising environment-friendly photocatalyst, titanium dioxide admittedly has two shortcomings of low sunlight utilization efficiency and poor quantum yield. Nitrogen doping and TiO〈sub〉2〈/sub〉 loading on carbon materials can improve the above two problems, respectively. But a facile synthetic method for titanium dioxide composites with stable structure and high visible-light-driven photocatalytic activity is still desired by researchers. Herein we obtained two-dimensional layered nitrogen-doped carbon-supported titanium dioxides (N-TiO〈sub〉2〈/sub〉@C) via a one-step in-situ fabrication way from a novel two-dimensional layered transition metal carbide Ti〈sub〉3〈/sub〉C〈sub〉2〈/sub〉 MXene as carbon skeleton and homologous titanium source. Based on the negatively charged and easily oxidized property of Ti〈sub〉3〈/sub〉C〈sub〉2〈/sub〉 MXene, it was assembled with nitrogen-containing cationic compound via electrostatic interactions and then in-situ transformed into nitrogen-doped carbon-supported TiO〈sub〉2〈/sub〉 in a CO〈sub〉2〈/sub〉 atmosphere at 550 °C. The obtained composites of porous 2D layered N-TiO〈sub〉2〈/sub〉@C with high stability, outstanding electron transfer performance and excellent visible-light photocatalytic activity exhibits the high efficiency of phenol degradation with the apparent rate constant 〈em〉k〈/em〉 of 1.646 × 10〈sup〉−2〈/sup〉 min〈sup〉−1〈/sup〉. It provides a facile new method for the preparation of visible-light-driven titanium dioxide with excellent catalytic performance, structural stability and good application prospects in the environmental purification.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉A new one-step in-situ synthetic method for nitrogen-doped TiO〈sub〉2〈/sub〉@C derived from Ti〈sub〉3〈/sub〉C〈sub〉2〈/sub〉 MXene is reported and the obtained N-TiO〈sub〉2〈/sub〉@C maintains 2D layered structure, has excellent visible-light driven photocatalytic activity and good cyclic stability for the photodegradation of phenol and other organic pollutants.〈/p〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319302887-ga1.jpg" width="289" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: Available online 29 March 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental〈/p〉 〈p〉Author(s): Pillaiyar Puthiaraj, Seenu Ravi, Kwangsun Yu, Wha-Seung Ahn〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉A new nanoporous N-heterocyclic carbene-based cross-linked aromatic polymer (NHC-CAP-1) incorporated with highly nucleophilic bromide anions and with a large surface area was synthesized by a simple Friedel-Crafts reaction of imidazolium salt, triphenylbenzene, and formaldehyde dimethylacetal. Subsequently, ZnBr〈sub〉2〈/sub〉 was grafted onto the NHC-CAP-1 to obtain NHC-CAP-1(Zn〈sup〉2+〈/sup〉) with enhanced Lewis acidity. After systematic evaluation of the structural and chemical properties using different analytical techniques, these were explored for CO〈sub〉2〈/sub〉 adsorption and CO〈sub〉2〈/sub〉 chemical fixation to cyclic carbonates. Whilst NHC-CAP-1 showed a high CO〈sub〉2〈/sub〉 capture capacity (188.2 mg g〈sup〉-1〈/sup〉 at 273 K/1 bar) with a moderate CO〈sub〉2〈/sub〉/N〈sub〉2〈/sub〉 selectivity, NHC-CAP-1(Zn〈sup〉2+〈/sup〉) displayed significantly enhanced CO〈sub〉2〈/sub〉/N〈sub〉2〈/sub〉 selectivity (100/80 at 273/298 K) at the expense of diminished CO〈sub〉2〈/sub〉 capture (123.0 mg g〈sup〉-1〈/sup〉 at 273 K/1 bar). These values are among the highest reported so far for porous cross-linked organic polymers. As a catalyst, NHC-CAP-1(Zn〈sup〉2+〈/sup〉) showed high catalytic activities for CO〈sub〉2〈/sub〉 cycloaddition to a series of epoxides to form cyclic carbonates in the absence of co-catalyst and solvent, producing a high turnover frequency (TOF) of 2202 h〈sup〉-1〈/sup〉 at 100 °C. The effect of reaction parameters including temperature, reaction time, and catalyst loading was examined. NHC-CAP-1(Zn〈sup〉2+〈/sup〉) could be separated readily and reuse for a minimum of 10 runs while maintaining high activity and stability owing to the strong covalent bonding of Lewis acidic Zn〈sup〉2+〈/sup〉 to the NHC-CAP-1 backbones. This work demonstrated that NHC-CAP-1 and NHC-CAP-1(Zn〈sup〉2+〈/sup〉) are viable porous materials that are highly efficient for both CO〈sub〉2〈/sub〉 capture and catalytic conversion of CO〈sub〉2〈/sub〉 to cyclic carbonates.〈/p〉〈/div〉 〈h5〉Graphical Abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319303066-ga1.jpg" width="301" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: Available online 28 March 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental〈/p〉 〈p〉Author(s): Paul A. DeSario, Catherine L. Pitman, Daniel J. Delia, Darren M. Driscoll, Andrew J. Maynes, John R. Morris, Ashley M. Pennington, Todd H. Brintlinger, Debra R. Rolison, Jeremy J. Pietron〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉We exploit interfacial charge transfer from titania (TiO〈sub〉2〈/sub〉) to copper (Cu) to design catalytic Cu/TiO〈sub〉2〈/sub〉 composite aerogels that shift the chemical state of Cu nanoparticles away from Cu〈sup〉2+〈/sup〉, making them highly active for low-temperature CO oxidation. The high degree of interfacial contact between ˜2–3 nm–diameter Cu particles and the networked ˜10 nm–diameter TiO〈sub〉2〈/sub〉 particles in ultraporous aerogel stabilizes a high ratio of Cu〈sup〉0/1+〈/sup〉:Cu〈sup〉2+〈/sup〉. The reduced nature of Cu in Cu/TiO〈sub〉2〈/sub〉 aerogels is evidenced by a strong surface plasmon resonance in its diffuse reflectance UV–Visible spectrum and by its X-ray photoelectron spectral features. In contrast, when larger diameter (˜50–60 nm), non–networked TiO〈sub〉2〈/sub〉 particles are used to support Cu nanoparticles, the single planar nanoscale interface between Cu and the support particle stabilizes a much lower fraction of low-valent Cu. The Cu〈sup〉0/1+〈/sup〉 speciation stabilized within the aerogel catalyzes low-temperature CO oxidation (〈100 °C) at high conversion rates and does not necessitate high-temperature activation in a reducing gas stream—performance that the non-networked catalyst cannot meet. Our work demonstrates how nanoscale interfacial materials design can be exploited to create active Cu nanoparticle–based catalysts that are stable under practical conditions.〈/p〉〈/div〉 〈h5〉Graphical Abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319302954-ga1.jpg" width="301" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: Available online 29 March 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental〈/p〉 〈p〉Author(s): Lays S.R. Silva, Caio V.S. Almeida, Cristiano T. Meneses, Elizete A. Batista, Sydney F. Santos, Katlin I.B. Eguiluz, Giancarlo R. Salazar-Banda〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Carbon-supported Pd, Au@Pd core–shell and Au〈sub〉1–〈/sub〉〈em〉〈sub〉x〈/sub〉〈/em〉Pd〈em〉〈sub〉x〈/sub〉〈/em〉-alloyed nanoparticles were prepared by a chemical reduction method and characterized by different experimental techniques, including X-ray powder diffraction, transmission electron microscopy, scanning-transmission electron microscopy using bright-field and high-angle annular dark field detectors and X-ray energy dispersive spectroscopy. The catalytic mass activity toward ethanol oxidation was assessed by cyclic voltammetry and chronoamperometry at room temperature. The measurements showed that the addition of Au enhances remarkably the electrocatalytic activity of the material, due to the bifunctional effect of Au〈sub〉1–〈/sub〉〈em〉〈sub〉x〈/sub〉〈/em〉Pd〈em〉〈sub〉x〈/sub〉〈/em〉/C alloys, and the synergetic effect on Au@Pd/C, resulting in a dissolution resistance of core–shell catalysts at potentials of 1.5 V versus reversible hydrogen electrode. In situ Fourier transform infrared spectroscopy measurements showed that the mechanism for ethanol oxidation depends on the electrocatalyst structure and morphology. Acetate was identified as the main product of ethanol electro-oxidation on the studied electrocatalysts. However, the presence of a core–shell structure on Au@Pd/C resulted in enhanced ethanol oxidation selectivity toward CO〈sub〉2〈/sub〉. The improvement of activity is attributed to the interaction between Pd shell and Au core.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319302899-ga1.jpg" width="301" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: Available online 28 March 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental〈/p〉 〈p〉Author(s): Wenting Hong, Chuanyong Jian, Genxiang Wang, Xu He, Jing Li, Qian Cai, Zhenhai Wen, Wei Liu〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉The morphology and crystallographic surface can influence the catalytic HER activity of electrocatalyst. With sufficient active sites and surface area, nanoporous materials with three-dimensional interconnected porous networks have shown the promising application in electrocatalyst. In this work, we report a simple method that can synthesize the self-supported nanoporous cobalt phosphosulfate (CoP|S) electrocatalyst. Theoretical calculation shows that the phosphorus substitution by sulfur can control the electronic structures of the active sites and accelerate charge transfer of CoP, therefore improving HER activity. The experimental study shows that nanoporous CoP|S electrodes present the improved HER performance compared with CoP in alkaline media and acidic media, respectively.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319302929-ga1.jpg" width="301" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: Available online 28 March 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental〈/p〉 〈p〉Author(s): Shuozhen Hu, Fanglin Che, Bita Khorasani, Mina Jeon, Chang Won Yoon, Jean-Sabin McEwen, Louis Scudier, Su Ha〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Pd-based bimetallic nanoparticles have a superior electrochemical activity and stability for formic acid oxidation (FAO) than pure Pd. Previous DFT-based calculations show that the catalytic properties of the Pd surface could be altered by modifying its electronic properties. However, only a few experimental studies investigate how the electronic properties of Pd are modified by introducing various metals and how the resulting electronic perturbation affects its electrochemical activity and stability for FAO. Here, we demonstrate a correlation between electrochemistry and electronic properites for Pd-M bimetallic nanoparticles (M = Ru, Pt, Cu, Au, and Ag). The volcano shape relationship obtained between activity and 〈em〉d〈/em〉-band center values suggests that the electronic effects play a major role in modifying the surface electrochemical properties of Pd-M bimetallic nanoparticles for FAO. Among all the bimetallic catalysts investigated in this study, Pd-Pt/C and Pd-Cu/C with 〈em〉d〈/em〉-band center values of 2.58 eV and 2.85 eV, respectively, demonstrate the highest activities and Pd-Cu/C exhibits the highest stability for FAO.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319302942-ga1.jpg" width="301" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: Available online 28 March 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental〈/p〉 〈p〉Author(s): Ranran Yuan, Cailiang Yue, Jinli Qiu, Fuqiang Liu, Aimin Li〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉TiO〈sub〉2〈/sub〉@NH〈sub〉2〈/sub〉-MIL-88B(Fe) heterostructures (TMFe-x) were successfully synthesized and used in an efficient sunlight-driven reduction towards Cr(VI) in a neutral aqueous media. Further, the prepared TMFe-x heterostructures exhibited higher photocatalytic activity when compared with those exhibited by pure TiO〈sub〉2〈/sub〉 and NH〈sub〉2〈/sub〉-MIL-88B(Fe) under simulated sunlight irradiation. The optical TiO〈sub〉2〈/sub〉 modification content was determined to be 10 wt.% (TMFe-b), with 98.6% Cr(VI) being converted to Cr(III) within 35 min using ammonium oxalate as the hole scavenger at pH = 7. In neutral conditions, the kinetic rate constant (0.0878 min〈sup〉-1〈/sup〉) was five times larger than the published values. Additionally, the photocatalytic performance of TMFe-b was maintained and Fe leaching was observed to be negligible after the completion of four reaction cycles. The superior photocatalytic property can be attributed to the high photoelectron-hole separation and migration efficiency. Subsequently, TMFe-b achieved Cr(VI) reduction under neutral conditions by capturing hydrogen from the water molecules or the hole scavengers. The photoelectrons and superoxide radicals were the main active species. Furthermore, TMFe-b was able to efficiently eliminate various pollutants through photocatalytic oxidation and reduction. This study suggests a novel strategy for the preparation of environmentally stable and efficient MOF-based photocatalysts to efficiently eliminate various pollutants. Further, there is a huge potential for the practical application of this technology to water purification.〈/p〉〈/div〉 〈h5〉Graphical Abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319302905-ga1.jpg" width="301" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: Available online 27 March 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental〈/p〉 〈p〉Author(s): Jili Yuan, Yanhong Tang, Xuanying Yi, Chengbin Liu, Can Li, Yunxiong Zeng, Shenglian Luo〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Exciton polarization dissociation, charge transfer and surface electron density in photocatalysts are crucial for photocatalytic hydrogen evolution reactions (HERs). In this study, crystalline carbon nitride with cyanamide defect edges (crystalline CCN) was synthesized by one step polymerization of urea in the presence of KCl. The texture and electronic band structure of carbon nitrides could be facilely tailored by changing KCl dosage. The light absorption edge of crystalline CCN extended to 736 nm due to n→π* electron transition. The enhanced dielectric constants of crystalline carbon nitrides promoted exciton polarization dissociation. The small effective electron mass (m〈sub〉e〈/sub〉*) in crystalline CCN facilitated m〈sub〉e〈/sub〉* diffusion. The efficient separation of electrons and holes benefited the formation of internal electric field, showing an 8.56-fold promotion in electron transfer compared to pristine CN. Significantly, femtosecond time-resolved transient absorption demonstrated that the surface electron density on crystalline CCN was enhanced in the presence of salt ions (NaCl). As a result, crystalline CCN exhibited 14.9 times higher HER rate than pristine CN under visible light irradiation. The apparent quantum yield for H〈sub〉2〈/sub〉 evolution on crystalline CCN reached to 42% at 420 nm and 9% at 500 nm. This study gets a comprehensive understanding of photocatalytic HERs using carbon nitride photocatalysts.〈/p〉〈/div〉 〈h5〉Graphical Abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319302917-ga1.jpg" width="301" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 5 May 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 244〈/p〉 〈p〉Author(s): Ruobai Li, Meixuan Cai, Zhijie Xie, Qianxin Zhang, Yongqin Zeng, Haijin Liu, Guoguang Liu, Wenying Lv〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉A copper ferrite modified graphitic carbon nitride (CuFe〈sub〉2〈/sub〉O〈sub〉4〈/sub〉/g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉) nanocomposite was successfully synthesized for the utilization as a visible-light responsive photocatalyst. The as-synthesized catalysts were characterized using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), UV–vis diffuse reflectance spectra (UV–vis/DRS), photoluminescence (PL) analysis, and an electrochemical workstation. Compared to g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 and CuFe〈sub〉2〈/sub〉O〈sub〉4〈/sub〉, the CuFe〈sub〉2〈/sub〉O〈sub〉4〈/sub〉/g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 composites possessed excellent photocatalytic performance for the destruction of propranolol (PRO). A removal efficiency of 82.2% was achieved with 1 g/L catalyst and 1 mM peroxydisulfate (PDS) under visible light irradiation (λ 〈 420 nm) within 120 min. The g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 coupled with CuFe〈sub〉2〈/sub〉O〈sub〉4〈/sub〉 improved the capacity for visible light capture, whereas the presence of PDS enhanced the transfer of photogenerated electron. Quenching experiments and electron spin resonance (ESR) suggested that the reactive oxygen species (ROS) were superoxide radicals (O〈sub〉2〈/sub〉〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉〈sup〉−〈/sup〉), h〈sup〉+〈/sup〉, hydroxyl radicals (〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉OH), and sulfate radicals (SO〈sub〉4〈/sub〉〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉〈sup〉−〈/sup〉). Moreover, the byproducts of PRO were investigated by HPLC-MS/MS, and the transformation pathways under the Vis/g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉/CuFe〈sub〉2〈/sub〉O〈sub〉4〈/sub〉/PDS process were tentatively proposed based on the intermediates. The research provided a potential approach of CuFe〈sub〉2〈/sub〉O〈sub〉4〈/sub〉 modified g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 as a photocatalyst combined with PDS for the treatment of contaminated water.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337318311974-ga1.jpg" width="359" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 May 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 245〈/p〉 〈p〉Author(s): Xiaoning Wang, Wenbo Dong, Marcello Brigante, Gilles Mailhot〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉In the present study, comparison of activation efficiencies of hydrogen peroxide (H〈sub〉2〈/sub〉O〈sub〉2〈/sub〉) and persulfate (PS, Na〈sub〉2〈/sub〉S〈sub〉2〈/sub〉O〈sub〉8〈/sub〉) induced by Fe(III)-Ethylenediamine-〈em〉N〈/em〉,〈em〉N'〈/em〉-disuccinic acid (EDDS) under polychromatic irradiation UVA and visible region at same conditions was studied for the first time. The effects of pH, Fe(III)-EDDS concentration, H〈sub〉2〈/sub〉O〈sub〉2〈/sub〉 and PS concentrations were investigated. 〈em〉p〈/em〉-hydroxyphenylacetic acid (〈em〉p〈/em〉-HPA) was taken as a model pharmaceutical intermediate pollutant to estimate the oxidative process efficiency. In these two systems, the degradation rate of 〈em〉p〈/em〉-HPA increased (not linearly) using higher concentrated solution of H〈sub〉2〈/sub〉O〈sub〉2〈/sub〉 and Na〈sub〉2〈/sub〉S〈sub〉2〈/sub〉O〈sub〉8〈/sub〉. However, when Fe(III)-EDDS concentration exceeding 250 μM, the degradation efficiency of 〈em〉p〈/em〉-HPA began to decrease. Surprisingly, results of pH effects showed that Fe(III)-EDDS/H〈sub〉2〈/sub〉O〈sub〉2〈/sub〉/UV system presents much higher degradation efficiency than Fe(III)-EDDS/PS/UV whatever the solution pH’s, especially in neutral and alkaline solutions. In the Fe(III)-EDDS/H〈sub〉2〈/sub〉O〈sub〉2〈/sub〉/UV reaction, 〈em〉p〈/em〉-HPA degradation rate (R〈em〉〈sub〉p〈/sub〉〈/em〉〈sub〉-HPA〈/sub〉) increased fast from pH 2.5 to 7.5, then it began to decrease when pH increased to 9.0. While R〈em〉〈sub〉p〈/sub〉〈/em〉〈sub〉-HPA〈/sub〉 started to decrease with pH increase to 3.9 in Fe(III)-EDDS/PS/UV system. To explain this phenomenon, the second order constant of 〈em〉p〈/em〉-HPA (for both molecular and mono-anionic forms) with HO〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉 and SO〈sub〉4〈/sub〉〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉〈sup〉−〈/sup〉 radicals were determined by laser flash photolysis (LFP) experiments for the first time. Results showed that 〈math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="si1.gif" overflow="scroll"〉〈mrow〉〈msub〉〈mi〉k〈/mi〉〈mrow〉〈mi〉p〈/mi〉〈mo〉−〈/mo〉〈mi〉H〈/mi〉〈mi〉P〈/mi〉〈mi〉A〈/mi〉〈mo〉,〈/mo〉〈mi〉H〈/mi〉〈msup〉〈mi〉O〈/mi〉〈mo〉•〈/mo〉〈/msup〉〈/mrow〉〈/msub〉〈/mrow〉〈/math〉 was higher than 〈math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="si2.gif" overflow="scroll"〉〈mrow〉〈msub〉〈mi〉k〈/mi〉〈mrow〉〈mi〉p〈/mi〉〈mo〉−〈/mo〉〈mi〉H〈/mi〉〈mi〉P〈/mi〉〈mi〉A〈/mi〉〈mo〉,〈/mo〉〈mi〉S〈/mi〉〈msubsup〉〈mi〉O〈/mi〉〈mn〉4〈/mn〉〈mrow〉〈mo〉•〈/mo〉〈mo〉−〈/mo〉〈/mrow〉〈/msubsup〉〈/mrow〉〈/msub〉〈/mrow〉〈/math〉 for both anionic and molecular forms of pollutant. These results demonstrated that iron-complex induced photo-Fenton process is more efficient than activation of persulfate process, particularly at environmentally closed pH values and sun-simulated wavelengths (λ 〉 300 nm).〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337318312050-ga1.jpg" width="418" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 May 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 245〈/p〉 〈p〉Author(s): Tingting Hou, Nengchao Luo, Yi-Tao Cui, Jianmin Lu, Lei Li, Katherine E. MacArthur, Marc Heggen, Ruotian Chen, Fengtao Fan, Wenming Tian, Shengye Jin, Feng Wang〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Engineering the electronic properties of heterogeneous catalysts is an important strategy to enhance their activity towards CO〈sub〉2〈/sub〉 reduction. Herein, we prepared partially sulfurized cerium oxide (CeO〈sub〉x〈/sub〉-S) nanoclusters with the size less than 2 nm on the surface of ZnIn〈sub〉2〈/sub〉S〈sub〉4〈/sub〉 layers. Surface electronic properties of CeO〈sub〉x〈/sub〉-S nanoclusters are facilely modulated by cerium coordination to sulfur, inducing the emergence of abundant Ce〈sup〉3+〈/sup〉 and oxygen vacancies. For the photoreduction of CO〈sub〉2〈/sub〉, CeO〈sub〉x〈/sub〉-S/ZnIn〈sub〉2〈/sub〉S〈sub〉4〈/sub〉 hybrid catalysts exhibited a CO productivity of 1.8 mmol g〈sup〉−1〈/sup〉 with a rate of 0.18 mmol g〈sup〉−1〈/sup〉 h〈sup〉−1〈/sup〉, which was twice as higher as that of ZnIn〈sub〉2〈/sub〉S〈sub〉4〈/sub〉 catalyst using triethylamine as a sacrificial electron donor. Further mechanistic studies reveal that the photogenerated electrons are trapped by oxygen vacancies on CeO〈sub〉x〈/sub〉-S/ZnIn〈sub〉2〈/sub〉S〈sub〉4〈/sub〉 catalysts and subsequently transfer to CO〈sub〉2〈/sub〉, benefiting the activation of CO〈sub〉2〈/sub〉. Moreover, the extremely high selectivity of CO is derived from the weak adsorption of CO on the surface of CeO〈sub〉x〈/sub〉-S/ZnIn〈sub〉2〈/sub〉S〈sub〉4〈/sub〉 catalysts.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337318312128-ga1.jpg" width="463" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 May 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 245〈/p〉 〈p〉Author(s): Manjot Kaur, Ahmad Umar, Surinder Kumar Mehta, Sushil Kumar Kansal〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Herein, we report the synthesis and characterization of rGO-CdS heterostructure and their utilization as an efficient material for sensing and visible-light driven photocatalytic degradation applications. The heterostructure was synthesized by facile hydrothermal process and characterized by several techniques which exhibited intriguing compositional, morphological, structural, thermal, textural and photo-physical properties. The high resolution transmission electron microscopy (HRTEM) images of the prepared rGO-CdS heterostructure showed the successful deposition of CdS nanoparticles (CdS NPs) on the surface of reduced graphene oxide (rGO) sheets. The synthesized rGO-CdS heterostructure was employed as an outstanding fluorescent sensor for the selective and sensitive detection of heavy transition metal ion; Ag(I) and a synthetic food colorant; sunset yellow (SY). The detection limit of 12.35 μM and 7.89 μM was found to be for Ag(I) and SY, respectively. The prepared rGO/CdS heterostructure was also successfully applied for the photocatalytic degradation of fluoroquinoline antibiotic, levofloxacin (LVX), and food colorant SY under visible-light irradiation. The removal efficiency of 82.7% was obtained for LVX (10 mg/L) using rGO-CdS heterostructure in 60 min under visible-light irradiation. The synthesized heterostructure displayed enhanced photocatalytic decomposition (82.7%) than pure CdS NPs (67.5%) under optimized reaction conditions (0.50 g/L photocatalyst amount, 10 mg/L LVX initial concentration and pH 9.0). Approximate 66% of SY was degraded in 270 min under visible-light using the prepared heterostructure. The scavenger study confirmed the pivotal role of e, O〈sub〉2〈/sub〉〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉, 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉OH〈sub〉s〈/sub〉 and 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉OH in the photocatalytic decomposition process. The amended photocatalytic behaviour of the rGO-CdS heterostructure could be accredited to the enhanced visible light harvesting capability, effective charge separation and transportation of photogenerated charge carriers across the heterojunctional interface. To the best of our knowledge, this is the first report till date on the utilization of rGO-CdS heterostructure for the fluorescence sensing of Ag(I) and SY as well as photocatalytic degradation of LVX and SY.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337318311962-ga1.jpg" width="259" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 May 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 245〈/p〉 〈p〉Author(s): Yu Han, Dongting Yue, Miao Kan, Yunwen Wu, Jun Zeng, Zhenfeng Bian, Yixin Zhao, Xufang Qian〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Improving the photocatalytic efficiency of commercial TiO〈sub〉2〈/sub〉 has important significance for practical application of TiO〈sub〉2〈/sub〉 based photocatalysts. A novel photocatalyst [Mo〈sub〉3〈/sub〉S〈sub〉13〈/sub〉]〈sup〉2−〈/sup〉/TiO〈sub〉2〈/sub〉 was fabricated by combining [Mo〈sub〉3〈/sub〉S〈sub〉13〈/sub〉]〈sup〉2−〈/sup〉 with commercial TiO〈sub〉2〈/sub〉 by an impregnation method. This composite photocatalyst presented a remarkable enhancement on photocatalytic mineralization of acetone in comparison with commercial TiO〈sub〉2〈/sub〉. The optimum loading amount of [Mo〈sub〉3〈/sub〉S〈sub〉13〈/sub〉]〈sup〉2−〈/sup〉 was 1.7wt%, which is more efficient than the Pt/TiO〈sub〉2〈/sub〉 (1.5wt%). Electrochemical impedance spectroscopy (EIS) showed the smooth electron transfer pathway in [Mo〈sub〉3〈/sub〉S〈sub〉13〈/sub〉]〈sup〉2−〈/sup〉/TiO〈sub〉2〈/sub〉 composite, facilitating the photo-charges separation during the photocatalysis process. Reactive oxygen species scavenging test illustrated that superoxide radical (〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉O〈sub〉2〈/sub〉〈sup〉−〈/sup〉), hydroxyl radical (〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉OH) and photo-induced hole (h〈sup〉+〈/sup〉) were all contributing to the acetone degradation. The [Mo〈sub〉3〈/sub〉S〈sub〉13〈/sub〉]〈sup〉2−〈/sup〉/TiO〈sub〉2〈/sub〉 photocatalyst was deposited on non-woven fabrics which showed obvious promotion on the photocatalytic degradation of acetone in comparison with pristine commercial TiO〈sub〉2〈/sub〉.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S092633731831213X-ga1.jpg" width="257" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 15 May 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 245〈/p〉 〈p〉Author(s): Jinshan Hu, Pengfei Zhang, Weijia An, Li Liu, Yinghua Liang, Wenquan Cui〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉In this work, an in-situ Fe-doped g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 catalyst was synthesized by thermal shrinkage polymerization. A heterogeneous photocatalysis-Fenton system was formed with the addition of H〈sub〉2〈/sub〉O〈sub〉2〈/sub〉 under visible irradiation and exhibited excellent and recyclable removal performance for refractory contaminants such as: phenol, bisphenol A, 2, 4-dichlorophenol and coking wastewater, which was due to the formation of σ-π bonds via Fe and N element in the triazine ring skeleton of Fe-g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉. The electrons generated can be quickly transferred to Fe〈sup〉3+〈/sup〉 to form Fe〈sup〉2+〈/sup〉 under the interaction of the chemical bond. The efficiency of photoelectron separation was accelerated, and 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉OH radicals were quickly generated with the reaction between Fe〈sup〉2+〈/sup〉 and H〈sub〉2〈/sub〉O〈sub〉2〈/sub〉. Specifically, the recycling of Fe can be achieved in the heterogeneous system, which avoids the problems for the recycling and secondary pollution of Fe ions in homogeneous Fenton reaction. Parameters such as Fe doping amount, hydrogen peroxide concentration, pH value, catalyst concentration, and complex wastewater (coking wastewater) were optimized. The degradation of coking wastewater were also performed, and the chemical oxygen demand (COD) and total organic carbon (TOC) values for 300 ml coking wastewater could be reduced from 64.6 and 25.3 mg/L to 22.8 and 12.3 mg/L in 60 min, respectively. These results demonstrate photocatalysis-Fenton reaction with Fe-g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 catalyst is promising for environmental remediation.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337318311810-ga1.jpg" width="209" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 5 May 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 244〈/p〉 〈p〉Author(s): Hong Pang, Xianguang Meng, Hui Song, Wei Zhou, Gaoliang Yang, Hongwei Zhang, Yasuo Izumi, Toshiaki Takei, Wipakorn Jewasuwan, Naoki Fukata, Jinhua Ye〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Photocatalytic CO〈sub〉2〈/sub〉 reduction reaction (CO〈sub〉2〈/sub〉RR) on a heterogeneous catalyst offers the possibility for CO〈sub〉2〈/sub〉 abatement and emerges as a promising avenue for renewable carbonaceous fuels production at ambient temperature and pressure using solar light as the sole energy input. Here, we report a newly aqueous colloidal comprised of monodispersed Ni-doped ZnS (ZnS:Ni) nanocrystals as excellent visible-light-responsive photocatalysts for CO〈sub〉2〈/sub〉RR into formate. The wavelength-dependent quantum yield shows a significant contribution of Ni doping for visible light activity. A high selectivity (〉95%) of HCOOH production and remarkable quantum efficiency of 59.1% at 340 nm and 5.6% at 420 nm are obtained over ZnS:Ni (0.1%) colloidal nanocrystals modified by Cd〈sup〉2+〈/sup〉. The proper balance between sulfur vacancies and extended visible light absorption of the constructed colloidal ZnS:Ni nanocrystals contributes to the prominent performance for CO〈sub〉2〈/sub〉RR. However, excessive doping of Ni does not guarantee an increase of photocatalytic CO〈sub〉2〈/sub〉RR due to a diminish of sulfur vacancies. The regulation of sulfur vacancies by Ni doping and their interplay on photocatalytic CO〈sub〉2〈/sub〉RR activity are presented and discussed. This work provides an in-depth insight of the role of dopant on vacancy modulation in photocatalyst beyond light absorption and a guidance for design of the potential photocatalyst for CO〈sub〉2〈/sub〉RR.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉Aqueous colloidal Ni-doped ZnS (ZnS:Ni) nanocrystals were constructed as excellent visible-light-responsive photocatalysts for CO〈sub〉2〈/sub〉RR into formate. The role of Ni dopant in light absorption, charge separation and sulfur vacancies regulation for photocatalytic CO〈sub〉2〈/sub〉RR activity are presented and discussed, providing an in-depth insight for design of the potential photocatalysts for CO〈sub〉2〈/sub〉RR.〈/p〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337318311639-ga1.jpg" width="303" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: 15 May 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 245〈/p〉 〈p〉Author(s): Yang Yang, Chen Zhang, Danlian Huang, Guangming Zeng, Jinhui Huang, Cui Lai, Chengyun Zhou, Wenjun Wang, Hai Guo, Wenjing Xue, Rui Deng, Min Cheng, Weiping Xiong〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Graphitic carbon nitride (g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉) has enormous potential for photocatalysis, but only possesses moderate activity because of excitonic effects and sluggish charge transfer. Herein, metal-free heterostructure photocatalyst constructed by boron nitride quantum dots (BNQDs) and ultrathin porous g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 (UPCN) was successfully developed for overcoming these defects. Results showed that the BNQDs loaded UPCN can simultaneously promote the dissociation of excitons and accelerate the transfer of charges owing to the negatively charged functional groups on the surface of BNQDs as well as the ultrathin and porous nanostructure of g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉. Benefiting from the intensified exciton dissociation and charge transfer, the BNQDs/UPCN (BU) photocatalyst presented superior visible-light-driven molecular oxygen activation ability, such as superoxide radical (〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉O〈sub〉2〈/sub〉〈sup〉−〈/sup〉) generation and hydrogen peroxide (H〈sub〉2〈/sub〉O〈sub〉2〈/sub〉) production. The average 〈sup〉〈img src="https://sdfestaticassets-eu-west-1.sciencedirectassets.com/shared-assets/16/entities/rad"〉〈/sup〉O〈sub〉2〈/sub〉〈sup〉−〈/sup〉 generation rate of the optimal sample (BU-3) was estimated to be 0.25 μmol L〈sup〉−1〈/sup〉 min〈sup〉−1〈/sup〉, which was about 2.3 and 1.6 times than that of bulk g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 and UPCN. Moreover, the H〈sub〉2〈/sub〉O〈sub〉2〈/sub〉 production by BU-3 was also higher than that of bulk g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 (22.77 μmol L〈sup〉−1〈/sup〉) and UPCN (36.13 μmol L〈sup〉−1〈/sup〉), and reached 72.30 μmol L〈sup〉−1〈/sup〉 over 60 min. This work reveals how rational combination of g-C〈sub〉3〈/sub〉N〈sub〉4〈/sub〉 with BNQDs can endow it with improved photocatalytic activity for molecular oxygen activation, and provides a novel metal-free and highly efficient photocatalyst for environmental remediation and energy conversion.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337318312037-ga1.jpg" width="334" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 5 May 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 244〈/p〉 〈p〉Author(s): Mona Kohantorabi, Stefanos Giannakis, Mohammad Reza Gholami, Ling Feng, Cesar Pulgarin〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉In this work, the role of dissolved oxygen in the solar and the photo-Fenton-mediated 〈em〉E. coli〈/em〉 inactivation process was put under scrutiny. The effect of transient species that were produced in the presence of various natural organic matter isolates (NOM), namely Suwannee River (SR) NOM, Nordic Reservoir (NR) NOM, SR Humic acid (SRHA), and SR Fulvic acid (SRFA) was studied in detail. The role of 〈sup〉1〈/sup〉 〈math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="si4.gif" overflow="scroll"〉〈msub〉〈mi〉O〈/mi〉〈mn〉2〈/mn〉〈/msub〉〈/math〉 in this reaction was systematically evaluated by modifying the O〈sub〉2〈/sub〉 concentration (N〈sub〉2〈/sub〉/O〈sub〉2〈/sub〉 purging) and the matrix composition (10, 50, and 100% deuterium oxide (D〈sub〉2〈/sub〉O) v/v). In the presence of NOM, 〈sup〉1〈/sup〉 〈math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="si4.gif" overflow="scroll"〉〈msub〉〈mi〉O〈/mi〉〈mn〉2〈/mn〉〈/msub〉〈/math〉 was generated and the enhancement of 〈em〉E. coli〈/em〉 inactivation rate due to charge transfer from triplet state to molecular oxygen. The comparison between SR and NR NOM showed that for these compounds, triplet state of NOM (〈sup〉3〈/sup〉NOM〈sup〉*〈/sup〉), and 〈sup〉1〈/sup〉 〈math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="si4.gif" overflow="scroll"〉〈msub〉〈mi〉O〈/mi〉〈mn〉2〈/mn〉〈/msub〉〈/math〉 were the more favorable active species in 〈em〉E. coli〈/em〉 inactivation, respectively. Also, the second order rate constants (〈math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="si5.gif" overflow="scroll"〉〈msubsup〉〈mi〉k〈/mi〉〈mrow〉〈mi〉E〈/mi〉〈mo〉.〈/mo〉〈mtext〉 〈/mtext〉〈mi〉c〈/mi〉〈mi〉o〈/mi〉〈mi〉l〈/mi〉〈mi〉i〈/mi〉〈/mrow〉〈mrow〉〈mn〉2〈/mn〉〈mi〉n〈/mi〉〈mi〉d〈/mi〉〈/mrow〉〈/msubsup〉〈/math〉) of 〈em〉E. coli〈/em〉 with 〈sup〉3〈/sup〉NOM〈sup〉*〈/sup〉, and 〈sup〉1〈/sup〉 〈math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="si4.gif" overflow="scroll"〉〈msub〉〈mi〉O〈/mi〉〈mn〉2〈/mn〉〈/msub〉〈/math〉 were calculated by using the steady state approximation. The obtained results showed that the rate values of 〈sup〉1〈/sup〉 〈math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="si4.gif" overflow="scroll"〉〈msub〉〈mi〉O〈/mi〉〈mn〉2〈/mn〉〈/msub〉〈/math〉 related to NR NOM was ∼ 5.6 times higher than SR NOM, while the rate values of 〈sup〉3〈/sup〉NOM〈sup〉*〈/sup〉 for SR NOM was ∼ 8.7 times higher than NR NOM. We also determined the effect of these organic matter isolates in the photo-Fenton process and its constituents (solar/Fe〈sup〉2+〈/sup〉, solar/H〈sub〉2〈/sub〉O〈sub〉2〈/sub〉, and solar/Fe〈sup〉2+〈/sup〉/H〈sub〉2〈/sub〉O〈sub〉2〈/sub〉). In presence of NOM, the photo-Fenton process inactivation rates increased which confirmed that the combined processes has additional pathways generated with disinfecting effect during solar exposure of bacteria.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337318311652-ga1.jpg" width="230" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: 5 May 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 244〈/p〉 〈p〉Author(s): Yamen AlSalka, Luis I. Granone, Wegdan Ramadan, Amer Hakki, Ralf Dillert, Detlef W. Bahnemann〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉The increasing demand for clean renewable energy needed for sustainable industrial progress and population growth is the driving force for the scientific community to achieve a continuous development in the field of photocatalysis and photoelectrochemistry. Nanostructures and nanomaterials have contributed significantly to the field of renewable energy due to their new physicochemical properties. Iron-based nanostructures have considerable advantages like small band gaps, allowing to harvest photons in the visible region of the solar spectrum, abundance, and important physical properties like magnetism and ferroelectricity. But they also have many shortcomings and drawbacks related to stability in the different photocatalytic media, low surface area, conductivity, and fast charge carrier recombination. In this review, the focus is placed on important members of the iron-based photocatalyst family such as, hematite, iron oxy-hydroxide, iron-based perovskites, and spinel ferrites. Also, iron doped titanium dioxide as visible light photocatalysts is covered. Various strategies employed for enhancing the photocatalytic and photoelectrocatalytic performance are discussed. Doping, oxygen vacancies, induced defects and formation of solid solutions seem to be a working strategy to address some of the challenges in photocatalysis and photoelectrocatalysis. Finally, photocatalytic and photoelectrocatalytic applications employing iron-based semiconductors are presented.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337318311676-ga1.jpg" width="243" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: January 2020〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 260〈/p〉 〈p〉Author(s): Wenhao Yang, Zi’ang Su, Zhenghao Xu, Weinan Yang, Yue Peng, Junhua Li〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉The structure-performance relationship of α-, β-, γ- and δ-MnO〈sub〉2〈/sub〉 catalysts were studied. The four samples exhibited different activities of toluene oxidation in terms of distinct tunnel sizes, surface-active oxygen and redox properties. δ-MnO〈sub〉2〈/sub〉 catalyst with K〈sup〉+〈/sup〉 in the mezzanines of its layers presented the highest toluene oxidation activity under a GHSV of 60,000 mL·g〈sup〉−1〈/sup〉 h〈sup〉−1〈/sup〉, as well as good water resistance. HAADF images and EELS results showed that oxygen vacancies preferred to form on δ-MnO〈sub〉2〈/sub〉 lattice with layer stack dislocations via Mn〈sup〉4+〈/sup〉 reduction rather than β-MnO〈sub〉2〈/sub〉 with good crystallization. These inherent-distorted structures with heterocations K〈sup〉+〈/sup〉 improved the emerge-annihilate cycling of oxygen vacancies. In-situ DRIFTS results showed that toluene adsorption was facilitated via rapid dehydrogenation of methyl due to abundant surface adsorbed oxygen on δ-MnO〈sub〉2〈/sub〉. In addition, benzoate, maleic and manganese carbonate on δ-MnO〈sub〉2〈/sub〉 were the key intermediate species during toluene oxidation at relatively low temperatures.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319308975-ga1.jpg" width="295" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: January 2020〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 260〈/p〉 〈p〉Author(s): Long Yang, Guoqiang Li, Jingfa Chang, Junjie Ge, Changpeng Liu, Fateev Vladimir, Guiling Wang, Zhao Jin, Wei Xing〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Uniform sea urchin-like Au@Pd formic acid oxidation reaction (FAOR) electrocatalysts with dendritic core-shell structure were successfully prepared via nanocatalysts self-assembly process. High electrochemical surface area with more exposed active sites as well as the suitable lattice strain were confirmed as influencing factor to enhance intrinsic activity and facilitate kinetic reaction rate, resulting improved FAOR performance. Specifically, as tuning the status of surface dendritic Pd, lattice strain presented different influence on the electrocatalytic performance. Stronger lattice strain would facilitate the surface adsorption of dissociate formic acid on the surface Pd. While, weaker lattice strain would make surface desorption of the intermediate species on surface Pd easily resulting regeneration of active sites. In this work, the optimized Au〈sub〉71〈/sub〉@Pd〈sub〉29〈/sub〉 DCS exhibits enhanced activity with the current density of 1405 A g〈sub〉Pd〈/sub〉〈sup〉−1〈/sup〉, which is 8.8 times higher than that of the commercial Pd black (160 A g〈sub〉Pd〈/sub〉〈sup〉−1〈/sup〉), as well as obvious enhanced durability.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319309476-ga1.jpg" width="500" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: January 2020〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 260〈/p〉 〈p〉Author(s): Junhua Zou, Zhitong Wang, Wei Guo, Binbin Guo, Yan Yu, Ling Wu〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉ZnTi-LDH nanosheets have been synthesized as photocatalysts for selective oxidation of benzyl alcohol (BA) to benzaldehyde (BAD) under visible light irradiation. Based on UV–vis DRS, in-situ FTIR and XPS results, it was revealed that BA would be efficiently chemisorbed and activated on ZnTi-LDH forming the surface coordination species, which contributed to harvesting visible light and induced the photocatalytic reaction. The ESR spectra suggested that oxygen vacancies would be produced in ZnTi-LDHs after the adsorption of BA molecules. More exposed surface OH groups would induce more oxygen vacancies, which would serve as the centers for capturing photoelectrons from the photoexcited surface coordination species and act as active sites for enhanced O〈sub〉2〈/sub〉 adsorption and activation, resulting outstanding photocatalytic activity. Finally, a possible mechanism was proposed to illustrate the photocatalytic process which mediated by surface coordination species formed by the interaction between ZnTi-LDH and BA.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319309324-ga1.jpg" width="200" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: January 2020〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 260〈/p〉 〈p〉Author(s): Kyungmin Im, Donghwi Kim, Jue-Hyuk Jang, Jinsoo Kim, Sung Jong Yoo〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Metal–nitrogen–carbon (M-NC) catalysts have been reported as promising electrocatalysts to replace noble-metal catalysts (Pt/C, Au/C, Ru/C etc.) in many industrial processes. In this regard, carbonized zeolite imidazole frameworks (ZIFs), as precursors of M-NC catalysts, have been extensively studied because of their porosity and ligand composition containing nitrogen and carbon. In this study, we synthesize Co-doped ZnO@ZIF-8 particles from a Co-doped ZnO sphere via the spray pyrolysis method and pseudomorphic replication. Ultrasonic spray pyrolysis is an attractive approach to operate mass production with high-purity homogeneous structures. Further, pseudomorphic replication makes it possible to control the morphology of the metal–organic framework (MOF) particles and easily prepare MOF composite particles. In the study, the pyrolyzed ZIF particles are applied to oxygen reduction reactions in alkaline media, and our results indicate that particles show a high half-wave potential of 0.904 V, which makes them suitable for diverse electrochemical applications.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319309397-ga1.jpg" width="276" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: January 2020〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 260〈/p〉 〈p〉Author(s): Reza Vakili, Rahman Gholami, Cristina E. Stere, Sarayute Chansai, Huanhao Chen, Stuart M. Holmes, Yilai Jiao, Christopher Hardacre, Xiaolei Fan〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Plasma-assisted dry reforming of methane (DRM) was performed in a dielectric barrier discharge (DBD) reactor. The effect of different packing materials including ZrO〈sub〉2〈/sub〉, UiO-67 MOF and PtNP@UiO-67 on plasma discharge was investigated, showing that ZrO〈sub〉2〈/sub〉 suppressed the plasma generation while UiO-67 improves it due to its porous nature which favours the formation of filamentary microdischarges and surface discharges. The improved plasma discharge increased the conversion of CH〈sub〉4〈/sub〉 and CO〈sub〉2〈/sub〉 by about 18% and 10%, respectively, compared to the plasma-alone mode. In addition, the distribution of hydrocarbon products changed from dominant C〈sub〉2〈/sub〉H〈sub〉6〈/sub〉 in the plasma-alone mode to C〈sub〉2〈/sub〉H〈sub〉2〈/sub〉 and C〈sub〉2〈/sub〉H〈sub〉4〈/sub〉 in the UiO-67 promoted plasma-assisted DRM. The UiO-67 MOF was stable in plasma, showing no significant changes in its properties under different treatment times, discharge powers and gases. Pt nanoparticles (NPs) on UiO-67 improved plasma-assisted DRM, especially the selectivity due to the presence of surface reactions. Due to the dehydrogenation of hydrocarbons over Pt NPs, the selectivity to hydrocarbons decreased by 30%, compared to the UiO-67 packing. 〈em〉In situ〈/em〉 diffuse reflectance infrared Fourier transformed spectroscopy (DRIFTS) was carried out to probe the surface reactions on PtNP@UiO-67 catalyst, showing the decomposition of surface formats to CO and C〈sub〉2〈/sub〉H〈sub〉4〈/sub〉 dehydrogenation over the metallic Pt. The PtNP@UiO-67 catalyst showed good reusability in the plasma-assisted DRM, and H〈sub〉2〈/sub〉 production was improved by high CH〈sub〉4〈/sub〉/CO〈sub〉2〈/sub〉 molar ratio and low feed flow rate.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319309427-ga1.jpg" width="343" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: Available online 14 September 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental〈/p〉 〈p〉Author(s): Xiaohu Luo, Shuo Du, Chengliang Zhou, Deshuai Zhen, Bo Chen, Ji Li, Qian Wu, Yoshyikazcu Iro, Dongchu Chen, Yali Liu〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Herein, we report a rational design of one-dimension (1D) porous hybrid heterostructures with the active HER (Mo〈sub〉2〈/sub〉C) and OER (Co〈sub〉4〈/sub〉S〈sub〉3〈/sub〉) embedded N and S co-doped carbon (Co〈sub〉4〈/sub〉S〈sub〉3〈/sub〉/Mo〈sub〉2〈/sub〉C-NSC) for the effective overall water splitting. Spectroscopic characterizations reveals that modulated electronic state behaviors are generated by the strong chemical couplings at the nanointerface which triggers the charge from Co〈sup〉2+〈/sup〉 to Mo〈sup〉4+〈/sup〉/Mo〈sup〉6+〈/sup〉 through the interfacial Mo-S-Co bond, resulting in producing the considerable amounts of the active sites (i.e., Co〈sup〉3+〈/sup〉, Mo〈sup〉2+〈/sup〉, and Mo〈sup〉3+〈/sup〉) for the HER and OER in the hybrid heterostructures. Interestingly, Co〈sub〉4〈/sub〉S〈sub〉3〈/sub〉/Mo〈sub〉2〈/sub〉C-NSC shows pronounced synergistic effects in electrocatalytic activity for the HER and OER. When Co〈sub〉4〈/sub〉S〈sub〉3〈/sub〉/Mo〈sub〉2〈/sub〉C-NSC is used as both anode and cathode for overall water splitting, a low cell voltage of 1.62 eV is generated at 10 mA cm〈sup〉-2〈/sup〉. The interesting work highlights the significance of optimization electronic structure based on transition metal-based bifunctional electrocatalysts for the HER and OER.〈/p〉〈/div〉 〈h5〉Graphical Abstract〈/h5〉 〈div〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319309440-ga1.jpg" width="301" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈p〉Co〈sub〉4〈/sub〉S〈sub〉3〈/sub〉/Mo〈sub〉2〈/sub〉C-NSC hybrid heterostructures exhibit the outsanding electrocatalytic activity for the HER and OER.〈/p〉 〈/div〉

Description: 〈p〉Publication date: January 2020〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 260〈/p〉 〈p〉Author(s): Guang Liu, Muheng Wang, Yun Wu, Na Li, Fei Zhao, Qiang Zhao, Jinping Li〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Three-dimensional (3D) self-supporting porous network NiCeO〈sub〉x〈/sub〉@NiFeO〈sub〉x〈/sub〉 electrocatalyst on Ni foam (denotes as NiCe@NiFe/NF-N) is prepared by a simple two step electrodepositing process. NiCe@NiFe/NF-N attains 100 mA/cm〈sup〉2〈/sup〉 at overpotential of 254 mV with Tafel slope of 59.9 mV/dec, which is much lower than that of NiCe@NiFe/NF-P, NiFe@NF, NiCe@NF and also commercial RuO〈sub〉2〈/sub〉 electrocatalysts. Furthermore, the obtained NiCe@NiFe/NF-N electrocatalyst only needs overpotential of 359 mV to deliver high current densities of 1 A/cm〈sup〉2〈/sup〉 and demonstrates excellent stability at such large current densities for 20 h, which is also superior to that of NiCe@NiFe/NF-P electrocatalyst. Further study reveals that the enhanced water oxidation performance of NiCe@NiFe/NF-N electrocatalyst with good stability at high current densities could be attributed to the optimal surface and electronic structures, fast reaction kinetics and high intrinsic catalytic activity. Collectively, such electrocatalyst paves new opportunities for development of low-cost water oxidation electrocatalysts with high current densities for practical water splitting applications.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉Taking advantage of the synergistic effects between NiCeO〈sub〉x〈/sub〉 and NiFeO〈sub〉x〈/sub〉, the 3D porous network heterostructure NiCe@NiFe electrocatalyst demonstrated excellent oxygen evolution reaction activities at high current densities towards water splitting.〈/p〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319309464-ga1.jpg" width="284" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: January 2020〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental, Volume 260〈/p〉 〈p〉Author(s): Wenzheng Cheng, Pengfei Yuan, Zirui Lv, Yingying Guo, Yueyang Qiao, Xiaoyi Xue, Xin Liu, Wenlong Bai, Kaixue Wang, Qun Xu, Jianan Zhang〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Experimental and computational studies show that topological defect and FeN〈sub〉4〈/sub〉 site in carbon materials would deliver high performances for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Either defect or FeN〈sub〉4〈/sub〉 site attracts numerous discussion, however, the synergetic effect between them is hardly explored. Herein, we design a facial strategy to synthesize N,P-doped defective carbon nanosheets first (N,P-DC), then cover doped sites with well-define metal-N〈sub〉4〈/sub〉 macrocyclic molecules (FePc@N,P-DC) through non-pyrolysis process. The defective carbon boosts the high spin state of Fe center, thus brings superior ORR performances with the half-wave potential of 0.903 V and excellent cycling-life stability in alkaline media. Theoretical calculations show that the overpotential of FePc@N,P-DC for ORR is 0.52 V, much lower than 0.80 V (N,P-DC). Interestingly, the OER activity is simultaneously improved. This metal-Pc@defective carbon hybrid opens a door to develop electrocatalysts combining atomically metal-N〈sub〉4〈/sub〉 sites with topological defect towards diverse energy conversion type.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉We design a facial and efficient strategy to synthesize N,P-doped defective carbon nanosheets first (N,P-DC), and then cover doped sites with well-define metal-N〈sub〉4〈/sub〉 organic macrocyclic molecules (FePc@N,P-DC) through non-pyrolysis process. The catalyst presents superior ORR and OER activity and stability.〈/p〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319309452-ga1.jpg" width="385" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉

Description: 〈p〉Publication date: Available online 4 November 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental〈/p〉 〈p〉Author(s): Bo Peng, Kenneth G. Rappé, Yanran Cui, Feng Gao, János Szanyi, Matthew J. Olszta, Eric D. Walter, Yong Wang, Jamie D. Holladay, Randal A. Goffe〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉ZrO〈sub〉2〈/sub〉 is introduced as a secondary phase to Cu-SSZ-13 via different approaches and tested for the NH〈sub〉3〈/sub〉-SCR reaction. It is shown that the vicinity between the two catalyst phases, i.e., ZrO〈sub〉2〈/sub〉 dispersion, influences interaction between copper oxide (CuO〈sub〉x〈/sub〉) on Cu-SSZ-13 and ZrO〈sub〉2〈/sub〉. A strong interaction is achieved when ZrO〈sub〉2〈/sub〉 is formed with high dispersion on Cu-SSZ-13, and leads to the chemical interaction of CuO〈sub〉x〈/sub〉 and ZrO〈sub〉2〈/sub〉 in hydrothermally aged catalysts. The result is formation of a Cu-stabilized t-ZrO〈sub〉2〈/sub〉 phase which greatly hinders the non-selective NH〈sub〉3〈/sub〉 oxidation due to CuO〈sub〉x〈/sub〉. With reduced ZrO〈sub〉2〈/sub〉 dispersion and less Cu-SSZ-13 and ZrO〈sub〉2〈/sub〉 interaction, the beneficial role of ZrO〈sub〉2〈/sub〉 is diminished. This strategy of CuO〈sub〉x〈/sub〉 passivation is able to significantly enhance the high-temperature selectivity of the state-of-the-art NH〈sub〉3〈/sub〉-SCR catalytic system while mitigating the adverse impact of CuO〈sub〉x〈/sub〉 clusters on the zeolite, potentially enabling higher Cu-content SCR catalysts and improved low-temperature activity.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319311051-ga1.jpg" width="301" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉〈/div〉

Description: 〈p〉Publication date: Available online 4 November 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental〈/p〉 〈p〉Author(s): Guoxia Jiang, Xin Zhang, Fenglian Zhang, Zizhong Liu, Zhuo Wang, Zhengping Hao, Caihong Lin〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉Simultaneous recovery of hydrogen and sulfur resources from acidic gas hydrogen sulfide (H〈sub〉2〈/sub〉S), whose content may reach 20-100% after hydrodesulfurization in oil refineries, is increasingly attractive. Nowadays, the widespread utilization of H〈sub〉2〈/sub〉S decomposition technology is mainly restricted by the low hydrogen and sulfur yield, ie 20% at 800 °C. In this work, for the first time a novel non-sulfide based LaFe〈sub〉x〈/sub〉Al〈sub〉12-x〈/sub〉O〈sub〉19〈/sub〉 hexaaluminate catalysts was used for high (50%) hydrogen yield at 800 °C. At the same time, the active phases and reaction mechanism were confirmed by various characterization techniques. The XRD, Raman, XPS, Mössbauer and XAFS results verified that the Fe species in the hexaaluminate structure, especially octahedral-coordinated Fe〈sup〉3+〈/sup〉, served as the main active phases. The reaction routes/mechanism for H〈sub〉2〈/sub〉S decomposition were also verified by density functional theory (DFT) method. H〈sub〉2〈/sub〉S was firstly adsorbed on the active sites and then completed the decomposition by direct dehydrogenation mechanism. Briefly, current study has minimized the challenges for H〈sub〉2〈/sub〉S decomposition at industrial scale. It is anticipated that our findings will offer potential application of H〈sub〉2〈/sub〉S decomposing technology.〈/p〉〈/div〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0926337319311002-ga1.jpg" width="301" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈p〉H〈sub〉2〈/sub〉S decomposed by a new direct dehydrogenation mechanism and 50% H〈sub〉2〈/sub〉 yield could be attained. The Fe species presented in the hexaaluminate structure, especially octahedral-coordinated Fe〈sup〉3+〈/sup〉, behaved as the main active phases. And H〈sub〉2〈/sub〉S was firstly adsorbed on the active sites and then completed the decomposition by direct dehydrogenation mechanism.〈/p〉 〈/div〉

Description: 〈p〉Publication date: Available online 4 November 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Catalysis B: Environmental〈/p〉 〈p〉Author(s): Andreina Alarcón, Jordi Guilera, Rodrigo Soto, Teresa Andreu〈/p〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉This study investigates the deactivation mechanism of CeO〈sub〉2〈/sub〉-promoted catalyst for the CO〈sub〉2〈/sub〉 methanation reaction. The catalytic performance was evaluated at high temperature (T = 500 °C, P = 5 bar·g) and under the presence of unfavourable H〈sub〉2〈/sub〉S impurities (1-5 ppm). The thermal stability of the CeO〈sub〉2〈/sub〉-promoted catalyst was excellent, while the non-promoted sample suffered from nickel sintering. In contrast, the presence of H〈sub〉2〈/sub〉S was detrimental for both catalysts. The tolerance to H〈sub〉2〈/sub〉S of CeO〈sub〉2〈/sub〉-promoted sample was higher; keeping one third of the initial catalytic activity under continuous addition of H〈sub〉2〈/sub〉S. The identification of crystallographic planes associated with Ce〈sub〉2〈/sub〉O〈sub〉2〈/sub〉S phase (HRSTEM) evidenced that the addition of CeO〈sub〉2〈/sub〉 to nickel catalyst minimized the formation of non-active NiS sites. This finding was further confirmed through DRIFT spectroscopy since for the Ni-CeO〈sub〉2〈/sub〉/γ-Al〈sub〉2〈/sub〉O〈sub〉3〈/sub〉, methane formation derived from formate dissociation was followed by hydrogenation of the adsorbed CO on the remaining available active sites.〈/p〉〈/div〉