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〉