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Intro to special issue artificial photosynthesis [Introductions] (2012)

Concepcion, J. J., House, R. L., Papanikolas, J. M., Meyer, T. J.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: In the early 1970s, the works by Fujishima and Honda (1) and Honda et al. (2) reported on the results of a now famous experiment. They showed that band gap excitation of anatase TiO2 in a photoelectrochemical cell with a Pt counter electrode and an applied bias resulted in water...

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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Narrow the gap of water oxidation to PS II [Chemistry] (2012)

Duan, L., Araujo, C. M., Ahlquist, M. S. G., Sun, L.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: Water oxidation catalysts are essential components of light-driven water splitting systems, which could convert water to H2 driven by solar radiation (H2O + hν → 1/2O2 + H2). The oxidation of water (H2O → 1/2O2 + 2H+ + 2e-) provides protons and electrons for the production of dihydrogen (2H+ + 2e- → H2), a clean-burning and high-capacity energy carrier. One of the obstacles now is the...

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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Photocatalytic CO2 reduction to formic acid [Chemistry] (2012)

Tamaki, Y., Morimoto, T., Koike, K., Ishitani, O.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: Previously undescribed supramolecules constructed with various ratios of two kinds of Ru(II) complexes—a photosensitizer and a catalyst—were synthesized. These complexes can photocatalyze the reduction of CO2 to formic acid with high selectivity and durability using a wide range of wavelengths of visible light and NADH model compounds as electron donors...

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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Step-by-step self-assembled hybrids that feature control over energy and charge transfer [Chemistry] (2012)

Grimm, B., Schornbaum, J., Jasch, H., Trukhina, O., Wessendorf, F., Hirsch, A., Torres, T., Guldi, D. M.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: In the current work, we have documented the use of two complementary supramolecular motifs, namely multipoint hydrogen bonding and metal complexation, as a means to control the step-by-step assembly of a panchromatically absorbing and highly versatile solar energy conversion system. On one hand, two different perylenediimides (1a/1b) have been integrated...

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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Long-lived ET state in nanosized silica-alumina [Chemistry] (2012)

Fukuzumi, S., Doi, K., Itoh, A., Suenobu, T., Ohkubo, K., Yamada, Y., Karlin, K. D.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: A simple donor-acceptor linked dyad, 9-mesityl-10-methylacridinium ion (Acr+-Mes) was incorporated into nanosized mesoporous silica-alumina to form a composite, which in acetonitrile is highly dispersed. In this medium, upon visible light irradiation, the formation of an extremely long-lived electron-transfer state (Acr•-Mes•+) was confirmed by EPR and laser flash photolysis spectroscopic methods....

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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Photodriven oxidation of a water-oxidation catalyst [Chemistry] (2012)

Vagnini, M. T., Smeigh, A. L., Blakemore, J. D., Eaton, S. W., Schley, N. D., D'Souza, F., Crabtree, R. H., Brudvig, G. W., Co, D. T., Wasielewski, M. R.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: Photodriving the activity of water-oxidation catalysts is a critical step toward generating fuel from sunlight. The design of a system with optimal energetics and kinetics requires a mechanistic understanding of the single-electron transfer events in catalyst activation. To this end, we report here the synthesis and photophysical characterization of two...

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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Calculation of thermodynamic hydricities [Chemistry] (2012)

Muckerman, J. T., Achord, P., Creutz, C., Polyansky, D. E., Fujita, E.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: We have developed a correlation between experimental and density functional theory-derived results of the hydride-donating power, or “hydricity”, of various ruthenium, rhenium, and organic hydride donors. This approach utilizes the correlation between experimental hydricity values and their corresponding calculated free-energy differences between the hydride donors and their conjugate acceptors in...

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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Cobalt-dithiolene complexes for proton reduction. [Chemistry] (2012)

Mc; Namara, W. R., Han, Z., Yin, C.-J., Brennessel, W. W., Holland, P. L., Eisenberg, R.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: Artificial photosynthesis (AP) is a promising method of converting solar energy into fuel (H2). Harnessing solar energy to generate H2 from H+ is a crucial process in systems for artificial photosynthesis. Widespread application of a device for AP would rely on the use of platinum-free catalysts due to the scarcity...

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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Visible light generation of I-I bonds [Chemistry] (2012)

Farnum, B. H., Jou, J. J., Meyer, G. J.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: Seven Ru-tris(diimine) compounds were prepared to study the photooxidation of iodide. Iodide oxidation results in the formation of I–I bonds, and it is therefore relevant to the conversion and storage of solar energy. Iodide oxidation is also a key step for electrical power generation in dye-sensitized solar cells. The mechanistic...

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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Splitting CO2 into CO and O2 by a single catalyst [Chemistry] (2012)

Chen, Z., Concepcion, J. J., Brennaman, M. K., Kang, P., Norris, M. R., Hoertz, P. G., Meyer, T. J.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: The metal complex [(tpy)(Mebim-py)RuII(S)]2+ (tpy = 2,2′ : 6′,2′′-terpyridine; Mebim-py = 3-methyl-1-pyridylbenzimidazol-2-ylidene; S = solvent) is a robust, reactive electrocatalyst toward both water oxidation to oxygen and carbon dioxide reduction to carbon monoxide. Here we describe its use as a single electrocatalyst for CO2 splitting, CO2 → CO + 1/2 O2, in a two-compartment electrochemical cell.

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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Water splitting in dye-sensitized solar cells [Chemistry] (2012)

Zhao, Y., Swierk, J. R., Megiatto, J. D., Sherman, B., Youngblood, W. J., Qin, D., Lentz, D. M., Moore, A. L., Moore, T. A., Gust, D., Mallouk, T. E.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: Photoelectrochemical water splitting directly converts solar energy to chemical energy stored in hydrogen, a high energy density fuel. Although water splitting using semiconductor photoelectrodes has been studied for more than 40 years, it has only recently been demonstrated using dye-sensitized electrodes. The quantum yield for water splitting in these dye-based systems...

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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Mimicking PS II electron transfer [Chemistry] (2012)

Megiatto, J. D., Antoniuk-Pablant, A., Sherman, B. D., Kodis, G., Gervaldo, M., Moore, T. A., Moore, A. L., Gust, D.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: In the photosynthetic photosystem II, electrons are transferred from the manganese-containing oxygen evolving complex (OEC) to the oxidized primary electron-donor chlorophyll P680•+ by a proton-coupled electron transfer process involving a tyrosine-histidine pair. Proton transfer from the tyrosine phenolic group to a histidine nitrogen positions the redox potential of the tyrosine...

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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H2 evolution: [Ni(P2N2)2]2+ in acidic ionic liq./H2O [Chemistry] (2012)

Pool, D. H., Stewart, M. P., O'Hagan, M., Shaw, W. J., Roberts, J. A. S., Bullock, R. M., Du; Bois, D. L.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: The electrocatalytic reduction of protons to H2 by (where in the highly acidic ionic liquid dibutylformamidium bis(trifluoromethanesulfonyl)amide shows a strong dependence on added water. A turnover frequency of 43,000–53,000 s-1 has been measured for hydrogen production at 25 °C when the mole fraction of water (χH2O) is 0.72. The same catalyst in...

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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Insights into proton-coupled electron transfer mechanisms of electrocatalytic H2 oxidation and production [Chemistry] (2012)

Horvath, S., Fernandez, L. E., Soudackov, A. V., Hammes-Schiffer, S.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: The design of molecular electrocatalysts for H2 oxidation and production is important for the development of alternative renewable energy sources that are abundant, inexpensive, and environmentally benign. Recently, nickel-based molecular electrocatalysts with pendant amines that act as proton relays for the nickel center were shown to effectively catalyze H2 oxidation...

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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Power curves for artificial leaves [Chemistry] (2012)

Surendranath, Y., Bediako, D. K., Nocera, D. G.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: An artificial leaf can perform direct solar-to-fuels conversion. The construction of an efficient artificial leaf or other photovoltaic (PV)-photoelectrochemical device requires that the power curve of the PV material and load curve of water splitting, composed of the catalyst Tafel behavior and cell resistances, be well-matched near the thermodynamic potential...

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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Artificial photosynthesis of CO [Chemistry] (2012)

Smieja, J. M., Benson, E. E., Kumar, B., Grice, K. A., Seu, C. S., Miller, A. J. M., Mayer, J. M., Kubiak, C. P.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: The effective design of an artificial photosynthetic system entails the optimization of several important interactions. Herein we report stopped-flow UV-visible (UV-vis) spectroscopy, X-ray crystallographic, density functional theory (DFT), and electrochemical kinetic studies of the Re(bipy-tBu)(CO)3(L) catalyst for the reduction of CO2 to CO. A remarkable selectivity for CO2 over H+...

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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Catalytic mechanism for water oxidation [Chemistry] (2012)

Lin, X., Hu, X., Concepcion, J. J., Chen, Z., Liu, S., Meyer, T. J., Yang, W.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: Water oxidation is a linchpin in solar fuels formation, and catalysis by single-site ruthenium complexes has generated significant interest in this area. Combining several theoretical tools, we have studied the entire catalytic cycle of water oxidation for a single-site catalyst starting with [RuII(tpy)(bpm)(OH2)]2+ (i.e., [RuII-OH2]2+; tpy is 2,2′∶6′,2′′-terpyridine and bpm...

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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Catalytic hydrogen evolution [Chemistry] (2012)

Valdez, C. N., Dempsey, J. L., Brunschwig, B. S., Winkler, J. R., Gray, H. B.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: A dicobaloxime in which monomeric Co(III) units are linked by an octamethylene bis(glyoxime) catalyzes the reduction of protons from p-toluenesulfonic acid as evidenced by electrocatalytic waves at -0.4 V vs. the saturated calomel electrode (SCE) in acetonitrile solutions. Rates of hydrogen evolution were determined from catalytic current peak heights (kapp = 1100 ± 70 M-1 s-1). Electrochemical...

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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Charge carrier dynamics in hematite photoanodes [Chemistry] (2012)

Barroso, M., Mesa, C. A., Pendlebury, S. R., Cowan, A. J., Hisatomi, T., Sivula, K., Gratzel, M., Klug, D. R., Durrant, J. R.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: This paper addresses the origin of the decrease in the external electrical bias required for water photoelectrolysis with hematite photoanodes, observed following surface treatments of such electrodes. We consider two alternative surface modifications: a cobalt oxo/hydroxo-based (CoOx) overlayer, reported previously to function as an efficient water oxidation electrocatalyst, and a...

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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Mass transport in Si wire-array photoelectrodes [Chemistry] (2012)

Xiang, C., Meng, A. C., Lewis, N. S.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: Physical integration of a Ag electrical contact internally into a metal/substrate/microstructured Si wire array/oxide/Ag/electrolyte photoelectrochemical solar cell has produced structures that display relatively low ohmic resistance losses, as well as highly efficient mass transport of redox species in the absence of forced convection. Even with front-side illumination, such wire-array based...

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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Photosystems by ruthenium oxo and native systems [Chemistry] (2012)

Tanaka, K., Isobe, H., Yamanaka, S., Yamaguchi, K.

National Academy of Sciences

In: PNAS - Proceedings of the National Academy of Sciences

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Publication Date: 2012-09-26

Description: The nature of chemical bonds of ruthenium(Ru)–quinine(Q) complexes, mononuclear [Ru(trpy)(3,5-t-Bu2Q)(OH2)](ClO4)2 (trpy = 2,2′:6′,2′′-terpyridine, 3,5-di-tert-butyl-1,2-benzoquinone) (1), and binuclear [Ru2(btpyan)(3,6-di-Bu2Q)2(OH2)]2+ (btpyan = 1,8-bis(2,2′:6′,2′′-terpyrid-4′-yl)anthracene, 3,6-t-Bu2Q = 3,6-di-tert-butyl-1,2-benzoquinone) (2), has been investigated by broken-symmetry (BS) hybrid density functional (DFT) methods. BS DFT computations for the Ru complexes have elucidated that the closed-shell structure (2b) Ru(II)–Q complex is less stable than...

Keywords: Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature

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