Towards a Molecular Level Understanding of the Multi-Electron Catalysis of Water Oxidation on Metal Oxide Surfaces

Zhang, Miao; Frei, Heinz

doi:10.1007/s10562-014-1437-8

Title: Towards a Molecular Level Understanding of the Multi-Electron Catalysis of Water Oxidation on Metal Oxide Surfaces

Journal Article · Sun Nov 23 00:00:00 EST 2014 · Catalysis Letters

DOI:https://doi.org/10.1007/s10562-014-1437-8· OSTI ID:1511411

Zhang, Miao ^[1]; Frei, Heinz ^[1]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Earth abundant metal oxides play a central role as catalysts in the essential chemical transformations of sunlight to fuel conversion, which are the oxidation of water and the reduction of carbon dioxide. The rapidly growing interest in renewable fuel generation by using the energy of the sun has recently led to substantial breakthroughs in the use of first row transition metal oxides as catalysts for oxygen evolution from water. Substantive improvements of rates and lowering of overpotentials have been achieved by exploiting materials properties on the nanoscale, or taking advantage of the synergy of multiple metals. Moreover, knowledge derived from mechanistic investigations with structure specific spectroscopy is accelerating efficiency improvements. Monitoring by time-resolved FT-infrared spectroscopy reveals the molecular nature of active sites, while in situ X-ray and optical spectroscopy under reaction conditions provides insights into the electronic structure of the surface metal centers participating in the catalysis. By combining the bond specificity of vibrational spectroscopy with the metal electronic structure specificity of optical, X-ray absorption or photoelectron spectroscopy, a complete understanding of active surface sites on metal oxides begins to emerge. Charge flow driving the chemical transformations probed by optical spectroscopy across time scales from ultrafast to very slow reveals the processes that control the productive use of charges delivered to the catalyst. Coupling of the water oxidation catalysis at a metal oxide catalyst with carbon dioxide reduction at a heterobinuclear chromophore, which is the goal of the artificial photosystem approach, is demonstrated by a well-defined all-inorganic polynuclear unit.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

DOE Contract Number:: AC02-05CH11231

OSTI ID:: 1511411

Journal Information:: Catalysis Letters, Vol. 145, Issue 1; ISSN 1011-372X

Publisher:: Springer

Country of Publication:: United States

Language:: English

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Coupling carbon dioxide reduction with water oxidation in nanoscale photocatalytic assemblies

Journal Article · Thu Apr 28 00:00:00 EDT 2016 · Chemical Society Reviews · OSTI ID:1511411

Kim, Wooyul; McClure, Beth Anne; Edri, Eran; +1 more

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Journal Article · Wed Jan 23 00:00:00 EST 2019 · Journal of Chemical Physics · OSTI ID:1511411

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
heterogeneous catalysis
photocatalysis
water oxidation
spectroscopy
surface reaction kinetics
oxide supports

Title: Towards a Molecular Level Understanding of the Multi-Electron Catalysis of Water Oxidation on Metal Oxide Surfaces

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