Toward Photochemical Water Splitting Using Band-Gap-Narrowed Semiconductors and Transition-Metal Based Molecular Catalysts

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We are carrying out coordinated theoretical and experimental studies of toward photochemical water splitting using band-gap-narrowed semiconductors (BGNSCs) with attached multi-electron molecular water oxidation and hydrogen production catalysts. We focus on the coupling between the materials properties and the H{sub 2}O redox chemistry, with an emphasis on attaining a fundamental understanding of the individual elementary steps in the following four processes: (1) Light-harvesting and charge-separation of stable oxide or oxide-derived semiconductors for solar-driven water splitting, including the discovery and characterization of the behavior of such materials at the aqueous interface; (2) The catalysis of the four-electron water oxidation by dinuclear ... continued below

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233 - 238

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Muckerman,J.T.; Rodriguez, J.A. & Fujita, E. June 7, 2009.

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We are carrying out coordinated theoretical and experimental studies of toward photochemical water splitting using band-gap-narrowed semiconductors (BGNSCs) with attached multi-electron molecular water oxidation and hydrogen production catalysts. We focus on the coupling between the materials properties and the H{sub 2}O redox chemistry, with an emphasis on attaining a fundamental understanding of the individual elementary steps in the following four processes: (1) Light-harvesting and charge-separation of stable oxide or oxide-derived semiconductors for solar-driven water splitting, including the discovery and characterization of the behavior of such materials at the aqueous interface; (2) The catalysis of the four-electron water oxidation by dinuclear hydroxo transition-metal complexes with quinonoid ligands, and the rational search for improved catalysts; (3) Transfer of the design principles learned from the elucidation of the DuBois-type hydrogenase model catalysts in acetonitrile to the rational design of two-electron hydrogen production catalysts for aqueous solution; (4) Combining these three elements to examine the function of oxidation catalysts on BGNSC photoanode surfaces and hydrogen production catalysts on cathode surfaces at the aqueous interface to understand the challenges to the efficient coupling of the materials functions.

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233 - 238

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  • The 31st DOE Solar Photochemistry Research Conference; Annapolis, MD; 20090607 through 20090610

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  • Report No.: BNL--90202-2009-CP
  • Grant Number: DE-AC02-98CH10886
  • Office of Scientific & Technical Information Report Number: 970420
  • Archival Resource Key: ark:/67531/metadc926020

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  • June 7, 2009

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  • Nov. 13, 2016, 7:26 p.m.

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  • Dec. 12, 2016, 8:36 p.m.

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Muckerman,J.T.; Rodriguez, J.A. & Fujita, E. Toward Photochemical Water Splitting Using Band-Gap-Narrowed Semiconductors and Transition-Metal Based Molecular Catalysts, article, June 7, 2009; United States. (digital.library.unt.edu/ark:/67531/metadc926020/: accessed October 20, 2017), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.