1. How Light-Harvesting Semiconductors Can Alter the Bias of Reversible Electrocatalysts in Favor of H 2 Production and CO 2 Reduction
- Author
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Yatendra S. Chaudhary, Vincent Wang, Thomas W. Woolerton, Sophie Bell, Stephen W. Ragsdale, Juan C. Fontecilla-Camps, Mehmet Can, Andreas Bachmeier, Fraser A. Armstrong, Inorganic Chemistry Laboratory [Oxford], University of Oxford, Institut de biologie structurale (IBS - UMR 5075 ), Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), University of Oxford [Oxford], Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)
- Subjects
Models, Molecular ,MESH: Aldehyde Oxidoreductases ,MESH: Oxidation-Reduction ,Light ,Protein Conformation ,Photochemistry ,Electrocatalyst ,Electrochemistry ,MESH: Carbon Dioxide ,MESH: Multienzyme Complexes ,7. Clean energy ,01 natural sciences ,Biochemistry ,Colloid and Surface Chemistry ,MESH: Protein Conformation ,Biomimetics ,Photosynthesis ,MESH: Photosynthesis ,biology ,[SDV.BBM.BS]Life Sciences [q-bio]/Biochemistry, Molecular Biology/Structural Biology [q-bio.BM] ,Chemistry ,MESH: Hydrogen ,Aldehyde Oxidoreductases ,MESH: Hydrogenase ,Electrode ,Oxidation-Reduction ,MESH: Models, Molecular ,Carbon monoxide dehydrogenase ,010402 general chemistry ,Redox ,Article ,Catalysis ,Hydrogenase ,Multienzyme Complexes ,MESH: Electrochemistry ,010405 organic chemistry ,business.industry ,General Chemistry ,Carbon Dioxide ,Solar fuel ,MESH: Catalysis ,MESH: Light ,0104 chemical sciences ,Semiconductor ,Semiconductors ,MESH: Biomimetics ,MESH: Semiconductors ,biology.protein ,business ,Hydrogen - Abstract
International audience; The most efficient catalysts for solar fuel production should operate close to reversible potentials, yet possess a bias for the fuel-forming direction. Protein film electrochemical studies of Ni-containing carbon monoxide dehydrogenase and [NiFeSe]-hydrogenase, each a reversible electrocatalyst, show that the electronic state of the electrode strongly biases the direction of electrocatalysis of CO2/CO and H(+)/H2 interconversions. Attached to graphite electrodes, these enzymes show high activities for both oxidation and reduction, but there is a marked shift in bias, in favor of CO2 or H(+) reduction, when the respective enzymes are attached instead to n-type semiconductor electrodes constructed from CdS and TiO2 nanoparticles. This catalytic rectification effect can arise for a reversible electrocatalyst attached to a semiconductor electrode if the electrode transforms between semiconductor- and metallic-like behavior across the same narrow potential range (
- Published
- 2013
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