Mechanistic insights into chemical and photochemical transformations of bismuth vanadate photoanodes

Francesca M. Toma (), Jason K. Cooper, Viktoria Kunzelmann, Matthew T. McDowell, Jie Yu, David M. Larson, Nicholas J. Borys, Christine Abelyan, Jeffrey W. Beeman, Kin Man Yu, Jinhui Yang, Le Chen, Matthew R. Shaner, Joshua Spurgeon, Frances A. Houle, Kristin A. Persson and Ian D. Sharp ()
Additional contact information
Francesca M. Toma: Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory
Jason K. Cooper: Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory
Viktoria Kunzelmann: Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory
Matthew T. McDowell: Joint Center for Artificial Photosynthesis, California Institute of Technology
Jie Yu: Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory
David M. Larson: Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory
Nicholas J. Borys: Molecular Foundry, Lawrence Berkeley National Laboratory
Christine Abelyan: Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory
Jeffrey W. Beeman: Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory
Kin Man Yu: Lawrence Berkeley National Laboratory
Jinhui Yang: Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory
Le Chen: Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory
Matthew R. Shaner: Joint Center for Artificial Photosynthesis, California Institute of Technology
Joshua Spurgeon: Joint Center for Artificial Photosynthesis, California Institute of Technology
Frances A. Houle: Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory
Kristin A. Persson: Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory
Ian D. Sharp: Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory

Nature Communications, 2016, vol. 7, issue 1, 1-11

Abstract: Abstract Artificial photosynthesis relies on the availability of semiconductors that are chemically stable and can efficiently capture solar energy. Although metal oxide semiconductors have been investigated for their promise to resist oxidative attack, materials in this class can suffer from chemical and photochemical instability. Here we present a methodology for evaluating corrosion mechanisms and apply it to bismuth vanadate, a state-of-the-art photoanode. Analysis of changing morphology and composition under solar water splitting conditions reveals chemical instabilities that are not predicted from thermodynamic considerations of stable solid oxide phases, as represented by the Pourbaix diagram for the system. Computational modelling indicates that photoexcited charge carriers accumulated at the surface destabilize the lattice, and that self-passivation by formation of a chemically stable surface phase is kinetically hindered. Although chemical stability of metal oxides cannot be assumed, insight into corrosion mechanisms aids development of protection strategies and discovery of semiconductors with improved stability.

Date: 2016
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DOI: 10.1038/ncomms12012

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