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Journal Article
Research Support, Non-U.S. Gov't
A Stable, Narrow-Gap Oxyfluoride Photocatalyst for Visible-Light Hydrogen Evolution and Carbon Dioxide Reduction.
Journal of the American Chemical Society 2018 May 31
Mixed anion compounds such as oxynitrides and oxychalcogenides are recognized as potential candidates of visible-light-driven photocatalysts since, as compared with oxygen 2p orbitals, p orbitals of less electronegative anion (e.g., N3- , S2- ) can form a valence band that has more negative potential. In this regard, oxyfluorides appear unsuitable because of the higher electronegativity of fluorine. Here we show an exceptional case, an anion-ordered pyrochlore oxyfluoride Pb2 Ti2 O5.4 F1.2 that has a small band gap (ca. 2.4 eV). With suitable modification of Pb2 Ti2 O5.4 F1.2 by promoters such as platinum nanoparticles and a binuclear ruthenium(II) complex, Pb2 Ti2 O5.4 F1.2 worked as a stable photocatalyst for visible-light-driven H2 evolution and CO2 reduction. Density functional theory calculations have revealed that the unprecedented visible-light-response of Pb2 Ti2 O5.4 F1.2 arises from strong interaction between Pb-6s and O-2p orbitals, which is enabled by a short Pb-O bond in the pyrochlore lattice due to the fluorine substitution.
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