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Citation
Tags
HERO ID
7111586
Reference Type
Journal Article
Title
A Stable, Narrow-Gap Oxyfluoride Photocatalyst for Visible-Light Hydrogen Evolution and Carbon Dioxide Reduction
Author(s)
Kuriki, Ryo; Ichibha, Tom; Hongo, K; Lu, D; Maezono, Ryo; Kageyama, H; Ishitani, O; Oka, K; Maeda, K; ,
Year
2018
Is Peer Reviewed?
Yes
Journal
Journal of the American Chemical Society
ISSN:
0002-7863
EISSN:
1520-5126
Publisher
AMER CHEMICAL SOC
Location
WASHINGTON
Page Numbers
6648-6655
PMID
29733632
DOI
10.1021/jacs.8b02822
Web of Science Id
WOS:000434101100021
Abstract
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 Pb2Ti2O5.4F1.2 that has a small band gap (ca. 2.4 eV). With suitable modification of Pb2Ti2O5.4F1.2 by promoters such as platinum nanoparticles and a binuclear ruthenium(II) complex, Pb2Ti2O5.F-4(1.2) worked as a stable photocatalyst for visible-light-driven H-2 evolution and CO2 reduction. Density functional theory calculations have revealed that the unprecedented visible-light-response of Pb2Ti2O5.F-4(1.2) 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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