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    Defect engineering of metal–oxide interface for proximity of photooxidation and photoreduction

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    Type
    Article
    Authors
    Zhou, Yangen
    Zhang, Zizhong
    Fang, Zhiwei
    Qiu, Mei
    Ling, Lan
    Long, Jinlin
    Chen, Lu
    Tong, Yuecong
    Su, Wenyue
    Zhang, Yongfan
    Wu, Jeffrey C S
    Basset, Jean-Marie cc
    Wang, Xuxu
    Yu, Guihua
    KAUST Department
    Chemical Science Program
    KAUST Catalysis Center (KCC)
    Physical Science and Engineering (PSE) Division
    Date
    2019-05-07
    Online Publication Date
    2019-05-07
    Print Publication Date
    2019-05-21
    Permanent link to this record
    http://hdl.handle.net/10754/652860
    
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    Abstract
    Close proximity between different catalytic sites is crucial for accelerating or even enabling many important catalytic reactions. Photooxidation and photoreduction in photocatalysis are generally separated from each other, which arises from the hole-electron separation on photocatalyst surface. Here, we show with widely studied photocatalyst Pt/[Formula: see text] as a model, that concentrating abundant oxygen vacancies only at the metal-oxide interface can locate hole-driven oxidation sites in proximity to electron-driven reduction sites for triggering unusual reactions. Solar hydrogen production from aqueous-phase alcohols, whose hydrogen yield per photon is theoretically limited below 0.5 through conventional reactions, achieves an ultrahigh hydrogen yield per photon of 1.28 through the unusual reactions. We demonstrated that such defect engineering enables hole-driven CO oxidation at the Pt-[Formula: see text] interface to occur, which opens up room-temperature alcohol decomposition on Pt nanoparticles to [Formula: see text] and adsorbed CO, accompanying with electron-driven proton reduction on Pt to [Formula: see text].
    Citation
    Zhou Y, Zhang Z, Fang Z, Qiu M, Ling L, et al. (2019) Defect engineering of metal–oxide interface for proximity of photooxidation and photoreduction. Proceedings of the National Academy of Sciences: 201901631. Available: http://dx.doi.org/10.1073/pnas.1901631116.
    Sponsors
    X.W., Y. Zhang, and W.S. acknowledge financial support from National Natural Science Foundation of China Grants U1305242, 21173044, 21373048, and 21373050. G.Y. acknowledges support from Welch Foundation Award F-1861 and the Sloan Research Foundation.
    Publisher
    Proceedings of the National Academy of Sciences
    Journal
    Proceedings of the National Academy of Sciences
    DOI
    10.1073/pnas.1901631116
    Additional Links
    https://www.pnas.org/content/early/2019/05/06/1901631116
    ae974a485f413a2113503eed53cd6c53
    10.1073/pnas.1901631116
    Scopus Count
    Collections
    Articles; Physical Science and Engineering (PSE) Division; Chemical Science Program; KAUST Catalysis Center (KCC)

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