Defect engineering of metal–oxide interface for proximity of photooxidation and photoreduction
Type
ArticleAuthors
Zhou, YangenZhang, Zizhong
Fang, Zhiwei
Qiu, Mei
Ling, Lan
Long, Jinlin
Chen, Lu
Tong, Yuecong
Su, Wenyue
Zhang, Yongfan
Wu, Jeffrey C S
Basset, Jean-Marie

Wang, Xuxu
Yu, Guihua
KAUST Department
Chemical Science ProgramKAUST Catalysis Center (KCC)
Physical Science and Engineering (PSE) Division
Date
2019-05-07Online Publication Date
2019-05-07Print Publication Date
2019-05-21Permanent link to this record
http://hdl.handle.net/10754/652860
Metadata
Show full item recordAbstract
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.Additional Links
https://www.pnas.org/content/early/2019/05/06/1901631116ae974a485f413a2113503eed53cd6c53
10.1073/pnas.1901631116