TY - JOUR
T1 - Defect engineering of metal–oxide interface for proximity of photooxidation and photoreduction
AU - Zhou, Yangen
AU - Zhang, Zizhong
AU - Fang, Zhiwei
AU - Qiu, Mei
AU - Ling, Lan
AU - Long, Jinlin
AU - Chen, Lu
AU - Tong, Yuecong
AU - Su, Wenyue
AU - Zhang, Yongfan
AU - Wu, Jeffrey C S
AU - Basset, Jean-Marie
AU - Wang, Xuxu
AU - Yu, Guihua
N1 - KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: 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.
PY - 2019/5/7
Y1 - 2019/5/7
N2 - 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].
AB - 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].
UR - http://hdl.handle.net/10754/652860
UR - https://www.pnas.org/content/early/2019/05/06/1901631116
UR - http://www.scopus.com/inward/record.url?scp=85066121922&partnerID=8YFLogxK
U2 - 10.1073/pnas.1901631116
DO - 10.1073/pnas.1901631116
M3 - Article
C2 - 31064878
SN - 0027-8424
VL - 116
SP - 10232
EP - 10237
JO - Proceedings of the National Academy of Sciences
JF - Proceedings of the National Academy of Sciences
IS - 21
ER -