Defect engineering of metal–oxide interface for proximity of photooxidation and photoreduction
Wu, Jeffrey C S
KAUST DepartmentChemical Science Program
KAUST Catalysis Center (KCC)
Physical Science and Engineering (PSE) Division
Online Publication Date2019-05-07
Print Publication Date2019-05-21
Permanent link to this recordhttp://hdl.handle.net/10754/652860
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AbstractClose 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].
CitationZhou 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.
SponsorsX.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.