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dc.contributor.authorZhou, Yangen
dc.contributor.authorZhang, Zizhong
dc.contributor.authorFang, Zhiwei
dc.contributor.authorQiu, Mei
dc.contributor.authorLing, Lan
dc.contributor.authorLong, Jinlin
dc.contributor.authorChen, Lu
dc.contributor.authorTong, Yuecong
dc.contributor.authorSu, Wenyue
dc.contributor.authorZhang, Yongfan
dc.contributor.authorWu, Jeffrey C S
dc.contributor.authorBasset, Jean-Marie
dc.contributor.authorWang, Xuxu
dc.contributor.authorYu, Guihua
dc.date.accessioned2019-05-13T11:38:16Z
dc.date.available2019-05-13T11:38:16Z
dc.date.issued2019-05-07
dc.identifier.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.
dc.identifier.issn0027-8424
dc.identifier.issn1091-6490
dc.identifier.doi10.1073/pnas.1901631116
dc.identifier.urihttp://hdl.handle.net/10754/652860
dc.description.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].
dc.description.sponsorshipX.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.
dc.publisherProceedings of the National Academy of Sciences
dc.relation.urlhttps://www.pnas.org/content/early/2019/05/06/1901631116
dc.rightsArchived with thanks to Proceedings of the National Academy of Sciences
dc.subjectPhotocatalyst
dc.subjectOxygen vacancy
dc.subjectDefect Engineering
dc.subjectSolar Hydrogen Production
dc.subjectMetal-oxide Interface
dc.titleDefect engineering of metal–oxide interface for proximity of photooxidation and photoreduction
dc.typeArticle
dc.contributor.departmentChemical Science Program
dc.contributor.departmentKAUST Catalysis Center (KCC)
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalProceedings of the National Academy of Sciences
dc.eprint.versionPublisher's Version/PDF
dc.contributor.institutionDepartment of Mechanical Engineering, The University of Texas at Austin, Austin, TX 78712
dc.contributor.institutionMaterials Science and Engineering Program, The University of Texas at Austin, Austin, TX 78712
dc.contributor.institutionState Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fuzhou 350002, China
dc.contributor.institutionDepartment of Chemistry, Fuzhou University, Fuzhou 350108, China
dc.contributor.institutionState Key Laboratory for Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
dc.contributor.institutionDepartment of Chemical Engineering, National Taiwan University, Taipei 10617, Taiwan
kaust.personBasset, Jean-Marie
refterms.dateFOA2019-11-07T00:00:00Z
dc.date.published-online2019-05-07
dc.date.published-print2019-05-21


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