文献类型：期刊文献

英文题名：Site Sensitivity of Interfacial Charge Transfer and Photocatalytic Efficiency in Photocatalysis: Methanol Oxidation on Anatase TiO2 Nanocrystals

作者：Fu, Cong[1,2];Li, Fei[3,4];Zhang, Jiachen[5];Li, Dan[1,2];Qian, Kun[1,2];Liu, Yong[6];Tang, Junwang[7];Fan, Fengtao[6,8];Zhang, Qun[5];Gong, Xue-Qing[3,4];Huang, Weixin[1,2,8]

机构：[1]Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Key Lab Surface & Interface Chem & Energy Catalys, Anhui Higher Educ Inst,CAS Key Lab Mat Energy Con, Hefei 230026, Peoples R China;[2]Univ Sci & Technol China, Dept Chem Phys, Hefei 230026, Peoples R China;[3]East China Univ Sci & Technol, Key Lab Adv Mat, Ctr Computat Chem, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China;[5]Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Dept Chem Phys, Synerget Innovat Ctr Quantum Informat & Quantum P, Hefei 230026, Peoples R China;[6]Chinese Acad Sci, State Key Lab Catalysis, Dalian Inst Chem Phys, Dalian 116023, Peoples R China;[7]UCL, Dept Chem Engn, London WC1E 7JE, England;[8]Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China

年份：2021

卷号：60

期号：11

起止页码：6160

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20210809946844);WOS:【SCI-EXPANDED(收录号:WOS:000618195100001)】；

基金：This work was financially supported by the National Natural Science Foundation of China (21525313, 91745202, 91945301, 21825301, 21573211, and 21633007), the National Key Research and Development Program of China (2016YFA0200602 and 2018YFA0303500), the Chinese Academy of Sciences, the Changjiang Scholars Program of Ministry of Education of China, and the Anhui Initiative in Quantum Information Technologies (AHY090200).

语种：英文

外文关键词：electronic structure; methanol; nanocrystals; surface chemistry; surface photochemistry

摘要：Photocatalytic oxidation of methanol on various anatase TiO2 nanocrystals was studied by in situ and time-resolved characterizations and DFT calculations. Surface site and resulting surface adsorbates affect the surface band bending/bulk-to-surface charge migration processes and interfacial electronic structure/interfacial charge transfer processes. TiO2 nanocrystals predominantly enclosed by the {001} facets expose a high density of reactive fourfold-coordinated Ti sites (Ti-4c) at which CH3OH molecules dissociate to form the CH3O adsorbate (CH3O(a)(Ti4c)). CH3O(a)(Ti4c) localized density of states are almost at the valence band maximum of TiO2 surface, facilitating the interfacial hole transfer process; CH3O(a)(Ti4c) with a high coverage promotes upward surface band bending, facilitating bulk-to-surface hole migration. CH3O(a)(Ti4c) exhibits the highest photocatalytic oxidation rate constant. TiO2 nanocrystals enclosed by the {001} facets are most active in photocatalytic methanol oxidation.