文献类型：期刊文献

英文题名：Identifying the key obstacle in photocatalytic oxygen evolution on rutile TiO2

作者：Wang, Dong[1,2];Sheng, Tian[1,2];Chen, Jianfu[1,2];Wang, Hai-Feng[1,2];Hu, P.[1,2,3]

机构：[1]East China Univ Sci & Technol, Key Lab Adv Mat, Ctr Computat Chem, Sch Chem & Mol Engn, Shanghai, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem & Mol Engn, Res Inst Ind Catalysis, Shanghai, Peoples R China;[3]Queens Univ Belfast, Sch Chem & Chem Engn, Belfast, Antrim, North Ireland

年份：2018

卷号：1

期号：4

起止页码：291

外文期刊名：NATURE CATALYSIS

收录：;EI(收录号：20184506042653);WOS:【SCI-EXPANDED(收录号:WOS:000430451900016)】；

基金：D.W. thanks the Chinese Scholarship Council for financial support for living abroad and P.H. thanks the Chinese Government for support from the "Thousands Talents" program. This work was financially supported by National Natural Science Foundation of China (21333003, 21421004, 21622305), Young Elite Scientist Sponsorship Program by the China Association for Science and Technology (YESS20150131), The Shanghai ShuGuang project (17SG30), and the Fundamental Research Funds for the Central Universities (WJ616007).

语种：英文

外文关键词：Oxide minerals - Oxygen - Catalyst activity - Efficiency

摘要：As the bottleneck in photocatalytic water splitting, the oxygen evolution reaction (OER) has drawn huge attention, but its efficiency still falls short of expectations. A widely accepted speculation is that the catalysts' activity is insufficient (high reaction barriers need to be overcome). Here, we develop a first-principles method to investigate the photocatalytic OER at the water/TiO2(110) interface. A full mechanism uncovering the importance of radicals is determined. Kinetic analysis further enables to quantitatively estimate each possible obstacle in the process. We demonstrate unambiguously that the rate-determining factor of the OER varies with the concentration of surface-reaching photoholes (Ch+). Under experimental conditions, the intrinsic catalytic activity of TiO2(110) does not represent the main obstacle, but all steps involving the photoholes are slow due to their low concentrations. This suggests that the key to enhance the OER efficiency is to increase Ch+ before Ch+ reaches the estimated threshold (Ch+ = similar to 10(-4)).