文献类型：期刊文献

英文题名：Fabricating a Au@TiO2 Plasmonic System To Elucidate Alkali-Induced Enhancement of Photocatalytic H2 Evolution: Surface Potential Shift or Methanol Oxidation Acceleration?

作者：Zhao, Ming[1,2];Xu, Hua[1,2];Ouyang, Shuxin[1,2];Tong, Hua[3];Chen, Huayu[1,2];Li, Yunxiang[4,5];Song, Lizhu[1,2];Ye, Jinhua[1,2,4,5]

机构：[1]Tianjin Univ, Sch Mat Sci & Engn, TJU NIMS Int Collaborat Lab, 92 Weijin Rd, Tianjin 300072, Peoples R China;[2]Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300072, Peoples R China;[3]East China Univ Sci & Technol, Sch Mat Sci & Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[4]Hokkaido Univ, Grad Sch Chem Sci & Engn, Sapporo, Hokkaido 0600814, Japan;[5]Natl Inst Mat Sci, Int Ctr Mat Nanoarchitecton WPI MANA, Environm Remediat Mat Unit, 1-1 Namiki, Tsukuba, Ibaraki 3050047, Japan

年份：2018

卷号：8

期号：5

起止页码：4266

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20182005193612);WOS:【SCI-EXPANDED(收录号:WOS:000431727300058)】；

基金：This work received financial support from the National Natural Science Foundation of China (21573158, 51502200, 51502198, 21633004), the National Basic Research Program of China (973 Program, No. 2014CB239301), and the Natural Science Foundation of Tianjin (15JCYBJC17400 and 15JCQNJC03500).

语种：英文

外文关键词：plasmonic photocatalysis; Au; anatase TiO2; alkaline environment; H-2 evolution

摘要：Enhancement in photocatalytic H-2 evolution induced by an alkaline reaction environment has been experimentally recognized, but there is not yet a consensus regarding the promotion mechanism (surface potential shift (SPS) or methanol oxidation (MO)). Herein, we construct a Au@TiO2 plasmonic system, since this architecture can easily separate the proton reduction process (only related to SPS) and the electron donor oxidation process (only related to MO) in physical space. The H-2 evolution rate over the Au@TiO2 system in a strongly basic environment is exponentially greater (by approximately 2 orders of magnitude) than that of the same reaction in a neutral environment. To explore which of these two processes is the dominant factor for the enhancement of the H-2 evolution, two investigation schemes are proposed. For Au@ST01 (ST01, a commercial anatase TiO2), the decisive role of the SPS on the enhancement of H-2 evolution is semiquantitatively deduced from the open-circuit potential (OCP) test (exceeds 80% at pH <13.5 and more than 50% at pH >= 13.5) and is further confirmed by electrochemical impedance spectroscopy (EIS) and photoresponse current tests. For Au@T-100 and Au@T-101, (T-100 and T-101, facet-controlled anatase TiO2), the irregular fluctuation of the ratio of H-2 evolution rates (rH(2)(Au@T-100)/rH(2)(Au@T-101)) suggests a secondary role of MO. This study clarifies the mechanism of the alkali-induced enhancement of H-2 evolution and provides a perspective for the modulation of reaction environments.