文献类型：期刊文献

英文题名：Non-oxidative Coupling of Methane: N-type Doping of Niobium Single Atoms in TiO2-SiO2 Induces Electron Localization

作者：Chen, Ziyu[1,2];Wu, Shiqun[1,2];Ma, Jiayu[1,2];Mine, Shinya[3];Toyao, Takashi[4,5];Matsuoka, Masaya[3];Wang, Lingzhi[1,2];Zhang, Jinlong[1,2,6]

机构：[1]East China Univ Sci & Technol, Key Lab Adv Mat, Sch Chem & Mol Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Joint Int Res Lab Precis Chem & Mol Engn, Sch Chem & Mol Engn, Feringa Nobel Prize Scientist Joint Res Ctr,Front, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]Osaka Prefecture Univ, Dept Appl Chem, Gakuen Cho 1-1, Sakai, Osaka 5998531, Japan;[4]Hokkaido Univ, Inst Catalysis, N-21,W-10, Sapporo, Hokkaido 0010021, Japan;[5]Kyoto Univ, Elements Strategy Initiat Catalysts & Batteries, Kyoto 6158520, Japan;[6]Yancheng Inst Technol, Sch Chem & Chem Engn, Yancheng 224051, Peoples R China

年份：2021

卷号：60

期号：21

起止页码：11901

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20211010017985);WOS:【SCI-EXPANDED(收录号:WOS:000623230700001)】；

基金：This work was supported by the National Natural Science Foundation of China (21972040, 21673073, 21677048 and 5171101651), the Science and Technology Commission of Shanghai Municipality (18520710200), Shanghai Pujiang Program (18PJD012), the PetroChina Innovation Foundation (2015D-5006-0402), Project supported by Shanghai Municipal Science and Technology Major Project (No.2018SHZDZX03) and the Program of Introducing Talents of Discipline to Universities (No. B20031, B16017). The X-ray absorption fine structure (XAFS) measurements were performed under the approval of the JASRI (Proposal No. 2019B1686).

语种：英文

外文关键词：C− H activation; desorption; NOCM; n-type doping; photocatalysis

摘要：Photodriven nonoxidative coupling of CH4 (NOCM) is an attractive potential way to use abundant methane resources. Herein, an n-type doped photocatalyst for NOCM is created by doping single-atom Nb into hierarchical porous TiO2-SiO2 (TS) microarray, which exhibits a high conversion rate of 3.57 mu mol g(-1) h(-1) with good recyclability. The Nb dopant replaces the 6-coordinated titanium on the (1 0 1) plane and forms shallow electron-trapped surface polarons along [0 1 0] direction and the comparison of different models proves that the electron localization caused by the n-type doping is beneficial to both methane activation and ethane desorption. The positive effect of n-type dopant on CH4 conversion is further verified on Mo-, W- and Ta-doped composites. In contrast, the doping of p-type dopant (Ga, Cu, Fe) shows a less active influence.