文献类型：期刊文献

英文题名：Identification of Active Area as Active Center for CO Oxidation over Single Au Atom Catalyst

作者：Lou, Yang[1,3];Cai, Yafeng[1];Hu, Wende[1];Wang, Li[1];Dai, Qiguang[1];Zhan, Wangcheng[1];Guo, Yanglong[1];Hu, P.[1];Cao, Xiao-Ming[1];Liu, Jingyue[2];Guo, Yun[1]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[2]Arizona State Univ, Dept Phys, Tempe, AZ 85287 USA;[3]Jiangnan Univ, Sch Chem & Mat Engn, Wuxi 214122, Jiangsu, Peoples R China

年份：2020

卷号：10

期号：11

起止页码：6094

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20202908951541);WOS:【SCI-EXPANDED(收录号:WOS:000538766900014)】；

基金：This project was financially supported by the National Key Research and Development Program of China (2016YFC0204300), the National Natural Science Foundation of China (21571061, 21673072, and 21908079), the Startup Funding of Jiangnan University (1045210322190170), and the Pujiang Program of the Shanghai Municipal Human Resources and Social Security Bureau (18PJD011). J.L. acknowledges the use of facilities within the John M. Cowley Center for HREM at Arizona State University.

语种：英文

外文关键词：single-atom Au; activity origin; isotope labeling; DFT calculation; CO oxidation

摘要：Identifying the activity origin of noble-metal-based catalysts is extremely important for fundamental research and practical application. We report that single Au atoms on Co3O4 (Au-1/Co3O4 single-atom catalysts (SAC)) exhibit excellent activity and stability for CO oxidation and that the activity origin of Au-1/Co3O4 SAC is an active area centered by Au-1 atom with one nearby Co and O atoms (and/or O vacancy). The turnover frequency is 3.1 s-1 at -75 degrees C, to our knowledge, which makes Au-1/Co3O4 SAC one of the most active Au catalysts for CO oxidation. The activity can be maintained after 10 cycles of temperature-programmed reaction from -100 to 300 degrees C or storage in air for 1 year, indicating the high stability of Au-1/Co3O4 SAC. The isotope, in situ DRIFTS, kinetics, and density functional theory (DFT) results further demonstrate that CO2 is produced through two reaction pathways, following the Langmuir-Hinshelwood (predominant) and Mars-van Krevelen mechanisms, respectively. The present findings pave the way for better understanding supported metal catalysts.