文献类型：期刊文献

英文题名：Dispersed Nickel Boosts Catalysis by Copper in CO2 Hydrogenation

作者：Wang, Ling-Xiang[1,2];Guan, Erjia[3];Wang, Zhiqiang[4,5];Wang, Liang[1];Gong, Zhongmiao[6];Cui, Yi[6];Yang, Zhiyuan[2];Wang, Chengtao[2];Zhang, Jian[2];Meng, Xiangju[2];Hu, Peijun[4,5,7];Gong, Xue-Qing[4,5];Gates, Bruce C.[3];Xiao, Feng-Shou[1]

机构：[1]Zhejiang Univ, Key Lab Biomass Chem Engn, Minist Educ, Coll Chem & Biol Engn, Hangzhou 310027, Peoples R China;[2]Zhejiang Univ, Dept Chem, Hangzhou 310027, Peoples R China;[3]Univ Calif Davis, Dept Chem Engn, Davis, CA 95616 USA;[4]East China Univ Sci & Technol, Key Lab Adv Mat, Ctr Computat Chem, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[5]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[6]Chinese Acad Sci, Vacuum Interconnected Nanotech Workstn Nano X, Suzhou Inst Nanotech & NanoBion SINANO, Suzhou 215123, Peoples R China;[7]Queens Univ, Sch Chem & Chem Engn, Belfast BT9 SAG, Antrim, North Ireland

年份：2020

卷号：10

期号：16

起止页码：9261

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20204109319728);WOS:【SCI-EXPANDED(收录号:WOS:000563749900022)】；

基金：This work was supported by the National Key Research and the Development Program of China (2018YFB0604801 and 2018YFA0208602), the National Natural Science Foundation of China (21822203, 91634201, and 21825301), the Natural Science Foundation of Zhejiang Province (LR18B030002), the Program of Shanghai Academic Research Leader (17XD1401400), the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (DE-FG02-04ER15513), and the Fundamental Research Funds for the Central Universities. The work at the Stanford Synchrotron Radiation Lightsource of the SLAC National Accelerator Laboratory was supported by DOE, Office of Science, Basic Energy Sciences (DE-AC02-76SF00515). We acknowledge Nano-X (SINANO, CAS) for the in situ XPS characterization. We thank Fang Chen and Prof. Wei Zhang for their kind help in TEM characterization. The authors from ECUST also thank the National Super Computing Center in Jinan for computing time.

语种：英文

外文关键词：CO2 hydrogenation; copper catalyst; nickel; reverse water-gas shift; alloy

摘要：The empirical optimization of the preparation of catalytically active copper-containing catalysts is far more advanced than the fundamental understanding of the catalyst performance because of the structural complexity of the catalysts. Here, we demonstrate the interplay between the catalyst structure and CO2 hydrogenation on Cu catalysts boosted with nickel species. The nickel dispersion on copper markedly affects the CO2 dissociation activity and catalytic reaction pathways, thus resulting in distinctive catalytic activity and selectivity attributed to Ni. Specifically, the catalyst incorporating nickel alloyed in copper maximizes the synergy between the two metals and is characterized by conversions close to the thermodynamic equilibrium to CO as a product-with switched off methanation-over a wide temperature range. Catalyst performance data, spectra characterizing the catalyst, and theoretical results demonstrate that surface copper with adjacent nickel atoms efficiently activates CO2 via a redox mechanism-with adsorption of CO being suppressed-so that methanation associated with deep hydrogenation of CO is inhibited. The results of this investigation highlight the importance of structures with copper-adjacent-nickel, which appear to offer appealing opportunities for tailoring efficient copper-containing catalysts for CO2 hydrogenation.