文献类型：期刊文献

英文题名：Unraveling Highly Tunable Selectivity in CO2 Hydrogenation over Bimetallic In-Zr Oxide Catalysts

作者：Chen, Tian-yuan[1];Cao, Chenxi[1];Chen, Tian-bao[1];Ding, Xiaoxu[1];Huang, Hai[1];Shen, Liang[1];Cao, Xinyu[1];Zhu, Minghui[1];Xu, Jing[1];Gao, Jian[2];Han, Yi-Fan[1,2]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]Zhengzhou Univ, Sch Chem Engn & Energy, Res Ctr Heterogeneous Catalysis & Engn Sci, Zhengzhou 450001, Henan, Peoples R China

年份：2019

卷号：9

期号：9

起止页码：8785

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20193907466231);WOS:【SCI-EXPANDED(收录号:WOS:000485090400116)】；

基金：We gratefully acknowledge financial support from the National Key R&D Program of China (2018YFB0605803), Shanghai Sailing Program (18YF1406100), National Natural Science Foundation of China (21878080, 21808058, and 21576084), Fundamental Research Funds for the Central Universities (222201718002 and 222201814006), and Innovation Scientists and Technicians Troop Construction Projects of Henan Province.

语种：英文

外文关键词：CO2 hydrogenation; methanol synthesis; reverse water-gas shift; indium catalysts; dynamic evolution

摘要：We present a comprehensive mechanistic study on the highly tunable selectivity over In-x/ZrO2 catalysts in CO2 hydrogenation. By variation of the indium loading between 0.1 and 5 wt %, either an admirable selectivity to CO methanol of 70-80% or up to 80% selectivity to CO could be obtained in the temperature range of 250-280 degrees C. It is shown that the shift in the product spectrum is related to the synergy between indium species and the zirconia substrate through variable interfacial structures. Zirconia-modulated crystalline In2O3, which prevails for indium loadings between 2.5 and 5 wt %, could enhance stepwise hydrogenation of *HCOO, leading to *H3CO and finally methanol due to the suitable bonding strengths of *HCOO and *H3CO. Regarding CO2 evidence has been provided that the synergistic effect between adjacent indium and zirconia sites is indispensable for the entire catalytic cycle. *HCOO is formed at the indium-zirconia interfaces and decomposes to CO subsequently. Highly dispersed InOx dominating for loadings below 0.5 wt % features an enormous indium-zirconia interface and suppresses hydrogenation ability for *HCOO, thus favoring the generation of CO. The study provides fundamental insights into the mechanism of CO2 conversion and reaction pathway tuning over oxide catalytic systems.