文献类型：期刊文献

英文题名：Structure-Activity Relationships of Copper- and Potassium-Modified Iron Oxide Catalysts during Reverse Water-Gas Shift Reaction

作者：Gu, Mengwei[1];Dai, Sheng[2,3];Qiu, Runfa[1];Ford, Michael E.[4];Cao, Chenxi[5];Wachs, Israel E.[4];Zhu, Minghui[1]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Sch Chem Engn, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Sch Chem & Mol Engn, Feringa Nobel Prize Scientist Joint Res Ctr, Shanghai 200237, Peoples R China;[4]Lehigh Univ, Operando Mol Spect & Catalysis Lab, Dept Chem & Biomol Engn, Bethlehem, PA 18015 USA;[5]East China Univ Sci & Technol, Key Lab Smart Mfg Energy Chem Proc, Minist Educ, Shanghai 200237, Peoples R China

年份：2021

卷号：11

期号：20

起止页码：12609

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20214211041435);WOS:【SCI-EXPANDED(收录号:WOS:000709692900017)】；

基金：This work is sponsored by the National Natural Science Foundation of China (22078089), Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning, Shanghai Sailing Program (19YF1410600) and Shanghai Rising-star Program (20QA1402400). The research at Lehigh University was supported by the Center for Understanding & Control of Acid Gas-Induced Evolution of Materials for Energy (UNCAGE-ME), an Energy Frontier Research Center funded by DOE, Office of Science, Office of Basic Energy Sciences under grant DE-SC0012577. Additional support was provided by the Feringa Nobel Prize Scientist Joint Research Center.

语种：英文

外文关键词：iron-based catalyst; CO2 activation; redox mechanism; associative mechanism; hydrogen dissociation

摘要：The reverse water-gas shift (RWGS) reaction is an initial and essential step for CO2 hydrogenation. In this study, Cu-and K-modified iron oxide catalysts were investigated with a series of in/ex-situ characterization techniques, including in situ XRD, in situ Raman, in situ DRIFTS quasi in situ XPS, quasi in situ HS-LEIS, H-2-TPR, CO2-TPD, and TPSR. The surface structure of the catalyst is found to strongly depend on the presence of Cu and K, leading to diverse reducibility and basicity. Adding K to the iron-based catalyst alters the reaction from a redox pathway that proceeds on surface redox sites to an associative pathway that proceeds on surface redox and basic sites. Metallic Cu facilitates hydrogen dissociation and promotes both mechanisms by either boosting surface vacancy sites or supplying abundant surface hydrogen atoms. These findings would be beneficial for the rational design of CO2 hydrogenation catalysts.