文献类型：期刊文献

英文题名：Surface Oxygen Vacancy and Hydride Species on Ceria Are Detrimental to Acetylene Semihydrogenation Reaction

作者：Li, Zhaorui[1];Chen, Lu[2];Wu, Zongfang[3];Jia, AiPing[4];Shi, Shucheng[5];Zhang, Hui[6];Wang, Jia[2];Liu, Zhi[7];Shao, Wei-Peng[7];Yang, Fan[7];Wu, Xin-Ping[2];Gong, Xue-Qing[2];Huang, Weixin[2]

机构：[1]Univ Sci & Technol China, Energy Catalysis Anhui Higher Educ Inst, Dept Chem Phys,Key Lab Surface & Interface, Key Lab Precise & Intelligent Chem,iChEM, Hefei 230026, Peoples R China;[2]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Ctr Computat Chem & Res Inst Ind Catalysis, Sch Chem & Mol Engney,Key Lab Adv Mat & Joint Int, Shanghai 200237, Peoples R China;[3]Univ Sci & Technol China, Hefei Nat Res Ctr Phys Sci Microscale, Key Lab Surface & Interface Chem & Energy Catalys, Hefei 230026, Peoples R China;[4]Zhejiang Normal Univ, Inst Phys Chem, Key Lab Minist Educ fo Adv Catalysis Mat, Jinhua 321004, Peoples R China;[5]Shanghai Tech Univ, Sch Phys Scie & Technol, Shanghai 201210, Peoples R China;[6]Chinese Acad Sci, State Key Lab Funct lMat Informat, Shanghai Inst Microsyst & Informatn Technol, Shanghai 200050, Peoples R China;[7]Shanghai Tech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China

年份：2023

卷号：13

期号：8

起止页码：5213

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20231513872746);WOS:【SCI-EXPANDED(收录号:WOS:000966998300001)】；

基金：This work was financially supported by the National Key R&D Program of MOST (2021YFA1501301) , the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB0450102) , the National Natural Science Foundation of China (91745202, 91945301, 92145302, U1930203, and 22003016) , the Fundamental Research Funds for the Central Universities (20720220008) , and the Changjiang Scholars Program of Ministry of Education of China. The authors thank BL02B at the Shanghai Synchrotron Radiation Facility supported by the National Natural Science Foundation of China under contract no. 11227902.

语种：英文

外文关键词：heterogeneous catalysis; reaction mechanism; active species; in situ characterization; DFT calculations

摘要：Reactivity of OH and hydride species in oxide catalyzed hydrogenation reactions has attracted great interest. Herein, we report a combined in situ spectroscopic characterization and density functional theory (DFT) calculation study of ceriacatalyzed acetylene semihydrogenation reaction. The ceria surface is fully hydroxylated during the adopted reaction condition. C2H2 adsorbs molecularly on the stoichiometric CeO2 surface and hydrogenates with OH groups selectively to produce C2H4. Semihydrogenation of C2H2 to C2H4 with either OH groups or hydride species on ceria surfaces with surface oxygen vacancies proceeds more facilely than on a stoichiometric CeO2 surface, but C2H4 adsorbs more strongly and further hydrogenates to C2H6 more facilely; moreover, dissociative adsorption of C2H2 to C2H species occurs, which facilely hydrogenates with the hydride species eventually to form C2H6 and react with each other to produce oligomers, decreasing the catalytic selectivity and stability, respectively. These results demonstrate that the ceria catalyst with a stoichiometric surface is extremely selective in catalyzing C2H2 semihydrogenation reaction to C2H4, whereas surface oxygen vacancies or hydride species on ceria are harmful to the catalytic performance.