文献类型：期刊文献

英文题名：Hydride Generation on the Cu-Doped CeO2(111) Surface and Its Role in CO2 Hydrogenation Reactions

作者：Wang, Zhi-Qiang[1,2,3];Liu, Hui-Hui[1,2,3];Wu, Xin-Ping[1,2,3];Hu, Peijun[1,2,3,4];Gong, Xue-Qing[1,2,3]

机构：[1]East China Univ Sci & Technol, Key Lab Adv Mat, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Ctr Computat Chem, Feringa Nobel Prize Scientist Joint Res Ctr, Joint Int Res Lab Precis Chem & Mol Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[4]Queens Univ Belfast, Sch Chem & Chem Engn, Belfast BT9 5AG, Antrim, North Ireland

年份：2022

卷号：12

期号：9

外文期刊名：CATALYSTS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000858137600001)】；

基金：This research was funded by National Key R&D Program of China (2018YFA0208602) and National Nature Science Foundation of China (21825301, 22003016, 92045303, 92145302) and Shanghai Sailing Program (21YF1409400) and China Postdoctoral Science Foundation (2020M671020).

语种：英文

外文关键词：ceria; hydride; CO2 hydrogenation; single Cu doping; density functional theory

摘要：Ceria-based catalysts exhibit great activity in catalyzing selective hydrogenation of CO2 to methanol. However, the underlying mechanism of this reaction, especially the generation of active H species, remains unclear. In this work, we performed extensive density functional theory calculations corrected by on-site Coulomb interaction (DFT + U) to investigate the H-2 dissociation and the reaction between the active H species and CO2 on the pristine and Cu-doped CeO2(111) (denoted as Cu/CeO2(111)) surfaces. Our calculations evidenced that the heterolytic H-2 dissociation for hydride generation can more readily occur on the Cu/CeO2(111) surface than on the pristine CeO2(111) surface. We also found that the Cu dopant can facilitate the formation of surface oxygen vacancies, further promoting the generation of hydride species. Moreover, the adsorption of CO2 and the hydrogenation of CO2 to HCOO* can be greatly promoted on the Cu/CeO2(111) surface with hydride species, which can lead to the high activity and selectivity toward CO2 hydrogenation to methanol.