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

Ceria-based catalysts exhibit great activity in catalyzing selective hydrogenation of CO2 to methanol. However, the underlying mechanism this reaction, especially generation active H species, remains unclear. In work, we performed extensive density functional theory calculations corrected by on-site Coulomb interaction (DFT + U) investigate H2 dissociation and reaction between species on pristine Cu-doped CeO2(111) (denoted as Cu/CeO2(111)) surfaces. Our evidenced that heterolytic for hydride can more readily occur Cu/CeO2(111) surface than surface. We also found Cu dopant facilitate formation oxygen vacancies, further promoting species. Moreover, adsorption HCOO* be greatly promoted with which lead high selectivity toward