异构化
氢化物
催化作用
离解(化学)
掺杂剂
化学
密度泛函理论
光化学
吸附
甲醇
无机化学
选择性
材料科学
兴奋剂
物理化学
氢
计算化学
有机化学
光电子学
作者
Zhiqiang Wang,Huihui Liu,Xin‐Ping Wu,P. Hu,Xue‐Qing Gong
出处
期刊:Catalysts
[MDPI AG]
日期:2022-08-29
卷期号:12 (9): 963-963
被引量:9
标识
DOI:10.3390/catal12090963
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 H2 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 H2 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.
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