Influence of Oxygen Vacancy Distribution on CO2 Hydrogenation: A Case Study of ZnO and In2O3

被引：0

作者：

Song, Dandan ^{[1
]}

Cui, Leyuan ^{[1
]}

Qin, Ruixuan ^{[1
,2
]}

Fu, Gang ^{[1
,2
]}

机构：

[1] Xiamen Univ, Coll Chem & Chem Engn, Collaborat Innovat Ctr Chem Energy Mat, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China

[2] Innovat Lab Sci & Technol Energy Mat Fujian Prov I, Xiamen 361102, Peoples R China

来源：

JACS AU | 2025年 / 5卷 / 07期

基金：

中国国家自然科学基金; 国家重点研发计划;

关键词：

oxygen vacancy distribution; ZnO; CO2; hydrogenation; surface polarization; machine learningpotential; SELECTIVE CONVERSION; CARBON-DIOXIDE; CATALYST; METHANOL;

D O I：

10.1021/jacsau.5c00304

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Oxygen vacancies (OVs) on metal oxide surfaces are widely recognized as catalytically active sites; however, the impact of their distribution on the catalytic performance remains underexplored. In this study, we used density functional theory (DFT) calculations combined with a machine learning potential to investigate the distribution of OVs on the ZnO(10 1 - 0) surface and their role in CO2 hydrogenation. We efficiently analyzed over 700,000 potential OV configurations by reducing them to unique, irreducible structures using the self-developed DefectMaker program. Our results revealed that higher OV concentrations led to the formation of linear OV structures, which, despite their energetic stability, exhibited lower CO2 hydrogenation efficiency compared to isolated OVs, due to the reduced surface polarization with linear OVs. Additionally, a comparative investigation on In2O3 surfaces revealed a scattered distribution of OVs, maintaining the material's catalytic activity in CO2 hydrogenation. This work provides a deeper understanding of defect engineering in metal oxides for a more efficient CO2 conversion

引用

页码：3156 / 3162

页数：7