A DFT study on the active surfaces of the ZnGa2O4 spinel catalyst for CO2 hydrogenation to methanol
2025-07
发表期刊MOLECULAR CATALYSIS (IF:3.9[JCR-2023],3.8[5-Year])
ISSN2468-8231
卷号582
发表状态已发表
DOI10.1016/j.mcat.2025.115166
摘要

In this work, we constructed the low Miller index surfaces of (100), (001), (111), and (110) of the ZnGa2O4 spinel catalyst. Through extensive DFT calculations, we found that the oxygen vacancy (VO) formation energies on the (100) and (001) surfaces were <1.0 eV, whereas those on the (111) and (110) surfaces were >3.0 eV. We further examined the dissociation of molecular hydrogen (H2) on these surfaces, and found that H2 homolytic dissociation tended to occur on surfaces with lower VO formation energies, while H2 heterolytic dissociation were favored on those with higher VO formation energies. CO2 adsorption and activation on the different surfaces of the ZnGa2O4 spinel catalyst were investigated, and on surfaces with lower VO formation energies, CO2 adsorbs in a linear configuration (ln-CO2*), while on surfaces with higher VO formation energies, CO2 adopts in a bent adsorption geometry (bt-CO2*) and is easier to dissociate. For HCOO formation from ln-CO2* + H*, the (110) surface has the lowest energy barrier, so it is likely the most active surface for CO2 hydrogenation to methanol (CH3OH). Thus, we compared the CH3OH formation pathway on the ZnGa2O4(110) surface with the pathways for direct and indirect CO2 dissociation, and predicted it to favor CH3OH production. Our calculations reveal the active surfaces of the ZnGa2O4 spinel catalyst for CO2 hydrogenation to CH3OH, and provide insights into the experimentally observed high CH3OH selectivity, which should be important for the rational design of Zn-based spinel catalysts for this reaction.

关键词ZnGa2O4 spinel catalyst Methanol synthesis CO2 hydrogenation DFT calculations Active surfaces
学科门类理学 ; 工学
收录类别SCI ; EI ; SCIE
语种英语
出版者Elsevier B.V.
EI入藏号20251818348287
EI主题词Hydrogenolysis
EI分类号802.2 Chemical Reactions
原始文献类型Journal article (JA)
文献类型期刊论文
条目标识符https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/527182
专题物质科学与技术学院
物质科学与技术学院_特聘教授组_李圣刚组
物质科学与技术学院_硕士生
通讯作者Shenggang Li
作者单位
1.School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, PR China
2.Low Carbon Conversion Science and Engineering Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201203, PR China
3.University of Chinese Academy of Sciences, Beijing 100049, PR China
4.State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, PR China
第一作者单位物质科学与技术学院
通讯作者单位物质科学与技术学院
第一作者的第一单位物质科学与技术学院
推荐引用方式
GB/T 7714
Ziqi Tang,YuanJie Bao,Zhangqian Wei,et al. A DFT study on the active surfaces of the ZnGa2O4 spinel catalyst for CO2 hydrogenation to methanol[J]. MOLECULAR CATALYSIS,2025,582.
APA Ziqi Tang,YuanJie Bao,Zhangqian Wei,&Shenggang Li.(2025).A DFT study on the active surfaces of the ZnGa2O4 spinel catalyst for CO2 hydrogenation to methanol.MOLECULAR CATALYSIS,582.
MLA Ziqi Tang,et al."A DFT study on the active surfaces of the ZnGa2O4 spinel catalyst for CO2 hydrogenation to methanol".MOLECULAR CATALYSIS 582(2025).
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