Coverage effect of surface oxygen vacancy on In2O3-catalyzed CO2 hydrogenation revealed by first principles-based microkinetic simulations

doi:10.1016/j.comptc.2023.114174

	Coverage effect of surface oxygen vacancy on In2O3-catalyzed CO2 hydrogenation revealed by first principles-based microkinetic simulations
	Li, Kun1,2,3 ; Wei, Zhangqian 1,3; Chang, Qingyu 1; Li, Shenggang1,2,3
	2023
发表期刊	COMPUTATIONAL AND THEORETICAL CHEMISTRY (IF:3.0[JCR-2023],2.3[5-Year])
ISSN	2210-271X
EISSN	1872-7999
卷号	1225
发表状态	已发表
DOI	10.1016/j.comptc.2023.114174
摘要	Density functional theory (DFT) calculations and microkinetic simulations were performed to study the effect of the surface oxygen vacancy (OV) coverage on the In2O3 catalyst for methanol synthesis from CO2 hydrogenation, focusing on the In2O3(1 1 0) surface with a high OV coverage of 1 ML (In2O3(1 1 0)-allov) and compared with that with a low OV coverage of < 0.1 ML (In2O3(1 1 0)-vac). We find that the In2O3(1 1 0)-allov surface is less favorable for CO2 and H2 adsorptions than the In2O3(1 1 0)-vac surface, but the former has lower energy barriers for both the HCOO and COOH routes than the latter. Furthermore, the high OV coverage for the In2O3(1 1 0)-allov surface results in a significant lower CO2 reactivity, but gives surprisingly higher CH3OH selectivity. Our simulations may explain the experimentally observed deactivation of the In2O3 catalyst when over-reduced towards metallic In. Physical insights from this work should contribute to the rational design of efficient oxide-based CO2 hydrogenation catalysts.
关键词	CO 2 utilization Methanol synthesis Reverse water gas shift Density functional theory calculations Reaction mechanism
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收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China["22172188","22293023"] ; Shanghai Sailing Program from the Science and Technology Commission of Shanghai Municipality[23YF1453400] ; Shell Global Solutions B.V.[CW373032]
WOS研究方向	Chemistry
WOS类目	Chemistry, Physical
WOS记录号	WOS:001013541600001
出版者	ELSEVIER
引用统计	正在获取...
文献类型	期刊论文
条目标识符	https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/306507
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	Chang, Qingyu; Li, Shenggang
作者单位	1.Chinese Acad Sci, Shanghai Adv Res Inst, CAS Key Lab Low Carbon Convers Sci & Engn, 100 Haike Rd, Shanghai 201210, Peoples R China 2.ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R 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
推荐引用方式 GB/T 7714	Li, Kun,Wei, Zhangqian,Chang, Qingyu,et al. Coverage effect of surface oxygen vacancy on In2O3-catalyzed CO2 hydrogenation revealed by first principles-based microkinetic simulations[J]. COMPUTATIONAL AND THEORETICAL CHEMISTRY,2023,1225.
APA	Li, Kun,Wei, Zhangqian,Chang, Qingyu,&Li, Shenggang.(2023).Coverage effect of surface oxygen vacancy on In2O3-catalyzed CO2 hydrogenation revealed by first principles-based microkinetic simulations.COMPUTATIONAL AND THEORETICAL CHEMISTRY,1225.
MLA	Li, Kun,et al."Coverage effect of surface oxygen vacancy on In2O3-catalyzed CO2 hydrogenation revealed by first principles-based microkinetic simulations".COMPUTATIONAL AND THEORETICAL CHEMISTRY 1225(2023).