Stability and Catalytic Performance of Single-Atom Catalysts Supported on Doped and Defective Graphene for CO2 Hydrogenation to Formic Acid: A First-Principles Study

doi:10.1021/acsanm.1c00959

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	Stability and Catalytic Performance of Single-Atom Catalysts Supported on Doped and Defective Graphene for CO2 Hydrogenation to Formic Acid: A First-Principles Study
	Ali, Sajjad 2,5; Iqbal, Rashid 1; Khan, Azim 2; Rehman, Shafiq Ur 3; Haneef, Muhammad 4; Yin, Lichang 2
通讯作者	Ali, Sajjad(sajjad@alum.imr.ac.cn)
	2021-07-23
发表期刊	ACS APPLIED NANO MATERIALS
ISSN	2574-0970
卷号	4 期号:7 页码:6893-6902
摘要	As an essential component of single-atom catalysts, support materials determine the dispersion, utilization, and stability of single metal atoms. Here, we reported the potential of defective and doped graphene as a single-atom catalyst (SAC) support for CO2 conversion to formic acid by hydrogenation. The support effect was screened based on the stability of a single-metal atom. Our calculation revealed that Cu, Pd, and Ru supported on defective graphene with monovacancy (m-VacG) have higher adsorption energy than the cohesive energy of their bulk counterparts; therefore we selected Cu, Pd, and Ru supported on m-VacG as potential SACs to examine the catalytic reaction. The stability and reactivity of SACs/ m-VacG were uncovered by molecular dynamics (MD) simulations, migration barrier calculation, and electronic structure analysis. The reaction of CO2 hydrogenation proceeds through two pathways starting from different initial states, i.e., the coadsorption of H-2 and CO2 on SACs/m-VacG (path A) and H-2 adsorption on SACs/m-VacG (path B). From the reaction pathways analysis, it is found that path B dominates the entire reaction thermodynamically with lower energy barrier compared with path A. Moreover, Pd supported on m-VacG is predicted to be the highest active SAC with the lowest energy barrier along the reaction path.
关键词	single-atom catalysts doped and defective carbon CO2 hydrogenation formic acid density functional theory
资助者	Southern University of Science and Technology, Shenzhen, China ; National Natural Science Foundation of China (NSFC) ; China Postdoc Council
DOI	10.1021/acsanm.1c00959
收录类别	SCI
语种	英语
资助项目	Southern University of Science and Technology, Shenzhen, China ; National Natural Science Foundation of China (NSFC)[51972312] ; China Postdoc Council
WOS研究方向	Science & Technology - Other Topics ; Materials Science
WOS类目	Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS记录号	WOS:000677582900040
出版者	AMER CHEMICAL SOC
引用统计	被引频次：58[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/159726
专题	中国科学院金属研究所
通讯作者	Ali, Sajjad
作者单位	1.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 3.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China 4.Hazara Univ, Dept Phys, Mansehra 21300, Pakistan 5.Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China
推荐引用方式 GB/T 7714	Ali, Sajjad,Iqbal, Rashid,Khan, Azim,et al. Stability and Catalytic Performance of Single-Atom Catalysts Supported on Doped and Defective Graphene for CO2 Hydrogenation to Formic Acid: A First-Principles Study[J]. ACS APPLIED NANO MATERIALS,2021,4(7):6893-6902.
APA	Ali, Sajjad,Iqbal, Rashid,Khan, Azim,Rehman, Shafiq Ur,Haneef, Muhammad,&Yin, Lichang.(2021).Stability and Catalytic Performance of Single-Atom Catalysts Supported on Doped and Defective Graphene for CO2 Hydrogenation to Formic Acid: A First-Principles Study.ACS APPLIED NANO MATERIALS,4(7),6893-6902.
MLA	Ali, Sajjad,et al."Stability and Catalytic Performance of Single-Atom Catalysts Supported on Doped and Defective Graphene for CO2 Hydrogenation to Formic Acid: A First-Principles Study".ACS APPLIED NANO MATERIALS 4.7(2021):6893-6902.