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 3,5; Iqbal, Rashid 2; Khan, Azim 3; Rehman, Shafiq Ur 4; Haneef, Muhammad 1; Yin, Lichang 3
刊名	ACS APPLIED NANO MATERIALS
	2021-07-23
卷号	4 期号:7 页码:6893-6902
关键词	single-atom catalysts doped and defective carbon CO2 hydrogenation formic acid density functional theory
ISSN号	2574-0970
DOI	10.1021/acsanm.1c00959
通讯作者	Ali, Sajjad(sajjad@alum.imr.ac.cn)
英文摘要	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.
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
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000677582900040
资助机构	Southern University of Science and Technology, Shenzhen, China ; National Natural Science Foundation of China (NSFC) ; China Postdoc Council
内容类型	期刊论文
源URL	[http://ir.imr.ac.cn/handle/321006/159725]
专题	金属研究所_中国科学院金属研究所
通讯作者	Ali, Sajjad
作者单位	1.Hazara Univ, Dept Phys, Mansehra 21300, Pakistan 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 4.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China 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.