Density Functional Theory Study of a Graphdiyne-Supported Single Au Atom Catalyst for Highly Efficient Acetylene Hydrochlorination

doi:10.1021/acsanm.1c00945

IMR OpenIR

	Density Functional Theory Study of a Graphdiyne-Supported Single Au Atom Catalyst for Highly Efficient Acetylene Hydrochlorination
	Ali, Sajjad 1,2; Lian, Zan 1; Li, Bo 1
通讯作者	Li, Bo(boli@imr.ac.cn)
	2021-06-25
发表期刊	ACS APPLIED NANO MATERIALS
ISSN	2574-0970
卷号	4 期号:6 页码:6152-6159
摘要	In this work, supported single Au on graphdiyne is examined as an efficient catalyst for acetylene hydrochlorination. The adsorption of reactants C2H2 and HCl has a paramount influence on the reaction mechanism. It is indicated that C2H2 adsorption is much stronger than the counterpart of HCl for most of the investigated cases. An Eley-Rideal (E-R) mechanism is first investigated, which is initiated with C2H2 adsorption. In the following steps, the adsorbed C2H2 becomes the site to bind and activate HCl, which leads to formation of the product. It is also revealed that single Au experienced a redox cycle along the reaction pathway. The largest barrier is calculated to be 0.57 eV, corresponding to the product desorption. On the other hand, a novel Langmuir-Hinshelwood (L-H)-like mechanism is also reported, which started with coadsorption of HCI and C2H2. It is noted that the barriers of the LH mechanism are smaller than those of the ER mechanism. Moreover, supported single Au on graphdiyne has much improved performance than the counterpart on pristine graphene and single-walled carbon nanotube support. This work clearly demonstrated the superior performance of supported single Au in acetylene hydrochlorination and the potential of novel support graphdiyne in single-atom catalysis.
关键词	single-atom catalyst graphdiyne acetylene hydrochlorination reaction mechanism density functional theory
资助者	National Natural Science Foundation of China ; ShenYang National Laboratory for Materials Science ; Southern University of Science and Technology ; China Postdoc Council ; Special Program for Applied Research on Super Computation of the NSFC Guangdong Joint Fund (the second phase)
DOI	10.1021/acsanm.1c00945
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China[21573255] ; ShenYang National Laboratory for Materials Science ; Southern University of Science and Technology ; China Postdoc Council ; Special Program for Applied Research on Super Computation of the NSFC Guangdong Joint Fund (the second phase)[U1501501]
WOS研究方向	Science & Technology - Other Topics ; Materials Science
WOS类目	Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS记录号	WOS:000668366800057
出版者	AMER CHEMICAL SOC
引用统计	被引频次：27[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/321006/160048
专题	中国科学院金属研究所
通讯作者	Li, Bo
作者单位	1.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Liaoning, Peoples R China 2.Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China
推荐引用方式 GB/T 7714	Ali, Sajjad,Lian, Zan,Li, Bo. Density Functional Theory Study of a Graphdiyne-Supported Single Au Atom Catalyst for Highly Efficient Acetylene Hydrochlorination[J]. ACS APPLIED NANO MATERIALS,2021,4(6):6152-6159.
APA	Ali, Sajjad,Lian, Zan,&Li, Bo.(2021).Density Functional Theory Study of a Graphdiyne-Supported Single Au Atom Catalyst for Highly Efficient Acetylene Hydrochlorination.ACS APPLIED NANO MATERIALS,4(6),6152-6159.
MLA	Ali, Sajjad,et al."Density Functional Theory Study of a Graphdiyne-Supported Single Au Atom Catalyst for Highly Efficient Acetylene Hydrochlorination".ACS APPLIED NANO MATERIALS 4.6(2021):6152-6159.