Probing the reaction mechanism of acetylene hydrochlorination on metal-free doped boron nitride: Decisive role of carbon dopant

doi:10.1016/j.apsusc.2021.150710

CORC > 金属研究所 > 中国科学院金属研究所

	Probing the reaction mechanism of acetylene hydrochlorination on metal-free doped boron nitride: Decisive role of carbon dopant
	Si, Chaowei ; Lian, Zan ; Yang, Min ; Li, Bo 1
刊名	APPLIED SURFACE SCIENCE
	2021-11-15
卷号	566 页码:7
关键词	Metal-free catalysis Boron Nitride DFT Acetylene hydroclorination Carbon doping
ISSN号	0169-4332
DOI	10.1016/j.apsusc.2021.150710
通讯作者	Li, Bo(boli@imr.ac.cn)
英文摘要	As emerging as highly active metal-free acetylene hydrochlorination catalyst, recently boron nitride attracted great attentions from both experimental and computational explorations. In this work, the carbon doping is verified to be indispensable to trigger the activities of pristine h-BN catalyst from first principles calculations. The effects on electronic structure of h-BN induced by carbon doping are examined from ELF, PDOS, and charge analysis which have direct impacts on the catalytic capabilities. The pathways can be categorized to be either C2H2 or HCl adsorption as first step. Although these two categories have distinct limiting step and mechanism, the shared feature is that the activation of C2H2 is key to the vinyl chloride formation. Furthermore, TOFs of different pathways are calculated to determine the most favorable catalytic route and is in a qualitatively agreement with largest barrier of elementary step. The importance of HCl-starting pathway is revealed from the comparison of TOF which is severely underestimated previously. In the end, the deep reactions which might be leading to precursor of cokes are explored and shed lights on the origin of superior stability of catalyst.
资助项目	National Natural Science Foundation of China[21573255] ; Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science ; State Key Laboratory of Catalytic Materials and Reaction Engineering (RIPP, SINOPEC) ; Special Program for Applied Research on Super Computation of the NSFC Guangdong Joint Fund[U1501501]
WOS研究方向	Chemistry ; Materials Science ; Physics
语种	英语
出版者	ELSEVIER
WOS记录号	WOS:000692110900003
资助机构	National Natural Science Foundation of China ; Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science ; State Key Laboratory of Catalytic Materials and Reaction Engineering (RIPP, SINOPEC) ; Special Program for Applied Research on Super Computation of the NSFC Guangdong Joint Fund
内容类型	期刊论文
源URL	[http://ir.imr.ac.cn/handle/321006/166889]
专题	金属研究所_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 Materials Sci, Shenyang 110016, Liaoning, Peoples R China 2.Univ Sci & Technol China, Sch Mat Sci & Engn, Shenyang 110016, Liaoning, Peoples R China
推荐引用方式 GB/T 7714	Si, Chaowei,Lian, Zan,Yang, Min,et al. Probing the reaction mechanism of acetylene hydrochlorination on metal-free doped boron nitride: Decisive role of carbon dopant[J]. APPLIED SURFACE SCIENCE,2021,566:7.
APA	Si, Chaowei,Lian, Zan,Yang, Min,&Li, Bo.(2021).Probing the reaction mechanism of acetylene hydrochlorination on metal-free doped boron nitride: Decisive role of carbon dopant.APPLIED SURFACE SCIENCE,566,7.
MLA	Si, Chaowei,et al."Probing the reaction mechanism of acetylene hydrochlorination on metal-free doped boron nitride: Decisive role of carbon dopant".APPLIED SURFACE SCIENCE 566(2021):7.