Screening of active center and reactivity descriptor in acetylene hydrochlorination on metal-free doped carbon catalysts from first principle calculations

doi:10.1016/j.apsusc.2019.02.007

IMR OpenIR

	Screening of active center and reactivity descriptor in acetylene hydrochlorination on metal-free doped carbon catalysts from first principle calculations
	Ali, Sajjad 1,2; Qiu, YiYang 4; Lian, Zan 1,3; Olanrele, Samson 1,3; Lan, GuoJun 4; Li, Ying 4; Su, Dang Sheng 1; Li, Bo 1
通讯作者	Li, Ying(liying@zjut.edu.cn) ; Su, Dang Sheng(dssu@imr.ac.cn) ; Li, Bo(boli@imr.ac.cn)
	2019-06-01
发表期刊	APPLIED SURFACE SCIENCE
ISSN	0169-4332
卷号	478 页码:574-580
摘要	In this work, first principle DFT calculations are carried out to identify the active center and reveal the reaction pathway on nitrogen and boron doped carbon catalysts in acetylene hydrochlorination. Various different dopant configurations including pyridine, graphitic, and pyrrolic are explored and compared. The different geometries of dopants give the distinct electronic structure, which indicate that pyridine configuration with three dopants around a vacancy, have more states around Fermi level. The adsorption of acetylene (C2H2) is predicted to be the first step of the reaction as it has much bigger binding energy than another reactant, HCl. Boron and nitrogen doping exhibit opposite effect on the charge transfer between adsorbed C2H2 and the catalyst. The curvature of tube also influences acetylene adsorption and the binding energy decreases with increasing tube diameter. Moreover, the detailed reaction pathway is revealed from the calculations. A balanced activity for C2H2 adsorption and HCl activation is required to improve catalytic performance and too strong binding of C2H2 hinders the followed steps on the pathway and cause large barrier. This work clarify the confusions facing by the metal-free doped carbon catalyst and lay out solid base for the future improvements in acetylene hydrochlorination.
关键词	Metal free catalyst Dopants Acetylene hydrochlorination Density functional theory
资助者	NSFC ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Liaoning Provincial Natural Science Foundation ; Institute of Metal Research, Chinese Academy of Sciences ; 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 (the second phase)
DOI	10.1016/j.apsusc.2019.02.007
收录类别	SCI
语种	英语
资助项目	NSFC[21573255] ; NSFC[51521091] ; Strategic Priority Research Program of the Chinese Academy of Sciences[XDA09030103] ; Liaoning Provincial Natural Science Foundation[20180510014] ; Institute of Metal Research, Chinese Academy of Sciences[Y3NBA211A1] ; 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 (the second phase)[U1501501]
WOS研究方向	Chemistry ; Materials Science ; Physics
WOS类目	Chemistry, Physical ; Materials Science, Coatings & Films ; Physics, Applied ; Physics, Condensed Matter
WOS记录号	WOS:000461150400069
出版者	ELSEVIER SCIENCE BV
引用统计	被引频次：22[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/321006/132111
专题	中国科学院金属研究所
通讯作者	Li, Ying; Su, Dang Sheng; Li, Bo
作者单位	1.Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, Shenyang 110016, Liaoning, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Univ Sci & Technol China, Sch Mat Sci & Engn, Shenyang 110016, Liaoning, Peoples R China 4.Zhejiang Univ Technol, Inst Ind Catalysis, Chaowang Rd 18, Hangzhou, Zhejiang, Peoples R China
推荐引用方式 GB/T 7714	Ali, Sajjad,Qiu, YiYang,Lian, Zan,et al. Screening of active center and reactivity descriptor in acetylene hydrochlorination on metal-free doped carbon catalysts from first principle calculations[J]. APPLIED SURFACE SCIENCE,2019,478:574-580.
APA	Ali, Sajjad.,Qiu, YiYang.,Lian, Zan.,Olanrele, Samson.,Lan, GuoJun.,...&Li, Bo.(2019).Screening of active center and reactivity descriptor in acetylene hydrochlorination on metal-free doped carbon catalysts from first principle calculations.APPLIED SURFACE SCIENCE,478,574-580.
MLA	Ali, Sajjad,et al."Screening of active center and reactivity descriptor in acetylene hydrochlorination on metal-free doped carbon catalysts from first principle calculations".APPLIED SURFACE SCIENCE 478(2019):574-580.