Revealing the origin of the reactivity of metal-free boron nitride catalysts in oxidative dehydrogenation of propane

doi:10.1016/j.apsusc.2020.146241

CORC > 金属研究所 > 中国科学院金属研究所

	Revealing the origin of the reactivity of metal-free boron nitride catalysts in oxidative dehydrogenation of propane
	Si, Chaowei 1,2; Lian, Zan 1,2; Olanrele, Samson O.1,2; Sun, XiaoYing 3; Li, Bo 1
刊名	APPLIED SURFACE SCIENCE
	2020-07-30
卷号	519 页码:8
关键词	Boron nitride Oxidative dehydrogenation Metal-free catalyst Reaction mechanism Density functional theory
ISSN号	0169-4332
DOI	10.1016/j.apsusc.2020.146241
通讯作者	Sun, XiaoYing(sunxiaoying78@163.com) ; Li, Bo(boli@imr.ac.cn)
英文摘要	Oxidative dehydrogenation (ODH) of propane is one of effective catalytic routes to produce value-added propene. Recently, boron nitride catalysts demonstrate extraordinary catalytic performance in ODH of propane with over 90% selectivity under 14% propane conversion. In this work, first principles calculations were performed to unravel the origin of activity of boron nitride catalyst. Three most active centers, including boron zigzag edge, nitrogen vacancies, and O = group, are identified from the screening propane first C-H bond activation among a large pool of candidates. The calculations verified the intrinsic reactivity of boron nitride which mostly comes from boron atoms at defective sites. The strong bonding between boron and carbon in propane dissociated fragments is accountable for the observed intrinsic reactivity. The detailed reaction pathway is revealed which cover from propene formation to active site regeneration. It is found that more critical step on pathway is regeneration rather than C-H bond activation. On the other hand, the active site could undergo conversion between each other at regeneration step. Furthermore, the deep dehydrogenation of propene is obstructed at the active site which uncovers the origin of high selectivity. Overall, current work gives a comprehensive description of catalytic properties of born nitride catalyst.
资助项目	NSFC[21573255] ; LiaoNing Natural Science Foundation[2019-ZD-0908] ; 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 (the second phase)[U1501501]
WOS研究方向	Chemistry ; Materials Science ; Physics
语种	英语
出版者	ELSEVIER
WOS记录号	WOS:000531753900005
资助机构	NSFC ; LiaoNing Natural Science Foundation ; 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 (the second phase)
内容类型	期刊论文
源URL	[http://ir.imr.ac.cn/handle/321006/138782]
专题	金属研究所_中国科学院金属研究所
通讯作者	Sun, XiaoYing; 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.Univ Sci & Technol China, Sch Mat Sci & Engn, Shenyang 110016, Liaoning, Peoples R China 3.ShenYang Normal Univ, Shenyang 110034, Liaoning, Peoples R China
推荐引用方式 GB/T 7714	Si, Chaowei,Lian, Zan,Olanrele, Samson O.,et al. Revealing the origin of the reactivity of metal-free boron nitride catalysts in oxidative dehydrogenation of propane[J]. APPLIED SURFACE SCIENCE,2020,519:8.
APA	Si, Chaowei,Lian, Zan,Olanrele, Samson O.,Sun, XiaoYing,&Li, Bo.(2020).Revealing the origin of the reactivity of metal-free boron nitride catalysts in oxidative dehydrogenation of propane.APPLIED SURFACE SCIENCE,519,8.
MLA	Si, Chaowei,et al."Revealing the origin of the reactivity of metal-free boron nitride catalysts in oxidative dehydrogenation of propane".APPLIED SURFACE SCIENCE 519(2020):8.