COx-Resistant Oxidative Dehydrogenation of Cyclohexane Catalyzed by sp(3)@sp(2) Nanodiamonds towards Highly Selective Cyclohexene Production

doi:10.1002/cctc.202001380

IMR OpenIR

	COx-Resistant Oxidative Dehydrogenation of Cyclohexane Catalyzed by sp(3)@sp(2) Nanodiamonds towards Highly Selective Cyclohexene Production
	Du, Pengfei 1,2; Zhang, Xin-Xing 3,4; Zhang, Shaoqian 5; Zhao, Yang 1; Zhang, Liyun 6; Zhang, Bingsen 6; Yang, Bing 1
通讯作者	Yang, Bing(byang@dicp.ac.cn)
	2020-11-04
发表期刊	CHEMCATCHEM
ISSN	1867-3880
页码	8
摘要	Deep oxidation/dehydrogenation are longstanding problems for decades in catalytic oxidative dehydrogenation (ODH) of cyclohexane and other alkanes. Here we show a metal-free catalyst of nanodiamonds (NDs) with unique sp(3)@sp(2) hybrid structure that catalyzes COx-resistant cyclohexane ODH with remarkable reactivity towards cyclohexene production. The selectivity of cyclohexene can reach as high as 67 % with significantly suppressed COx emission (<5 %), which is on top of the highest reported values among other metal(oxide)/metal-free catalysts. Structural evolution of sp(3)@sp(2) NDs under annealing treatments and their specific surface functional groups are systematically studied using TEM, XPS, Raman and TPD. By comparing with carbon nanotubes (CNTs), we found that the carbonyl groups stabilized on strained sp(3)@sp(2) core-shell NDs enhanced the cyclohexene selectivity via preferential cleavage of C-H over C-C bond. Kinetic studies further revealed the underlying reaction pathways that cyclohexane is rapidly dehydrogenated to cyclohexene which subsequently transforms into benzene (fast) and COx (slow). Deep oxidation of both cyclic hydrocarbons is largely suppressed due to the low density of electrophilic functional groups on strongly curved graphitic surface of sp(3)@sp(2) NDs.
关键词	cyclohexane oxidative dehydrogenation cyclohexene nanocatalysis
资助者	Talents Innovation Project of Dalian ; Natural Science Foundation of China ; Foundation of Dalian Institute of Chemical Physics
DOI	10.1002/cctc.202001380
收录类别	SCI
语种	英语
资助项目	Talents Innovation Project of Dalian[2016RD04] ; Natural Science Foundation of China[21872145] ; Foundation of Dalian Institute of Chemical Physics[DICP I201943]
WOS研究方向	Chemistry
WOS类目	Chemistry, Physical
WOS记录号	WOS:000584508700001
出版者	WILEY-V C H VERLAG GMBH
引用统计	被引频次：5[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/321006/141343
专题	中国科学院金属研究所
通讯作者	Yang, Bing
作者单位	1.Chinese Acad Sci, Dalian Natl Lab Clean Energy, Dalian Inst Chem Phys, 457 Zhongshan Rd, Dalian 116023, Peoples R China 2.Univ Chinese Acad Sci, 19 Yuquan Rd, Beijing 100049, Peoples R China 3.Univ Chicago, James Franck Inst, Dept Chem, Chicago, IL 60637 USA 4.Univ Chicago, Inst Biophys Dynam, Chicago, IL 60637 USA 5.Chinese Acad Sci, Key Lab Chem Lasers, Dalian Inst Chem Phys, 457 Zhongshan Rd, Dalian 116023, Peoples R China 6.Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, 72 Wenhua Rd, Shenyang 110016, Peoples R China
推荐引用方式 GB/T 7714	Du, Pengfei,Zhang, Xin-Xing,Zhang, Shaoqian,et al. COx-Resistant Oxidative Dehydrogenation of Cyclohexane Catalyzed by sp(3)@sp(2) Nanodiamonds towards Highly Selective Cyclohexene Production[J]. CHEMCATCHEM,2020:8.
APA	Du, Pengfei.,Zhang, Xin-Xing.,Zhang, Shaoqian.,Zhao, Yang.,Zhang, Liyun.,...&Yang, Bing.(2020).COx-Resistant Oxidative Dehydrogenation of Cyclohexane Catalyzed by sp(3)@sp(2) Nanodiamonds towards Highly Selective Cyclohexene Production.CHEMCATCHEM,8.
MLA	Du, Pengfei,et al."COx-Resistant Oxidative Dehydrogenation of Cyclohexane Catalyzed by sp(3)@sp(2) Nanodiamonds towards Highly Selective Cyclohexene Production".CHEMCATCHEM (2020):8.