IMR OpenIR
COx-Resistant Oxidative Dehydrogenation of Cyclohexane Catalyzed by sp(3)@sp(2) Nanodiamonds towards Highly Selective Cyclohexene Production
Du, Pengfei1,2; Zhang, Xin-Xing3,4; Zhang, Shaoqian5; Zhao, Yang1; Zhang, Liyun6; Zhang, Bingsen6; Yang, Bing1
Corresponding AuthorYang, Bing(byang@dicp.ac.cn)
2020-11-04
Source PublicationCHEMCATCHEM
ISSN1867-3880
Pages8
AbstractDeep 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.
Keywordcyclohexane oxidative dehydrogenation cyclohexene nanocatalysis
Funding OrganizationTalents Innovation Project of Dalian ; Natural Science Foundation of China ; Foundation of Dalian Institute of Chemical Physics
DOI10.1002/cctc.202001380
Indexed BySCI
Language英语
Funding ProjectTalents Innovation Project of Dalian[2016RD04] ; Natural Science Foundation of China[21872145] ; Foundation of Dalian Institute of Chemical Physics[DICP I201943]
WOS Research AreaChemistry
WOS SubjectChemistry, Physical
WOS IDWOS:000584508700001
PublisherWILEY-V C H VERLAG GMBH
Citation statistics
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/141343
Collection中国科学院金属研究所
Corresponding AuthorYang, Bing
Affiliation1.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
Recommended Citation
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.
Files in This Item:
There are no files associated with this item.
Related Services
Recommend this item
Bookmark
Usage statistics
Export to Endnote
Google Scholar
Similar articles in Google Scholar
[Du, Pengfei]'s Articles
[Zhang, Xin-Xing]'s Articles
[Zhang, Shaoqian]'s Articles
Baidu academic
Similar articles in Baidu academic
[Du, Pengfei]'s Articles
[Zhang, Xin-Xing]'s Articles
[Zhang, Shaoqian]'s Articles
Bing Scholar
Similar articles in Bing Scholar
[Du, Pengfei]'s Articles
[Zhang, Xin-Xing]'s Articles
[Zhang, Shaoqian]'s Articles
Terms of Use
No data!
Social Bookmark/Share
All comments (0)
No comment.
 

Items in the repository are protected by copyright, with all rights reserved, unless otherwise indicated.