| 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 Author | Yang, Bing(byang@dicp.ac.cn) |
| 2020-11-04 | |
| Source Publication | CHEMCATCHEM
 |
| ISSN | 1867-3880 |
| Pages | 8 |
| Abstract | 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. |
| Keyword | cyclohexane oxidative dehydrogenation cyclohexene nanocatalysis |
| Funding Organization | Talents Innovation Project of Dalian ; Natural Science Foundation of China ; Foundation of Dalian Institute of Chemical Physics |
| DOI | 10.1002/cctc.202001380 |
| Indexed By | SCI |
| Language | 英语 |
| Funding Project | Talents Innovation Project of Dalian[2016RD04] ; Natural Science Foundation of China[21872145] ; Foundation of Dalian Institute of Chemical Physics[DICP I201943] |
| WOS Research Area | Chemistry |
| WOS Subject | Chemistry, Physical |
| WOS ID | WOS:000584508700001 |
| Publisher | WILEY-V C H VERLAG GMBH |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://ir.imr.ac.cn/handle/321006/141343 |
| Collection | 中国科学院金属研究所 |
| Corresponding Author | Yang, Bing |
| Affiliation | 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 |
| 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. |
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