COx-Resistant Oxidative Dehydrogenation of Cyclohexane Catalyzed by sp(3)@sp(2) Nanodiamonds towards Highly Selective Cyclohexene Production
文献类型：期刊论文
| 作者 | Du, Pengfei2,3; Zhang, Xin-Xing4,5; Zhang, Shaoqian1; Zhao, Yang2; Zhang, Liyun6; Zhang, Bingsen6; Yang, Bing2 |
| 刊名 | CHEMCATCHEM
 |
| 出版日期 | 2020-11-04 |
| 页码 | 8 |
| 关键词 | cyclohexane oxidative dehydrogenation cyclohexene nanocatalysis |
| ISSN号 | 1867-3880 |
| DOI | 10.1002/cctc.202001380 |
| 通讯作者 | Yang, Bing(byang@dicp.ac.cn) |
| 英文摘要 | 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. |
| 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 |
| 语种 | 英语 |
| WOS记录号 | WOS:000584508700001 |
| 出版者 | WILEY-V C H VERLAG GMBH |
| 资助机构 | Talents Innovation Project of Dalian ; Natural Science Foundation of China ; Foundation of Dalian Institute of Chemical Physics |
| 源URL | [http://ir.imr.ac.cn/handle/321006/141342]  |
| 专题 | 金属研究所_中国科学院金属研究所 |
| 通讯作者 | Yang, Bing |
| 作者单位 | 1.Chinese Acad Sci, Key Lab Chem Lasers, Dalian Inst Chem Phys, 457 Zhongshan Rd, Dalian 116023, Peoples R China 2.Chinese Acad Sci, Dalian Natl Lab Clean Energy, Dalian Inst Chem Phys, 457 Zhongshan Rd, Dalian 116023, Peoples R China 3.Univ Chinese Acad Sci, 19 Yuquan Rd, Beijing 100049, Peoples R China 4.Univ Chicago, James Franck Inst, Dept Chem, Chicago, IL 60637 USA 5.Univ Chicago, Inst Biophys Dynam, Chicago, IL 60637 USA 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. |
入库方式： OAI收割
来源：金属研究所
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