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COx-Resistant Oxidative Dehydrogenation of Cyclohexane Catalyzed by sp(3)@sp(2) Nanodiamonds towards Highly Selective Cyclohexene Production
Du, Pengfei; Zhang, Xin-Xing; Zhang, Shaoqian; Zhao, Yang; Zhang, Liyun; Zhang, Bingsen; Yang, Bing
2020-11-04
Source PublicationCHEMCATCHEM
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.
DOI10.1002/cctc.202001380
WOS IDWOS:000584508700001
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Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/82374
Collection中国科学院金属研究所
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.
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.
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).
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