Molybdenum Carbide Modified Nanocarbon Catalysts for Alkane Dehydrogenation Reactions | |
Liu, Wei; Chen, Bingxu; Duan, Xuezhi; Wu, Kuang-Hsu; Qi, Wei; Guo, Xiaoling; Zhang, Bingsen; Su, Dangsheng; Qi, W; Su, DS (reprint author), Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, 72 Wenhua Rd, Shenyang 110016, Liaoning, Peoples R China. | |
刊名 | AMER CHEMICAL SOC |
2017-09-01 | |
卷号 | 7期号:9页码:5820-5827 |
关键词 | Nanocarbon Molybdenum Carbide C-h Bond Activation Dehydrogenation Hybrid Catalysts |
ISSN号 | 2155-5435 |
英文摘要 | Nucleophilic sites on nanocarbon catalysts act as promoters for homolytic cleavage of aliphatic C-H bond. In this study, we report a hybrid catalyst composed of Mo2C and nitrogen-doped onion-like carbon (NOLC) with enhanced capability for C-H bond activation in direct dehydrogenation (DH) reaction of ethylbenzene (EB). The enhanced activity of the Mo2C/NOLC catalyst over unmodified NOLC in EB DH is attributable to the promoted C-H bond activation by Mo2C, as characterized by the lower activation energy and the kinetic isotope effect using deuterated EB. Our XPS, XRD, and Raman spectroscopy results show that the hybrid catalyst is structurally robust under the reaction condition. The increase in nucleophilicity of the oxygen active sites in NOLC is evidenced by an overall shift of the O is peaks to lower binding energies after Mo2C modification. The DFT calculation further provides mechanistic insights into the electron-transfer process from Mo2C to the ketonic carbonyl groups.; Nucleophilic sites on nanocarbon catalysts act as promoters for homolytic cleavage of aliphatic C-H bond. In this study, we report a hybrid catalyst composed of Mo2C and nitrogen-doped onion-like carbon (NOLC) with enhanced capability for C-H bond activation in direct dehydrogenation (DH) reaction of ethylbenzene (EB). The enhanced activity of the Mo2C/NOLC catalyst over unmodified NOLC in EB DH is attributable to the promoted C-H bond activation by Mo2C, as characterized by the lower activation energy and the kinetic isotope effect using deuterated EB. Our XPS, XRD, and Raman spectroscopy results show that the hybrid catalyst is structurally robust under the reaction condition. The increase in nucleophilicity of the oxygen active sites in NOLC is evidenced by an overall shift of the O is peaks to lower binding energies after Mo2C modification. The DFT calculation further provides mechanistic insights into the electron-transfer process from Mo2C to the ketonic carbonyl groups. |
学科主题 | Chemistry, Physical |
语种 | 英语 |
资助机构 | NSFC of China [91645114, 21573256, 2161101164, 51521091]; "Joint Research Program of Natural Science Foundation of Liaoning Province-Shenyang National Laboratory for Materials Science" [2015021010]; Youth Innovation Promotion Association, CAS |
公开日期 | 2018-01-10 |
内容类型 | 期刊论文 |
源URL | [http://ir.imr.ac.cn/handle/321006/79125] |
专题 | 金属研究所_中国科学院金属研究所 |
通讯作者 | Qi, W; Su, DS (reprint author), Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, 72 Wenhua Rd, Shenyang 110016, Liaoning, Peoples R China.; Su, DS (reprint author), Univ Chinese Acad Sci, Beijing 100049, Peoples R China. |
推荐引用方式 GB/T 7714 | Liu, Wei,Chen, Bingxu,Duan, Xuezhi,et al. Molybdenum Carbide Modified Nanocarbon Catalysts for Alkane Dehydrogenation Reactions[J]. AMER CHEMICAL SOC,2017,7(9):5820-5827. |
APA | Liu, Wei.,Chen, Bingxu.,Duan, Xuezhi.,Wu, Kuang-Hsu.,Qi, Wei.,...&Su, DS .(2017).Molybdenum Carbide Modified Nanocarbon Catalysts for Alkane Dehydrogenation Reactions.AMER CHEMICAL SOC,7(9),5820-5827. |
MLA | Liu, Wei,et al."Molybdenum Carbide Modified Nanocarbon Catalysts for Alkane Dehydrogenation Reactions".AMER CHEMICAL SOC 7.9(2017):5820-5827. |
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