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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.; Su, DS (reprint author), Univ Chinese Acad Sci, Beijing 100049, Peoples R China.
2017-09-01
发表期刊AMER CHEMICAL SOC
ISSN2155-5435
卷号7期号:9页码:5820-5827
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.
部门归属[liu, wei ; wu, kuang-hsu ; qi, wei ; guo, xiaoling ; zhang, bingsen ; su, dangsheng] chinese acad sci, shenyang natl lab mat sci, inst met res, 72 wenhua rd, shenyang 110016, liaoning, peoples r china ; [liu, wei ; qi, wei ; zhang, bingsen ; su, dangsheng] univ chinese acad sci, beijing 100049, peoples r china ; [chen, bingxu ; duan, xuezhi] east china univ sci & technol, state key lab chem engn, 130 meilong rd, shanghai 200237, peoples r china ; [wu, kuang-hsu] univ new south wales, sch chem engn, sydney, nsw 2052, australia
关键词Nanocarbon Molybdenum Carbide C-h Bond Activation Dehydrogenation Hybrid Catalysts
学科领域Chemistry, Physical
资助者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
收录类别SCI
语种英语
文献类型期刊论文
条目标识符http://ir.imr.ac.cn/handle/321006/79125
专题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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