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Nitrogen-doped carbon nanotubes as bifunctional catalysts with enhanced catalytic performance for selective oxidation of ethanol
Wang, Jia; Huang, Rui; Zhang, Yajie; Diao, Jiangyong; Zhang, Jiayun; Liu, Hongyang; Su, Dangsheng; Liu, HY; Su, DS (reprint author), Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, Shenyang 110016, Peoples R China.
2017
发表期刊CARBON
ISSN0008-6223
卷号111页码:519-528
摘要The gas-phase selective oxidation of ethanol to acetaldehyde is a promising alternative to current Wacker process in which ethylene is catalyzed to acetaldehyde by palladium and copper chlorides in strong acidic solutions. The supported gold catalyst has been reported and showed excellent catalytic performance in gas-phase oxidation of ethanol. But its high price stimulates the studies to focus on non-noble metal catalysts, or non-metal catalysts. Here, we report that nitrogen-doped carbon nanotubes as a bifunctional catalyst exhibits robust performance in the selective oxidation of ethanol to acetaldehyde. A stable catalytic,performance with ethanol conversion of 72% and acetaldehyde selectivity of 90% at 270 degrees C was obtained. The substantial enhancement of acetaldehyde yield was ascribed to the synergistic effect of synchronously promoting the dissociative adsorption of O-2 and ethanol adsorption when incorporating graphite-like and pyridine-like nitrogen species. The kinetic analysis indicates that the introduction of nitrogen species can significantly decrease the activation energy of the reaction. The study of this bifunctional carbocatalyst may also provide guidance for the design of new carbon-based catalytic systems for the selective oxidation of alcohols via regulating the adsorption and activation ability of catalyst to reactants. (C) 2016 Elsevier Ltd. All rights reserved.; The gas-phase selective oxidation of ethanol to acetaldehyde is a promising alternative to current Wacker process in which ethylene is catalyzed to acetaldehyde by palladium and copper chlorides in strong acidic solutions. The supported gold catalyst has been reported and showed excellent catalytic performance in gas-phase oxidation of ethanol. But its high price stimulates the studies to focus on non-noble metal catalysts, or non-metal catalysts. Here, we report that nitrogen-doped carbon nanotubes as a bifunctional catalyst exhibits robust performance in the selective oxidation of ethanol to acetaldehyde. A stable catalytic,performance with ethanol conversion of 72% and acetaldehyde selectivity of 90% at 270 degrees C was obtained. The substantial enhancement of acetaldehyde yield was ascribed to the synergistic effect of synchronously promoting the dissociative adsorption of O-2 and ethanol adsorption when incorporating graphite-like and pyridine-like nitrogen species. The kinetic analysis indicates that the introduction of nitrogen species can significantly decrease the activation energy of the reaction. The study of this bifunctional carbocatalyst may also provide guidance for the design of new carbon-based catalytic systems for the selective oxidation of alcohols via regulating the adsorption and activation ability of catalyst to reactants. (C) 2016 Elsevier Ltd. All rights reserved.
部门归属[wang, jia ; huang, rui ; zhang, yajie ; diao, jiangyong ; zhang, jiayun ; liu, hongyang ; su, dangsheng] chinese acad sci, shenyang natl lab mat sci, inst met res, shenyang 110016, peoples r china ; [zhang, yajie ; zhang, jiayun] univ sci & technol china, sch chem & mat sci, hefei 230026, peoples r china
学科领域Chemistry, Physical ; Materials Science, Multidisciplinary
资助者Ministry of Science and Technology (MOST) [2016YFA0204100]; National Natural Science Foundation of China [21573254, 91545110, 21133010, 51221264, 21261160487, 11504386, 21403261]; Youth Innovation Promotion Association (CAS); Sinopec China; MOST [2011CBA00504]; "Strategic Priority Research Program" of the Chinese Academy of Sciences [XDA09030103]
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/321006/78385
专题中国科学院金属研究所
通讯作者Liu, HY; Su, DS (reprint author), Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, Shenyang 110016, Peoples R China.
推荐引用方式
GB/T 7714
Wang, Jia,Huang, Rui,Zhang, Yajie,et al. Nitrogen-doped carbon nanotubes as bifunctional catalysts with enhanced catalytic performance for selective oxidation of ethanol[J]. CARBON,2017,111:519-528.
APA Wang, Jia.,Huang, Rui.,Zhang, Yajie.,Diao, Jiangyong.,Zhang, Jiayun.,...&Su, DS .(2017).Nitrogen-doped carbon nanotubes as bifunctional catalysts with enhanced catalytic performance for selective oxidation of ethanol.CARBON,111,519-528.
MLA Wang, Jia,et al."Nitrogen-doped carbon nanotubes as bifunctional catalysts with enhanced catalytic performance for selective oxidation of ethanol".CARBON 111(2017):519-528.
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