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Methanol oxidative dehydrogenation and dehydration on carbon nanotubes: active sites and basic reaction kinetics

文献类型：期刊论文

作者Yan, Pengqiang1,3; Zhang, Xuefei1; Herold, Felix2; Li, Fan1; Dai, Xueya1; Cao, Tianlong1; Etzold, Bastian J. M.2; Qi, Wei1
刊名CATALYSIS SCIENCE & TECHNOLOGY
出版日期2020-08-07
卷号10期号:15页码:4952-4959
ISSN号2044-4753
DOI10.1039/d0cy00619j
通讯作者Qi, Wei(wqi@imr.ac.cn)
英文摘要Methanol dehydrogenation to formaldehyde or dehydration to dimethyl ether are high-value-added industrial processes. Here, we applied oxidized multi-walled carbon nanotubes (oCNTs) in a methanol conversion reaction in the presence of oxygen. oCNT catalysts exhibit a methanol conversion of 60% under gentle reaction conditions, yielding DME (65%) and FA (30%) as the main products, and long term stability for over 150 h is achieved. The catalytic performance of oCNTs is even comparable to industrial metal catalysts. An in situ site titration experiment revealed that carboxyl groups were the active sites for the formation of dimethyl ether. Small organic molecules as model catalysts suggested that quinoidic carbonyl groups may be responsible for methanol ODH producing formaldehyde, while both quinoidic and ketonic carbonyl groups are responsible for total oxidation to carbon dioxide. Basic reaction kinetics and mechanisms such as reaction orders, apparent activation energy, rate determining step, etc. for the oxidative dehydrogenation and dehydration of methanol were studied systematically. A unique gentle redox catalytic activity of oCNT catalysts could be realized to reduce the overoxidation losses.
资助项目NSFC of China[21761132010] ; NSFC of China[91645114] ; NSFC of China[21573256] ; Youth Innovation Promotion Association, CAS ; Deutsche Bundesstiftung Umwelt (DBU) ; Deutsche Forschungsgemeinschaft (DFG, German Research Foundation)[ET-101/13-1]
WOS研究方向Chemistry
语种英语
WOS记录号WOS:000556422000037
出版者ROYAL SOC CHEMISTRY
资助机构NSFC of China ; Youth Innovation Promotion Association, CAS ; Deutsche Bundesstiftung Umwelt (DBU) ; Deutsche Forschungsgemeinschaft (DFG, German Research Foundation)
源URL[http://ir.imr.ac.cn/handle/321006/140134]  
专题金属研究所_中国科学院金属研究所
通讯作者Qi, Wei
作者单位1.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China
2.Tech Univ Darmstadt, Ernst Berl Inst Tech & Makromol Chem, D-64287 Darmstadt, Germany
3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
推荐引用方式
GB/T 7714		 Yan, Pengqiang,Zhang, Xuefei,Herold, Felix,et al. Methanol oxidative dehydrogenation and dehydration on carbon nanotubes: active sites and basic reaction kinetics[J]. CATALYSIS SCIENCE & TECHNOLOGY,2020,10(15):4952-4959.
APA Yan, Pengqiang.,Zhang, Xuefei.,Herold, Felix.,Li, Fan.,Dai, Xueya.,...&Qi, Wei.(2020).Methanol oxidative dehydrogenation and dehydration on carbon nanotubes: active sites and basic reaction kinetics.CATALYSIS SCIENCE & TECHNOLOGY,10(15),4952-4959.
MLA Yan, Pengqiang,et al."Methanol oxidative dehydrogenation and dehydration on carbon nanotubes: active sites and basic reaction kinetics".CATALYSIS SCIENCE & TECHNOLOGY 10.15(2020):4952-4959.

入库方式： OAI收割

来源：金属研究所

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