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

doi:10.1039/d0cy00619j

CORC > 金属研究所 > 中国科学院金属研究所

	Methanol oxidative dehydrogenation and dehydration on carbon nanotubes: active sites and basic reaction kinetics
	Yan, Pengqiang 1,2; Zhang, Xuefei 2; Herold, Felix 3; Li, Fan 2; Dai, Xueya 2; Cao, Tianlong 2; Etzold, Bastian J. M.3; Qi, Wei 2
刊名	CATALYSIS SCIENCE & TECHNOLOGY
	2020-08-07
卷号	10 期号:15 页码:4952-4959
ISSN号	2044-4753
DOI	10.1039/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
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000556422000037
资助机构	NSFC of China ; Youth Innovation Promotion Association, CAS ; Deutsche Bundesstiftung Umwelt (DBU) ; Deutsche Forschungsgemeinschaft (DFG, German Research Foundation)
内容类型	期刊论文
源URL	[http://ir.imr.ac.cn/handle/321006/140135]
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.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 3.Tech Univ Darmstadt, Ernst Berl Inst Tech & Makromol Chem, D-64287 Darmstadt, Germany
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.