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

doi:10.1039/d0cy00619j

IMR OpenIR

	Methanol oxidative dehydrogenation and dehydration on carbon nanotubes: active sites and basic reaction kinetics
	Yan, Pengqiang 1,2; Zhang, Xuefei 1; Herold, Felix 3; Li, Fan 1; Dai, Xueya 1; Cao, Tianlong 1; Etzold, Bastian J. M.3; Qi, Wei 1
通讯作者	Qi, Wei(wqi@imr.ac.cn)
	2020-08-07
发表期刊	CATALYSIS SCIENCE & TECHNOLOGY
ISSN	2044-4753
卷号	10 期号:15 页码:4952-4959
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.
资助者	NSFC of China ; Youth Innovation Promotion Association, CAS ; Deutsche Bundesstiftung Umwelt (DBU) ; Deutsche Forschungsgemeinschaft (DFG, German Research Foundation)
DOI	10.1039/d0cy00619j
收录类别	SCI
语种	英语
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
WOS类目	Chemistry, Physical
WOS记录号	WOS:000556422000037
出版者	ROYAL SOC CHEMISTRY
引用统计	被引频次：25[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/140136
专题	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.Univ Chinese Acad Sci, Beijing 100049, 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.