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Methanol oxidative dehydrogenation and dehydration on carbon nanotubes: active sites and basic reaction kinetics
Yan, Pengqiang1,2; Zhang, Xuefei1; Herold, Felix3; Li, Fan1; Dai, Xueya1; Cao, Tianlong1; Etzold, Bastian J. M.3; Qi, Wei1
Corresponding AuthorQi, Wei(wqi@imr.ac.cn)
2020-08-07
Source PublicationCATALYSIS SCIENCE & TECHNOLOGY
ISSN2044-4753
Volume10Issue:15Pages:4952-4959
AbstractMethanol 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.
Funding OrganizationNSFC of China ; Youth Innovation Promotion Association, CAS ; Deutsche Bundesstiftung Umwelt (DBU) ; Deutsche Forschungsgemeinschaft (DFG, German Research Foundation)
DOI10.1039/d0cy00619j
Indexed BySCI
Language英语
Funding ProjectNSFC 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 Research AreaChemistry
WOS SubjectChemistry, Physical
WOS IDWOS:000556422000037
PublisherROYAL SOC CHEMISTRY
Citation statistics
Cited Times:5[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/140137
Collection中国科学院金属研究所
Corresponding AuthorQi, Wei
Affiliation1.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
Recommended Citation
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.
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