| 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 Author | Qi, Wei(wqi@imr.ac.cn) |
| 2020-08-07 | |
| Source Publication | CATALYSIS SCIENCE & TECHNOLOGY
 |
| ISSN | 2044-4753 |
| Volume | 10Issue:15Pages:4952-4959 |
| Abstract | 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. |
| Funding Organization | NSFC of China ; Youth Innovation Promotion Association, CAS ; Deutsche Bundesstiftung Umwelt (DBU) ; Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) |
| DOI | 10.1039/d0cy00619j |
| Indexed By | SCI |
| Language | 英语 |
| Funding Project | 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 Research Area | Chemistry |
| WOS Subject | Chemistry, Physical |
| WOS ID | WOS:000556422000037 |
| Publisher | ROYAL SOC CHEMISTRY |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://ir.imr.ac.cn/handle/321006/140136 |
| Collection | 中国科学院金属研究所 |
| Corresponding Author | Qi, Wei |
| Affiliation | 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 |
| 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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