| A promising plasma-catalytic approach towards single-step methane conversion to oxygenates at room temperature | |
Chawdhury, Piu1; Wang, Yaolin2; Ray, Debjyoti1; Mathieu, Stephanie2; Wang, Ni2; Harding, Jonathan2; Bin F(宾峰)2,3 ; Tu, Xin2; Subrahmanyam, Ch1
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| Corresponding Author | Tu, Xin([email protected]) ; Subrahmanyam, Ch.([email protected]) |
| Source Publication | APPLIED CATALYSIS B-ENVIRONMENTAL
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| 2021-05-05 | |
| Volume | 284Pages:13 |
| ISSN | 0926-3373 |
| Abstract | Direct conversion of methane into chemicals and fuels under mild conditions has been considered as a 'holy grail' of chemistry and catalysis in the 21st century. Plasma-catalytic partial oxidation of methane (POM) to higher-value liquid fuels and chemicals over supported transition metal catalysts (Ni/gamma-Al2O3, Cu/gamma-Al2O3 and Fe/gamma-Al2O3) has been investigated in a co-axial dielectric barrier discharge (DBD) reactor at room temperature and atmospheric pressure. The selectivity of oxygenates was 58.3% in the plasma POM reaction without a catalyst, while the combination of DBD with the catalysts enhanced the selectivity of oxygenates up to 71.5%. Of the three catalysts, Fe/gamma-Al2O3 showed the highest methanol selectivity of 36.0% and a significant methanol yield of 4.7%, while the use of Cu/gamma-Al2O3 improved the selectivity of C-2 oxygenates to 9.4%, which can be attributed to the presence of more acid sites on the surfaces of the Cu catalyst. The possible reaction pathways in the plasmacatalytic POM reaction have been explored by combined means of plasma electrical and optical diagnostics, analysis of gas and liquid products, as well as comprehensive catalyst characterization. The plausible reaction routes for the production of major oxygenate (methanol) on the Fe/gamma-Al2O3 surfaces have been proposed. The surface CHx species are found to be critical for methanol synthesis; they can be formed through the direct adsorption of CHx radicals generated in the plasma gas-phase reactions or through the dissociation of adsorbed CH4 on the catalyst surface. |
| Keyword | Partial oxidation of methane Non-thermal plasma Plasma-catalysis Methanol synthesis Oxygenates |
| DOI | 10.1016/j.apcatb.2020.119735 |
| Indexed By | SCI ; EI |
| Language | 英语 |
| WOS ID | WOS:000655536100001 |
| WOS Keyword | BARRIER DISCHARGE REACTOR ; DIRECT PARTIAL OXIDATION ; ATMOSPHERIC-PRESSURE ; HYDROGEN-PRODUCTION ; NONTHERMAL PLASMA ; PART 1 ; FUELS ; CO2 ; CU ; CHEMICALS |
| WOS Research Area | Chemistry ; Engineering |
| WOS Subject | Chemistry, Physical ; Engineering, Environmental ; Engineering, Chemical |
| Funding Project | MHRD ; European Union (EU) ; Horizon 2020[722346] |
| Funding Organization | MHRD ; European Union (EU) ; Horizon 2020 |
| Classification | 一类 |
| Ranking | 3+ |
| Contributor | Tu, Xin ; Subrahmanyam, Ch. |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://dspace.imech.ac.cn/handle/311007/86799 |
| Collection | 高温气体动力学国家重点实验室 |
| Affiliation | 1.Indian Inst Technol Hyderabad, Dept Chem, Hyderabad 502285, Telangana, India; 2.Univ Liverpool, Dept Elect Engn & Elect, Liverpool L69 3GJ, Merseyside, England; 3.Chinese Acad Sci, State Key Lab High Temp Gas Dynam, Inst Mech, Beijing 100190, Peoples R China |
| Recommended Citation GB/T 7714 | Chawdhury, Piu,Wang, Yaolin,Ray, Debjyoti,et al. A promising plasma-catalytic approach towards single-step methane conversion to oxygenates at room temperature[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2021,284:13.Rp_Au:Tu, Xin, Subrahmanyam, Ch. |
| APA | Chawdhury, Piu.,Wang, Yaolin.,Ray, Debjyoti.,Mathieu, Stephanie.,Wang, Ni.,...&Subrahmanyam, Ch.(2021).A promising plasma-catalytic approach towards single-step methane conversion to oxygenates at room temperature.APPLIED CATALYSIS B-ENVIRONMENTAL,284,13. |
| MLA | Chawdhury, Piu,et al."A promising plasma-catalytic approach towards single-step methane conversion to oxygenates at room temperature".APPLIED CATALYSIS B-ENVIRONMENTAL 284(2021):13. |
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| Jp2021F234.pdf（9051KB） | 期刊论文 | 出版稿 | 开放获取 | CC BY-NC-SA | View Download | |
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