A promising plasma-catalytic approach towards single-step methane conversion to oxygenates at room temperature

doi:10.1016/j.apcatb.2020.119735

CORC > 力学研究所 > 中国科学院力学研究所 > 高温气体动力学国家重点实验室

	A promising plasma-catalytic approach towards single-step methane conversion to oxygenates at room temperature
	Chawdhury, Piu 3; Wang, Yaolin 2; Ray, Debjyoti 3; Mathieu, Stephanie 2; Wang, Ni 2; Harding, Jonathan 2; Bin F(宾峰)1,2; Tu, Xin 2; Subrahmanyam, Ch 3
刊名	APPLIED CATALYSIS B-ENVIRONMENTAL
	2021-05-05
卷号	284 页码:13
关键词	Partial oxidation of methane Non-thermal plasma Plasma-catalysis Methanol synthesis Oxygenates
ISSN号	0926-3373
DOI	10.1016/j.apcatb.2020.119735
通讯作者	Tu, Xin(xin.tu@liverpool.ac.uk) ; Subrahmanyam, Ch.(csubbu@iith.ac.in)
英文摘要	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.
分类号	一类
资助项目	MHRD ; European Union (EU) ; Horizon 2020[722346]
WOS关键词	BARRIER DISCHARGE REACTOR ; DIRECT PARTIAL OXIDATION ; ATMOSPHERIC-PRESSURE ; HYDROGEN-PRODUCTION ; NONTHERMAL PLASMA ; PART 1 ; FUELS ; CO2 ; CU ; CHEMICALS
WOS研究方向	Chemistry ; Engineering
语种	英语
WOS记录号	WOS:000655536100001
资助机构	MHRD ; European Union (EU) ; Horizon 2020
其他责任者	Tu, Xin ; Subrahmanyam, Ch.
内容类型	期刊论文
源URL	[http://dspace.imech.ac.cn/handle/311007/86798]
专题	力学研究所_高温气体动力学国家重点实验室
作者单位	1.Chinese Acad Sci, State Key Lab High Temp Gas Dynam, Inst Mech, Beijing 100190, Peoples R China 2.Univ Liverpool, Dept Elect Engn & Elect, Liverpool L69 3GJ, Merseyside, England; 3.Indian Inst Technol Hyderabad, Dept Chem, Hyderabad 502285, Telangana, India;
推荐引用方式 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.
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.