Plasma-catalytic direct oxidation of methane to methanol over Cu-MOR: Revealing the zeolite-confined Cu2+active sites

被引:2
|
作者
Lv, Huan [1 ,2 ]
Meng, Shengyan [1 ]
Cui, Zhaolun [3 ]
Li, Shangkun [4 ]
Li, Dongxing [4 ]
Gao, Xiaoxia [5 ]
Guo, Hongchen [1 ]
Bogaerts, Annemie [4 ]
Yi, Yanhui [1 ]
机构
[1] Dalian Univ Technol, Frontier Sci Ctr Smart Mat, Sch Chem Engn, State Key Lab Fine Chem, Dalian 116024, Peoples R China
[2] Baotou Elect Ind Vocat Sch, Baotou 014000, Peoples R China
[3] South China Univ Technol, Sch Elect Power Engn, Guangzhou 510630, Peoples R China
[4] Univ Antwerp, Res Grp PLASMANT, Dept Chem, Univ Pl 1, BE-2610 Antwerp, Belgium
[5] Dalian Univ Technol, Instrumental Anal Ctr, Dalian 116024, Peoples R China
基金
中国国家自然科学基金;
关键词
Methane conversion; Direct oxidation; Methanol production; Plasma catalysis; Copper-mordenite catalysts; CO2; HYDROGENATION; ACTIVE-SITES; TO-METHANOL; MORDENITE; PROMOTION; OXIDE;
D O I
10.1016/j.cej.2024.154337
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Efficient methane conversion to methanol remains a significant challenge in chemical industry. This study investigates the direct oxidation of methane to methanol under mild conditions, employing a synergy of non- thermal plasma and Cu-MOR (Copper-Mordenite) catalysts. Catalytic tests demonstrate that the Cu-MOR IE-3 catalyst (i.e., prepared by three cycles of ion exchange) exhibits superior catalytic performance (with 51 % methanol selectivity and 7.9 % methane conversion). Conversely, the Cu-MOR catalysts prepared via wetness impregnation tend to over-oxidize CH4 4 to CO and CO2. 2 . Through systematic catalyst characterizations (XRD, TPR, UV-Vis, HRTEM, XPS), we elucidate that ion exchange mainly leads to the formation of zeolite-confined Cu2+ 2+ species, while wetness impregnation predominantly results in CuO particles. Based on the catalytic performance, catalyst characterizations and in-situ FTIR spectra, we conclude that zeolite-confined Cu2+ 2+ species serve as the active sites for plasma-catalytic direct oxidation of methane to methanol.
引用
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页数:11
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