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

来源：

CHEMICAL ENGINEERING JOURNAL | 2024年 / 496卷

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

页数：11