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
收藏
页数:11
相关论文
共 16 条
  • [1] Distinct activation of Cu-MOR for direct oxidation of methane to methanol
    Kim, Younhwa
    Kim, Tae Yong
    Lee, Hyunjoo
    Yi, Jongheop
    CHEMICAL COMMUNICATIONS, 2017, 53 (29) : 4116 - 4119
  • [2] Evolution of active sites during selective oxidation of methane to methanol over Cu-CHA and Cu-MOR zeolites as monitored by operando XAS
    Borfecchia, Elisa
    Pappas, Dimitrios K.
    Dyballa, Michael
    Lomachenko, Kirill A.
    Negri, Chiara
    Signorile, Matteo
    Berlier, Gloria
    CATALYSIS TODAY, 2019, 333 : 17 - 27
  • [3] Plasma-catalytic one-step steam reforming of methane to methanol: Revealing the catalytic cycle on Cu/mordenite
    Hao, Yingzi
    Li, Shangkun
    Fang, Wei
    Wang, Ximiao
    Cui, Zhaolun
    Bal, Kristof M.
    Gerrits, Nick
    Guo, Hongchen
    Neyts, Erik C.
    Bogaerts, Annemie
    Yi, Yanhui
    AICHE JOURNAL, 2025, 71 (01)
  • [4] Highly dispersed Cu-anchored nanoparticles based mordenite zeolite catalyst (Cu-MOR): Influence of the different preparation methods for direct methane oxidation (DMTM) to methanol
    Hussain, Ijaz
    Ganiyu, Saheed
    Alasiri, Hassan
    Alhooshani, Khalid
    JOURNAL OF THE ENERGY INSTITUTE, 2023, 109
  • [5] Conditions to meet for the [CuOH]+ site to be favorable and reactive toward the conversion of methane to methanol over Cu-MOR zeolite
    Mahyuddin, Muhammad Haris
    Lasiman, Elbert Timothy
    Saputro, Adhitya Gandaryus
    Casuarina, Suci Valerie
    Dipojono, Hermawan Kresno
    CATALYSIS SCIENCE & TECHNOLOGY, 2023, 13 (19) : 5767 - 5775
  • [6] Confined Cu-OH single sites in SSZ-13 zeolite for the direct oxidation of methane to methanol
    Zhang, Hailong
    Han, Peijie
    Wu, Danfeng
    Du, Congcong
    Zhao, Jiafei
    Zhang, Kelvin H. L.
    Lin, Jingdong
    Wan, Shaolong
    Huang, Jianyu
    Wang, Shuai
    Xiong, Haifeng
    Wang, Yong
    NATURE COMMUNICATIONS, 2023, 14 (01)
  • [7] Effect of the Preparation Method on Cu-MOR/g-C3N4 for Direct Methanol Synthesis from Methane Oxidation by Photothermal Catalysis
    Hao, Jun-Cai
    Zhang, Rui-Xin
    Ren, Miao
    Zhao, Jia-Xuan
    Gao, Zhi-Hua
    Liu, Lei
    Zhang, Zhu-Xia
    Zuo, Zhi-Jun
    CATALYSTS, 2023, 13 (05)
  • [8] Direct Stepwise Oxidation of Methane to Methanol over Cu-SiO2
    Bozbag, Selmi E.
    Sot, Petr
    Nachtegaal, Maarten
    Ranocchiari, Marco
    van Bolchoven, Jeroen A.
    Mesters, Carl
    ACS CATALYSIS, 2018, 8 (07): : 5721 - 5731
  • [9] Enhanced plasma-catalytic oxidation of methanol over MOF-derived CeO2 catalysts with exposed active sites
    Chen, Gui
    Mao, Mengqi
    Chen, Longwen
    Zhang, Guangyi
    Wang, Zikun
    Liu, Feng
    Ye, Daiqi
    Wu, Junliang
    JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING, 2022, 10 (06):
  • [10] Plasma-Catalytic Methanol Synthesis from CO2 Hydrogenation over a Supported Cu Cluster Catalyst: Insights into the Reaction Mechanism
    Cui, Zhaolun
    Meng, Shengyan
    Yi, Yanhui
    Jafarzadeh, Amin
    Li, Shangkun
    Neyts, Erik Cornelis
    Hao, Yanpeng
    Li, Licheng
    Zhang, Xiaoxing
    Wang, Xinkui
    Bogaerts, Annemie
    ACS CATALYSIS, 2022, 12 (02) : 1326 - 1337