Selective oxidation of CH4 to CH3OH through plasma catalysis: Insights from catalyst characterization and chemical kinetics modelling



Yi, Yanhui, Li, Shangkun, Cui, Zhaolun, Hao, Yingzi, Zhang, Yang, Wang, Li, Liu, Pei, Tu, Xin ORCID: 0000-0002-6376-0897, Xu, Xianming, Guo, Hongchen
et al (show 1 more authors) (2021) Selective oxidation of CH4 to CH3OH through plasma catalysis: Insights from catalyst characterization and chemical kinetics modelling. APPLIED CATALYSIS B-ENVIRONMENTAL, 296. p. 120384.

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Abstract

The selective oxidation of methane to methanol (SOMTM) by molecular oxygen is a holy grail in catalytic chemistry and remains a challenge in chemical industry. We perform SOMTM in a CH4/O2 plasma, at low temperature and atmospheric pressure, promoted by Ni-based catalysts, reaching 81 % liquid oxygenates selectivity and 50 % CH3OH selectivity, with an excellent catalytic stability. Chemical kinetics modelling shows that CH3OH in the plasma is mainly produced through radical reactions, i.e., CH4 + O(1D) → CH3O + H, followed by CH3O + H + M→ CH3OH + M and CH3O + HCO → CH3OH + CO. The catalyst characterization shows that the improved production of CH3OH is attributed to abundant chemisorbed oxygen species, originating from highly dispersed NiO phase with strong oxide support interaction with γ-Al2O3, which are capable of promoting CH3OH formation through E-R reactions and activating H2O molecules to facilitate CH3OH desorption.

Item Type: Article
Uncontrolled Keywords: Methane conversion, Plasma catalysis, Selective oxidation, Methanol synthesis, Plasma chemistry
Divisions: Faculty of Science and Engineering > School of Electrical Engineering, Electronics and Computer Science
Depositing User: Symplectic Admin
Date Deposited: 20 May 2021 09:15
Last Modified: 18 Jan 2023 22:46
DOI: 10.1016/j.apcatb.2021.120384
Related URLs:
URI: https://livrepository.liverpool.ac.uk/id/eprint/3123395