Title
|
|
|
|
Selective oxidation of CH4 to CH3OH through plasma catalysis : insights from catalyst characterization and chemical kinetics modelling
| |
Author
|
|
|
|
| |
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. |
| |
Language
|
|
|
|
English
| |
Source (journal)
|
|
|
|
Applied catalysis : B : environmental. - Amsterdam
| |
Publication
|
|
|
|
Amsterdam
:
2021
| |
ISSN
|
|
|
|
0926-3373
| |
DOI
|
|
|
|
10.1016/J.APCATB.2021.120384
| |
Volume/pages
|
|
|
|
296
(2021)
, 11 p.
| |
Article Reference
|
|
|
|
120384
| |
ISI
|
|
|
|
000706860000003
| |
Medium
|
|
|
|
E-only publicatie
| |
Full text (Publisher's DOI)
|
|
|
|
| |
Full text (open access)
|
|
|
|
| |
Full text (publisher's version - intranet only)
|
|
|
|
| |
|