Indexed by:
Abstract:
A comprehensive density functional theory calculation was employed to investigate the possible reaction pathways and mechanisms of methane complete oxidation (CH4 + 2O(2) -> CO2 + 2H(2)O) on different manganese oxides including alpha-MnO2(100) and beta-MnO2(111) surfaces. According to a coupling of the Mars-van Krevelen and Langmuir-Hinshelwood mechanism, the activation energy barrier and the reaction energy of each elementary surface reaction were determined. Our calculated results show that the detailed processes for methane oxidation on two surfaces are different due to the differences in the surface structure. The breaking of the last C-H bond of CH4 molecule is the rate-determining step with an activation barrier of 0.85 eV for alpha-MnO2(100) surface. By contrast, the overall reaction rate on beta-MnO2(111) surface is limited by the dissociation of the second O-2 molecule adsorbed on the vacancy site, and re-oxidation of the reduced beta-MnO2(111) surface by the gaseous oxygen requires a much higher energy barrier of 1.44 eV As a result, the alpha-MnO2(100) exhibits superior activity and durability in the methane oxidation reaction than beta-MnO2(111) surface. The present study provides insight into understanding the structure-catalytic activity relationship of the catalysts based on manganese oxides towards the methane oxidation reaction.
Keyword:
Reprint 's Address:
Email:
Version:
Source :
CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
ISSN: 0254-5861
CN: 35-1112/TQ
Year: 2020
Issue: 8
Volume: 39
Page: 1405-1421
0 . 8 9 3
JCR@2020
5 . 9 0 0
JCR@2023
ESI Discipline: CHEMISTRY;
ESI HC Threshold:160
JCR Journal Grade:4
CAS Journal Grade:3
Cited Count:
WoS CC Cited Count: 0
SCOPUS Cited Count:
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 1
Affiliated Colleges: