A proposed reaction mechanism for the selective oxidation of methane with nitrous oxide over Co-ZSM-5 catalyst forming synthesis gas (CO + H 2 )

N.A. Khan; E.M. Kennedy; B.Z. Dlugogorski; A.A. Adesina; M. Stockenhuber

doi:10.1016/j.ijhydene.2018.05.026

Back

A proposed reaction mechanism for the selective oxidation of methane with nitrous oxide over Co-ZSM-5 catalyst forming synthesis gas (CO + H 2 )

Journal article

Peer reviewed

A proposed reaction mechanism for the selective oxidation of methane with nitrous oxide over Co-ZSM-5 catalyst forming synthesis gas (CO + H 2 )

N.A. Khan, E.M. Kennedy, B.Z. Dlugogorski, A.A. Adesina and M. Stockenhuber

International Journal of Hydrogen Energy, Vol.43(29), pp.13133-13144

2018

DOI: https://doi.org/10.1016/j.ijhydene.2018.05.026

Files and links (1)

url

Link to Published Version *Subscription may be requiredView

Abstract

Probable reaction intermediates and mechanistic steps involved for the selective oxidation of methane (CH4) with nitrous oxide (N2O) forming synthesis gas (CO + H2) over Co-ZSM-5 was examined. To assess the reaction kinetics reactions were conducted within a temperature range of 300 °C–550 °C and at atmospheric pressure, and the composition of reactant feed (N2O/CH4) was varied between three fixed ratios (5, 3, and 1). TPD, XRD, TEM and FT-IR techniques were used for catalyst characterization and mechanistic studies. It was found, that H2 selectivity is higher for feeds with lower N2O concentration. Furthermore, CO formation commences at lower temperatures in comparison to H2 gas which is a result of the formation of methanol (CH3OH) and carbon oxides (CO and CO2) at low CH4 conversions. Based on the reaction conditions, the literature proposes direct and an indirect mechanistic route for synthesis gas formation. Our catalytic study suggests a direct route for the synthesis gas formation; i.e. H2 gas is formed by the decomposition of intermediate species (methoxy and CH2O). This is supported by spectroscopic investigation. Under favourable reaction conditions and over the Co-ZSM-5 catalyst, N2O first oxidizes CH4 to CH3OH, an active reaction intermediate, which then subsequently is converted into (formaldehyde) CH2O and H2. CH2O is highly reactive and decomposes into CO and H2.

Details

Title: A proposed reaction mechanism for the selective oxidation of methane with nitrous oxide over Co-ZSM-5 catalyst forming synthesis gas (CO + H 2 )
Authors/Creators: N.A. Khan (Author/Creator) - University of Newcastle Australia
E.M. Kennedy (Author/Creator) - University of Newcastle Australia
B.Z. Dlugogorski (Author/Creator) - Murdoch University
A.A. Adesina (Author/Creator) - Product Innovation and Engineering (United States) (United States, Saint James) - LLC
M. Stockenhuber (Author/Creator) - University of Newcastle Australia
Publication Details: International Journal of Hydrogen Energy, Vol.43(29), pp.13133-13144
Publisher: Elsevier BV
Identifiers: 991005542096407891
Copyright: © 2018 Hydrogen Energy Publications LLC.
Murdoch Affiliation: School of Engineering and Information Technology
Language: English
Resource Type: Journal article

UN Sustainable Development Goals (SDGs)

This output has contributed to the advancement of the following goals:

Source: InCites

Metrics

66 Record Views

4 Times Cited - Web of Science

InCites Highlights

These are selected metrics from InCites Benchmarking & Analytics tool, related to this output

Collaboration types: Domestic collaboration; International collaboration
Citation topics: 2 Chemistry; 2.41 Catalysts; 2.41.366 Selective Catalytic Reduction
Web Of Science research areas: Chemistry, Physical; Electrochemistry; Energy & Fuels
ESI research areas: Engineering