Quasicatalytic and Catalytic Oxidation of Methane to Methanol by Nitrous Oxide over FeZSM-5 Zeolite Full article
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Journal of Catalysis
ISSN: 0021-9517 , E-ISSN: 1090-2694 |
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| Output data | Year: 2014, Volume: 318, Pages: 14-21 Pages count : 8 DOI: 10.1016/j.jcat.2014.07.009 | ||
| Tags | Biomimetic oxidation, FeZSM-5 zeolite, Methane oxidation, Methane to methanol, Nitrous oxide, Product extraction, Quasicatalytic reaction, Surface diffusion, α-Oxygen | ||
| Authors |
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| Affiliations |
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Funding (1)
| 1 | Russian Foundation for Basic Research | 12-03-00063 |
Abstract:
Methane oxidation by N2O at 200 °C and below was shown to proceed in a quasicatalytic mode resulting in product accumulation on FeZSM-5 surface. Methanol that formed via methane oxidation by α-oxygen, CH4 + (FeIII–O−)α, migrated from α-sites, initiating new reaction cycles. At 200 °C, a 4-h run provided turnover number close to 7. Methanol and dimethyl ether (DME) were the products extracted from the surface.
At above 200 °C, the reaction moved to conventional catalytic mode with product desorption into gas phase. Water strongly increased methanol selectivity, which attained 62% at 275 °C (accounting coke). Contrary to expectations, DME was not detected among the gas-phase products being converted to coke.
Comparison of quasicatalytic and catalytic data can provide new information on the reaction mechanism including a possibility of identifying potential intermediates invisible under catalytic conditions. Mechanistic scheme presenting main steps of both reaction modes was suggested.
Cite:
Parfenov M.V.
, Starokon E.V.
, Pirutko L.V.
, Panov G.I.
Quasicatalytic and Catalytic Oxidation of Methane to Methanol by Nitrous Oxide over FeZSM-5 Zeolite
Journal of Catalysis. 2014. V.318. P.14-21. DOI: 10.1016/j.jcat.2014.07.009 WOS Scopus РИНЦ ANCAN OpenAlex
Quasicatalytic and Catalytic Oxidation of Methane to Methanol by Nitrous Oxide over FeZSM-5 Zeolite
Journal of Catalysis. 2014. V.318. P.14-21. DOI: 10.1016/j.jcat.2014.07.009 WOS Scopus РИНЦ ANCAN OpenAlex
Dates:
| Submitted: | Apr 17, 2014 |
| Accepted: | Jul 13, 2014 |
| Published online: | Aug 13, 2014 |
| Published print: | Oct 1, 2014 |
Identifiers:
| Web of science: | WOS:000343360800002 |
| Scopus: | 2-s2.0-84906099573 |
| Elibrary: | 23982751 |
| Chemical Abstracts: | 2014:1257386 |
| Chemical Abstracts (print): | 161:337855 |
| OpenAlex: | W2016656388 |