The Direct Partial Oxidation of Methane to Dimethyl Ether over Pt/Y 2 O 3 Catalysts Using an NO/O 2 Shuttle

Using a mixture of NO + O 2 as the oxidant enabled the direct selective oxidation of methane to dimethyl ether (DME) over Pt/Y 2 O 3 . The reaction was carried out in a fixed bed reactor at 0.1 MPa over a temperature range of 275–375 °C. During the activity tests, the only carbon‐containing products...

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Veröffentlicht in:Angewandte Chemie International Edition 2020-09, Vol.59 (38), p.16644-16650
Hauptverfasser: Vargheese, Vibin, Kobayashi, Yasukazu, Oyama, S. Ted
Format: Artikel
Sprache:eng
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Zusammenfassung:Using a mixture of NO + O 2 as the oxidant enabled the direct selective oxidation of methane to dimethyl ether (DME) over Pt/Y 2 O 3 . The reaction was carried out in a fixed bed reactor at 0.1 MPa over a temperature range of 275–375 °C. During the activity tests, the only carbon‐containing products were DME and CO 2 . The DME productivity (μmol g cat −1  h −1 ) was comparable to oxygenate productivities reported in the literature for strong oxidants (N 2 O, H 2 O 2 , O 3 ). The NO + O 2 mixture formed NO 2 , which acted as the oxygen atom carrier for the ultimate oxidant O 2 . During the methane partial oxidation reaction, NO and NO 2 were not reduced to N 2 . In situ FTIR showed the formation of surface nitrate species, which are considered to be key intermediate species for the selective oxidation.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202006020