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The Direct Partial Oxidation of Methane to Dimethyl Ether over Pt/Y 2 O 3 Catalysts Using an NO/O 2 Shuttle
Author(s) -
Vargheese Vibin,
Kobayashi Yasukazu,
Oyama S. Ted
Publication year - 2020
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202006020
Subject(s) - dimethyl ether , oxygenate , catalysis , chemistry , partial oxidation , methane , anaerobic oxidation of methane , inorganic chemistry , ether , alkane , oxygen , organic chemistry
Abstract 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.