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• W3185670147 endingPage "412" @default.
• W3185670147 startingPage "401" @default.
• W3185670147 abstract "• Silica-supported oxides oxidized CH 4 with NO 2 , formed by the gas-phase reaction of NO and O 2 . • The reaction proceeded at moderate pressure (0.10 MPa) and temperatures (300–400 °C). • Oxides of V, Mo, W formed formaldehyde while oxides of Cr, Mn, and Nb formed only CO 2 . • Infrared spectroscopy indicated the involvement of adsorbed nitrate species. Methane oxidation using O 2 over transition metal oxides often requires severe conditions (>500 °C) to achieve detectable conversion. In this study, NO was used to transfer oxygen atoms from O 2 , through the facile gas-phase formation of NO 2 at moderate conditions (0.1 MPa and 300–400 °C), to oxidize methane over silica-supported transition metal oxides (VO x , CrO x , MnO x , NbO x , MoO x , and WO x ). In situ infrared spectroscopy measurements indicated that the reaction likely proceeded by the formation of surface monodentate nitrate intermediates. These nitrate species were formed by the interaction between adsorbed NO 2 and the supported metal oxides. During the reaction, the oxides of vanadium, molybdenum, and tungsten formed formaldehyde and CO 2 , whereas the oxides of chromium, manganese, and niobium produced only CO 2 . These results are consistent with the known hydrocarbon oxidation chemistry of the metal oxides. Contact time measurements on VO x /SiO 2 indicated that formaldehyde was a primary product and CO 2 was the final product; conversely, analogous measurements on MnO x /SiO 2 showed that CO 2 was the sole product. The formaldehyde production rate on VO x /SiO 2 , MoO x /SiO 2 , and WO x /SiO 2 , based on surface sites measured by high temperature oxygen chemisorption, compared favorably to oxygenate production rates for stronger oxidants (N 2 O and H 2 O 2 ) reported in the literature." @default.
• W3185670147 created "2021-08-02" @default.
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• W3185670147 date "2022-04-01" @default.
• W3185670147 modified "2023-10-13" @default.
• W3185670147 title "Methane selective oxidation on metal oxide catalysts at low temperatures with O2 using an NO/NO2 oxygen atom shuttle" @default.
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• W3185670147 doi "https://doi.org/10.1016/j.jcat.2021.07.014" @default.
• W3185670147 hasPublicationYear "2022" @default.
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