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  Methane selective oxidation on metal oxide catalysts at low temperatures with O2 using an NO/NO2 oxygen atom shuttle

Ghampson, I. T., Lundin, S.-T.-B., Vargheese, V., Kobayashi, Y., Huff, G., Schlögl, R., et al. (2022). Methane selective oxidation on metal oxide catalysts at low temperatures with O2 using an NO/NO2 oxygen atom shuttle. Journal of Catalysis, 408, 401-412. doi:10.1016/j.jcat.2021.07.014.

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Ghampson, I. Tyrone1, 2, Author
Lundin, Sean-Thomas B.2, Author
Vargheese, Vibin2, Author
Kobayashi, Yasukazu3, Author
Huff, Gregory4, Author           
Schlögl, Robert4, 5, Author           
Trunschke, Annette4, Author           
Oyama, S. Ted2, 6, 7, Author
Affiliations:
1Department of Applied Chemistry for Environment, Graduate School of Urban Environmental Sciences, Tokyo Metropolitan University, 1-1 Minami-Osawa, Hachioji, Tokyo 192-0397, Japan, ou_persistent22              
2Department of Chemical Systems Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan, ou_persistent22              
3Interdisciplinary Research Center for Catalytic Chemistry, National Institute of Advanced Industrial Science and Technology (AIST), Central 5, 1-1-1 Higashi, Tsukuba, Ibaraki 305-8565, Japan, ou_persistent22              
4Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
5Department of Heterogeneous Reactions, Max-Planck-Institut für Chemische Energiekonversion, Stiftstraße 34-36, 45470 Mülheim a. d. Ruhr, Germany, ou_persistent22              
6School of Chemical Engineering, Fuzhou University, Fuzhou 350116, China, ou_persistent22              
7Department of Chemical Engineering, Virginia Tech, Blacksburg, VA 24061, United States, ou_persistent22              

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 Abstract: Methane oxidation using O2 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 O2, through the facile gas-phase formation of NO2 at moderate conditions (0.1 MPa and 300–400 °C), to oxidize methane over silica-supported transition metal oxides (VOx, CrOx, MnOx, NbOx, MoOx, and WOx). 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 NO2 and the supported metal oxides. During the reaction, the oxides of vanadium, molybdenum, and tungsten formed formaldehyde and CO2, whereas the oxides of chromium, manganese, and niobium produced only CO2. These results are consistent with the known hydrocarbon oxidation chemistry of the metal oxides. Contact time measurements on VOx/SiO2 indicated that formaldehyde was a primary product and CO2 was the final product; conversely, analogous measurements on MnOx/SiO2 showed that CO2 was the sole product. The formaldehyde production rate on VOx/SiO2, MoOx/SiO2, and WOx/SiO2, based on surface sites measured by high temperature oxygen chemisorption, compared favorably to oxygenate production rates for stronger oxidants (N2O and H2O2) reported in the literature.

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Language(s): eng - English
 Dates: 2021-04-152021-07-112021-07-202022-04
 Publication Status: Published in print
 Pages: 12
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1016/j.jcat.2021.07.014
 Degree: -

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Title: Journal of Catalysis
  Abbreviation : J. Catal.
Source Genre: Journal
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Publ. Info: Amsterdam : Elsevier
Pages: 12 Volume / Issue: 408 Sequence Number: - Start / End Page: 401 - 412 Identifier: ISSN: 0021-9517
CoNE: https://pure.mpg.de/cone/journals/resource/954922645027