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author:

Ghampson, I. Tyrone (Ghampson, I. Tyrone.) [1] | Lundin, Sean-Thomas B. (Lundin, Sean-Thomas B..) [2] | Vargheese, Vibin (Vargheese, Vibin.) [3] | Kobayashi, Yasukazu (Kobayashi, Yasukazu.) [4] | Huff, Gregory S. (Huff, Gregory S..) [5] | Schlogl, Robert (Schlogl, Robert.) [6] | Trunschke, Annette (Trunschke, Annette.) [7] | Oyama, S. Ted (Oyama, S. Ted.) [8]

Indexed by:

EI SCIE

Abstract:

Methane oxidation using O-2 over transition metal oxides often requires severe conditions (>500 degrees 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 NO2 at moderate conditions (0.1 MPa and 300-400 degrees 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. (c) 2021 Elsevier Inc. All rights reserved.

Keyword:

CH4 oxidation Formaldehyde Nitrate species Metal oxide catalysts NO and O-2 shuttle

Community:

  • [ 1 ] [Oyama, S. Ted]Fuzhou Univ, Sch Chem Engn, Fuzhou 350116, Peoples R China
  • [ 2 ] [Ghampson, I. Tyrone]Tokyo Metropolitan Univ, Grad Sch Urban Environm Sci, Dept Appl Chem Environm, 1-1 Minami Osawa, Hachioji, Tokyo 1920397, Japan
  • [ 3 ] [Ghampson, I. Tyrone]Univ Tokyo, Dept Chem Syst Engn, Bunkyo Ku, 7-3-1 Hongo, Tokyo 1138656, Japan
  • [ 4 ] [Lundin, Sean-Thomas B.]Univ Tokyo, Dept Chem Syst Engn, Bunkyo Ku, 7-3-1 Hongo, Tokyo 1138656, Japan
  • [ 5 ] [Vargheese, Vibin]Univ Tokyo, Dept Chem Syst Engn, Bunkyo Ku, 7-3-1 Hongo, Tokyo 1138656, Japan
  • [ 6 ] [Oyama, S. Ted]Univ Tokyo, Dept Chem Syst Engn, Bunkyo Ku, 7-3-1 Hongo, Tokyo 1138656, Japan
  • [ 7 ] [Kobayashi, Yasukazu]Natl Inst Adv Ind Sci & Technol, Interdisciplinary Res Ctr Catalyt Chem, Cent 5,1-1-1 Higashi, Tsukuba, Ibaraki 3058565, Japan
  • [ 8 ] [Huff, Gregory S.]Max Planck Gesell, Fritz Haber Inst, Faradayweg 4-6, D-14195 Berlin, Germany
  • [ 9 ] [Schlogl, Robert]Max Planck Gesell, Fritz Haber Inst, Faradayweg 4-6, D-14195 Berlin, Germany
  • [ 10 ] [Trunschke, Annette]Max Planck Gesell, Fritz Haber Inst, Faradayweg 4-6, D-14195 Berlin, Germany
  • [ 11 ] [Schlogl, Robert]Max Planck Inst Chem Energiekonvers, Dept Heterogeneous React, Stiftstr 34-36, D-45470 Mulheim, Germany
  • [ 12 ] [Oyama, S. Ted]Virginia Tech, Dept Chem Engn, Blacksburg, VA 24061 USA

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Source :

JOURNAL OF CATALYSIS

ISSN: 0021-9517

Year: 2022

Volume: 408

Page: 401-412

7 . 3

JCR@2022

6 . 5 0 0

JCR@2023

ESI Discipline: CHEMISTRY;

ESI HC Threshold:74

JCR Journal Grade:1

CAS Journal Grade:2

Cited Count:

WoS CC Cited Count: 7

SCOPUS Cited Count: 9

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 0

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