Zeolite Surface Methoxy Groups as Key Intermediates in the Stepwise Conversion of Methane to Methanol

Abstract: This contribution clarifies the overoxidation‐preventing key step in the methane‐to‐methanol (MTM) conversion over copper mordenite zeolites. We followed the methane‐to‐methanol conversion over copper mordenite zeolites by NMR spectroscopy supported by DRIFTS to show that surface methoxy groups (SMGs) located at zeolite Brønsted sites are the key intermediates. The SMGs with chemical shift of 59 ppm are identical to those formed on a copper‐free reference zeolite after reaction with methanol and react with water, methanol, or carbon monoxide to yield methanol, dimethyl ether, and acetate. This reactivity corroborates the location of SMGs at Brønsted sites. We find no evidence for stable SMGs directly at copper sites and explain mechanistically why H‐form mordenites outperform their Na‐form analogues. This finding is of interest for any future process that tries to trap the intermediate methane oxidation product towards methanol.

Standort
Deutsche Nationalbibliothek Frankfurt am Main
Umfang
Online-Ressource
Sprache
Englisch

Erschienen in
Zeolite Surface Methoxy Groups as Key Intermediates in the Stepwise Conversion of Methane to Methanol ; volume:11 ; number:20 ; year:2019 ; pages:5022-5026 ; extent:5
ChemCatChem ; 11, Heft 20 (2019), 5022-5026 (gesamt 5)

Urheber
Dyballa, Michael
Thorshaug, Knut
Pappas, Dimitrios K.
Borfecchia, Elisa
Kvande, Karoline
Bordiga, Silvia
Berlier, Gloria
Lazzarini, Andrea
Olsbye, Unni
Beato, Pablo
Svelle, Stian
Arstad, Bjørnar

DOI
10.1002/cctc.201901315
URN
urn:nbn:de:101:1-2022080208310502115398
Rechteinformation
Open Access; Der Zugriff auf das Objekt ist unbeschränkt möglich.
Letzte Aktualisierung
15.08.2025, 07:36 MESZ

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Beteiligte

  • Dyballa, Michael
  • Thorshaug, Knut
  • Pappas, Dimitrios K.
  • Borfecchia, Elisa
  • Kvande, Karoline
  • Bordiga, Silvia
  • Berlier, Gloria
  • Lazzarini, Andrea
  • Olsbye, Unni
  • Beato, Pablo
  • Svelle, Stian
  • Arstad, Bjørnar

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