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Catalysis02:50

Catalysis

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Methane Oxidation over Cu

Jörg Wolfram Anselm Fischer1, Andreas Brenig2,3, Daniel Klose1

  • 1Institute for Molecular Physical Science, ETH Zurich, Vladimir-Prelog-Weg 1-5/10, 8093, Zurich, Switzerland.

Angewandte Chemie (International Ed. in English)
|June 9, 2023
PubMed
Summary
This summary is machine-generated.

This study reveals a new pathway for methane oxidation using copper-exchanged mordenite (Cu-MOR). Paired copper sites, not previously recognized, are key to this catalytic process.

Keywords:
Copperheterogeneous catalysismethane to methanoloperando spectroscopyzeolites

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Area of Science:

  • Catalysis
  • Materials Science
  • Chemical Spectroscopy

Background:

  • Copper-exchanged mordenite (Cu-MOR) is a key catalyst for partial methane (CH4) oxidation.
  • Understanding the diverse copper (Cu) species in Cu-MOR is crucial for identifying active sites and their properties.

Purpose of the Study:

  • To elucidate the speciation of Cu in Cu-MOR with varying loadings.
  • To identify active Cu sites and determine their redox and kinetic properties for CH4 oxidation.

Main Methods:

  • Operando electron paramagnetic resonance (EPR) and UV-Visible (UV/Vis) spectroscopy.
  • In situ photoluminescence (PL) and Fourier-transform infrared (FTIR) spectroscopy.
  • Site-specific kinetic measurements.

Main Results:

  • A novel CH4 oxidation pathway involving paired [CuOH]+ and bare Cu2+ species was identified.
  • Adjacent [CuOH]+ facilitates the reduction of bare Cu2+, challenging the assumption of redox-inert Cu2+.
  • Dimeric Cu species showed faster reaction rates and higher activation energy than monomeric Cu2+ sites.

Conclusions:

  • The study identified specific active Cu sites and a new reaction pathway for methane oxidation over Cu-MOR.
  • The findings highlight the importance of considering paired Cu species and their redox behavior in catalysis.
  • Site-specific kinetics reveal differences in catalytic potential between monomeric and dimeric Cu sites.