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Area of Science:

  • Catalysis
  • Materials Science
  • Green Chemistry

Background:

  • Direct methane oxidation to acetic acid is challenging due to methane's inertness and over-oxidation risks.
  • Developing selective catalysts for C-H activation and C-C coupling is crucial for value-added chemical production.

Purpose of the Study:

  • To develop an efficient and selective heterogeneous catalyst for direct methane to acetic acid conversion.
  • To investigate the catalytic mechanism and the role of the metal-organic framework support.

Main Methods:

  • Synthesis of a single-site mono-copper(II) hydroxyl catalyst supported on porous aluminium metal-organic framework (MIL-53(Al)-Cu(OH)).
  • Direct oxidation of methane to acetic acid in water using molecular oxygen (O2) at 175 °C.
  • Characterization using computational studies and spectroscopic analyses.

Main Results:

  • Achieved high acetic acid productivity (11,796 mmolCH molCu-1 h-1) with 9.3% methane conversion and 95% selectivity.
  • Demonstrated catalyst reusability for at least 6 cycles.
  • Identified a catalytic cycle involving methyl radical formation and proposed confinement effects within the MOF.

Conclusions:

  • The developed MIL-53(Al)-Cu(OH) catalyst enables efficient and selective direct conversion of methane to acetic acid under mild conditions.
  • The MOF structure plays a key role in facilitating C-C coupling and enhancing selectivity through mass transfer limitations.
  • This work presents a promising approach for utilizing earth-abundant metal catalysts in MOFs for sustainable chemical synthesis.