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Tailoring Methane Oxidative Coupling Pathways through Cluster-Modified Photocatalysts.

Hui-Ling Luo1, Hui-Li Chai1, Fang-Yu Cao1

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This study developed an Au24Zn1 nanocluster-embedded ZnO catalyst for efficient photocatalytic methane coupling to valuable C2+ chemicals. The catalyst achieved high selectivity and yield, offering new mechanistic insights.

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Area of Science:

  • Catalysis
  • Materials Science
  • Chemical Engineering

Background:

  • Photocatalytic methane coupling is a key strategy for producing C2+ chemicals.
  • Developing efficient catalysts is crucial for this process.

Purpose of the Study:

  • To design and evaluate an Au24Zn1 nanocluster-embedded ZnO catalyst for enhanced photocatalytic methane coupling.
  • To elucidate the reaction mechanism and identify key active species.

Main Methods:

  • Synthesis of Au24Zn1/ZnO catalyst.
  • Photocatalytic methane coupling experiments in a batch reactor.
  • Characterization using XPS and CO-DRIFTS.
  • Radical trapping and isotope-labeling studies.

Main Results:

  • The Au24Zn1/ZnO catalyst achieved 93.5% C2+ selectivity and a yield of 663.1 μmol·gcat−1·h−1.
  • Au24Zn1 nanoclusters acted as hole acceptors, improving charge carrier separation.
  • •OH radicals from water, not photogenerated holes, were the primary methane activators.
  • •OOH radicals played a supporting role in modulating •OH concentration and the catalytic cycle.

Conclusions:

  • The rational design of metal nanocluster-based catalysts significantly enhances photocatalytic methane conversion.
  • The identified reaction pathway involving •OH and •OOH radicals provides new mechanistic understanding.
  • This work demonstrates the potential of nanocluster-decorated semiconductors for sustainable chemical production.