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<p>Photocatalytic oxidative coupling of methane (POCM) is a promising strategy for the production of sustainable C<sub>2+</sub> hydrocarbons; however, it typically relies on large quantities of noble metals, such as gold, to serve as active sites for methyl coupling. In this study, we demonstrate that ZnO-supported gold nanoclusters with an average diameter of 1.1&#xa0;nm provide a robust alternative to conventional gold nanoparticles, enabling efficient POCM even at ultralow gold loadings of 0.1 wt%. The optimized photocatalyst affords a C<sub>2</sub>–C<sub>4</sub> hydrocarbon production rate of 3.89&#xa0;mmol/(g&#xa0;h) with 94.8% selectivity under 365&#xa0;nm irradiation in a batch reactor. Results reveal that the abundant interfaces between highly dispersed gold nanoclusters and ZnO substrates facilitate charge carrier separation and promote a light-induced Mars–van Krevelen reaction pathway. Methyl adsorption causes gold nanoclusters to exhibit a more intense d-<i>σ</i> hybridization state compared to gold nanoparticles, enhancing electron transfer interactions and substantially reducing the transition-state energy barrier for methyl coupling.</p>

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Low-Loading Gold Nanoclusters on Zinc Oxide Enable Efficient Photocatalytic Oxidative Coupling of Methane

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月19日

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  • Xiaotong Zhang,
  • Tingxuan Ran,
  • Jiaqi Zhao,
  • Lingsong Wang,
  • Run Shi,
  • Tierui Zhang

摘要

Photocatalytic oxidative coupling of methane (POCM) is a promising strategy for the production of sustainable C2+ hydrocarbons; however, it typically relies on large quantities of noble metals, such as gold, to serve as active sites for methyl coupling. In this study, we demonstrate that ZnO-supported gold nanoclusters with an average diameter of 1.1 nm provide a robust alternative to conventional gold nanoparticles, enabling efficient POCM even at ultralow gold loadings of 0.1 wt%. The optimized photocatalyst affords a C2–C4 hydrocarbon production rate of 3.89 mmol/(g h) with 94.8% selectivity under 365 nm irradiation in a batch reactor. Results reveal that the abundant interfaces between highly dispersed gold nanoclusters and ZnO substrates facilitate charge carrier separation and promote a light-induced Mars–van Krevelen reaction pathway. Methyl adsorption causes gold nanoclusters to exhibit a more intense d-σ hybridization state compared to gold nanoparticles, enhancing electron transfer interactions and substantially reducing the transition-state energy barrier for methyl coupling.