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<p>Direct photocatalytic oxidation of methane to high-value-added oxygenated products remains a great challenge due to the unavoidable overoxidation of target products. Here, we report an efficient and highly selective TiO<sub>2</sub> photocatalyst anchored with subnanometric MoO<sub>x</sub> clusters for photocatalytic methane oxidation to organic oxygenates by oxygen. A high organic oxygenates yield of 3.8 mmol/g with nearly 100% selectivity was achieved after 2 h of light irradiation, resulting in a 13.3% apparent quantum yield at 365 nm. Mechanistic studies reveal a photocatalytic cycle for methane oxidation on the MoO<sub>x</sub> anchored TiO<sub>2</sub>, which not only largely inhibits the formation of hydroxyl and superoxide radicals and the overoxidation of oxygenate products but also facilitates the activation of the first carbon-hydrogen bond of methane. This work would promote the rational design of efficient non-noble metal&#xa0;catalysts for direct conversion of methane to high-value-added oxygenates.</p>

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Subnanometric MoOx clusters limit overoxidation during photocatalytic CH4 conversion to oxygenates over TiO2

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年5月6日

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  • Panpan Wu,
  • Yueying Chu,
  • Maoling Wang,
  • Ningdong Feng,
  • Jun Xu,
  • Ding Ma,
  • Jinhua Ye,
  • Feng Deng

摘要

Direct photocatalytic oxidation of methane to high-value-added oxygenated products remains a great challenge due to the unavoidable overoxidation of target products. Here, we report an efficient and highly selective TiO2 photocatalyst anchored with subnanometric MoOx clusters for photocatalytic methane oxidation to organic oxygenates by oxygen. A high organic oxygenates yield of 3.8 mmol/g with nearly 100% selectivity was achieved after 2 h of light irradiation, resulting in a 13.3% apparent quantum yield at 365 nm. Mechanistic studies reveal a photocatalytic cycle for methane oxidation on the MoOx anchored TiO2, which not only largely inhibits the formation of hydroxyl and superoxide radicals and the overoxidation of oxygenate products but also facilitates the activation of the first carbon-hydrogen bond of methane. This work would promote the rational design of efficient non-noble metal catalysts for direct conversion of methane to high-value-added oxygenates.