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<p>Selective photocatalytic oxidation of methane to liquid oxygenates under ambient conditions remains challenging due to the inert C–H bond and propensity for over-oxidation. Controlling carrier transfer and reactive oxygen species is therefore essential to the selective methane photooxidation. Ultrasmall zirconium metal–organic framework (UiO-66-H) nanocrystals in situ grown on titania form a heterojunction that promotes efficient charge separation and tunes the interfacial band alignment. Comprehensive experiments and characterization reveal that this heterojunction precisely regulates <sup>•</sup>OH and <sup>•</sup>OOH generation, enabling controlled, radical-mediated oxidation of methane with a competitive oxygenate yield and nearly 100% selectivity at room temperature using air as an oxidant. In this work, ultrasmall metal–organic framework–semiconductor heterojunctions with a built-in electric field provide an effective route for developing&#xa0;efficient, low-cost photocatalysts for methane chemical valorization under mild, solar-driven conditions.</p>

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Decorating titania with ultrasmall UiO-66-H crystallites enables quantitative photocatalytic oxidation of methane to oxygenates

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年4月29日

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  • Geqian Fang,
  • Nour Alhajjar,
  • Wenjun Yu,
  • Maya Marinova,
  • Karima Ben Tayeb,
  • Jian Lin,
  • Thomas Roland,
  • Pardis Simon,
  • Vincent De Waele,
  • Vitaly V. Ordomsky,
  • Andrei Y. Khodakov

摘要

Selective photocatalytic oxidation of methane to liquid oxygenates under ambient conditions remains challenging due to the inert C–H bond and propensity for over-oxidation. Controlling carrier transfer and reactive oxygen species is therefore essential to the selective methane photooxidation. Ultrasmall zirconium metal–organic framework (UiO-66-H) nanocrystals in situ grown on titania form a heterojunction that promotes efficient charge separation and tunes the interfacial band alignment. Comprehensive experiments and characterization reveal that this heterojunction precisely regulates •OH and •OOH generation, enabling controlled, radical-mediated oxidation of methane with a competitive oxygenate yield and nearly 100% selectivity at room temperature using air as an oxidant. In this work, ultrasmall metal–organic framework–semiconductor heterojunctions with a built-in electric field provide an effective route for developing efficient, low-cost photocatalysts for methane chemical valorization under mild, solar-driven conditions.