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<p>Aqueous photocatalytic CH<sub>4</sub> oxidation offers a promising route for converting natural gas into oxygenates, a process governed by multi-electron and proton transfer at the catalyst-water interface. Here, we demonstrate that spatially confining water within Au/TiO<sub>2</sub>@pSiO<sub>2</sub> core-shell catalysts—by reducing silica pore size to 1.7 nm—increases CH<sub>4</sub> conversion three-fold and H<sub>2</sub>O<sub>2</sub> production 22-fold compared to Au/TiO<sub>2</sub>. This strategy is generalizable to other semiconductors and cocatalysts, with Pt/TiO<sub>2</sub>@pSiO<sub>2</sub>-1.7 exhibiting oxygenate yields of 32.7 mmol g<sup>-1</sup> h<sup>-1</sup> and a 14.1% apparent quantum yield at 365 nm. Spectroscopic studies and molecular dynamics simulations reveal that water confined within pores, with a weakened hydrogen-bonding network, alters proton-coupled electron transfer pathways. Water oxidation transits to a concerted pathway, favoring •OH production for CH<sub>4</sub> conversion, while oxygen reduction shifts to a two-electron process, directly producing H<sub>2</sub>O<sub>2</sub>. This work highlights the potential of water confinement for designing efficient photocatalysts for CH<sub>4</sub> conversion.</p>

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Simultaneous promotion of photocatalytic CH4 conversion and H2O2 production via nanopore water confinement

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年2月17日

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  • Fanxun Lv,
  • Shengwei Wei,
  • Xiaoyan Wu,
  • Chenghang Qi,
  • Xuan Wang,
  • Xiaoning Liu,
  • Yi Yu,
  • Bo Yang,
  • Chenlu Xie

摘要

Aqueous photocatalytic CH4 oxidation offers a promising route for converting natural gas into oxygenates, a process governed by multi-electron and proton transfer at the catalyst-water interface. Here, we demonstrate that spatially confining water within Au/TiO2@pSiO2 core-shell catalysts—by reducing silica pore size to 1.7 nm—increases CH4 conversion three-fold and H2O2 production 22-fold compared to Au/TiO2. This strategy is generalizable to other semiconductors and cocatalysts, with Pt/TiO2@pSiO2-1.7 exhibiting oxygenate yields of 32.7 mmol g-1 h-1 and a 14.1% apparent quantum yield at 365 nm. Spectroscopic studies and molecular dynamics simulations reveal that water confined within pores, with a weakened hydrogen-bonding network, alters proton-coupled electron transfer pathways. Water oxidation transits to a concerted pathway, favoring •OH production for CH4 conversion, while oxygen reduction shifts to a two-electron process, directly producing H2O2. This work highlights the potential of water confinement for designing efficient photocatalysts for CH4 conversion.