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<p>Mild-condition methane (CH<sub>4</sub>) oxidation into valuable chemicals using earth-abundant oxygen (O<sub>2</sub>) is a highly desirable yet challenging process due to the chemical inertness of CH<sub>4</sub> and the low reactivity of O<sub>2</sub>. Herein, we report an ultrasound-catalysis coupling strategy for highly efficient conversion of CH<sub>4</sub> into high-value oxygenates under mild conditions, using O<sub>2</sub> as an oxidant and carbon nanotube-supported platinum nanoparticles (Pt/CNT) as a catalyst. It achieves a superior formation rate of 3727 μmol g<sub>cat.</sub><sup>−1</sup> h<sup>−1</sup> and a selectivity of 92% for C<sub>1-2</sub> oxygenates at 5 <sup>o</sup>C and 0.1 MPa, significantly surpassing both previously reported thermo-catalytic and ultrasound-driven processes under low-temperature conditions. We find that ultrasound-driven surface cleaning effect enhances the exposure of active Pt sites, thereby facilitating the adsorption of CH<sub>4</sub> and O<sub>2</sub>. Furthermore, the localized and instantaneous high-temperature and high-pressure microenvironment generated by ultrasonic cavitation not only promotes the activation of CH<sub>4</sub> and O<sub>2</sub> for C−H cleavage and C−O coupling, but also accelerates the mass transfer of reactants and products.</p>

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Mild-condition methane conversion with oxygen by an ultrasound-catalysis coupling process

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年5月4日

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  • Yunlong Zhang,
  • Qiming Bing,
  • Yunchuan Tu,
  • Shiming Chen,
  • Xiaoju Cui,
  • Lingxing Zan,
  • Mingrun Li,
  • Jingting Hu,
  • Liang Yu,
  • Dehui Deng

摘要

Mild-condition methane (CH4) oxidation into valuable chemicals using earth-abundant oxygen (O2) is a highly desirable yet challenging process due to the chemical inertness of CH4 and the low reactivity of O2. Herein, we report an ultrasound-catalysis coupling strategy for highly efficient conversion of CH4 into high-value oxygenates under mild conditions, using O2 as an oxidant and carbon nanotube-supported platinum nanoparticles (Pt/CNT) as a catalyst. It achieves a superior formation rate of 3727 μmol gcat.−1 h−1 and a selectivity of 92% for C1-2 oxygenates at 5 oC and 0.1 MPa, significantly surpassing both previously reported thermo-catalytic and ultrasound-driven processes under low-temperature conditions. We find that ultrasound-driven surface cleaning effect enhances the exposure of active Pt sites, thereby facilitating the adsorption of CH4 and O2. Furthermore, the localized and instantaneous high-temperature and high-pressure microenvironment generated by ultrasonic cavitation not only promotes the activation of CH4 and O2 for C−H cleavage and C−O coupling, but also accelerates the mass transfer of reactants and products.