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<p>The partial oxidation of methane (POM) into value-added C<sub>1</sub> chemicals (e.g., CH<sub>3</sub>OH, HCHO, and CO) offers a promising approach for natural gas utilization under mild conditions. However, existing POM systems often rely on complex catalyst designs and the addition of extra oxidants. Here, we developed a catalyst-free POM system by integrating mechanical stirring with a low-frequency ultrasonic field. A high production rate of C<sub>1</sub> chemicals (129.26 µmol h<sup>−1</sup>) and methane conversion rate (22%) were achieved under ambient conditions (298 K, P<sub>CH4</sub> = 0.1 bar, P<sub>O2</sub> = 0.1 bar, P<sub>N2</sub> = 0.8 bar). Mechanism studies revealed that the introduction of mechanical stirring amplified the ultrasonic cavitation effect, promoting the in-situ release of reactive oxygen species. Reaction pathway investigation confirmed that hydroxyl radicals facilitated the cleavage of methane C-H bonds and that oxygen participated in the generation of POM products. This strategy provides a sustainable avenue for the value-added conversion of methane.</p>

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Catalyst-free partial oxidation of methane under ambient conditions boosted by mechanical stirring-enhanced ultrasonic cavitation

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年8月13日

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  • Yingtong Pan,
  • Ruofan Li,
  • Ling Zhang,
  • Ji-Xuan Liu,
  • Wenzhong Wang,
  • Guo-Jun Zhang

摘要

The partial oxidation of methane (POM) into value-added C1 chemicals (e.g., CH3OH, HCHO, and CO) offers a promising approach for natural gas utilization under mild conditions. However, existing POM systems often rely on complex catalyst designs and the addition of extra oxidants. Here, we developed a catalyst-free POM system by integrating mechanical stirring with a low-frequency ultrasonic field. A high production rate of C1 chemicals (129.26 µmol h−1) and methane conversion rate (22%) were achieved under ambient conditions (298 K, PCH4 = 0.1 bar, PO2 = 0.1 bar, PN2 = 0.8 bar). Mechanism studies revealed that the introduction of mechanical stirring amplified the ultrasonic cavitation effect, promoting the in-situ release of reactive oxygen species. Reaction pathway investigation confirmed that hydroxyl radicals facilitated the cleavage of methane C-H bonds and that oxygen participated in the generation of POM products. This strategy provides a sustainable avenue for the value-added conversion of methane.