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

Pan, Yingtong; Li, Ruofan; Zhang, Ling; Liu, Ji-Xuan; Wang, Wenzhong; Zhang, Guo-Jun · Nat Commun · 2025

basic_science · Level V

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Abstract

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.