Pan Yingtong, Li Ruofan, Zhang Ling, Liu Ji-Xuan, Wang Wenzhong, Zhang Guo-Jun
State Key Laboratory of Advanced Fiber Materials, College of Materials Science and Engineering, Institute of Functional Materials, Donghua University, Shanghai, China.
State Key Laboratory of High Performance Ceramics, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, China.
Nat Commun. 2025 Aug 13;16(1):7506. doi: 10.1038/s41467-025-62924-2.
The partial oxidation of methane (POM) into value-added C chemicals (e.g., CHOH, 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 chemicals (129.26 µmol h) and methane conversion rate (22%) were achieved under ambient conditions (298 K, P = 0.1 bar, P = 0.1 bar, P = 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.
将甲烷部分氧化（POM）转化为增值碳化学品（如CHOH、HCHO和CO）为温和条件下的天然气利用提供了一种很有前景的方法。然而，现有的POM系统通常依赖复杂的催化剂设计和添加额外的氧化剂。在此，我们通过将机械搅拌与低频超声场相结合，开发了一种无催化剂的POM系统。在环境条件（298 K，P = 0.1 bar，P = 0.1 bar，P = 0.8 bar）下实现了高碳化学品生产率（129.26 µmol h）和甲烷转化率（22%）。机理研究表明，机械搅拌的引入放大了超声空化效应，促进了活性氧的原位释放。反应途径研究证实，羟基自由基促进了甲烷C-H键的裂解，并且氧气参与了POM产物的生成。该策略为甲烷的增值转化提供了一条可持续的途径。
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