Methane C(sp)-H bond activation by water microbubbles

Microbubble-induced oxidation offers an effective approach for activating the C(sp 3 )-H bond of methane under mild conditions, achieving a methane activation rate of up to 6.7% per hour under optimized parameters. In this study, microbubbles provided an extensive gas-liquid interface that promoted...

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Veröffentlicht in:Chemical science (Cambridge) 2024-10, Vol.15 (41), p.1726-1731
Hauptverfasser: Li, Juan, Xu, Jinheng, Song, Qingyuan, Zhang, Xinxing, Xia, Yu, Zare, Richard N
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Sprache:eng
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Zusammenfassung:Microbubble-induced oxidation offers an effective approach for activating the C(sp 3 )-H bond of methane under mild conditions, achieving a methane activation rate of up to 6.7% per hour under optimized parameters. In this study, microbubbles provided an extensive gas-liquid interface that promoted the formation of hydroxyl (OH&z.rad;) and hydrogen radicals (H&z.rad;), which facilitated the activation of methane, leading to the generation of methyl radicals (CH 3 &z.rad;). These species further participated in free-radical reactions at the interface, resulting in the production of ethane and formic acid. The microbubble system was optimized by adjusting gas-liquid interaction time, water temperature, and bubble size, with the optimal conditions (150 s of water-gas interaction, 15 °C, 50 μm bubble size) yielding a methane conversion rate of 171.5 ppm h −1 , an ethane production rate of 23.5 ppm h −1 , and a formic acid production rate of 2.3 nM h −1 during 8 h of continuous operation. The stability and efficiency of this process, confirmed through electron spin resonance, high-resolution mass spectrometry, and gas chromatography, suggest that microbubble-based methane activation offers a scalable and energy-efficient pathway for methane utilization. Microbubble-induced oxidation offers an effective approach for activating the C(sp 3 )-H bond of methane under mild conditions, achieving a methane activation rate of up to 6.7% per hour under optimized parameters.
ISSN:2041-6520
2041-6539
DOI:10.1039/d4sc05773b