DOI: 10.1021/jacs.6c17330 ISSN: 0002-7863

Continuous-Flow Irradiation Facilitates Catalyst-Free Methane-to-Methanol Conversion

Songbai Tang, Xianhuan Hao, Daopeng Sheng, Zining Wang, Zhiyong Peng, Dan Zhou, Qianhui Wu, Song Yu, Weiqiang Liao, Congchong Yan, Lixi Chen, Jun Ma, Yanlong Wang, Zhifang Chai, Shuao Wang

Abstract

Converting methane to methanol (MTM) holds far-reaching practical implications, yet achieving both high productivity and high selectivity remains a longstanding challenge owing to the inertness of methane and the susceptibility of methanol to overoxidation. Here, we propose a continuous-flow irradiation system (CIS) by coupling radiation technology and flow chemistry for efficient MTM under ambient conditions. High-energy radiation promises direct methane activation in an oxidant-independent and catalyst-free manner with high efficiency, which enables its integration with continuous-flow synthesis that decouples CH4 activation from methanol formation in time and space, thereby preventing overoxidation and undesirable cascade side reactions. The CIS–MTM achieves a superior methanol production rate (68.3 μmol·h–1, at a dose rate of 7.2 kGy·min–1, 83.2 RH%, CH4 flow rate 60 mL·min–1) than most existing indirect activation routes, with economic scalability comparable to industrial methods. This work introduces radiation technology as a potential direct activation method for methane conversion.

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