Title: Direct conversion of methane with O2 at room temperature over edge-rich MoS2

Authors: Jun Mao, Huan Liu, Xiaoju Cui, Yunlong Zhang, Xiangyu Meng, Yanping Zheng, Mingshu Chen, Yang Pan, Zhenchao Zhao, Guangjin Hou, Jingting Hu, Yanan Li, Guilan Xu, Rui Huang, Liang Yu* & Dehui Deng*

Abstract: Conversion of methane to value-added chemicals at low temperature by directly using inexpensive O₂ as oxidant offers an ideal route for methane utilization but remains a great challenge due to the chemical inertness of methane and the low activity of O₂. Methane monooxygenase is the only known natural catalyst that can convert methane with O₂ at room temperature. Here we report the realization of an artificial process for the direct methane conversion to C1 oxygenates with O₂ on an edge-rich MoS₂ catalyst at 25 °C, which delivers a remarkable methane conversion of 4.2% with >99% selectivity for C1 oxygenates. In situ spectroscopic and microscopic characterizations and theoretical calculations reveal that the binuclear molybdenum sites of sulfur vacancies at the MoS₂ edge can directly dissociate O₂ to form O=Mo=O* active species, which can activate the C–H bond and enable methane conversion at room temperature.

Full-Link: https://www.nature.com/articles/s41929-023-01030-2