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Direct conversion of methane with O2 at room temperature over edge-rich MoS2
Nature Catalysis ( IF 42.8 ) Pub Date : 2023-09-21 , DOI: 10.1038/s41929-023-01030-2
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

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.



中文翻译:

室温下甲烷与 O2 在边缘富集的 MoS2 上直接转化

直接使用廉价的O 2作为氧化剂在低温下将甲烷转化为增值化学品为甲烷利用提供了理想的途径,但由于甲烷的化学惰性和O 2的低活性,仍然是一个巨大的挑战。甲烷单加氧酶是唯一已知可以在室温下将甲烷与O 2转化的天然催化剂。在这里,我们报告了在边缘富集的 MoS 2上利用 O 2将甲烷直接转化为 C1 含氧化合物的人工过程的实现催化剂在 25 °C 下可实现 4.2% 的显着甲烷转化率,并且对 C1 含氧化合物的选择性 > 99%。原位光谱和微观表征以及理论计算表明,MoS 2边缘硫空位的双核钼位点可以直接解离O 2形成O=Mo=O*活性物种,从而激活C-H键并使甲烷能够生成室温下的转化。

更新日期:2023-09-21
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