Efficient direct transformation of methane into value-added chemicals has great significance for long-termsustainability of fuels and chemicals, but remains a major challenge due to its high inertness.Compared with the direct activation and conversion of methane alone, the introduction of small molecule coupling can effectively reduce the reaction temperature required for methane activation and improve the conversion efficiency of methane.

Recently，research team led by Prof. ZHU wenliang has made new progress in the study of coupling reaction of methane and CO, and successfully prepared a type of zinc modified HZSM-5 zeolite catalyst that exhibited excellent catalytic performance in the coupling reaction of methane and CO.

It is found that increasing the temperature and pressure is beneficial to the conversion of methane, and the products at low reaction temperature (673K) are mainly low-carbon hydrocarbons (the selectivity of C2 hydrocarbons is as high as 92%), and the high reaction temperature is mainly aromatics (823K, aromatics selectivity isup to 80%). isotope labellingexperiments demonstrate that approximately 50% of the carbon atoms in all the hydrocarbon products originatefrom carbon monoxide, whereas another half of the carbons come from methane. In-situ infrared andNMR characterizations indicate that acyl compounds and/or acetic acid formatted by carbonylation of methane and CO maybe the intermediate species in the formation of hydrocarbons.

This work provides a new research idea for the direct conversion of methane to produce high value-added products.

Related research results, entitled "Coupling conversion of methane with carbon monoxide via carbonylation over Zn/HZSM-5 catalysts", werepublished onCatalysis Science & Technologyrecently. This research was supported by the National Natural Science Foundation of China and Chinese Academy of Sciences (XDA). (Text by WEN fuli, ZHU wenliang)

Coupling conversion of methane with carbonmonoxide via carbonylation over Zn/HZSM-5catalysts. Fuli Wen, Jin Zhang, Zhiyang Chen, Ziqiao Zhou,Hongchao Liu*,Wenliang Zhu*, Zhongmin Liu, CatalysisScience &Technology, 11:1358-1364,2021.