The Deng Feng research group of the State Key Laboratory of Spectroscopy and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences, has made important progress in the study of the reaction mechanism of the catalytic conversion of methane and carbon monoxide to acetic acid. Related research results have been published online in Angew. Chem. Int. Ed.

Methane is the main component of natural gas. As a chemical raw material with abundant reserves and low prices, it has important economic value to convert it into high value-added chemicals. However, methane is the most stable natural organic small molecule, and its activation and conversion has always been one of the most challenging problems in the field of catalytic chemistry. The biggest difficulty comes from the lack of catalysts for efficient activation and conversion and less clear catalysis Reaction mechanism.

The heterogeneous catalytic magnetic resonance research group led by Researcher Deng Feng has long been devoted to the development of solid-state NMR methods and the study of the structure and reaction performance of environmentally friendly solid catalysts. Aiming at the characteristics of methane C−H bond activation, Associate Researcher Xu Jun and Dr. Wang Xiumei of the research group prepared a bifunctional Zn-modified zeolite molecular sieve catalyst (ZnZSM-5) with acidity and redox properties, and Using this catalyst, the mild conversion of methane and carbon monoxide to acetic acid was achieved at 523K.

In-situ 13C solid-state NMR tracking of the reaction process showed that methane and carbon monoxide produced acetic acid through two pathways controlled by the reaction intermediates (ZnCH3 and ZnOCH3). By adjusting the redox atmosphere of the reaction system, the formation of reaction intermediates can be controlled, thereby achieving the purpose of regulating the reaction channel.

The results of this study are expected to provide a new way for the activation and selective conversion of methane and other lower alkanes. The research work has received key support from the National Natural Science Foundation of China, the Ministry of Science and Technology and the Chinese Academy of Sciences.

Reaction mechanism of methane carbonylation to acetic acid on Zn modified zeolite molecular sieve

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