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 methane activation mechanism at room temperature. The research results were published online in the Journal of the Royal Society of Chemistry, Chemical Science (DOI: 10.1039 / C2SC20434G).

Methane is the main component of natural gas, but due to its extremely high inertness, its activation is often difficult. The activation and conversion of methane is considered to be one of the most challenging research directions in catalysis and the entire chemical research field. Recently, Deng Feng's research team prepared a highly active zinc-modified molecular sieve catalyst (ZnZSM-5) that can activate methane at room temperature. Using in-situ solid 13C NMR technology, the researchers found that methane can be cracked at room temperature to generate a large number of surface methoxy (-OCH3) species, which is an active intermediate, generally made of methanol or olefins on acidic molecular sieve catalyst Get. But for methane, the formation of this species was observed at room temperature in a heterogeneous catalytic system, indicating the high reactivity of the ZnZSM-5 catalyst.

Further research found that surface methoxy species can react with water to produce methanol at room temperature, and then methanol can also be converted into high value-added gasoline components through the MTG process. Through NMR and other experimental techniques combined with quantitative calculations, the researchers found that the Zn-O-Zn active center with an open shell structure can homogenize methane to generate methyl radicals, which are combined with the molecular sieve framework through migration Generate surface methoxy species.

These research results have certain reference significance for the activation and conversion of methane and other lower alkanes in the heterogeneous catalytic system and the design of related catalysts.

In the previous work, the research team also found that the ZnZSM-5 catalyst can convert methane and carbon monoxide into acetic acid under mild conditions of 523 K, and revealed its catalytic reaction mechanism by in situ 13C NMR experiments (Angew. . Ed. 2012, 51, 3850 -3853).

The research was supported by the National Natural Science Foundation of China, the Ministry of Science and Technology and the Chinese Academy of Sciences.

Progress in research on activation mechanism of methane at room temperature

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