CHEMICAL SCIENCE

The new catalyst enables efficient conversion of methane


With the large-scale exploitation of shale gas, the direct selective conversion of its main product methane into high value-added oxygenated compounds under mild conditions has attracted widespread attention from researchers. Recently, Wang Xiaodong, researcher Wang Xiaodong, researcher Lin Jian, researcher of Dalian Institute of Chemical Physics, Chinese Academy of Sciences, and Lin Sen, professor of Fuzhou University, have made new progress in the research of single-atom catalytic enhancement of direct oxidation of methane. The cooperative team developed a single-atom Ru catalyst assembled with MOFs zirconium oxygen cluster node, which realized the efficient conversion of methane and can be hydroxylated to oxygen-containing compounds by nearly 100%. The results were published in the Journal of the American Chemical Society.

Schematic diagram of the catalytic structure

Methane molecules have a highly symmetrical tetrahedral structure, and the C-H bonds contained in them are difficult to polarize, and the efficient activation and directional conversion of methane by modulating the active center structure of the catalyst is known as the “holy grail topic” in the field of catalysis. So far, the strategy of combining metal single/diatomic catalysts with the addition or synthesis of hydrogen peroxide oxidants has been mainly used, although it can promote methane activation to a certain extent, but there is still the problem of excessive oxidation of target products.

In this work, based on the unique geometric and electronic properties of UiO-66-based MOFs discovered earlier, the researchers developed a high-performance Ru1/UiO-66 single-atom catalyst, which can achieve hydroxylation of methane to oxygenated compounds under mild conditions with nearly 100% selectivity and a conversion frequency of 185.4h-1. Compared with nano-Ru catalysts and traditional carrier-supported Ru single atoms, Ru1/UiO-66 has higher oxygen-containing yield and no excessive oxidation product carbon dioxide. The biposition synergy between monatomic Ru and UiO-66 is an intrinsic factor that improves the hydroxylation activity of methane and the selectivity of oxygenated compounds.

In recent years, the team has been committed to the development of high-efficiency low-carbon alkane selective oxidation catalysts, which provides reference for the construction of single-atom catalysts for low-carbon alkanes to produce high value-added products. (Source: Sun Danning, China Science News)

Related paper information:https://doi.org/10.1021/jacs.3c02121



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