4.8 Article

Zeolite-encaged mononuclear copper centers catalyze CO2 selective hydrogenation to methanol

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NATIONAL SCIENCE REVIEW
卷 10, 期 7, 页码 -

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OXFORD UNIV PRESS
DOI: 10.1093/nsr/nwad043

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CO2 hydrogenation; zeolite; methanol; catalysis; mononuclear copper

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This study reports a method for selectively hydrogenating carbon dioxide to methanol using renewable hydrogen sources, which is both environmentally friendly and carbon neutral. By designing faujasite-encaged mononuclear Cu centers, stable methanol production and selectivity were achieved. This work provides a clear example of structure-activity relationship in catalysis and highlights the advantages of zeolite catalysis in complex chemical transformations.
The selective hydrogenation of CO2 to methanol by renewable hydrogen source represents an attractive route for CO2 recycling and is carbon neutral. Stable catalysts with high activity and methanol selectivity are being vigorously pursued, and current debates on the active site and reaction pathway need to be clarified. Here, we report a design of faujasite-encaged mononuclear Cu centers, namely Cu@FAU, for this challenging reaction. Stable methanol space-time-yield (STY) of 12.8 mmol g(cat)(-1) h(-1) and methanol selectivity of 89.5% are simultaneously achieved at a relatively low reaction temperature of 513 K, making Cu@FAU a potential methanol synthesis catalyst from CO2 hydrogenation. With zeolite-encaged mononuclear Cu centers as the destined active sites, the unique reaction pathway of stepwise CO2 hydrogenation over Cu@FAU is illustrated. This work provides a clear example of catalytic reaction with explicit structure-activity relationship and highlights the power of zeolite catalysis in complex chemical transformations. Zeolite with confined mononuclear Cu ions can efficiently catalyze the selective hydrogenation of CO2 to methanol by dihydrogen at relatively low reaction temperatures.

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