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

The selective hydrogenation of CO₂ to methanol by renewable hydrogen source represents an attractive route for CO₂  recycling and carbon neutral. Stable catalysts with high activity and  methanol selectivity are being hotly pursued, and current debates on the  active site and reaction pathway need to be clarified. Here, we report  the 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/h 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.