Silicification-Engineered Robust Copper Catalysts for Hydrogenation

Copper phyllosilicate-derived catalysts are promising for hydrogenation reactions to produce important alcohols but often suffer from deactivation due to copper sintering and leaching. Here, we present a robust 20Cu@SiO2 catalyst, fabricated via a kinetically modulated silicification process, for the hydrogenation of ethylene carbonate. A secondary step of quick silicification redistributed copper and formed a mesoporous structure through Cu-phyllosilicate intermediates, enhancing the stability and mass transfer at active sites. Performance tests and ICP analysis showed improved stability, with copper leaching reduced from 17.9% to 1.1% while maintaining excellent activity and selectivity. NH3-temperature-programmed desorption and Auger electron spectroscopy confirmed increased Cu+ species after secondary silicification. This strategy effectively tunes the Cu+/(Cu+ + Cu0) ratio and suppresses copper leaching. This work provides a novel stabilization method with the potential to extend the lifespan of Cu/SiO2 catalysts and advance the design of durable, high-performance hydrogenation catalysts.