Synergetic catalysis via zeolite-encapsulated PdCu alloy for highly efficient CO2 hydrogenation to ethanol

ABSTRACT CO2 catalytic hydrogenation presents a highly promising and alternative pathway for ethanol production, offering the dual benefits of large-scale CO2 emission reduction and green H2 storage. However, this approach faces major challenges such as low ethanol selectivity and activity, stemming from the complex reaction network and the lack of efficient catalyst design strategies. In this work, we proposed an effective catalyst design strategy for CO2 hydrogenation to ethanol by constructing synergetic catalytic sites between alloy nanoparticles and zeolite to decouple key competing reaction steps. The developed PdCu alloy catalyst encapsulated by Y zeolite achieved simultaneously high ethanol selectivity (>93%) and activity (>200 mg gcat−1 h−1), outperforming most previously reported heterogeneous catalysts. Mechanistic investigations revealed that the alloy–zeolite synergetic sites facilitate controllable C–C coupling and enhance C–O bond cleavage, thereby balancing selectivity and catalytic activity toward CO2 hydrogenation to ethanol. This work offers a feasible catalyst design strategy for the efficient conversion of CO2 into high-value-added and structurally complex products.