Single-Crystal Metal–Organic and Covalent Organic Framework Hybrids Enable Efficient Photoelectrochemical CO2 Reduction to Ethanol

-to-ethanol conversion. Particularly, the Pt-MOCOF delivers a Faradaic efficiency (FE) of 83.5% at -1.0 V with 91.7% carbon selectivity, surpassing state-of-the-art COF or MOF catalysts and ranking it among the top-performing catalysts. The catalyst system displays remarkable stability, maintaining 95% of its activity after 100 h of continuous operation. Experiments and theoretical calculations revealed that the cooperative catalyst enriches and stabilizes intermediates in the channels, guiding the reaction pathway toward ethanol production.