Atomic Layered ZnO Between Cu Nanoparticles and a PVP Polymer Layer Enable Exceptional Selectivity and Stability in Electrocatalytic CO2 Reduction to C2H4

Abstract This study employs a chemically controlled strategy to construct a few‐atomic‐layer ZnO structure integrated with polyvinylpyrrolidone (PVP) and nanoscale metallic copper on active carbon. Hydrogen‐bond interactions from PVP's N‐vinylpyrrolidone allow ZnO to retain a specific proportion of metal atoms, confining electrons at the Cu/ZnO interface to form CuZn nanoalloy clusters. The nanoalloy's dual role in promoting CO adsorption and C─C coupling synergistically boosts C 2 H 4 production during electrochemical CO 2 reduction (ECR). Rapid Cu regeneration further increases adsorbed hydrogen (H ads ) from water splitting, achieving a remarkable C 2 H 4 selectivity of ≈50.2% with stable performance over 10 h. The Zn→Cu electron confinement and interfacial synergy at the organic‐oxide‐metal heterojunction underscore the catalyst's superior efficiency, offering a promising pathway for sustainable CO 2 ‐to‐C 2 H 4 conversion.