Ag‐Regulated Cu‐Sites on a Conductive Cu‐Metal‐Organic Framework for Enhanced CO 2 Electroreduction to CH 4

ABSTRACT Electrochemical reduction of CO 2 into value‐added chemicals using renewable electricity offers a promising pathway for sustainable fuel production, yet its industrial implementation has been hindered by lack of efficient and stable catalysts. Here we present a series of silver nanoparticles (Ag NPs) modified 2D conductive Cu‐MOF, namely Cu 3 (HHTP) 2 (H 6 HHTP = 2,3,6,7,10,11‐hexahydroxytriphenylene), demonstrating enhanced catalytic activity and selectivity. The optimized Ag@Cu 3 (HHTP) 2 composite exhibits superior electrocatalytic performance, achieving a Faradaic efficiency (FE) of 65.1% for CH 4 production at commercially relevant current density (−240 mA cm −2 ) while maintaining stable operation for 24 h under industrial‐grade current density. Mechanistic investigations show that the incorporation of Ag NPs induces dual‐functional effects: (1) electronic structure optimization through interfacial charge redistribution and (2) enhanced CO 2 adsorption and activation capacity. This study establishes a fundamental paradigm for designing high‐performance MOF‐based electrocatalysts for CO 2 reduction through rational metal decoration strategy.