Boosting C2+ Selectivity in CO₂ Electroreduction on Cu Nanoparticles via Molecular Dispersion of Cobalt Phthalocyanine

Cu‐based tandem catalysts have been widely studied due to their excellent performance in electrocatalytic reduction of carbon dioxide (CO2RR) to produce C2+ products. However, during the CO2RR process, Cu atoms face the issue of dynamic restructuring, resulting in relatively poor stability and single‐product selectivity. Herein, Cobalt phthalocyanine (CoPc) was integrated with Cu nanoparticles (NPs) to prepare a tandem catalyst (Cu/CoPcx) by in‐situ growth method, significantly enhancing the selectivity of Cu‐based catalysts for C2+ products. The optimal material, Cu/CoPc0.004, achieved a Faradaic efficiency (FE) of 73.17% for C2+ products, with a C2+ product current density exceeding 377 mA/cm2. More importantly, tandem catalyst Cu/CoPc0.004 exhibits high selectivity for ethylene, achieving a FE of 52.35% at ‐1.26 V (versus reversible hydrogen electrode) with a high ethylene current density (270 mA/cm2). The experimental results indicate that the interaction between CoPc and Cu NPs introduces numerous oxygen vacancies and stabilizes the presence of Cu+. Moreover, the unique structure of the cascade catalyst enables CoPc to provide a large amount of CO intermediates for Cu active sites, thus promoting C‐C coupling and facilitating the formation of C2+ products.