Electrocatalytic reduction can convert excess emissions of CO2 into high value-added chemicals, but the highly active and selective of electrocatalytic CO2 reduction is still facing great challenges. Molecular catalysts with well-defined structures are conducive to elucidate the essential causes of high selectivity in electrocatalysis. Here, we report the ethylene Faradaic efficiency (FE) of 50%, a highest FE for C2+ of about 65% at -1.19 V vs. reversible hydrogen electrode (RHE) on strain-assisted dual copper complex Cu2(Ophen)2. Also, the catalyst can exhibit stable for 15 hours at 180 mA/cm2. Operando X-ray absorption spectroscopy (XAS) experiments proved that reveal that the copper complex immobilized in mesoporous carbon stably exists in the oxidation state of Cu(I) and inhibits the generation of copper particles. Moreover, the density functional theory (DFT) calculations also demonstrate that the strain effect can regulate the d-band center of the catalyst to decrease the Gibbs free energy change of potential determining step (*COCO → *COCOH).

Strain-assisted dual copper complex for highly selective electrochemical CO2 reduction to ethylene

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