Single‐Site Metal–Organic Framework and Copper Foil Tandem Catalyst for Highly Selective CO2 Electroreduction to C2H4

Tandem catalysis is a promising way to break the limitation of linear scaling relationship for enhancing efficiency, and the desired tandem catalysts for electrochemical CO₂ reduction reaction (CO₂ RR) are urgent to be developed. Here, a tandem electrocatalyst created by combining Cu foil (CF) with a single-site Cu(II) metal-organic framework (MOF), named as Cu-MOF-CF, to realize improved electrochemical CO₂ RR performance, is reported. The Cu-MOF-CF shows suppression of CH₄ , great increase in C₂ H₄ selectivity (48.6%), and partial current density of C₂ H₄ at -1.11 V versus reversible hydrogen electrode. The outstanding performance of Cu-MOF-CF for CO₂ RR results from the improved microenvironment of the Cu active sites that inhibits CH₄ production, more CO intermediate produced by single-site Cu-MOF in situ for CF, and the enlarged active surface area by porous Cu-MOF. This work provides a strategy to combine MOFs with copper-based electrocatalysts to establish high-efficiency electrocatalytic CO₂ RR.