Self-exfoliating Bimetallic Metal–Organic Framework Layer with Intralayer π–π Interactions for Efficient Electrical Transport and CO2 Electroreduction

Two-dimensional metal–organic frameworks (2D MOF) have attracted great attention in the electrocatalytic reduction of CO₂ owing to their well-defined structure and high surface area. Nevertheless, how to combine accessible metal active sites with high electron transfer still poses challenges in structural assembly. Herein, two-dimensional AgCe-MOFs with intralayer π–π stacking interactions were assembled by linking one-dimensional Ce–O chains to Ag(I). Its nanosheet can be facilely prepared via self-exfoliation upon the loss of uncoordinated interlayer acetonitrile. The 2D AgCe-MOF nanosheets’ merits of more exposed active sites and efficient electron transfer channels have displayed outstanding electrochemical performance and 99.5% selectivity in electrocatalytic CO₂ reduction to CO. The establishment of efficient electrical transport channels and high exposure of catalytic sites in a framework through designed supramolecular interactions is expected to be a potential strategy for the construction of efficient electrocatalysts.