Rational Construction of an Exceptionally Stable MOF Catalyst with Metal‐Adeninate Vertices toward CO2 Cycloaddition under Mild and Co‐Catalyst Free Conditions

: CO2 is considered as the primary greenhouse gas, resulting in a series of serious environmental problems that affect people's life and health. Carbon capture and sequestration has been implemented as one of the most appealing pathways to control and use CO2 . Here, we rationally integrate various functional sites within the confined nanospace of a microporous metal-organic framework (MOF) material, which is constructed by mixed-ligand strategy based on metal-adeninate vertices. It not only exhibits excellent stability but also can efficiently transform CO2 and epoxides to cyclic carbonates under mild and cocatalyst-free conditions. Additionally, this catalyst shows extraordinary recyclability for the CO2 cycloaddition reaction.