Assembling a Heterobimetallic Actinide Metal‐Organic Framework by a Reaction‐Induced Preorganization Strategy

Periodically arranging coordination‐distinct actinides into one crystalline architecture is intriguing but of great synthetic challenge. We report a rare example of a heterobimetallic actinide metal–organic framework (An‐MOF) by a unique reaction‐induced preorganization strategy. A thorium MOF (SCU‐16) with the largest unit cell among all Th‐MOFs was prepared as the precursor, then the uranyl was precisely embedded into the MOF precursor under oxidation condition. Single crystal of the resulting thorium‐uranium MOF (SCU‐16‐U) shows that a uranyl‐specific site was in situ induced by the formate‐to‐carbonate oxidation reaction. The heterobimetallic SCU‐16‐U exhibits multifunction catalysis properties derived from two distinct actinides. The strategy proposed here offers a new avenue to create mixed‐actinide functional material with unique architecture and versatile functionality. Benefiting from the unique architecture of the largest‐unit‐cell thorium metal–organic framework (MOF), a second actinide, uranyl, with dintinct coordination behaviour was successfully assembled into the framework via a novel reaction‐induced preorganization strategy to yield a rare single crystalline heterobimetallic actinide MOF.