Confinement Self-Assembly of Metal-Organic Cages within Mesoporous Carbon for One-Pot Sequential Reactions

Well-defined discrete metal-organic cages have been very attractive in the field of supramolecular catalysis. However, their potential to serve as heterogeneous catalysts for one-pot reactions remains unexplored. Herein, we present the success of confinement self-assembly of TEMPO-containing M₁₂L₂₄ cage within the cavity of amino-functionalized mesoporous carbon FDU-ED, which gave rise to a highly efficient heterogeneous catalyst for one-pot oxidation-Knoevenagel condensation reaction. The orthogonal feature of the isolated catalytic sites within the obtained bifunctional heterogeneous catalyst leads to enhanced catalytic activities, selectivity, and recyclability for the overall transformation, which provides valuable information and methodology for design of the next-generation heterogeneous catalysts based on supramolecular architectures. The longer-term ambition is to put forward a new platform for the advent of catalysts with unique and exciting reactivity.