(513ei) Mesoporous Core?Shell Nanostructures Bridging Metal and Biocatalyst for Highly Efficient Cascade Reactions

Chemocatalysis and biocatalysis are usually considered two complementary fields, each with its distinct advantages and limitations. The combination of chemo- and biocatalysts in one-pot acquires synergistic catalytic abilities for cascade reactions that cannot be achieved by either separately. However, the integration of metal and enzyme is still in its infancy due to incompatibility and mutual inactivation. Spatial separation caused by the integration of metal and enzyme on the same defined matrix provides an effective and straightforward avenue to circumvent the incompatibility problems.

In this work mesoporous core−shell structured nanocatalysts with a PdPt bimetallic core and enzyme-immobilized polydopamine (PDA) shell were designed, in which the PDA shell worked as a barrier to position the bimetallic core and enzyme in separated locations. The obtained various bifunctional nanocatalysts with different enzyme enabled efficient two-step one-pot cascade reactions of different types: dynamic kinetic resolution of primary amines in organic solvent with high yield and enantioselectivity (up to 99% yield and 98% ee) and degradation of organophosphate nerve agent in aqueous solution with high rate constant and turnover frequency number values (0.8 min^−1and 20 min^−1, respectively).