Programmable Micelles from DNA-Block Copolymers: Hierarchical Assembly of Catalytically Active Nanostructures

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The DNA molecule, one of the icons of modern science, represents one of the most versatile molecular structures in nature. The use of DNA to build up 2D- and 3D-nanostructures is based on its unique and reversible recognition properties. DNA alone can form the skeleton of these nanostructures, alternatively DNA can serve as an interconnector or template to form DNA-hybrid-nanostructures with other materials. In this proposal we will explore the hierarchical assembly of DNA-based nanoparticles, i.e. DNA block copolymer micelles, and their application as a scaffold for new catalytic systems. The following three applications will be pursued:1) Chiral Catalysis in the corona of ds-DNA block copolymer micelles by intercalating catalysts. It is envisioned that combination of high enantioselectivity of the recently developed DNA-based asymmetric catalysis with the extraordinary rate enhancements observed in micellar catalysis, leading to catalytic systems that combine high activity in aqueous environments with high enantioselectivity.2) Cascade reactions on the corona of DNA block copolymer micelles. In this proposal the modular assembly of different catalytic moieties in the corona of DNA block copolymer micelles will be explored to perform catalytic cascade reactions in a well-defined compartmentalised space.3) Controlled release of encapsulated compounds from the core of the micelle by a catalyst attached to the corona. This could lead to important applications in the area of drug delivery, since the combination of DNA-block copolymer micelles and catalysis will allow the release process to be triggered at a specific time during treatment. This proposed research, which is at the interface of polymer chemistry, bio-nanotechnology, and chemical catalysis, represents a fundamentally new approach towards the hierarchical assembly of new catalytic systems. As such is expected to have a profound impact on both the supramolecular chemistry and catalysis community.