Tailored Organocatalysis for Novel Macromolecular Architectures and Macromolecules for Enzyme-Inspired Catalysis

​Tailored Soft Materials for Catalysis and Transport/Encapsulation

Branched macromolecules can be prepared with a high degree of control over their nanoscale structures, approximating the useful features of natural biopolymers. Aiming to create materials for enzyme-like catalysis, we develop general approaches for ready accessibility of complex macromolecular assemblies and for the rapid generation of structural diversity. Catalytic moieties are immobilized on these polymer scaffolds using a few extremely efficient “click” reactions, or through “phase tags.” The macromolecular toolbox thus developed enables us to perform systematic studies of reactivity in nanoscale phases.

Controlled Nanoenvironments for Catalysis

The remarkable catalytic performance of enzymes is the result of precise control over the relative positions of the active center and incoming substrates, finely-tuned local solvent environment and the participation of metal ions and cofactors. We aim to devise systems with enzyme-like pre-organization of functional groups around the active sites. We are particularly interested in the use of supramolecular interactions for imparting selectivity to nanocatalysts and in chiral environments for enantioselective catalysis.

Efficient Polymerization Strategy for Preparing Polypeptides with Well-Defined Macromolecular Architectures

A novel highly efficient strategy based on an "alliance" of primary and secondary amine initiators was successfully developed, allowing for the fast and living ring-opening polymerization (ROP) of α-amino acid N-carboxyanhydrides (NCAs) at room temperature. The polypeptides are being explored for their applications in catalysis. 

Well-defined (co)polypeptides bearing pendant alkyne groups for “click” chemistry

A novel metal-free strategy using hydrogen-bonding catalytic ring opening polymerization of alkyne-functionalized N-carboxy anhydrides of α-amino acids was developed for the synthesis of well-defined polypeptides bearing pendant alkyne groups. This method provides an efficient way to synthesize novel alkyne-functionalized homopolypeptides (A) and copolypeptides such as AB diblock (B) non-functionalized), ABA triblock and star-AB diblock as well as linear and star random copolypeptides, which are the precursors of a plethora of complex macromolecular architectures achieved by "click" chemistry.

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