Single-chain polymeric systems: design, synthesis, and applications

Abstract

Single-chain polymeric nanoparticles (SCNPs) have been explored for applications in biomedicine such as drug delivery, catalysis, and imaging. These SCNPs are generated from the intramolecular folding or collapse of the single-chain polymer where the collapse is achieved by self-assembly or covalent crosslinking. In this thesis, the intramolecular self-assembly of single-chain polymeric systems is explored in catalysis and fluorescence. In Chapter 2, we developed an amphiphilic ruthenium-containing single-chain polymer that promotes allyl carbamate cleavage reactions in aqueous and biologically relevant conditions. This polymeric catalyst works in synergy with the enzyme β-galactosidase to perform a tandem reaction on a single substrate. Additionally, the polymer catalyst was characterized by various methods to study its self-assembly. In Chapter 3, we investigated a modular approach to SCNPs for catalysis that consists of an amphiphilic single-chain polymer that folds under dilute aqueous conditions resulting in unimolecular micelle-like structures. This modular approach allows binding of various catalysts and substrates leading to reaction rate enhancement. In Chapter 4, we developed fluorophore-containing single-chain polymers that may be useful in bioimaging. The polymers solubilized and stabilized various types of organic fluorophores leading to brighter and more stable fluorophores.