"Design and synthesis of crosslinkable amphiphilic PEGylated poly(amino" by Adekunle Titus Akinmola

Date of Award

2025

Document Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

Department

Materials Science

Committee Chair

Carmen Scholz

Committee Member

Bernhard Vogler

Committee Member

Geoffrey Bothun

Committee Member

Judith Schneider

Committee Member

Kyung-Ho Roh

Research Advisor

Carmen Scholz

Subject(s)

Polymerization, Block copolymers, Iron oxides--Magnetic properties, Nanoparticles, Drug delivery systems

Abstract

The development of polymeric micelles for biomedical applications has been of significant interest due to their potential for targeted delivery for therapeutic and diagnostic agents. This dissertation focusses on the synthesis, characterization, and application of amphiphilic PEGylated poly(amino acid) block copolymers as nanocarriers for superparamagnetic iron oxide nanoparticles (SPIONs) in magnetic particle imaging (MPI). Series of novel diblock and triblock copolymers were synthesized through ring-opening polymerization of amino acid N-Carboxyanhydrides (NCAs) to afford HO-PEG77-b-p(L-Leu)m and HO-PEGx-b-p(Allyl-L-Gly)10-b-p(L-Leu)n. These polymers were further functionalized to yield their folate conjugates through dicyclohexylcarbodiimide (DCC) coupling. NMR and FTIR were used to verify the chemical structures of the block copolymeers. The copolymers were further characterized by TGA and DSC and it was found that increasing the hydrophobic block led to copolymers that were thermally more stable. The resulting amphiphilic block copolymers were self-assembled into micelles. The encapsulation of SPIONs within the micelle core was explored, thus confirming their potential for magnetic particle imaging (MPI). Photoinitiated crosslinking was employed to enhance micelle stability. It was shown that these crosslinked micelles were able to retain structural integrity after lyophilization and exhibited no measurable critical micelle concentration (CMC), which signifies successful crosslinking. TEM measurements showed the micelles morphology and size. The size data were corroborated by DLS studies, which also indicated a narrow size distribution.

Comments

Submitted ... in the joint Interdisciplinary Materials Science program.

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