Publication Date

Summer 2023

Degree Type

Thesis

Degree Name

Master of Science (MS)

Department

Chemistry

Advisor

Madalyn Radlauer; Philip Dirlam; Roy Okuda

Abstract

Enzymes, nature’s catalysts, are a crucial component in biological reactions because they help lower the activation energy and speed up these reactions. They display impressive selectivity, catalytic activity, and specificity. However, they can be difficult to produce synthetically, especially on a large scale, and they are not suitable for all reactions for which synthetic catalysts are needed. Metalloenzymes contain a transition metal active site inside the primary coordination sphere (PCS) (ligands directly bound to the metal) that is surrounded by a secondary coordination sphere (SCS) (made up of more distant amino acids) which provides steric bulk and intramolecular interactions between the enzyme and its substrate. These interactions help enzymes achieve their impressive characteristics and selectivity. We aim to synthesize a single chain nanoparticle (SCNP) as an enzyme mimic capable of catalytic activity by using synthetic block polymers that contain both a hydrophilic and crosslinkable (A) block as well as a hydrophobic (B) block to mimic the SCS. The metal and the PCS are mimicked by using a small molecule transition metal complex that will be covalently connected to the AB diblock polymers. To form the SCNPs from linear polymers, the A block will be crosslinked. We have successfully synthesized our target A and B polymers separately as well as introduced crosslinking to the A block to form SCNPs via a Michael addition reaction. Our future work includes chain extension to complete the AB diblock polymer and attach the polymers to the ligand precursor by aminolysis and thiol-ene reactions to form an ABA triblock polymer of the form AB-active site mimic-BA linear polymer, then crosslink to form SCNPs.

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Available for download on Wednesday, November 08, 2028

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