Date of Award

2025

Document Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

Program

Biomedical Sciences

Track

Molecular and Systems Pharmacology

Research Advisor

Richard Lee

Committee

Alejandro Dopico; Daniel Blair; Kirk Hevener; Tommaso Cupido

Abstract

Purpose. Design and synthesize novel compounds to treat Staphylococcus aureus infections by targeting the dysregulation of the Casein Protease P, ClpP. Methods. Utilize established chemical methods to synthesize ureadepsipeptides, small-molecule ClpP activators, and ureadepsipeptide hybrids. Assess their effectiveness by using minimum inhibitory concentration assays and in vitro biochemical assays for ClpP activation. Explore their potential as antibiotics through mitochondrial toxicity tests, glucose/galactose assays, and biophysical measurements related to metabolism and clearance, including thermal shift and surface plasmon resonance assays. Results. Synthesized and tested 33 novel compounds, comprising a total of 80 synthetic steps. Conclusion. The three-part conclusion from the dissertation is that: Heterocycles and bulky side chains are not well tolerated in the ureadepsipeptide structure at the phenylurea position, and a LogD of approximately 2 serves as a good marker for whole-cell activity. Small-molecule ClpP activators can achieve MIC activity but require further optimization for specificity against S. aureus. Biasing the pucker state of the southern proline on the UDEP macrocycle increases MIC activity, but attaching siderophore sidechains to the southern proline via a short linker does not confer broad-spectrum activity to UDEPs.

ORCID

0009-0007-0397-0896

DOI

10.21007/etd.cghs.2025.0699

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