Abstract

Antibiotics are facing significant challenges due to the emergence of resistance and the slow pace of discovery. A deeper understanding of the enzymes responsible for antibiotic resistance and virulence is important to address this growing threat. This dissertation focuses on investigating key enzymatic mechanisms underlying tetracycline resistance and tabtoxin biosynthesis. Specifically, a series of inhibitors, including two covalent inhibitors, were rationally designed and synthesized to target tetracycline destructases, with the goal of restoring the efficacy of tetracycline antibiotics through combination therapy. In parallel, the early steps of tabtoxin biosynthesis were explored. A SAM-dependent enzyme TblA was found to exhibit unexpected cyclopropane synthase activity, expanding the known catalytic repertoire of this enzyme family. These findings provide new insights into antibiotic resistance and biosynthetic enzymes, offering promising strategies for combating antibiotic resistance and expanding our knowledge of enzyme functions.

Committee Chair

Timothy Wencewicz

Committee Members

Gautam Dantas; John-Stephen Taylor; Joseph Jez; Kevin Moeller

Degree

Doctor of Philosophy (PhD)

Author's Department

Chemistry

Author's School

Graduate School of Arts and Sciences

Document Type

Dissertation

Date of Award

8-4-2025

Language

English (en)

Available for download on Wednesday, August 14, 2030

Included in

Chemistry Commons

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