Authors

Rong Zhou

Type

Text

Type

Dissertation

Advisor

Li, Qiang | Dale G. Drueckhammer | Daniel P. Raleigh | Peter J. Tonge | Subramanyam Swaminathan.

Date

2010-08-01

Keywords

Biochemistry | Drug target, MbtI, Menaquinone, MenE, Mycobacterium Tuberculosis, Staphylococcus aureus

Department

Department of Chemistry

Language

en_US

Source

This work is sponsored by the Stony Brook University Graduate School in compliance with the requirements for completion of degree.

Identifier

http://hdl.handle.net/11401/72734

Publisher

The Graduate School, Stony Brook University: Stony Brook, NY.

Format

application/pdf

Abstract

A detailed understanding of the catalytic mechanism of enzyme drug targets is required to guide structure-based drug discovery. In my thesis research I have primarily focused on the catalytic mechanism and inhibition of MenE the OSB-CoA synthetase from three different organisms: M. tuberculosis, S. aureus and E. coli. MenE catalyzes the formation of OSB-CoA through a two step reaction that proceeds via acyl adenylate intermediate and utilizes ATP and CoA as cofactors. In chapter 2, I discuss the catalytic mechanism of MenE from S. aureus (saMenE) where steady state kinetics coupled with site-directed mutagenesis has been used to identify key catalytic residues in the active site of MenE and to elucidate the molecular details of each half reaction. In chapter 3, I present data on the inhibition of saMenE as well as the enzymes from M. tuberculosis (tbMenE) and E. coli (ecMenE). These studies have focused on a series of OSB-AMP intermediate analogs synthesized by our collaborator Dr. Tan at Memorial Sloan-Kettering Cancer Center. The most potent compound inhibits MenE with a Kid value of 11.2ñ0.9 nM. While the majority of my work has focused on MenE, I have also undertaken kinetic studies of the charismata-dependent enzymes Men from E. coli and MbtI from M. tuberculosis (chapter 4). These enzymes catalyze the initial reaction in menaquinone biosynthetic pathway and mycobactin biosynthetic pathway, respectively. Interestingly, in the absence of Mg2+, MenF and MbtI show chorismate mutase activity, although these enzymes have no similarity to the AroQ/H chorismate mutase. Because tbEntC, which is annotated as isochorismate synthase in M. tuberculosis menaquinone pathway, cannot yet be well expressed by using a heterologous E. coli expression system, I propose that MbtI might have a dual function and produce isochorismate for menaquinone in vitro.

Share

COinS
 
 

To view the content in your browser, please download Adobe Reader or, alternately,
you may Download the file to your hard drive.

NOTE: The latest versions of Adobe Reader do not support viewing PDF files within Firefox on Mac OS and if you are using a modern (Intel) Mac, there is no official plugin for viewing PDF files within the browser window.