Computer-Aided Lead Optimization: Improved Small-Molecule Inhibitor of the Zinc Endopeptidase of Botulinum Neurotoxin Serotype A

Abstract

Optimization of a serotype-selective, small-molecule inhibitor of botulinum neurotoxin serotype A (BoNTA) endopeptidase is a formidable challenge because the enzyme-substrate interface is unusually large and the endopeptidase itself is a large, zincbinding protein with a complex fold that is difficult to simulate computationally. We conducted multiple molecular dynamics simulations of the endopeptidase in complex with a previously described inhibitor (Ki(exp app) of 7+/-2.4 micrometers) using the cationic dummy atom approach. Based on our computational results, we hypothesized that introducing a hydroxyl group to the inhibitor could improve its potency. Synthesis and testing of the hydroxyl-containing analog as a BoNTA endopeptidase inhibitor showed a twofold improvement in inhibitory potency (Ki(exp app) of 3.8+/-0.8 micrometers) with a relatively small increase in molecular weight (16 Da). The results offer an improved template for further optimization of BoNTA endopeptidase inhibitors and demonstrate the effectiveness of the cationic dummy atom approach in the design and optimization of zinc protease inhibitors.

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Document Details

Document Type
Technical Report
Publication Date
Aug 01, 2007
Accession Number
ADA520371

Entities

People

  • Charles B. Millard
  • James J. Schmidt
  • Jewn G. Park
  • Jing Tang
  • Yuan-Ping Pang

Organizations

  • Mayo Clinic

Tags

Communities of Interest

  • Biomedical

DTIC Thesaurus Topics

  • Chemical Synthesis
  • Chemistry
  • Computational Science
  • Computer Simulations
  • Computers
  • Enzyme Inhibitors
  • Hydrogen Bonds
  • Inhibitors
  • Liquid Chromatography
  • Molecular Dynamics
  • Molecular Weight
  • Molecules
  • Neurotoxins
  • Optimization
  • Simulations
  • Small Molecules
  • United States

Readers

  • Microbial Pathology
  • Molecular and Cellular Biochemistry
  • Systems Analysis and Design