Structural Basis for the Inhibition of Helicobacter pylori α-Carbonic Anhydrase by Sulfonamides

PLoS One. 2015 May 26;10(5):e0127149. doi: 10.1371/journal.pone.0127149. eCollection 2015.

Abstract

Periplasmic α-carbonic anhydrase of Helicobacter pylori (HpαCA), an oncogenic bacterium in the human stomach, is essential for its acclimation to low pH. It catalyses the conversion of carbon dioxide to bicarbonate using Zn(II) as the cofactor. In H. pylori, Neisseria spp., Brucella suis and Streptococcus pneumoniae this enzyme is the target for sulfonamide antibacterial agents. We present structural analysis correlated with inhibition data, on the complexes of HpαCA with two pharmacological inhibitors of human carbonic anhydrases, acetazolamide and methazolamide. This analysis reveals that two sulfonamide oxygen atoms of the inhibitors are positioned proximal to the putative location of the oxygens of the CO2 substrate in the Michaelis complex, whilst the zinc-coordinating sulfonamide nitrogen occupies the position of the catalytic water molecule. The structures are consistent with acetazolamide acting as site-directed, nanomolar inhibitors of the enzyme by mimicking its reaction transition state. Additionally, inhibitor binding provides insights into the channel for substrate entry and product exit. This analysis has implications for the structure-based design of inhibitors of bacterial carbonic anhydrases.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Acetazolamide / pharmacology
  • Amino Acid Sequence
  • Anti-Bacterial Agents / pharmacology
  • Carbonic Anhydrase Inhibitors / pharmacology*
  • Carbonic Anhydrases / metabolism*
  • Helicobacter Infections / drug therapy
  • Helicobacter Infections / microbiology
  • Helicobacter pylori / drug effects*
  • Helicobacter pylori / metabolism*
  • Humans
  • Methazolamide / pharmacology
  • Molecular Sequence Data
  • Periplasm / drug effects
  • Periplasm / metabolism
  • Sequence Alignment
  • Sulfonamides / pharmacology*

Substances

  • Anti-Bacterial Agents
  • Carbonic Anhydrase Inhibitors
  • Sulfonamides
  • Carbonic Anhydrases
  • Acetazolamide
  • Methazolamide

Associated data

  • PDB/4YGF
  • PDB/4YHA

Grants and funding

This work was supported by the Australian Research Council Fellowship to AR (grant number DP1094619). The funders had no role in study design, data collection and analysis, decision to publish, or preparation of the manuscript.