Design and synthesis of 2-(2-isonicotinoylhydrazineylidene)propanamides as InhA inhibitors with high antitubercular activity

Eur J Med Chem. 2021 Nov 5:223:113668. doi: 10.1016/j.ejmech.2021.113668. Epub 2021 Jun 23.

Abstract

Based on successful antitubercular isoniazid scaffold we have designed its "mee-too" analogues by a combination of this drug linked with substituted anilines through pyruvic acid as a bridge. Lipophilicity important for passive diffusion through impenetrable mycobacterial cell wall was increased by halogen substitution on the aniline. We prepared twenty new 2-(2-isonicotinoylhydrazineylidene)propanamides that were assayed against susceptible Mycobacterium tuberculosis H37Rv, nontuberculous mycobacteria, and also multidrug-resistant tuberculous strains (MDR-TB). All the compounds showed excellent activity not only against Mtb. (minimum inhibitory concentrations, MIC, from ≤0.03 μM), but also against M. kansasii (MIC ≥2 μM). The most active molecules have CF3 and OCF3 substituent in the position 4 on the aniline ring. MIC against MDR-TB were from 8 μM. The most effective derivatives were used for the mechanism of action investigation. The treatment of Mtb. H37Ra with tested compounds led to decreased production of mycolic acids and the strains overproducing InhA were more resistant to them. These results confirm that studied compounds inhibit the enoyl-acyl carrier protein reductase (InhA) in mycobacteria. The compounds did not show any cytotoxic and cytostatic activity for HepG2 cells. The amides can be considered as a promising scaffold for antitubercular drug discovery having better antimicrobial properties than original isoniazid together with a significantly improved pharmaco-toxicological profile.

Keywords: Antimycobacterial activity; InhA; Isoniazid; Mechanism of action; Multidrug resistance; Pyruvic acid; Tuberculosis.

MeSH terms

  • Amides / chemistry*
  • Amides / metabolism
  • Amides / pharmacology
  • Amides / therapeutic use
  • Aniline Compounds / chemistry
  • Antitubercular Agents / chemical synthesis*
  • Antitubercular Agents / metabolism
  • Antitubercular Agents / pharmacology
  • Antitubercular Agents / therapeutic use
  • Bacterial Proteins / antagonists & inhibitors*
  • Bacterial Proteins / metabolism
  • Cell Survival / drug effects
  • Drug Design*
  • Drug Resistance, Bacterial / drug effects
  • Hep G2 Cells
  • Humans
  • Microbial Sensitivity Tests
  • Mycobacterium tuberculosis / drug effects
  • Mycobacterium tuberculosis / metabolism
  • Oxidoreductases / antagonists & inhibitors*
  • Oxidoreductases / metabolism
  • Pyruvic Acid / chemistry
  • Structure-Activity Relationship
  • Tuberculosis / drug therapy

Substances

  • Amides
  • Aniline Compounds
  • Antitubercular Agents
  • Bacterial Proteins
  • Pyruvic Acid
  • Oxidoreductases
  • InhA protein, Mycobacterium