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Designer broad-spectrum polyimidazolium antibiotics.

Wenbin Zhong1,2, Zhenyu Shi1,2, Surendra H Mahadevegowda1,2

  • 1School of Chemical and Biomedical Engineering, Nanyang Technological University, Singapore 637459.

Proceedings of the National Academy of Sciences of the United States of America
|November 24, 2020
PubMed
Summary

New synthetic cationic polyimidazolium (PIM) mimics show potent, broad-spectrum antibiotic activity against resistant bacteria. A PIM1 derivative (PIM1D) demonstrated reduced toxicity and efficacy in preclinical models, offering potential new antimicrobial drugs.

Keywords:
bactericidalcationic antimicrobial polymerscolistin-resistant

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Area of Science:

  • Medicinal Chemistry
  • Microbiology
  • Drug Discovery

Background:

  • Most antimicrobial peptides (AMPs) face challenges in clinical use due to toxicity, low potency, or limited spectrum.
  • Developing novel antibiotics is crucial to combat the rise of pan-antibiotic-resistant bacteria.

Purpose of the Study:

  • To synthesize and evaluate novel cationic peptide mimics, specifically main-chain cationic polyimidazoliums (PIMs), as potential antimicrobial agents.
  • To investigate the mechanism of action and in vivo efficacy of promising PIM candidates against resistant bacterial pathogens.

Main Methods:

  • Synthesis of cationic polyimidazoliums (PIMs) and evaluation of their antibacterial activity against Gram-positive, Gram-negative, and mycobacterial species.
  • Mechanistic studies on PIM1, including membrane interaction, cell entry, and activity dependence on membrane potential.
  • Laboratory evolution experiments to determine resistance mechanisms in *Staphylococcus aureus* and *Pseudomonas aeruginosa*.
  • Assessment of PIM1 and its derivative PIM1D for toxicity and efficacy in murine models of infection.

Main Results:

  • Several PIMs exhibited potent, broad-spectrum antibacterial activity, including against pan-drug-resistant strains, with low acute mammalian cell toxicity.
  • PIM1 demonstrated membrane binding, cell entry, and bacterial killing, requiring membrane electric potential but not membrane permeabilization.
  • Resistance to PIM1 in *S. aureus* was associated with menaquinone mutations; *P. aeruginosa* did not readily develop resistance.
  • PIM1 showed topical efficacy but systemic toxicity in mice, while the less hydrophobic derivative PIM1D was non-toxic and effective in a murine sepsis model.

Conclusions:

  • Main-chain cationic polyimidazoliums (PIMs) represent a promising class of synthetic antimicrobial agents with broad-spectrum activity.
  • PIM1D, a non-toxic derivative, shows potential for development into new therapeutics to treat challenging pan-resistant bacterial infections.