Remodeling of Cross-bridges Controls Peptidoglycan Cross-linking Levels in Bacterial Cell Walls

ACS Chem Biol. 2020 May 15;15(5):1261-1267. doi: 10.1021/acschembio.0c00002. Epub 2020 Apr 3.

Abstract

Cell walls are barriers found in almost all known bacterial cells. These structures establish a controlled interface between the external environment and vital cellular components. A primary component of cell wall is a highly cross-linked matrix called peptidoglycan (PG). PG cross-linking, carried out by transglycosylases and transpeptidases, is necessary for proper cell wall assembly. Transpeptidases, targets of β-lactam antibiotics, stitch together two neighboring PG stem peptides (acyl-donor and acyl-acceptor strands). We recently described a novel class of cellular PG probes that were processed exclusively as acyl-donor strands. Herein, we have accessed the other half of the transpeptidase reaction by developing probes that are processed exclusively as acyl-acceptor strands. The critical nature of the cross-bridge on the PG peptide was demonstrated in live bacterial cells, and surprising promiscuity in cross-bridge primary sequence was found in various bacterial species. Additionally, acyl-acceptor probes provided insight into how chemical remodeling of the PG cross-bridge (e.g., amidation) can modulate cross-linking levels, thus establishing a physiological role of PG structural variations. Together, the acyl-donor and -acceptor probes will provide a versatile platform to interrogate PG cross-linking in physiologically relevant settings.

Publication types

  • Research Support, N.I.H., Extramural

MeSH terms

  • Amino Acid Sequence
  • Anti-Bacterial Agents / metabolism*
  • Bacterial Proteins / metabolism*
  • Binding Sites
  • Cell Wall / metabolism
  • Cross-Linking Reagents / metabolism*
  • Diaminopimelic Acid / metabolism
  • Drug Design
  • Enterococcus faecalis / metabolism
  • Enterococcus faecalis / ultrastructure
  • Enterococcus faecium / metabolism
  • Enterococcus faecium / ultrastructure
  • Peptidoglycan / metabolism*
  • Peptidoglycan Glycosyltransferase / metabolism
  • Peptidyl Transferases / metabolism
  • Signal Transduction
  • beta-Lactams / metabolism*

Substances

  • Anti-Bacterial Agents
  • Bacterial Proteins
  • Cross-Linking Reagents
  • Peptidoglycan
  • beta-Lactams
  • Diaminopimelic Acid
  • Peptidyl Transferases
  • Peptidoglycan Glycosyltransferase