Peracetylated 4-fluoro-glucosamine reduces the content and repertoire of N- and O-glycans without direct incorporation

J Biol Chem. 2011 Jun 17;286(24):21717-31. doi: 10.1074/jbc.M110.194597. Epub 2011 Apr 14.

Abstract

Prior studies have shown that treatment with the peracetylated 4-fluorinated analog of glucosamine (4-F-GlcNAc) elicits anti-skin inflammatory activity by ablating N-acetyllactosamine (LacNAc), sialyl Lewis X (sLe(X)), and related lectin ligands on effector leukocytes. Based on anti-sLe(X) antibody and lectin probing experiments on 4-F-GlcNAc-treated leukocytes, it was hypothesized that 4-F-GlcNAc inhibited sLe(X) formation by incorporating into LacNAc and blocking the addition of galactose or fucose at the carbon 4-position of 4-F-GlcNAc. To test this hypothesis, we determined whether 4-F-GlcNAc is directly incorporated into N- and O-glycans released from 4-F-GlcNAc-treated human sLe(X) (+) T cells and leukemic KG1a cells. At concentrations that abrogated galectin-1 (Gal-1) ligand and E-selectin ligand expression and related LacNAc and sLe(X) structures, MALDI-TOF and MALDI-TOF/TOF mass spectrometry analyses showed that 4-F-GlcNAc 1) reduced content and structural diversity of tri- and tetra-antennary N-glycans and of O-glycans, 2) increased biantennary N-glycans, and 3) reduced LacNAc and sLe(X) on N-glycans and on core 2 O-glycans. Moreover, MALDI-TOF MS did not reveal any m/z ratios relating to the presence of fluorine atoms, indicating that 4-F-GlcNAc did not incorporate into glycans. Further analysis showed that 4-F-GlcNAc treatment had minimal effect on expression of 1200 glycome-related genes and did not alter the activity of LacNAc-synthesizing enzymes. However, 4-F-GlcNAc dramatically reduced intracellular levels of uridine diphosphate-N-acetylglucosamine (UDP-GlcNAc), a key precursor of LacNAc synthesis. These data show that Gal-1 and E-selectin ligand reduction by 4-F-GlcNAc is not caused by direct 4-F-GlcNAc glycan incorporation and consequent chain termination but rather by interference with UDP-GlcNAc synthesis.

Publication types

  • Research Support, N.I.H., Extramural
  • Research Support, Non-U.S. Gov't

MeSH terms

  • Acetylation
  • Acetylglucosamine / analogs & derivatives*
  • Acetylglucosamine / chemistry
  • Amino Sugars / chemistry
  • Gas Chromatography-Mass Spectrometry / methods
  • Gene Expression Profiling
  • Gene Expression Regulation
  • Humans
  • Inflammation
  • Lectins / chemistry
  • Leukocytes / metabolism
  • Ligands
  • Oligosaccharides / chemistry
  • Polysaccharides / chemistry*
  • Sialyl Lewis X Antigen
  • beta-Galactosidase / chemistry

Substances

  • Amino Sugars
  • Lectins
  • Ligands
  • Oligosaccharides
  • Polysaccharides
  • Sialyl Lewis X Antigen
  • N-acetyllactosamine
  • N-fluoroacetyl-D-glucosamine
  • beta-Galactosidase
  • Acetylglucosamine