Synthesis of Asparagine Derivatives Harboring a Lewis X Type DC-SIGN Ligand and Evaluation of their Impact on Immunomodulation in Multiple Sclerosis

Chemistry. 2021 Feb 5;27(8):2742-2752. doi: 10.1002/chem.202004076. Epub 2020 Dec 28.

Abstract

The protein myelin oligodendrocyte glycoprotein (MOG) is a key component of myelin and an autoantigen in the disease multiple sclerosis (MS). Post-translational N-glycosylation of Asn31 of MOG seems to play a key role in modulating the immune response towards myelin. This is mediated by the interaction of Lewis-type glycan structures in the N-glycan of MOG with the DC-SIGN receptor on dendritic cells (DCs). Here, we report the synthesis of an unnatural Lewis X (LeX )-containing Fmoc-SPPS-compatible asparagine building block (SPPS=solid-phase peptide synthesis), as well as asparagine building blocks containing two LeX -derived oligosaccharides: LacNAc and Fucα1-3GlcNAc. These building blocks were used for the glycosylation of the immunodominant portion of MOG (MOG31-55 ) and analyzed with respect to their ability to bind to DC-SIGN in different biological setups, as well as their ability to inhibit the citrullination-induced aggregation of MOG31-55 . Finally, a cytokine secretion assay was carried out on human monocyte-derived DCs, which showed the ability of the neoglycopeptide decorated with a single LeX to alter the balance of pro- and anti-inflammatory cytokines, inducing a tolerogenic response.

Keywords: bioorganic chemistry; glycoconjugates; glycoimmunology; glycopeptides; multiple sclerosis.

MeSH terms

  • Asparagine / chemistry
  • Asparagine / metabolism*
  • Cell Adhesion Molecules / genetics
  • Cell Adhesion Molecules / immunology*
  • Cell Adhesion Molecules / metabolism*
  • Humans
  • Immunomodulation*
  • Lectins, C-Type / genetics
  • Lectins, C-Type / immunology*
  • Lectins, C-Type / metabolism*
  • Ligands
  • Multiple Sclerosis / immunology*
  • Multiple Sclerosis / metabolism
  • Myelin-Oligodendrocyte Glycoprotein / chemistry*
  • Myelin-Oligodendrocyte Glycoprotein / immunology
  • Myelin-Oligodendrocyte Glycoprotein / metabolism*
  • Receptors, Cell Surface / genetics
  • Receptors, Cell Surface / immunology*
  • Receptors, Cell Surface / metabolism*

Substances

  • Cell Adhesion Molecules
  • DC-specific ICAM-3 grabbing nonintegrin
  • Lectins, C-Type
  • Ligands
  • Myelin-Oligodendrocyte Glycoprotein
  • Receptors, Cell Surface
  • Asparagine