One-pot N-glycosylation remodeling of IgG with non-natural sialylglycopeptides enables glycosite-specific and dual-payload antibody-drug conjugates

Org Biomol Chem. 2016 Oct 12;14(40):9501-9518. doi: 10.1039/c6ob01751g.

Abstract

Chemoenzymatic transglycosylation catalyzed by endo-S mutants is a powerful tool for in vitro glycoengineering of therapeutic antibodies. In this paper, we report a one-pot chemoenzymatic synthesis of glycoengineered Herceptin using an egg-yolk sialylglycopeptide (SGP) substrate. Combining this one-pot strategy with novel non-natural SGP derivatives carrying azido or alkyne tags, glycosite-specific conjugation was enabled for the development of new antibody-drug conjugates (ADCs). The site-specific ADCs and semi-site-specific dual-drug ADCs were successfully achieved and characterized with SDS-PAGE, intact antibody or ADC mass spectrometry analysis, and PNGase-F digestion analysis. Cancer cell cytotoxicity assay revealed that small-molecule drug release of these ADCs relied on the cleavable Val-Cit linker fragment embedded in the structure. These results represent a new approach for glycosite-specific and dual-drug ADC design and rapid synthesis, and also provide the structural requirement for their biologic activities.

MeSH terms

  • Cell Line, Tumor
  • Glycopeptides / metabolism*
  • Glycosylation
  • Humans
  • Immunoconjugates / chemistry
  • Immunoconjugates / metabolism*
  • Immunoglobulin G / chemistry*
  • Immunoglobulin G / metabolism*
  • Models, Molecular
  • Nitrogen / chemistry*
  • Protein Conformation

Substances

  • Glycopeptides
  • Immunoconjugates
  • Immunoglobulin G
  • Nitrogen