Orthogonal liquid chromatography-mass spectrometry methods for the comprehensive characterization of therapeutic glycoproteins, from released glycans to intact protein level

J Chromatogr A. 2017 May 19:1498:128-146. doi: 10.1016/j.chroma.2017.02.072. Epub 2017 Mar 27.

Abstract

Proteins are increasingly used as therapeutics. Their characterization is challenging due to their size and inherent heterogeneity notably caused by post-translational modifications, among which glycosylation is probably the most prominent. The glycosylation profile of therapeutic proteins must therefore be thoroughly analyzed. Here, we illustrate how the use of a combination of various cutting-edge LC or LC/MS(/MS) methods, and operating at different levels of analysis allows the comprehensive characterization of both the N- and O-glycosylations of therapeutic proteins without the need for other approaches (capillary electrophoresis, MALDI-TOF). This workflow does not call for the use of highly specialized/custom hardware and software nor an extensive knowledge of glycan analysis. Most notably, we present the point of view of a contract research organization, with the constraints associated to the work in a regulated environment (GxP). Two salient points of this work are i) the use of mixed-mode chromatography as a fast and straightforward mean of profiling N-glycans sialylation as well as an orthogonal method to separate N-glycans co-eluting in the HILIC mode; and ii) the use of widepore HILIC/MS to analyze challenging N/O-glycosylation profiles at both the peptide and subunit levels. A particular attention was given to the sample preparations in terms of duration, specificity, versatility, and robustness, as well as the ease of data processing.

Keywords: High-resolution mass spectrometry; Hydrophilic interaction chromatography; Mixed-mode chromatography; Porous graphitic carbon chromatography; Protein glycosylation; Therapeutic proteins.

MeSH terms

  • Adalimumab / metabolism
  • Amino Acid Sequence
  • Antibodies, Monoclonal / metabolism
  • Carbohydrate Sequence
  • Cetuximab / metabolism
  • Chromatography, High Pressure Liquid*
  • Electrophoresis, Capillary
  • Etanercept / metabolism
  • Glycopeptides / analysis
  • Glycopeptides / isolation & purification
  • Glycoproteins / metabolism*
  • Glycosylation
  • Hydrophobic and Hydrophilic Interactions
  • Polysaccharides / analysis*
  • Polysaccharides / isolation & purification
  • Spectrometry, Mass, Matrix-Assisted Laser Desorption-Ionization*

Substances

  • Antibodies, Monoclonal
  • Glycopeptides
  • Glycoproteins
  • Polysaccharides
  • Adalimumab
  • Etanercept
  • Cetuximab