Top-Down Analysis of Branched Proteins Using Mass Spectrometry

Anal Chem. 2018 Mar 20;90(6):4032-4038. doi: 10.1021/acs.analchem.7b05234. Epub 2018 Mar 7.

Abstract

Post-translational modifications by the covalent attachment of Rub1 (NEDD8), ubiquitin, SUMO, and other small signaling proteins have profound impacts on the functions and fates of cellular proteins. Investigations of the relationship of these bioactive structures and their functions are limited by analytical methods that are scarce and tedious. A novel strategy is reported here for the analysis of branched proteins by top-down mass spectrometry and illustrated by application to four recombinant proteins and one synthetic peptide modified by covalent bonds with ubiquitin or Rub1. The approach allows an analyte to be recognized as a branched protein; the participating proteins to be identified; the site of conjugation to be defined; and other chemical, native, and recombinant modifications to be characterized. In addition to the high resolution and high accuracy provided by the mass spectrometer, success is based on sample fragmentation by electron-transfer dissociation assisted by collisional activation and on software designed for graphic interpretation and adapted for branched proteins. The strategy allows for structures of unknown, two-component branched proteins to be elucidated directly the first time and can potentially be extended to more complex systems.

Publication types

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

MeSH terms

  • Amino Acid Sequence
  • Humans
  • Models, Molecular
  • NEDD8 Protein / chemistry
  • PTEN Phosphohydrolase / chemistry
  • Protein Processing, Post-Translational*
  • Proteins / chemistry*
  • Recombinant Proteins / chemistry
  • Saccharomyces cerevisiae / chemistry
  • Saccharomyces cerevisiae Proteins / chemistry
  • Tandem Mass Spectrometry / methods*
  • Ubiquitin / chemistry
  • Ubiquitination
  • Ubiquitins / chemistry

Substances

  • NEDD8 Protein
  • Proteins
  • RUB1 protein, S cerevisiae
  • Recombinant Proteins
  • Saccharomyces cerevisiae Proteins
  • Ubiquitin
  • Ubiquitins
  • PTEN Phosphohydrolase