Proteome-wide detection of S-nitrosylation targets and motifs using bioorthogonal cleavable-linker-based enrichment and switch technique

Nat Commun. 2019 May 16;10(1):2195. doi: 10.1038/s41467-019-10182-4.

Abstract

Cysteine modifications emerge as important players in cellular signaling and homeostasis. Here, we present a chemical proteomics strategy for quantitative analysis of reversibly modified Cysteines using bioorthogonal cleavable-linker and switch technique (Cys-BOOST). Compared to iodoTMT for total Cysteine analysis, Cys-BOOST shows a threefold higher sensitivity and considerably higher specificity and precision. Analyzing S-nitrosylation (SNO) in S-nitrosoglutathione (GSNO)-treated and non-treated HeLa extracts Cys-BOOST identifies 8,304 SNO sites on 3,632 proteins covering a wide dynamic range of the proteome. Consensus motifs of SNO sites with differential GSNO reactivity confirm the relevance of both acid-base catalysis and local hydrophobicity for NO targeting to particular Cysteines. Applying Cys-BOOST to SH-SY5Y cells, we identify 2,151 SNO sites under basal conditions and reveal significantly changed SNO levels as response to early nitrosative stress, involving neuro(axono)genesis, glutamatergic synaptic transmission, protein folding/translation, and DNA replication. Our work suggests SNO as a global regulator of protein function akin to phosphorylation and ubiquitination.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Chromatography, High Pressure Liquid / instrumentation
  • Chromatography, High Pressure Liquid / methods
  • Cysteine / analysis*
  • Cysteine / metabolism
  • HeLa Cells
  • Humans
  • Nitrosation / physiology
  • Protein Processing, Post-Translational / physiology
  • Proteome / analysis
  • Proteome / metabolism*
  • Proteomics / instrumentation
  • Proteomics / methods*
  • S-Nitrosoglutathione / chemistry
  • S-Nitrosoglutathione / metabolism
  • Tandem Mass Spectrometry / instrumentation
  • Tandem Mass Spectrometry / methods

Substances

  • Proteome
  • S-Nitrosoglutathione
  • Cysteine