Mapping spatial proximities of sulfhydryl groups in proteins using a fluorogenic cross-linker and mass spectrometry

Anal Biochem. 2004 Aug 1;331(1):27-32. doi: 10.1016/j.ab.2004.03.075.

Abstract

Chemical cross-linking of proteins in combination with mass spectrometric analysis of the reaction products has gained renewed interest as a method of obtaining distance constraints within a protein and determining a low-resolution three-dimensional structure. We present a method for identifying spatially close sulfhydryl groups in proteins employing chemical cross-linking with the fluorogenic, homobifunctional cross-linker dibromobimane, which cross-links thiol pairs within approximately 3-6A. The applicability of our strategy was demonstrated by cross-linking the sulfhydryl groups of Cys-18 and Cys-78 in gamma-crystallin F, which are within a distance of 3.57A according to the X-ray structure. Intramolecularly cross-linked gamma-crystallin was first separated from reaction side products by reversed-phase chromatography on a C-4 column. Subsequently, the fraction containing the reacted protein was enzymatically digested with trypsin, and the resulting peptide mixture was separated by a second reversed-phase chromatographic step on a C-18 column, in which the cross-linked peptides were tracked by their fluorescence. The cross-linking product between Cys-18 and Cys-78 in gamma-crystallin F was identified by matrix-assisted laser desorption/ionization-time of flight mass spectrometry. This strategy presents a rapid method for mapping sulfhydryl groups separated by a distance of approximately 3-6A within a protein.

MeSH terms

  • Animals
  • Bridged Bicyclo Compounds / chemistry*
  • Cattle
  • Chromatography, High Pressure Liquid
  • Cross-Linking Reagents / chemistry*
  • Cysteine / chemistry
  • Fluorescence
  • Peptide Mapping
  • Spectrometry, Mass, Matrix-Assisted Laser Desorption-Ionization / methods*
  • Sulfhydryl Compounds / chemistry*
  • gamma-Crystallins / chemistry*

Substances

  • Bridged Bicyclo Compounds
  • Cross-Linking Reagents
  • Sulfhydryl Compounds
  • gamma-Crystallins
  • dibromobimane
  • Cysteine