Clinical assay of four thiol amino acid redox couples by LC-MS/MS: utility in thalassemia

J Chromatogr B Analyt Technol Biomed Life Sci. 2009 Oct 15;877(28):3418-27. doi: 10.1016/j.jchromb.2009.06.041. Epub 2009 Jul 2.

Abstract

The total concentrations of four sulfur amino acid (SAA) metabolite redox couples (reduced and oxidized forms of homocysteine, cysteine, glutathione, and cysteinylglycine) in human blood are assayed with a simple and sensitive method by liquid chromatography-electrospray positive ionization-tandem mass spectrometry. To prevent ex vivo thiol oxidation, iodoacetamide (IAM) is used immediately following the blood draw. To selectively enrich for S-carboxyamidomethylated SAA, and other cationic amino acids metabolites, proprietary strong cation-exchange solid phase extraction tips are used. Analytes are further derivatized with isopropylchloroformate (IPCF) to esterify the amino and the carboxylic groups. Double derivatization with IAM and IPCF improves the reverse phase liquid chromatography separation of SAA metabolites. The use of detection mode of multiple-reaction monitoring (MRM) allows sensitive and specific simultaneous detection of SAA. The internal standards used to account for the matrix effects of human plasma and erythrocytes were plant glutathione analogue, homoglutathione, and stable isotopes of cystine and homocystine. The method was validated for its linearity, accuracy, and precision. Excellent linearity of detection (r(2)>0.98) was observed over relevant ranges for plasma and erythrocyte samples, and the limits of detection were established to be between 5 and 20nM. Relative standard deviations were <9% for within-day variations and <15% for between-day variations. The method was used to assess thiol redox states in plasma and erythrocytes isolated from healthy subjects and thalassemia patients.

Publication types

  • Evaluation Study
  • Research Support, N.I.H., Extramural
  • Research Support, Non-U.S. Gov't
  • Research Support, U.S. Gov't, P.H.S.

MeSH terms

  • Adult
  • Amino Acids, Sulfur / blood*
  • Amino Acids, Sulfur / metabolism
  • Case-Control Studies
  • Chromatography, Liquid / methods*
  • Clinical Chemistry Tests / methods*
  • Erythrocytes / chemistry
  • Erythrocytes / metabolism
  • Female
  • Humans
  • Male
  • Middle Aged
  • Oxidation-Reduction
  • Sulfhydryl Compounds / blood*
  • Sulfhydryl Compounds / metabolism
  • Tandem Mass Spectrometry / methods*
  • Thalassemia / blood*
  • Thalassemia / metabolism

Substances

  • Amino Acids, Sulfur
  • Sulfhydryl Compounds