Investigations into the role of methylcobalamin and glutathione for the methylation of antimony using isotopically enriched antimony (V).

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Abstract

Glutathione (gamma-Glu-Cys-Gly, GSH) and methylcobalamin (CH3-B-12) may play a role in the biomethylation process of antimony. To understand better the transformation of antimony in biological systems, we studied abiotic and biomethylation processes and the influence of GSH in the methylation.

CH3-B-12, acting as a possible methylating agent for antimony, was studied with GSH and in the absence of GSH. The most abundant product of this reaction was monomethylantimony, with a small concentration of the dimethylantimony species, as identified by hydride generation cryotrapping gas chromatography inductively coupled plasma mass spectrometry (HG-CT-GC-ICP-MS). In the same experiments we found that tris(gamma-Glu-Cys-Gly)trithioantimonite [Sb(GS)(3)] and di(gamma-Glu-Cys-Gly)methyldithioantimonite [(CH3)Sb(GS)(2)] complexes were present using flow-injection electrospray ionization MS. Both complexes were also identified in a fermented sewage sample, suggesting that these complexes may play a role as intermediates in the biomethylation of antimony.

However, CH3-B-12 is not the sole methylation agent, since it does not produce any trimethylantimony species as identified in anaerobic sewage sludge cultures inoculated with enriched Sb-123(V). Species-specific Sb-123/121 isotope ratio measurements of the different methylantimony species suggest a stepwise methylation of antimony according to the Challenger mechanism. Copyright (C) 2004 John Wiley Sons, Ltd.

Original languageEnglish
Pages (from-to)631-639
Number of pages8
JournalApplied Organometallic Chemistry
Volume18
Issue number18
DOIs
Publication statusPublished - 2004

Keywords

  • antimony
  • biomethylation
  • methylcobalamin
  • glutathione
  • electrospray mass spectrometry
  • GC-ICP-MS
  • speciation
  • CHROMATOGRAPHY-MASS-SPECTROMETRY
  • GENERATION GAS-CHROMATOGRAPHY
  • HPLC-ICP-MS
  • SCOPULARIOPSIS-BREVICAULIS
  • HYDRIDE GENERATION
  • CRYPTOCOCCUS-HUMICOLUS
  • ENZYMATIC METHYLATION
  • BILIARY-EXCRETION
  • ARSENIC COMPOUNDS
  • MERCURY COMPOUNDS

Cite this

@article{ec310c32a79c48f0a597804a7df26450,
title = "Investigations into the role of methylcobalamin and glutathione for the methylation of antimony using isotopically enriched antimony (V).",
abstract = "Glutathione (gamma-Glu-Cys-Gly, GSH) and methylcobalamin (CH3-B-12) may play a role in the biomethylation process of antimony. To understand better the transformation of antimony in biological systems, we studied abiotic and biomethylation processes and the influence of GSH in the methylation.CH3-B-12, acting as a possible methylating agent for antimony, was studied with GSH and in the absence of GSH. The most abundant product of this reaction was monomethylantimony, with a small concentration of the dimethylantimony species, as identified by hydride generation cryotrapping gas chromatography inductively coupled plasma mass spectrometry (HG-CT-GC-ICP-MS). In the same experiments we found that tris(gamma-Glu-Cys-Gly)trithioantimonite [Sb(GS)(3)] and di(gamma-Glu-Cys-Gly)methyldithioantimonite [(CH3)Sb(GS)(2)] complexes were present using flow-injection electrospray ionization MS. Both complexes were also identified in a fermented sewage sample, suggesting that these complexes may play a role as intermediates in the biomethylation of antimony.However, CH3-B-12 is not the sole methylation agent, since it does not produce any trimethylantimony species as identified in anaerobic sewage sludge cultures inoculated with enriched Sb-123(V). Species-specific Sb-123/121 isotope ratio measurements of the different methylantimony species suggest a stepwise methylation of antimony according to the Challenger mechanism. Copyright (C) 2004 John Wiley Sons, Ltd.",
keywords = "antimony, biomethylation, methylcobalamin, glutathione, electrospray mass spectrometry, GC-ICP-MS, speciation, CHROMATOGRAPHY-MASS-SPECTROMETRY, GENERATION GAS-CHROMATOGRAPHY, HPLC-ICP-MS, SCOPULARIOPSIS-BREVICAULIS, HYDRIDE GENERATION, CRYPTOCOCCUS-HUMICOLUS, ENZYMATIC METHYLATION, BILIARY-EXCRETION, ARSENIC COMPOUNDS, MERCURY COMPOUNDS",
author = "Silvia Wehmeier and Andrea Raab and Jorg Feldmann",
year = "2004",
doi = "10.1002/aoc.692",
language = "English",
volume = "18",
pages = "631--639",
journal = "Applied Organometallic Chemistry",
issn = "0268-2605",
publisher = "John Wiley and Sons Ltd",
number = "18",

}

TY - JOUR

T1 - Investigations into the role of methylcobalamin and glutathione for the methylation of antimony using isotopically enriched antimony (V).

AU - Wehmeier, Silvia

AU - Raab, Andrea

AU - Feldmann, Jorg

PY - 2004

Y1 - 2004

N2 - Glutathione (gamma-Glu-Cys-Gly, GSH) and methylcobalamin (CH3-B-12) may play a role in the biomethylation process of antimony. To understand better the transformation of antimony in biological systems, we studied abiotic and biomethylation processes and the influence of GSH in the methylation.CH3-B-12, acting as a possible methylating agent for antimony, was studied with GSH and in the absence of GSH. The most abundant product of this reaction was monomethylantimony, with a small concentration of the dimethylantimony species, as identified by hydride generation cryotrapping gas chromatography inductively coupled plasma mass spectrometry (HG-CT-GC-ICP-MS). In the same experiments we found that tris(gamma-Glu-Cys-Gly)trithioantimonite [Sb(GS)(3)] and di(gamma-Glu-Cys-Gly)methyldithioantimonite [(CH3)Sb(GS)(2)] complexes were present using flow-injection electrospray ionization MS. Both complexes were also identified in a fermented sewage sample, suggesting that these complexes may play a role as intermediates in the biomethylation of antimony.However, CH3-B-12 is not the sole methylation agent, since it does not produce any trimethylantimony species as identified in anaerobic sewage sludge cultures inoculated with enriched Sb-123(V). Species-specific Sb-123/121 isotope ratio measurements of the different methylantimony species suggest a stepwise methylation of antimony according to the Challenger mechanism. Copyright (C) 2004 John Wiley Sons, Ltd.

AB - Glutathione (gamma-Glu-Cys-Gly, GSH) and methylcobalamin (CH3-B-12) may play a role in the biomethylation process of antimony. To understand better the transformation of antimony in biological systems, we studied abiotic and biomethylation processes and the influence of GSH in the methylation.CH3-B-12, acting as a possible methylating agent for antimony, was studied with GSH and in the absence of GSH. The most abundant product of this reaction was monomethylantimony, with a small concentration of the dimethylantimony species, as identified by hydride generation cryotrapping gas chromatography inductively coupled plasma mass spectrometry (HG-CT-GC-ICP-MS). In the same experiments we found that tris(gamma-Glu-Cys-Gly)trithioantimonite [Sb(GS)(3)] and di(gamma-Glu-Cys-Gly)methyldithioantimonite [(CH3)Sb(GS)(2)] complexes were present using flow-injection electrospray ionization MS. Both complexes were also identified in a fermented sewage sample, suggesting that these complexes may play a role as intermediates in the biomethylation of antimony.However, CH3-B-12 is not the sole methylation agent, since it does not produce any trimethylantimony species as identified in anaerobic sewage sludge cultures inoculated with enriched Sb-123(V). Species-specific Sb-123/121 isotope ratio measurements of the different methylantimony species suggest a stepwise methylation of antimony according to the Challenger mechanism. Copyright (C) 2004 John Wiley Sons, Ltd.

KW - antimony

KW - biomethylation

KW - methylcobalamin

KW - glutathione

KW - electrospray mass spectrometry

KW - GC-ICP-MS

KW - speciation

KW - CHROMATOGRAPHY-MASS-SPECTROMETRY

KW - GENERATION GAS-CHROMATOGRAPHY

KW - HPLC-ICP-MS

KW - SCOPULARIOPSIS-BREVICAULIS

KW - HYDRIDE GENERATION

KW - CRYPTOCOCCUS-HUMICOLUS

KW - ENZYMATIC METHYLATION

KW - BILIARY-EXCRETION

KW - ARSENIC COMPOUNDS

KW - MERCURY COMPOUNDS

U2 - 10.1002/aoc.692

DO - 10.1002/aoc.692

M3 - Article

VL - 18

SP - 631

EP - 639

JO - Applied Organometallic Chemistry

JF - Applied Organometallic Chemistry

SN - 0268-2605

IS - 18

ER -