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Determination of picomolar levels of methylmercury complexes with low molecular mass thiols by liquid chromatography tandem mass spectrometry and online preconcentration
Umeå University, Faculty of Science and Technology, Department of Chemistry.
Umeå University, Faculty of Science and Technology, Department of Chemistry.ORCID iD: 0000-0001-6657-3336
Umeå University, Faculty of Science and Technology, Department of Chemistry.
2020 (English)In: Analytical and Bioanalytical Chemistry, ISSN 1618-2642, E-ISSN 1618-2650Article in journal (Refereed) Epub ahead of print
Abstract [en]

Methylmercury (MeHg) is one of the most potent neurotoxins. It is produced in nature through the methylation of inorganic divalent mercury (HgII) by phylogenetically diverse anaerobic microbes. The mechanistic understanding of the processes that govern the extent of bacterial export of MeHg, its bioaccumulation, and bio-toxicity depends on accurate quantification of its species, especially its complexation with low molecular mass thiols; organometallic complexes that are difficult to detect and measure in natural conditions. Here, we report the development of a novel analytical method based on liquid chromatography tandem mass spectrometry (LC-MS/MS) to determine 13 MeHg complexes with important thiol compounds which have been observed in the environment and in biological systems. By using online preconcentration via solid phase extraction (SPE), the method offers picomolar (12–530 pM) detection limits, the lowest reported so far for the determination of MeHg compounds. Among three different SPE materials, a weak cation exchange phase showed the best efficiency at a low pH of 2.5. We further report the presence of MeHg-cysteine, MeHg-cysteamine, MeHg-penicillamine, MeHg-cysteinylglycine, and MeHg-glutamylcysteine as the predominant MeHg–thiol complexes in the extracellular milieu of an important HgII methylating bacterium, Geobacter sulfurreducens PCA, exposed to 100 nM of HgII.

Place, publisher, year, edition, pages
Springer Berlin/Heidelberg, 2020.
Keywords [en]
Methylmercury-thiol complex, Low molecular mass thiols, Liquid chromatography tandem mass spectrometry, Online preconcentration
National Category
Analytical Chemistry
Identifiers
URN: urn:nbn:se:umu:diva-167613DOI: 10.1007/s00216-020-02389-yISI: 000507709500001PubMedID: 31950236Scopus ID: 2-s2.0-85078592237OAI: oai:DiVA.org:umu-167613DiVA, id: diva2:1392202
Available from: 2020-02-06 Created: 2020-02-06 Last updated: 2020-02-06

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Adediran, Gbotemi A.Björn, Erik

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