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Determination of Methylmercury, Ethylmercury, and Inorganic Mercury in Mouse Tissues, Following Administration of Thimerosal, by Species-Specific Isotope Dilution GC-Inductively Coupled Plasma-MS
Umeå University, Faculty of Science and Technology, Department of Chemistry.
Umeå University, Faculty of Science and Technology, Department of Chemistry. Umeå University, Faculty of Science and Technology, Umeå Marine Sciences Centre (UMF). (UMFpub)
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2003 (English)In: Analytical Chemistry, Vol. 75, no 16, 4120-4 p.Article in journal (Refereed) Published
Abstract [en]

Isotopically enriched HgO standards were used to synthesize CH3200Hg+ and C2H5199Hg+ using Grignard reagents. These species were employed for isotope dilution GC-ICPMS to study uptake and biotransformation of ethylmercury in mice treated with thimerosal, (sodium ethylmercurithiosalicylate) 10 mg L-1 in drinking water ad libitum for 1, 2.5, 6, or 14 days. Prior to analysis, samples were spiked with aqueous solutions of CH3200Hg+, C2H5199Hg+, and 201Hg2+ and then digested in 20% tetramethylammonium hydroxide and extracted at pH 9 with DDTC/toluene. Extracted mercury species were reacted with butylmagnesium chloride to form butylated derivatives. Absolute detection limits for CH3Hg+, C2H5Hg+, and Hg2+ were 0.4, 0.2, and 0.6 pg on the basis of 3 of five separate blanks. Up to 9% of the C2H5Hg+ was decomposed to Hg2+ during sample preparation, and it is therefore crucial to use a species-specific internal standard when determining ethylmercury. No demethylation, methylation, or ethylation during sample preparation was detected. The ethylmercury component of thimerosal was rapidly taken up in the organs of the mice (kidney, liver, and mesenterial lymph nodes), and concentrations of C2H5Hg+ as well as Hg2+ increased over the 14 days of thimerosal treatment. This shows that C2H5Hg+ in mice to a large degree is degraded to Hg2+. Increased concentrations of CH3Hg+ were also observed, which was found to be due to impurities in the thimerosal.

Place, publisher, year, edition, pages
2003. Vol. 75, no 16, 4120-4 p.
Identifiers
URN: urn:nbn:se:umu:diva-9948DOI: 10.1021/ac0342370OAI: oai:DiVA.org:umu-9948DiVA: diva2:149619
Available from: 2008-05-29 Created: 2008-05-29 Last updated: 2017-10-24Bibliographically approved
In thesis
1. On the reliability of methods for the speciation of mercury based on chromatographic separation coupled to atomic spectrometric detection
Open this publication in new window or tab >>On the reliability of methods for the speciation of mercury based on chromatographic separation coupled to atomic spectrometric detection
2003 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This thesis deals with the reliability of methods for the speciation of mercury in environmental and biological samples. Problems with speciation methods that couple chromatography to atomic spectrometric detection and how to overcome the problems are discussed. Analytical techniques primarily studied and evaluated are high performance liquid chromatography-cold vapour-atomic absorption spectrometry (HPLC-CV-AAS), HPLC-inductively coupled plasma-mass spectrometry (HPLC-ICP-MS), capillary electrophoresis-ICP-MS (CE-ICP-MS) and gas chromatography-ICP-MS (GC-ICP-MS). Applying a multi-capillary approach increased the analyte amount injected into a CE-ICP-MS system and improved the overall sensitivity. A microconcentric nebulizer with a cyclone spray chamber was shown to improve the detection limits for mercury species 3-13 times in HPLC-ICP-MS and 11-19 times in CE-ICP-MS compared to a cross-flow nebulizer with a Scott spray chamber. To decrease the interference of water vapour in HPLC-CV-AAS a Nafion dryer tube was inserted between the CV-generation and the detector. Methyl mercury was however lost in the Nafion unless it was reduced to elemental mercury prior transport through the dryer tube.

During sample pre-treatment, incomplete extraction, losses and transformation (alkylation, dealkylation, oxidation and reduction) of mercury species can lead to significant errors (underestimation and overestimation) in the determination of the concentrations. Methods to detect and determine the degree of transformation as well as correct for errors caused by transformation are presented in the thesis. The preferable method use species-specific enriched stable isotope standards in combination with MS detection and a matrix based calculation scheme. This approach is very powerful as both the concentrations of the species as well as the degrees of transformation can be determined within each individual sample.

Publisher
35 p.
Keyword
Analytical chemistry, Mercury, speciation, hyphenated techniques, HPLC, CE, GC, CV-AAS, ICP-MS, species-specific enriched stable isotope, Analytisk kemi
National Category
Analytical Chemistry
Research subject
Analytical Chemistry
Identifiers
urn:nbn:se:umu:diva-111 (URN)91-7305-429-1 (ISBN)
Public defence
2003-05-23, Umeå, 13:00 (English)
Available from: 2003-09-25 Created: 2003-09-25 Last updated: 2009-05-25Bibliographically approved
2. Mercury species transformations in marine and biological systems studied by isotope dilution mass spectrometry and stable isotope tracers
Open this publication in new window or tab >>Mercury species transformations in marine and biological systems studied by isotope dilution mass spectrometry and stable isotope tracers
2005 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This thesis focuses on the implementation of species-specific isotope dilution (SSID) methodology and stable isotope tracers to determine mercury species occurrence and transformation processes in-situ and during sample treatment. Isotope enriched tracers of methyl-, ethyl- and inorganic mercury were synthesised and applied in different combinations to marine and biological samples. Experimental results were obtained using gas chromatography-inductively coupled plasma-mass spectrometry (GC-ICP-MS).

Mercury methylation and methylmercury demethylation processes in surface sediments were studied in the brackish Öre River estuary, Bothnian Bay. Uni- and multivariate data evaluation identified the organic material content and mercury methylation potential in the sediments as important factors controlling incipient methylmercury levels. Mercury species distribution in mice treated with the pharmaceutical preservative Thimerosal (ethylmercurithiosalicylate) was studied. The ethylmercury moiety of Thimerosal was observed to rapidly convert to inorganic mercury in the mice during the treatment period as well as during sample treatment, hence necessitating SSID methodology for accurate ethylmercury determinations in biological samples.

To facilitate the introduction of SSID as a routine quantitative method in mercury speciation, a methylmercury isotopic certified reference material (ICRM) was produced. Prior to certification, the stability of the material was examined in conventional and isochronous stability studies spanning 12 months, which permitted uncertainty estimation of the methylmercury amount content for two years of shelf-life.

Finally, a field-adapted SSID method for methylmercury determinations in natural water samples was developed. The proposed analytical protocol significantly simplified sample storage- and treatment procedures without sacrifices in analytical accuracy.

Place, publisher, year, edition, pages
Umeå: Kemi, 2005. 38 p.
Keyword
Analytical chemistry, Mercury, methylmercury, ethylmercury, Thimerosal, speciation, methylation, demethylation, brackish water sediment, natural waters, GC-ICP-MS, species-specific isotope dilution, isotope enriched tracers, Analytisk kemi
National Category
Analytical Chemistry
Research subject
Analytical Chemistry
Identifiers
urn:nbn:se:umu:diva-467 (URN)91-7305-838-6 (ISBN)
Public defence
2005-04-01, KB3A9, Kemiskt Biologiskt Centrum (KBC), Umeå Universitet 90187, Umeå, 10:00 (English)
Opponent
Supervisors
Available from: 2005-03-09 Created: 2005-03-09 Last updated: 2009-05-25Bibliographically approved

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