Validation of Methylmercury Determinations in Aquatic Systems by Alkyl Derivatization Methods for GC Analysis Using ICP-IDMS
Isotope dilution mass spectrometry (IDMS), using an inductively coupled plasma quadrupole mass spectrometer (ICPMS) and a species-specific methylmercury spike was applied to validate the commonly used GC method for methylmercury (MeHg+) determination, which is based on the formation of volatile meth...
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| Veröffentlicht in: | Analytical chemistry (Washington) 2001-08, Vol.73 (16), p.4020-4027 |
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| creator | Demuth, Natascha Heumann, Klaus G |
| description | Isotope dilution mass spectrometry (IDMS), using an inductively coupled plasma quadrupole mass spectrometer (ICPMS) and a species-specific methylmercury spike was applied to validate the commonly used GC method for methylmercury (MeHg+) determination, which is based on the formation of volatile methylethylmercury by derivatization with NaBEt4. The spike compound, Me201Hg+, was synthesized by reaction of 201Hg-enriched mercury chloride with methylcobalamin. By analyzing different environmental aquatic samples, it was found that in most cases, transformation of MeHg+ into elemental mercury (Hg0) took place. From investigations of synthetic solutions, it could be followed that halide ions are responsible for this transformation process. Chloride and bromide converted MeHg+ into Hg0, whereas iodide caused transformation into Hg2+ and Hg0. It could also be shown that transformation of MeHg+ took place only during the derivatization step. In contrast to ethylation, propylation by NaBPr4 did not cause any transformation; however, accurate results of MeHg+ determinations could be obtained by propylation as well as by ethylation when GC/ICP-IDMS was applied. This work demonstrates the great power of isotopically labeled element compounds for the validation of element speciation methods and for species-specific IDMS analyses. |
| doi_str_mv | 10.1021/ac010366+ |
| format | Article |
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The spike compound, Me201Hg+, was synthesized by reaction of 201Hg-enriched mercury chloride with methylcobalamin. By analyzing different environmental aquatic samples, it was found that in most cases, transformation of MeHg+ into elemental mercury (Hg0) took place. From investigations of synthetic solutions, it could be followed that halide ions are responsible for this transformation process. Chloride and bromide converted MeHg+ into Hg0, whereas iodide caused transformation into Hg2+ and Hg0. It could also be shown that transformation of MeHg+ took place only during the derivatization step. In contrast to ethylation, propylation by NaBPr4 did not cause any transformation; however, accurate results of MeHg+ determinations could be obtained by propylation as well as by ethylation when GC/ICP-IDMS was applied. This work demonstrates the great power of isotopically labeled element compounds for the validation of element speciation methods and for species-specific IDMS analyses.</description><identifier>ISSN: 0003-2700</identifier><identifier>EISSN: 1520-6882</identifier><identifier>DOI: 10.1021/ac010366+</identifier><identifier>PMID: 11534731</identifier><identifier>CODEN: ANCHAM</identifier><language>eng</language><publisher>Washington, DC: American Chemical Society</publisher><subject>Analysis methods ; Analytical chemistry ; Applied sciences ; Chemistry ; Chromatographic methods and physical methods associated with chromatography ; Exact sciences and technology ; Gas chromatographic methods ; Isotopes ; Natural water pollution ; Pollution ; Spectrum analysis ; Toxicity ; Water treatment and pollution</subject><ispartof>Analytical chemistry (Washington), 2001-08, Vol.73 (16), p.4020-4027</ispartof><rights>Copyright © 2001 American Chemical Society</rights><rights>2001 INIST-CNRS</rights><rights>Copyright American Chemical Society Aug 15, 2001</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a433t-e250004ee493d606fbb3fbf2029f541ba80c692c52c9c8cd84a81ffd058939a43</citedby><cites>FETCH-LOGICAL-a433t-e250004ee493d606fbb3fbf2029f541ba80c692c52c9c8cd84a81ffd058939a43</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/ac010366+$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/ac010366+$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,777,781,2752,27057,27905,27906,56719,56769</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=1100469$$DView record in Pascal Francis$$Hfree_for_read</backlink><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/11534731$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Demuth, Natascha</creatorcontrib><creatorcontrib>Heumann, Klaus G</creatorcontrib><title>Validation of Methylmercury Determinations in Aquatic Systems by Alkyl Derivatization Methods for GC Analysis Using ICP-IDMS</title><title>Analytical chemistry (Washington)</title><addtitle>Anal. Chem</addtitle><description>Isotope dilution mass spectrometry (IDMS), using an inductively coupled plasma quadrupole mass spectrometer (ICPMS) and a species-specific methylmercury spike was applied to validate the commonly used GC method for methylmercury (MeHg+) determination, which is based on the formation of volatile methylethylmercury by derivatization with NaBEt4. The spike compound, Me201Hg+, was synthesized by reaction of 201Hg-enriched mercury chloride with methylcobalamin. By analyzing different environmental aquatic samples, it was found that in most cases, transformation of MeHg+ into elemental mercury (Hg0) took place. From investigations of synthetic solutions, it could be followed that halide ions are responsible for this transformation process. Chloride and bromide converted MeHg+ into Hg0, whereas iodide caused transformation into Hg2+ and Hg0. It could also be shown that transformation of MeHg+ took place only during the derivatization step. In contrast to ethylation, propylation by NaBPr4 did not cause any transformation; however, accurate results of MeHg+ determinations could be obtained by propylation as well as by ethylation when GC/ICP-IDMS was applied. This work demonstrates the great power of isotopically labeled element compounds for the validation of element speciation methods and for species-specific IDMS analyses.</description><subject>Analysis methods</subject><subject>Analytical chemistry</subject><subject>Applied sciences</subject><subject>Chemistry</subject><subject>Chromatographic methods and physical methods associated with chromatography</subject><subject>Exact sciences and technology</subject><subject>Gas chromatographic methods</subject><subject>Isotopes</subject><subject>Natural water pollution</subject><subject>Pollution</subject><subject>Spectrum analysis</subject><subject>Toxicity</subject><subject>Water treatment and pollution</subject><issn>0003-2700</issn><issn>1520-6882</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2001</creationdate><recordtype>article</recordtype><recordid>eNqFkV1v0zAYhS3ExMrggj-ALDQhJBTwR-Ikl6VlXaVNTHQD7izHscGbk2x-E7RM_Pi5tFAEF1xZ1nn0yMcHoWeUvKGE0bdKE0q4EK8foAnNGElEUbCHaEII4QnLCdlHjwEuCaGUUPEI7VOa8TTndIJ-fFLe1ap3XYs7i09N_230jQl6CCOem96ExrU_Y8CuxdObIV40Xo3QmwZwNeKpvxp9RIP7HqO7jWrt6WrAtgt4McPTVvkRHOALcO1XvJydJcv56eoJ2rPKg3m6PQ_QxdH789lxcvJhsZxNTxKVct4nhmWxSWpMWvJaEGGritvKMsJKm6W0UgXRomQ6Y7rUha6LVBXU2ppkRcnL6DhALzfe69DdDAZ62TjQxnvVmm4AmVOaCkH5f0FaRGVWrsEXf4GX3RBiS5CM5kXO8kxE6NUG0qEDCMbK6-AaFUZJiVwPJ38NF9HnW99QNabegduhInC4BRRo5W1QrXbwBxc_SJQRSzaYi_vc_o5VuJIi53kmz89W8vjzl8XH1dE7Od9plYZdhX-edw-oArlJ</recordid><startdate>20010815</startdate><enddate>20010815</enddate><creator>Demuth, Natascha</creator><creator>Heumann, Klaus G</creator><general>American Chemical Society</general><scope>BSCLL</scope><scope>IQODW</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7QF</scope><scope>7QO</scope><scope>7QQ</scope><scope>7SC</scope><scope>7SE</scope><scope>7SP</scope><scope>7SR</scope><scope>7TA</scope><scope>7TB</scope><scope>7TM</scope><scope>7U5</scope><scope>7U7</scope><scope>7U9</scope><scope>8BQ</scope><scope>8FD</scope><scope>C1K</scope><scope>F28</scope><scope>FR3</scope><scope>H8D</scope><scope>H8G</scope><scope>H94</scope><scope>JG9</scope><scope>JQ2</scope><scope>KR7</scope><scope>L7M</scope><scope>L~C</scope><scope>L~D</scope><scope>P64</scope><scope>7QH</scope><scope>7UA</scope><scope>7X8</scope></search><sort><creationdate>20010815</creationdate><title>Validation of Methylmercury Determinations in Aquatic Systems by Alkyl Derivatization Methods for GC Analysis Using ICP-IDMS</title><author>Demuth, Natascha ; Heumann, Klaus G</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a433t-e250004ee493d606fbb3fbf2029f541ba80c692c52c9c8cd84a81ffd058939a43</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2001</creationdate><topic>Analysis methods</topic><topic>Analytical chemistry</topic><topic>Applied sciences</topic><topic>Chemistry</topic><topic>Chromatographic methods and physical methods associated with chromatography</topic><topic>Exact sciences and technology</topic><topic>Gas chromatographic methods</topic><topic>Isotopes</topic><topic>Natural water pollution</topic><topic>Pollution</topic><topic>Spectrum analysis</topic><topic>Toxicity</topic><topic>Water treatment and pollution</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Demuth, Natascha</creatorcontrib><creatorcontrib>Heumann, Klaus G</creatorcontrib><collection>Istex</collection><collection>Pascal-Francis</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>Aluminium Industry Abstracts</collection><collection>Biotechnology Research Abstracts</collection><collection>Ceramic Abstracts</collection><collection>Computer and Information Systems Abstracts</collection><collection>Corrosion Abstracts</collection><collection>Electronics & Communications Abstracts</collection><collection>Engineered Materials Abstracts</collection><collection>Materials Business File</collection><collection>Mechanical & Transportation Engineering Abstracts</collection><collection>Nucleic Acids Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>Toxicology Abstracts</collection><collection>Virology and AIDS Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>ANTE: Abstracts in New Technology & Engineering</collection><collection>Engineering Research Database</collection><collection>Aerospace Database</collection><collection>Copper Technical Reference Library</collection><collection>AIDS and Cancer Research Abstracts</collection><collection>Materials Research Database</collection><collection>ProQuest Computer Science Collection</collection><collection>Civil Engineering Abstracts</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>Computer and Information Systems Abstracts Academic</collection><collection>Computer and Information Systems Abstracts Professional</collection><collection>Biotechnology and BioEngineering Abstracts</collection><collection>Aqualine</collection><collection>Water Resources Abstracts</collection><collection>MEDLINE - Academic</collection><jtitle>Analytical chemistry (Washington)</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Demuth, Natascha</au><au>Heumann, Klaus G</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Validation of Methylmercury Determinations in Aquatic Systems by Alkyl Derivatization Methods for GC Analysis Using ICP-IDMS</atitle><jtitle>Analytical chemistry (Washington)</jtitle><addtitle>Anal. Chem</addtitle><date>2001-08-15</date><risdate>2001</risdate><volume>73</volume><issue>16</issue><spage>4020</spage><epage>4027</epage><pages>4020-4027</pages><issn>0003-2700</issn><eissn>1520-6882</eissn><coden>ANCHAM</coden><abstract>Isotope dilution mass spectrometry (IDMS), using an inductively coupled plasma quadrupole mass spectrometer (ICPMS) and a species-specific methylmercury spike was applied to validate the commonly used GC method for methylmercury (MeHg+) determination, which is based on the formation of volatile methylethylmercury by derivatization with NaBEt4. The spike compound, Me201Hg+, was synthesized by reaction of 201Hg-enriched mercury chloride with methylcobalamin. By analyzing different environmental aquatic samples, it was found that in most cases, transformation of MeHg+ into elemental mercury (Hg0) took place. From investigations of synthetic solutions, it could be followed that halide ions are responsible for this transformation process. Chloride and bromide converted MeHg+ into Hg0, whereas iodide caused transformation into Hg2+ and Hg0. It could also be shown that transformation of MeHg+ took place only during the derivatization step. In contrast to ethylation, propylation by NaBPr4 did not cause any transformation; however, accurate results of MeHg+ determinations could be obtained by propylation as well as by ethylation when GC/ICP-IDMS was applied. This work demonstrates the great power of isotopically labeled element compounds for the validation of element speciation methods and for species-specific IDMS analyses.</abstract><cop>Washington, DC</cop><pub>American Chemical Society</pub><pmid>11534731</pmid><doi>10.1021/ac010366+</doi><tpages>8</tpages></addata></record> |
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| subjects | Analysis methods Analytical chemistry Applied sciences Chemistry Chromatographic methods and physical methods associated with chromatography Exact sciences and technology Gas chromatographic methods Isotopes Natural water pollution Pollution Spectrum analysis Toxicity Water treatment and pollution |
| title | Validation of Methylmercury Determinations in Aquatic Systems by Alkyl Derivatization Methods for GC Analysis Using ICP-IDMS |
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