Abstract
Mercury (Hg) isotopic analysis via multi-collector inductively coupled plasma (ICP)-mass spectrometry (MC-ICP-MS) can provide relevant biogeochemical information by revealing sources, pathways, and sinks of this highly toxic metal. In this work, the capabilities and limitations of two different sample introduction systems, based on pneumatic nebulization (PN) and cold vapor generation (CVG), respectively, were evaluated in the context of Hg isotopic analysis via MC-ICP-MS. The effect of (i) instrument settings and acquisition parameters, (ii) concentration of analyte element (Hg), and internal standard (Tl)—used for mass discrimination correction purposes—and (iii) different mass bias correction approaches on the accuracy and precision of Hg isotope ratio results was evaluated. The extent and stability of mass bias were assessed in a long-term study (18 months, n = 250), demonstrating a precision ≤0.006 % relative standard deviation (RSD). CVG-MC-ICP-MS showed an approximately 20-fold enhancement in Hg signal intensity compared with PN-MC-ICP-MS. For CVG-MC-ICP-MS, the mass bias induced by instrumental mass discrimination was accurately corrected for by using either external correction in a sample-standard bracketing approach (SSB) or double correction, consisting of the use of Tl as internal standard in a revised version of the Russell law (Baxter approach), followed by SSB. Concomitant matrix elements did not affect CVG-ICP-MS results. Neither with PN, nor with CVG, any evidence for mass-independent discrimination effects in the instrument was observed within the experimental precision obtained. CVG-MC-ICP-MS was finally used for Hg isotopic analysis of reference materials (RMs) of relevant environmental origin. The isotopic composition of Hg in RMs of marine biological origin testified of mass-independent fractionation that affected the odd-numbered Hg isotopes. While older RMs were used for validation purposes, novel Hg isotopic data are provided for the latest generations of some biological RMs.
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References
Fitzgerald WF, Lamborg CH (2003). Geochemistry of mercury in the environment. In: Treatise on geochemistry, vol. 9. Elservier, New York, pp. 107–148
Ridley WI, Stetson SJ (2006) Appl Geochem 21:1889–1899
National Research Council (1978) An assessment of mercury in the environment. National Academy of Sciences, Washington, DC
Mergler D, Anderson HA, Chan LHM, Mahaffey KR, Murray M, Sakamoto M, Stern AH (2007) Ambio 36:3–11
Baya PA, Gosselin M, Lehnherr I, St.Louis VL, Hintelmann H (2015) Environ Sci Technol 49:223–232
Fitzgerald WF, Engström DR, Mason RP, Nater EA (1998) Environ Sci Technol 32:1–7
Blum JD (2011) Applications of stable mercury isotopes to biogeochemistry. In: Bskaran M (ed) Handbook of environmental isotope geochemistry, advances in isotope geochemistry. Springer, Berlin
Hintelmann H (2012) Use of stable isotopes in mercury research. In: Bank MS (ed) Mercury in the environment. Univ Calif Press, Berkeley
Blum JD, Sherman LS, Johnson MW (2014) Annu Rev Earth Planet Sci 42:249–269
Yin R, Feng X, Li X, Yu B, Du B (2014) Trends Environ Anal Chem 2:1–10
Vanhaecke F, Balcaen L, Malinovsky D (2009) J Anal At Spectrom 24:863–886
Yin R, Feng X, Shi W (2010) Appl Geochem 25:1467–1477
Young ED, Galy A, Nagahara H (2002) Geochim Cosmochim Acta 66:1095–1104
Biegeleisen J (1996) J Am Chem Soc 118:3676–3680
Buchachenko AL (2001) J Phys Chem A 105:9995–10011
Chen J, Hintelmann H, Feng X, Dimock B (2012) Geochim Cosmochim Acta 90:33–46
Wang Z, Chen J, Feng X, Hintelmann H, Yuan S, Cai H, Huang Q, Wang S, Wang F (2015) Compt Rendus Geosci. doi:10.1016/j.crte.2015.1002.1006
Theimens MH (1999) Science 283:341–345
Farqijar J, Bao H, Tjoe ME (2000) Science 289:756–759
Gantner N, Hintelmann H, Zheng W, Muir DC (2009) Environ Sci Technol 43:9148–9154
Laffont L, Sonke JE, Maurice L, Hintelmann H, Pouilly M, Bacarreza YS, Perez T, Behra P (2009) Environ Sci Technol 43:8985–8990
Zambardi T, Sonke JE, Toutain JP, Sortino F, Shinohara H (2009) Earh Planet Sci Lett 277:236–243
Perrot V, Epov VN, Pastukhov MV, Grebenshchikova VI, Zouiten C, Sonke JE, Husted S, Donard OFX, Amouroux D (2010) Environ Sci Technol 44:8030–8037
Masbou J, Point D, Sonke J (2013) J Anal At Spectrom 28:1620–1628
Albarède F, Telouk P, Blichert-Toft J, Boyet M, Agranier A, Nelson B (2004) Geochim Cosmochim Acta 68:2725–2744
Meija J, Yang L, Mester Z, Sturgeon RE (2012) Correction of instrumental mass discrimination for isotope ratio determination with multi-collector inductively coupled plasma mass spectrometry. In: Vanhaecke F, Degryse P (eds) Isotopic analysis fundamentals and applications using ICP-MS. Wiley-VCH, Germany
Yang L (2009) Mass Spectrom Rev 28:990–1011
Kivel N, Potthast H-D, Günther-Leopold I, Vanhaecke F, Günther D (2014) Spectrochim Acta B 93:34–40
Barling J, Weis D (2008) J Anal At Spectrom 23:1017–1025
Barling J, Weis D (2012) J Anal At Spectrom 27:653–662
Yang L, Sturgeon RE (2003) J Anal At Spectrom 18:1452–1457
Taylor PDP, De Bièvre P, Walder AJ, Entwistle A (1995) J Anal At Spectrom 10:395–398
Devulder V, Lobo L, Van Hoecke K, Degryse P, Vanhaecke F (2013) Spectrochim Acta B 89:20–29
Vanhaecke F, Vanhoe H, Dams R (1992) Talanta 39:737–742
Albarède F, Albalat E, Télouk P (2015) J Anal At Spectrom 30:1736–1742
Russell WA, Papanastassiou DA, Tombrello TA (1978) Geochim Cosmochim Acta 42:1075–1090
Hirata T (1996) Analyst 121:1407–1411
White WM, Albarède F, Télouk P (2000) Chem Geol 167:257–270
Woodhead J (2002) J Anal At Spectrom 17:1381–1385
Baxter DC, Rodushkin I, Engström E, Malinovsky D (2006) J Anal At Spectrom 21:427–430
Wombacher F, Rehkämper M (2003) J Anal At Spectrom 18:1371–1375
Mead C, Johnson TM (2010) Anal Bioanal Chem 397:1529–1538
Evans RD, Hintelmann H, Dillon PJ (2001) J Anal At Spectrom 16:1064–1069
Sonke JE, Zambardi T, Toutain J-P (2008) J Anal At Spectrom 23:569–573
Leopold K, Foulkes M, Worsfold PJ (2009) TrAC Trends Anal Chem 28:426–435
Hintelmann H, Lu S (2003) Analyst 128:635–639
Foucher D, Hintelmann H (2006) Anal Bioanal Chem 384:1470–1478
Vanhaecke F, Van Holderbeke M, Moens L, Dams R (1996) J Anal At Spectrom 11:543–548
Kritee K, Blum JD, Johnson MW, Bergquist BA, Barkay T (2007) Environ Sci Technol 41:1889–1895
Foucher D, Ogrinc N, Hintelmann H (2009) Environ Sci Technol 43:33–39
Sonke JE, Schäfer J, Chmeleff J, Audry S, Blanc G, Dupré B (2010) Chem Geol 279:90–100
Aramendía M, Resano M, Vanhaecke F (2010) J Anal At Spectrom 25:390–404
Epov VN, Rodriguez-Gonzalez P, Sonke JE, Tessier E, Amouroux D, Bourgoin LM, Donard OFX (2008) Anal Chem 80:3530–3538
Yang L, Mester Z, Zhou L, Gao S, Sturgeon RE, Meija J (2011) Anal Chem 83:8999–9004
Blum JB, Bergquist BA (2007) Anal Bioanal Chem 388:353–359
Meija J, Yang L, Sturgeon RE, Mester Z (2010) J Anal At Spectrom 25:384–389
Evans EH, Giglio JJ (1993) J Anal At Spectrom 8:1–18
Agatemor C, Beauchemin D (2011) Anal Chim Acta 706:66–83
Rehkämper M, Mezger K (2000) J Anal At Mass Spectrom 15:1451–1460
Fontaine GH, Hattendorf B, Bourdon B, Günther D (2009) J Anal At Mass Spectrom 24:637–648
Bergquist BA, Blum JD (2007) Science 318:417–420
Malinovsky D, Sturgeon RE, Yang L (2008) Anal Chem 80:2548–2555
Kwon SY, Blum JD, Chen CY, Meattey DE, Mason RP (2014) Environ Sci Technol 48:10089–10097
Perrot V, Pastukhov MV, Epov VN, Husted S, Donard OFX, Amouroux D (2012) Environ Sci Technol 46:5902–5911
Sherman LS, Blum JB (2013) Sci Total Environ 448:163–175
Acknowledgments
The authors acknowledge the European Metrology Research Programme (EMRP) for the organizational research excellence grant (REG) provided in the context of the SIB09-Elements project. The EMRP is jointly funded by the EMRP-participating countries within the Euramet and the EU. The authors sincerely thank (i) Prof. Dr. Olivier Donard and Dr. Sylvain Bérail from the Université de Pau et des Pays de l’Adour, Pau (France) for providing them with an aliquot of UM-Almaden digest and (ii) Dr. Patricia Grinberg and Dr. Ralph Sturgeon from the Canadian National Research Centre (NRC) for providing them with reference materials that are no longer commercially available.
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Published in the topical collection Applications of Isotopes in Analytical Ecogeochemistry with guest editors Thomas Prohaska, Andreas Zitek, and Johanna Irrgeher.
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Rua-Ibarz, A., Bolea-Fernandez, E. & Vanhaecke, F. An in-depth evaluation of accuracy and precision in Hg isotopic analysis via pneumatic nebulization and cold vapor generation multi-collector ICP-mass spectrometry. Anal Bioanal Chem 408, 417–429 (2016). https://doi.org/10.1007/s00216-015-9131-2
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DOI: https://doi.org/10.1007/s00216-015-9131-2