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A Method for Methylmercury and Inorganic Mercury in Biological Samples Using High Performance Liquid Chromatography- Inductively Coupled Plasma Mass Spectrometry

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Abstract

A new determination method was developed for the measurement of methylmercury (Me-Hg) and inorganic mercury (i-Hg) in biological samples using high-performance liquid chromatography-inductively coupled plasma-mass spectrometry (HPLC-ICP-MS) following alkaline extraction. Mercury species in biological samples were extracted with 10% (w/w) tetramethylammonium hydroxide (TMAH) solution at 80°C for 2 h. Methylmercury was completely separated from i-Hg by adamantyl type and octadecylsilyl type columns within 6 and 4 min using isocratic elution, respectively. The detection limits (3(3σ)) of adamantyl and octadecylsilyl columns using the proposed system were 0.08 and 0.13 ng g−1 (as Hg), respectively. Inorganic Hg completely separates from Me-Hg without tailing. The proposed determination methods were applied to several biological certified reference materials (CRMs). The measurement results of Me-Hg obtained by the present method were in good agreement within the expanded uncertainties (k = 2) with the certified values. The analytical precision (n = 3) of Me-Hg was less than 2%, and the recoveries of Me-Hg and i-Hg were 101 ± 1 and 103 ± 3%, respectively. In addition, this method enables the determination of Me-Hg and i-Hg for 20 samples in 1 h.

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References

  1. FAO, “The State of World Fisheries and Aquaculture 2014”, 2014, ISSN 1020-5489, Rome.

    Google Scholar 

  2. Codex, “Codex General Standard for Contaminants and Toxins and Food and Feed”, 2015, CODEX STAN, 193-1995.

    Google Scholar 

  3. R. S. Hellberg, C. A. M. DeWitt, and M. T. Morrissey, Compr. Rev. Food Sci. Food Saf., 2012, 11, 490.

    Article  CAS  Google Scholar 

  4. B. Laird, H. M. Chan, K. Kannan, A. Husain, H. Al-Amiri, B. Dashti, A. Sultan, A. Al-Othman, and F. Al-Mutawa, Sci. Total Environ., 2017, 607-608, 375.

    Article  PubMed  Google Scholar 

  5. Ministry of the Environmental, Government of Japan: http://www.env.go.jp/en/chemi/mercury/mcm.html.

  6. C. Ibánez-Palomino, J. F. Lopez-Sanchez, and A. Sahuquillo, Anal. Chim. Acta, 2012, 720, 9.

    Article  PubMed  Google Scholar 

  7. M. Morita, J. Yoshinaga, and J. S. Edmonds, Pure Appl. Chem., 1998, 70, 1585.

    Article  CAS  Google Scholar 

  8. J. Yoshinaga, M. Morita, and K. Okamoto, Fresenius J. Anal. Chem., 1997, 357, 279.

    Article  CAS  Google Scholar 

  9. Ministry of the Environment, Government of Japan, “Manual for Mercury Analysis”, 2004, http://www.env.go.jp/chemi/report/h15-04/index.html.

    Google Scholar 

  10. M. Loger, M. Horvat, H. Akagi, T. Ando, T. Tomiyasu, and V. Fajon, Appl. Organometal. Chem., 2001, 15, 515.

    Article  Google Scholar 

  11. T. Sakamoto, K. Akaki, T. Watanabe, R. Matsuda, and H. Hiwaki, Bunseki Kagaku, 2012, 61, 327.

    Article  CAS  Google Scholar 

  12. A. Chow and D. Buksak, Canadian J. Chem., 1975, 53, 1373.

    Article  CAS  Google Scholar 

  13. Ministry of the Environment, Government of Japan, “Manual for Mercury Analysis”, March 2004, http://www.env.go.jp/chemi/report/h15-04/index.html.

    Google Scholar 

  14. F. V. M. Pontes, M. C. Carneiro, D. S. Vaitsman, M. I. C. Monteiro, A. A. Neto, and M. L. B. Tristao, Fuel, 2014, 116, 421.

    Article  CAS  Google Scholar 

  15. P. Kumkrong, B. Thiensong, P. M. Le, G. McRae, A. Windust, S. Deawtong, J. Meija P. Maxwell, L. Yang, and Z. Mester, Anal. Chim. Acta, 2016, 943, 41.

    Article  CAS  PubMed  Google Scholar 

  16. H. Tao, T. Murakami, M. Tominaga, and A. Miyazaki, J. Anal. At. Spectrom., 1998, 13, 1085.

    Article  CAS  Google Scholar 

  17. Q. Tu, J. Qiana, and W. Frech, J. Anal. At. Spectrom., 2000, 15, 1583.

    Article  CAS  Google Scholar 

  18. G. M. M. Rahman, M. M. Wolle, T. Fahrenholz, H. M. S. Kingston, and M. Pamuku, Anal. Chem., 2014, 86, 6130.

    Article  CAS  PubMed  Google Scholar 

  19. S. Clémens, M. Monperrus, O. F. X. Donard, D. Amouroux, and T. Guerin, Anal. Bioanal. Chem., 2011, 401, 2699.

    Article  PubMed  Google Scholar 

  20. H. Pietilä, P. Perämäki, J. Piispanen, M. Starr, T. Nieminen, M. Kantola, and L. Ukonmaanaho, Chemosphere, 2015, 124, 47.

    Article  PubMed  Google Scholar 

  21. L. D’Ulivo, L. Yang, Y.-L. Feng, and Z. Mester, Anal. Methods, 2013, 5, 7127.

    Article  Google Scholar 

  22. L. Yang, Z. Mester, and R. E. Sturgeon, J. Anal. At. Spectrom., 2003, 18, 431.

    Article  CAS  Google Scholar 

  23. S. Zhu, B. Chen, M. He, T. Huang, and B. Hu, Talanta, 2017, 171, 213.

    Article  CAS  PubMed  Google Scholar 

  24. R. Koplfk, I. Klimesová, K. Malisová, and O. Mestek, Czech J. Food Sci., 2014, 32, 249.

    Article  Google Scholar 

  25. S. C. Hight and J. Cheng, Anal. Chim. Acta, 2006, 567, 160.

    Article  CAS  Google Scholar 

  26. S. Sannac, P. Fisicaro, G. Labarraque, F. Pannier, and M. Potin-Gautie, Accred. Qual. Assur, 2009, 14, 263.

    Article  CAS  Google Scholar 

  27. M. Amde, Y. Yin, D. Zhang, and J. Liu, Chem. Spec. Bioavailab., 2016, 28, 51.

    Article  CAS  Google Scholar 

  28. R. Rai, W. Maher, and F. Kirkowa, J. Anal. At. Spectrom., 2002, 12, 1560.

    Article  Google Scholar 

  29. R. Jagtap, F. Krikowa, W. Maher, S. Foster, and M. Ellwood, Talanta, 2011, 85, 49.

    Article  CAS  PubMed  Google Scholar 

  30. M. Lemes and F. Wang, J. Anal. At. Spectrom., 2009, 24, 663.

    Article  CAS  Google Scholar 

  31. C. C. Brombach, Z. Gajdosechova, B. Chen, A. Brownlow, W. T. Corns, J. Feldmann, and E. M. Krupp, Anal. Bioanal. Chem., 2015, 407, 973.

    Article  CAS  PubMed  Google Scholar 

  32. C. C. Brombach, B. Chen, W. T. Corns, J. Feldmann, and E. M. Krupp, Spectrochim. Acta, Part B, 2015, 105, 103.

    Article  CAS  Google Scholar 

  33. M. E. Pichichero, E. Cernichiari, J. Lopreiato, and J. Treanor, Lancet, 2002, 360, 1737.

    Article  CAS  PubMed  Google Scholar 

  34. T. M. Burbacher, D. D. Shen, N. Liberato, K. S. Grant, E. Cernichiari, and T. Clarkson, Environ. Health Perspect., 2005, 113, 1015.

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  35. A. Krata, E. Vassileva, and E. Bulska, Talanta, 2016, 160, 562.

    Article  CAS  PubMed  Google Scholar 

  36. J. Qvarnström, L. Lambertsson, S. Havarinasab, P. Hultman, and W. Frech, Anal. Chem., 2003, 75, 4120.

    Article  PubMed  Google Scholar 

  37. C. C. Brombach, P. Manorut, P. P. P. Kolambage-Dona, M. F. Ezzeldin, B. Chen, W. T. Corns, J. Feldmann, and E. M. Krupp, Food Chem., 2017, 214, 360.

    Article  CAS  PubMed  Google Scholar 

  38. M. A. Vieira, A. S. Ribeiro, A. J. Curtius, and R. E. Sturgeon, Anal. Bioanal. Chem., 2007, 388, 837.

    Article  CAS  PubMed  Google Scholar 

  39. C. M. Tseng, A. De Diego, F. M. Martin, D. Amouroux, and O. F. X. Donard, J. Anal. At. Spectrom., 1997, 12, 743.

    Article  CAS  Google Scholar 

  40. C. C. Brombach, M. F. Ezzeldin, B. Chen, W. T. Corns, J. Feldmann, and E. M. Krupp, Anal. Methods, 2015, 7, 8584.

    Article  CAS  Google Scholar 

  41. H. Matusiewicz and E. Stanisz, Cent. Eur. J. Chem., 2010, 8, 594.

    CAS  Google Scholar 

  42. L. Carrasco and E. Vassileva, Talanta, 2014, 122, 106.

    Article  CAS  PubMed  Google Scholar 

  43. R. Falter, H. Hintelmann, and P. Quevauviller, Chemosphere, 1999, 39, 1039.

    Article  CAS  Google Scholar 

  44. H. Hintelmann, Chemosphere, 1999, 39, 1093.

    Article  CAS  Google Scholar 

  45. H. Hintelmann, R. Falter, G. Ilgen, and R. D. Evans, Fresenius J. Anal. Chem., 1997, 358, 363.

    Article  CAS  Google Scholar 

  46. C. R. Hammerschmidt and W. F. Fitzgerald, Anal. Chem., 2001, 73, 5930.

    Article  CAS  PubMed  Google Scholar 

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Acknowledgments

We thank Prof. Jun Yoshinaga of Toyo University for kindly providing the mercury materials.

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Authors and Affiliations

  1. National Metrology Institute of Japan (NMIJ), National Institute of Advanced Industrial Science and Technology (AIST), 1-1-1 Umezono, Tsukuba, Ibaraki, 305-8563, Japan

    Tomohiro Narukawa

  2. Department of Environmental and Applied Chemistry, School of Science and Technology, Kwansei Gakuin University, 2-1 Gakuen, Sanda, Hyogo, 669-1337, Japan

    Takahiro Iwai & Koichi Chiba

  3. Environmental Analytical Chemistry TESLA-Trace Element Speciation Laboratory, University of Aberdeen, Meston Building Rm G26, Aberdeen AB24 3UE, Scotland, UK

    Joerg Feldmann

Authors
  1. Tomohiro Narukawa
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  2. Takahiro Iwai
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  3. Koichi Chiba
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  4. Joerg Feldmann
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Correspondence to Tomohiro Narukawa.

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Narukawa, T., Iwai, T., Chiba, K. et al. A Method for Methylmercury and Inorganic Mercury in Biological Samples Using High Performance Liquid Chromatography- Inductively Coupled Plasma Mass Spectrometry. ANAL. SCI. 34, 1329–1334 (2018). https://doi.org/10.2116/analsci.18P255

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  • DOI: https://doi.org/10.2116/analsci.18P255

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