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Development and Validation of the Simultaneous Analytical Method of Urinary Metals and Metalloids for the National Biomonitoring Programs

국가 바이오모니터링 프로그램을 위한 소변 중 금속류 동시분석법 개발 및 검증

  • Cho, Yong Min (Institute for Life & Environmental Technology, Smartive Corporation) ;
  • Yang, Minho (Institute for Life & Environmental Technology, Smartive Corporation) ;
  • Im, Hosub (Institute for Life & Environmental Technology, Smartive Corporation) ;
  • Cha, Sangwon (Department of Chemistry, Hankuk University of Foreign Studies) ;
  • Lee, Jaeick (Doping Control Center, Korea Institute of Science and Technology) ;
  • Kim, Ki Hun (Doping Control Center, Korea Institute of Science and Technology) ;
  • Han, Sang Beom (Department of Pharmaceutical Analysis, College of Pharmacy, Chung-Ang University)
  • 조용민 (주식회사 스마티브 생명환경연구소) ;
  • 양민호 (주식회사 스마티브 생명환경연구소) ;
  • 임호섭 (주식회사 스마티브 생명환경연구소) ;
  • 차상원 (한국외국어대학교 화학과) ;
  • 이재익 (한국과학기술연구원 도핑콘트롤센터) ;
  • 김기훈 (한국과학기술연구원 도핑콘트롤센터) ;
  • 한상범 (중앙대학교 약학대학)
  • Received : 2019.09.17
  • Accepted : 2019.11.06
  • Published : 2019.12.31

Abstract

Objectives: This study developed and validated an analysis method of urinary metals and metalloids that can be applied inductively with coupled plasma mass spectrometry (ICP-MS). Methods: 0.3 mL of urine was used to analyze 25 metal and metalloid compounds using ICP-MS. The validation of the analytical method included linearity, accuracy, precision, and the calculation of detection limits. In addition, a comparison test was performed with the graphite furnace atomic absorption spectrometry (GF-AAS) method, which is the current standard method, with urine samples of 66 healthy subjects. Results: The linearities (R2) of calibration curves of all 25 compounds were ≥ 0.999. Of the 25 compounds, the intra-day and inter-day accuracy% of 17 and 20 met ≤15%, respectively. In addition, fifteen compounds showed ≤15% recovery% for certificated reference materials. Intraclass correlation coefficients of the comparison between the current methods and new methods in this study were 0.952 (p-value<0.001) and 0.911 (p-value<0.001) for urinary cadmium and mercury, respectively. Conclusion: This study proposes an efficient simultaneous methodology that can analyze multi elements in smaller sample amounts. More reproduction experiments are needed in the future.

Keywords

References

  1. Angerer J, Ewers U, Wilhelm M. Human biomonitoring: state of the art. Int J Hyg Environ Health 2007; 210(3-4): 201-228. https://doi.org/10.1016/j.ijheh.2007.01.024
  2. Angerer J, Aylward LL, Hays SM, Heinzow B, Wilhelm M. Human biomonitoring assessment values: approaches and data requirements. Int J Hyg Environ Health 2011; 214(5): 348-360. https://doi.org/10.1016/j.ijheh.2011.06.002
  3. Kim S. Application of biomonitoring to activities on environmental health and recommendations for Korean National Environmental Health Survey. The Korean Journal of Public Health 2015; 52(1): 59-74.
  4. Lee JH, Lee CK, Moon CS, Choi IJ, Lee KJ, Yi SM, et al. Korea National Survey for environmental pollutants in the human body 2008: heavy metals in the blood urine of the Korean population. Int J Environ Health 2012; 215(4): 449-457. https://doi.org/10.1016/j.ijheh.2012.01.002
  5. Park C, Yu SD. Status and prospects of the Korean National Environmental Health Survey (KoNEHS). J Environ Health Sci 2014; 40(1): 1-9.
  6. Becker K, Conrad A, Kirsch N, Kolossa-Gehring M, Schulz C, Seiwert M, et al. German Environmental Survey (GerES): human biomonitoring as a tool to identify exposure pathways. Int J Hyg Environ Health 2007; 210(3-4): 267-269. https://doi.org/10.1016/j.ijheh.2007.01.010
  7. Haines DA, Saravanabhavan G, Werry K, Khoury C. An overview of human biomonitoring of environmental chemicals in the Canadian Health Measures Survey: 2007-2019. Int J Hyg Environ Health 2017; 220(2 Pt A): 13-28. https://doi.org/10.1016/j.ijheh.2016.08.002
  8. Awata H, Linder S, Mitchell LE, Delclos GL. Biomarker Levels of Toxic Metals among Asian Populations in the United States: NHANES 2011-2012. Environ Health Perspect 2017; 125(3): 306-313. https://doi.org/10.1289/EHP27
  9. Butler O, Evans H, Fisher A, Hill S, Harrinton C, et al. Atomic spectrometry updates: a 25-year retrospective. J Anal At Spectrom 2010; 25(10): 1546-1566. https://doi.org/10.1039/c005518m
  10. Fukui Y, Ohashi F, Sakuragi S, Moriguchi J, Ikeda M. Comparative evaluation of GFAAS and ICP-MS for analyses of cadmium in blood. Ind Health 2011; 49(3): 338-343. https://doi.org/10.2486/indhealth.MS1194
  11. Basu N, Tutino R, Zhang Z, Cantonwine DE, Goodrich JM, Somers EC, et al. Mercury levels in pregnant women, children, and seafood from Mexico City. Environ Res 2014; 135: 63-39 https://doi.org/10.1016/j.envres.2014.08.029
  12. Vriens A, Nawrot TS, Janssen BG, Baeyens W, Bruckers L, Covaci A, et al. Exposure to Environmental Pollutants and Their Association with Biomarkers of Aging: A Multipollutant Approach. Environ Sci Technol 2019; doi: 10.1021/acs.est/ 8b07141. [Epub ahead of print]
  13. Goulle JP, Saussereau E, Mahieu L, Guerbet M. Current role of ICP-MS in clinical toxicology and forensic toxicology: a metallic profile. Bioanalysis 2014; 6(17): 2245-2259. https://doi.org/10.4155/bio.14.190
  14. Kwon JY, Kim BG, Lim HJ, Seo JW, Kang MK, Kim YM, et al. Comparison of human blood cadmium concentrations using graphite furnace atomic absorption spectrometry (GF-AAS) and inductively coupled plasma-mass spectrometry (ICP-MS). J Environ Health Sci 2018; 44(5): 491-501.
  15. Goulle JP, Mahieu L, Castermant J, Neveu N, Bonneau L, Laine G, et al. Metal and metalloid multielementary ICP-MS validation in whole blood, plasma, urine and hair. Reference values. Forensic Sci Int 2005; 153(1): 39-44. https://doi.org/10.1016/j.forsciint.2005.04.020
  16. Caldwell KL, Hartel J, Jarrett J, Jones RL. Inductively coupled plasma mass spectrometry to measure multiple toxic elements in urine in NHANES 1999-2000. Atomic Spectroscopy 2005; 26(1): 1-7.
  17. Haines DA, Saravanabhavan G, Werry K, Khoury C. An overview of human biomonitoring of environmental chemicals in the Canadian Health Measures Survey: 2007-2019. Int J Hyg Environ Health 2017; 220(2 Pt A): 13-28. https://doi.org/10.1016/j.ijheh.2016.08.002
  18. CDC (Centers for Disease Control and Prevention). Laboratory Procedure Manual-Urine Multi-Element ICP-DRC-MS. CDC Method No. 3018.6-02 (15 element panel) and 3018A.4-02 (total arsenic). NHANES 2015-2016. P. 91.
  19. Kim K, Hong SY, Yoo EJ, Ko SH, Kim MO, Kim MJ, et al. Study on the validation of environmental test methods. J Korean Society for Environmental Analysis 2018; 21(2): 87-94.
  20. Ministry of Food and Drug Safety. Guideline on bioanalytical method validation. 11-1471000-000028-01; 2013. P. 40.
  21. National Institute of Environmental Research. A manual for analysis of environmental pollutants in the human specimen. NIER GOVP1200717001; 2006. P. 302.
  22. Kong KA. Statistical methods: reliability assessment and method comparison. Ewha Med J 2017; 40(1): 9-16. https://doi.org/10.12771/emj.2017.40.1.9
  23. Becker K, Schulz C, Kaus S, Seiwert M, Seifert B. German Environmental Survey 1998 (GerES III): environmental pollutants in the urine of the German population. Int J Hyg Environ Health 2003; 206(1): 15-24. https://doi.org/10.1078/1438-4639-00188
  24. Fukui Y, Ohashi F, Sakuragi S, Moriguchi J, Ikeda M. Comparative evaluation of GFAAS and ICP-MS for analyses of cadmium in blood. Ind Health 2011; 49(3): 338-343. https://doi.org/10.2486/indhealth.MS1194
  25. Lee W, Hur YH, Park KS. A study of analytical method for trace metal ions in whole blood and urine by inductively coupled plasma-mass spectrometry using solid-liquid extraction technique. Anal Sci Technol 1998; 11(4): 281-291.
  26. Kim YH, Kim WI, Hwang SR, Song KB, Park JS, Kang YY, et al. Establishment of analytical methods for blood and urine using ICP/MS (II). Environmental Health Risk Research Department. NIER 2009-01-1057; 2009. P. 62.
  27. Lee SY, Oh HJ, Choi YH, Kim JW, Kim SH. Trace metal analysis using inductively plasma-mass spectrometry (ICP-MS). Korean J Lab 2004; 24: 362-370.
  28. Trzcinka-Ochocka M, Brodzka R, Janasik B. Useful and Fast Method for Blood Lead and Cadmium Determination Using ICP-MS and GF-AAS; Validation Parameters. J Clin Lab Anal 2016; 30(2): 130-139. https://doi.org/10.1002/jcla.21826
  29. DeBord DG, Carreon T, Lentz TJ, Middendorf PJ, Hoover MD, Schulte PA. Use of the "Exposome" in the Practice of Epidemiology: A Primer on -Omic Technologies. Am J Epidemiol 2016; 184(4): 302-314. https://doi.org/10.1093/aje/kwv325
  30. Palmer CD, Lewis Jr ME, Geraghty CM, Barbosa Jr F, Parsons PJ. Determination of lead, cadmium and mercury in blood for assessment of environmental exposure: A comparison between inductively coupled plasma-mass spectrometry and atomic absorption spectrometry. Spectrochimica Acta Part B 2006; 61: 980-990. https://doi.org/10.1016/j.sab.2006.09.001