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Urinary arsenic species, toenail arsenic, and arsenic intake estimates in a Michigan population with low levels of arsenic in drinking water

Journal of Exposure Science & Environmental Epidemiology volume 22, pages 182–190 (2012)Cite this article

Abstract

The large disparity between arsenic concentrations in drinking water and urine remains unexplained. This study aims to evaluate predictors of urinary arsenic in a population exposed to low concentrations (≤50 μg/l) of arsenic in drinking water. Urine and drinking water samples were collected from a subsample (n=343) of a population enrolled in a bladder cancer case–control study in southeastern Michigan. Total arsenic in water and arsenic species in urine were determined using ICP-MS: arsenobetaine (AsB), arsenite (As[III]), arsenate (As[V]), methylarsenic acid (MMA[V]), and dimethylarsenic acid (DMA[V]). The sum of As[III], As[V], MMA[V], and DMA[V] was denoted as SumAs. Dietary information was obtained through a self-reported food intake questionnaire. Log10-transformed drinking water arsenic concentration at home was a significant (P<0.0001) predictor of SumAs (R2=0.18). Associations improved (R2=0.29, P<0.0001) when individuals with less than 1 μg/l of arsenic in drinking water were removed and further improved when analyses were applied to individuals who consumed amounts of home drinking water above the median volume (R2=0.40, P<0.0001). A separate analysis indicated that AsB and DMA[V] were significantly correlated with fish and shellfish consumption, which may suggest that seafood intake influences DMA[V] excretion. The Spearman correlation between arsenic concentration in toenails and SumAs was 0.36 and between arsenic concentration in toenails and arsenic concentration in water was 0.42. Results show that arsenic exposure from drinking water consumption is an important determinant of urinary arsenic concentrations, even in a population exposed to relatively low levels of arsenic in drinking water, and suggest that seafood intake may influence urinary DMA[V] concentrations.

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References

  • Adair B., Hudgens E., Shmitt M., Calderon R., and Thomas D. Total arsenic concentrations in toenails quantified by two techniques provide a useful biomarker of chronic arsenic exposure in drinking water. Environ Res 2006: 19: 213–220.

    Article  Google Scholar 

  • Aposhian H., and Aposhian M. Arsenic toxicology: five questions. Chem Res Toxicol 2006: 19: 1–15.

    Article  CAS  Google Scholar 

  • Brima EI., Haris PI., Jenkins RO., Polea DA., Gault AG., and Harrington CF. Understanding arsenic metabolism through a comparative study of arsenic levels in the urine, hair and fingernails of healthy volunteers from three unexposed ethnic groups in the United Kingdom. Toxicol and Appl Pharmacol 2006: 216: 122–130.

    Article  CAS  Google Scholar 

  • Caldwell K., Jones R., Verdon C., Jarrett J., Caudill S., and Osterloh J. Levels of urinary total and speciated arsenic in the US population: National Health and Nutrition Examination Survey 2003–2004. J Expo Sci Environ Epidemiol 2009: 19: 59–68.

    Article  CAS  Google Scholar 

  • Chen Y., Su H., Guo Y., Hsueh Y., Smith T., and Ryan L., et al. Arsenic methylation and bladder cancer risk in Taiwan. Cancer Causes Control 2003: 14: 303–310.

    Article  Google Scholar 

  • Choi B., Choi S., Kim D., Huang Y., Kim N., and Park K. Effects of repeated seafood consumption on urinary excretion of arsenic species by volunteers. Arch Envrion Contam Toxicol 2010: 58: 222–229.

    Article  CAS  Google Scholar 

  • Das D., Chatterjee A., Mandal B., Samanta G., Chakraborti D., and Chanda B. Arsenic in ground water in six districts of West Bengal, India: the biggest arsenic calamity in the world. Part 2. Arsenic concentration in drinking water, hair, nails, urine, skin-scale and liver tissue (biopsy) of the affected people. Analyst 1995: 120: 917–924.

    Article  CAS  Google Scholar 

  • Devesa V., Súñer M., Algora S., Vélez D., Montoro R., and Jalón M., et al. Organoarsenical species contents in cooked seafood. J Agric Food Chem 2005: 53: 8813–8819.

    Article  CAS  Google Scholar 

  • Fillol C., Dor F., Labat L., Boltz P., Le Bouard J, and Mantey K., et al. Urinary arsenic concentrations and speciation in residents living in an area with naturally contaminated soils. Sci Total Environ 2010: 408: 1190–1194.

    Article  CAS  Google Scholar 

  • Francesconi K., and Kuehnelt D. Determination of arsenic species: a critical review of methods and applications, 2000–2003. Analyst 2004: 129: 327–335.

    Google Scholar 

  • Francesconi K., Tanggaar R., McKenzie C., and Goessler W. Arsenic metabolites in human urine after ingestion of an arsenosugar. Clin Chem 2002: 48: 92–101.

    CAS  PubMed  Google Scholar 

  • Hopenhayn-Rich C., Biggs M., Smith A., Kalman D., and Moore L. Methylation study of a population environmentally exposed to arsenic in drinking water. Environ Health Perspect 1996: 104: 620–628.

    Article  CAS  Google Scholar 

  • Hsueh Y., Chiou H., Huang Y., Wu W., Huang C., and Yang M., et al. Serum beta-carotene level, arsenic methylation capability, and incidence of skin cancer. Cancer Epidemiol BiomarkersPrev 1997: 6: 589–596.

    CAS  Google Scholar 

  • Karagas M., Le X., Morris S., Blum J., Lu X., and Spate V., et al. Markers of low levels arsenic exposure for evaluating human cancer risks in a US population. Intern J Occup Med Environ Health 2001: 14: 171–175.

    CAS  Google Scholar 

  • Karagas M., Nelson H., Kelsey K., Morris S., Blum J., and Tosteson T., et al. Urinary arsenic species in relation to drinking water, toenail arsenic concentrations and genetic polymorphism in GSTMI in New Hampshire. In: Wilson S.H., and Suk W.A. (Eds.). Biomarkers of Environmentally Associated Disease: Technologies, Concepts, and Perspectives. Lewis Publisher, New York, 2002, pp. 249–260.

    Google Scholar 

  • Karagas M., Tosteson T., Blum J., Klaue B., Weiss J., and Stannard V. Measurement of low levels of arsenic exposure: a comparison of water and toenail concentrations. Am J Epidemiol 2000: 152: 84–90.

    Article  CAS  Google Scholar 

  • Karagas M., Tosteston T., Morris J.S., Demidenko E., Mott L., and Heaney J., et al. Incidence of transitional cell carcinoma of the bladder cancer and arsenic exposure in New Hampshire. Cancer Causes Control 2004: 15: 465–472.

    Article  Google Scholar 

  • Lai V., Sun Y., Ting E., Cullen W., and Reimer K. Arsenic speciation in human urine: are we all the same? Toxicol Appl Pharmacol 2004: 198: 297–306.

    Article  CAS  Google Scholar 

  • Le X., Cullen W., and Reimer K. Determination of urinary arsenic and impact of dietary arsenic intake. Talanta 1993: 40: 185–193.

    Article  CAS  Google Scholar 

  • Le X., Cullen W., and Reimer K. Human urinary arsenic excretion following one-time ingestion of arsenosugars present in seaweed and arsenobetaine present in crab and shrimp. Clin Chem 1994: 40: 617–625.

    CAS  PubMed  Google Scholar 

  • Lindberg A., Goessler W., Gurzau E., Koppova K., Rudnai P., and Kumar R., et al. Arsenic in Hungary, Romania and Slovakia. J Environ Monit 2006: 8: 203–208.

    Article  CAS  Google Scholar 

  • Ma M., and Le X. Effect of arsenosugar ingestion on urinary arsenic speciation. Clin Chem 1998: 44: 539–550.

    CAS  PubMed  Google Scholar 

  • Maskiell K., Heyworth J., and McCaul K. Validation of a water consumption questionnaire for a study of the adverse health outcomes associated with disinfection by-products. Int J Environ Health Res 2006: 16: 145–153.

    Article  CAS  Google Scholar 

  • Meacher D., Menzel D., Dillencourt D., Bic L., Schoof R., and Yost L., et al. Estimation of multimedia inorganic arsenic in take in the US population. Hum Ecol Risk Assess 2002: 8: 1697–1721.

    Article  CAS  Google Scholar 

  • Meliker J., Slotnick M., AvRuskin G., Schottenfeld D., Jacquez G., and Wilson M., et al. Lifetime exposure to arsenic in drinking water and bladder cancer: a population-based case–control study in Michigan, USA. Cancer Causes Control 2010: 21: 745–757.

    Article  Google Scholar 

  • Meza M., Kopplin M., Burgess J., and Gandolfi A. Arsenic drinking water exposure and urinary excretion among adults in the Yaqui Valley, Sonora, Mexico. Environ Res 2004: 96: 119–126.

    Article  CAS  Google Scholar 

  • Navas-Acien A., Francesconi K., Silbergeld E., and Guallar E. Seafood intake and urine concentrations of total arsenic, dimethylarsinate and arsenobetaine in the US population. Environ Res 2011: 111: 110–118.

    Article  CAS  Google Scholar 

  • Navas-Acien A., Silbergeld E., Pastor-Barriuso R., and Guallar E. Arsenic exposure and prevalence of type 2 diabetes in US adults. JAMA 2008: 300: 814–822.

    Article  CAS  Google Scholar 

  • Navas-Acien A., Umans J.G., Howard B.V., Goessler W., Franscesconi K.A., Crainiceanu C.M., and Silbergeld E. Urine arsenic concentrations and species excretion patterns in American Indian communities over 10-year period: the Strong Heart Study. Environ Health Perspect 2009: 117: 1428–1433.

    Article  CAS  Google Scholar 

  • Ritsema R., Dukan L., i Navarro T., van Leeuwen W., Oliviera N., and Wolfs P., et al. Speciation of arsenic compounds in urine by LC-ICP MS. Appl Organometal Chem 1998: 12: 591–599.

    Article  CAS  Google Scholar 

  • Rivera-Núñez Z., Linder A.M., Chen B., and Nriagu J.O. Low level determination of six arsenic species in urine by high performance liquid chromatography inductively coupled plasma mass spectrometry (HPLC ICP MS). Anal Methods 2011: 3: 1122–1129.

    Article  Google Scholar 

  • Rivera-Núñez Z., Meliker J., Linder A., and Nriagu J. Reliability of spot urine samples in assessing arsenic exposure. Int J Hyg Environ Health 2010: 213: 359–364.

    Article  Google Scholar 

  • Schoof R., Yost L., Eickhoff J., Crecelius E., Cragin D., and Meacher D., et al. A market basket survey of inorganic arsenic in food. Food Chem Toxicol 1999: 37: 839–846.

    Article  CAS  Google Scholar 

  • Silbergeld E.K., and Nachman K. The environmental and public health risks associated with arsenical use in animal feed. Ann NY Acad Sci 2008: 1140: 346–357.

    Article  CAS  Google Scholar 

  • Slotnick M.J., Meliker J., AvRuskin G.A., Ghosh D., and Nriagu J.O. Toenails as a biomarker of inorganic arsenic intake from drinking water and foods. J Toxicol Environ Health A 2007: 70: 148–158.

    Article  CAS  Google Scholar 

  • Steinmaus C., Bates M., Yuan Y., Kalman D., Atallah R., and Rey O., et al. Arsenic methylation and bladder cancer risk in case–control studies in Argentina and the United States. J Occup Environ Med 2006: 48: 478–488.

    Article  CAS  Google Scholar 

  • Steinmaus C., Carrigan K., Kalman D., Atallah R., Yuan Y., and Smith A. Dietary intake and arsenic methylation in a US population. Environ Health Perspect 2005: 113: 1153–1159.

    Article  CAS  Google Scholar 

  • Steinmaus C., Yuan Y., Liaw J., and Smith A. Low-level population exposure to inorganic arsenic in the United States and diabetes mellitus. Epidemiology 2009: 20: 807–815.

    Article  Google Scholar 

  • Tseng C., Huan Y., Huang Y.C., Chung C.J., Yang M., Chen C., and Hsueh Y. Arsenic exposure, urinary arsenic speciation and peripheral vascular disease in blackfoot disease-hyperendemic villages in Taiwan. Toxicol Appl Pharmacol 2005: 206: 299–308.

    Article  CAS  Google Scholar 

  • Vahter M. Methylation of inorganic arsenic in different mammalian species and population groups. Sci Prog 1999: 82: 69–88.

    CAS  PubMed  Google Scholar 

  • Wright J., Murphy P., Nieuwenhuijsen M., and Savitz D. The impact of water consumption, point-of-use filtration and exposure categorization on exposure misclassification of ingested drinking water contaminants. Sci Total Environ 2006: 366: 65–73.

    Article  CAS  Google Scholar 

  • Xue J., Zartarian V., Wang S., Liu S., and Georgopoulos P. Probabilistic model of dietary arsenic exposure and dose and evaluation with 2003–2004 NHANES Data. Environ Health Perspect 2010: 118: 345–350.

    Article  CAS  Google Scholar 

Download references

Acknowledgements

We appreciate the involvement of all study participants for taking part in this research. We also thank the collaboration of Aaron M. Linder, Lingling Zhang, Luis O. Rivera-González, Stacey Fedewa, Gillian AvRuskin, Angela Hungerink, Roni Kobrosly, Nicholas Mank, and Caitlyn Meservey for valuable assistance with different aspects of this project. This research was funded by the National Cancer Institute, Grant RO-1 CA96002-10. The first author received support from the Comprehensive Minority Biomedical Branch of the National Cancer Institute. The perspectives are those of the authors and do not necessarily represent the official position of the funding agency.

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Authors and Affiliations

  1. Department of Environmental Health Sciences, School of Public Health, University of Michigan, 6655 SPH I, Ann Arbor, Michigan, USA

    Zorimar Rivera-Núñez, John D Meeker, Melissa J Slotnick & Jerome O Nriagu

  2. Department of Preventive Medicine, Graduate Program in Public Health, Stony Brook University Medical Center, Stony Brook, HSC L3, New York, USA

    Jaymie R Meliker

Authors
  1. Zorimar Rivera-Núñez
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Correspondence to Zorimar Rivera-Núñez.

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Supplementary Information accompanies the paper on the Journal of Exposure Science and Environmental Epidemiology website

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Rivera-Núñez, Z., Meliker, J., Meeker, J. et al. Urinary arsenic species, toenail arsenic, and arsenic intake estimates in a Michigan population with low levels of arsenic in drinking water. J Expo Sci Environ Epidemiol 22, 182–190 (2012). https://doi.org/10.1038/jes.2011.27

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