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Drug Monitoring and Toxicology |
a Author for correspondence. Fax 403-492-0364; e-mail xc.le{at}ualberta.ca.
We developed and evaluated a method for the determination of µg/L concentrations of individual arsenic species in urine samples. We have mainly studied arsenite [As(III)], arsenate [As(V)], monomethylarsonic acid (MMAA), and dimethylarsinic acid (DMAA) because these are the most commonly used biomarkers of exposure by the general population to inorganic arsenic and because of concerns over these arsenic species on their toxicity and carcinogenicity. We have also detected five unidentified urinary arsenic species resulting from the metabolism of arsenosugars. We combined ion pair liquid chromatography with on-line hydride generation and subsequent atomic fluorescence detection (HPLC/HGAFS). Detection limits, determined as three times the standard deviation of the baseline noise, are 0.8, 1.2, 0.7, and 1.0 µ/L arsenic for arsenite, arsenate, MMAA, and DMAA, respectively. These correspond to 16, 24, 14, and 20 pg of arsenic, respectively, for a 20-µL sample injected for analysis. The excellent detection limit enabled us to determine trace concentrations of arsenic species in urine samples from healthy subjects who did not have excess exposure to arsenic. There was no need for any sample pretreatment step. We used Standard Reference Materials, containing both normal and increased concentrations of arsenic, to validate the method. Interlaboratory studies with independent techniques also confirmed the results obtained with the HPLC/HGAFS method. We demonstrated an application of the method to the determination of arsenic species in urine samples after the ingestion of seaweed by four volunteers. We observed substantial increases of DMAA concentrations in the samples collected from the volunteers after the consumption of seaweed. The increase of urinary DMAA concentration is due to the metabolism of arsenosugars that are present in the seaweed. Our results suggest that the commonly used biomarkers of exposure to inorganic arsenic, based on the measurement of arsenite, arsenate, MMAA, and DMAA, are not reliable when arsenosugars are ingested from the diet.
The following articles in journals at HighWire Press have cited this article:
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  C. Yuan, X. Lu, N. Oro, Z. Wang, Y. Xia, T. J. Wade, J. Mumford, and X. C. Le Arsenic Speciation Analysis in Human Saliva Clin. Chem., January 1, 2008; 54(1): 163 - 171. [Abstract] [Full Text] [PDF]
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 E. Guillamet, A. Creus, J. Ponti, E. Sabbioni, S. Fortaner, and R. Marcos In vitro DNA damage by arsenic compounds in a human lymphoblastoid cell line (TK6) assessed by the alkaline Comet assay Mutagenesis, March 1, 2004; 19(2): 129 - 135. [Abstract] [Full Text] [PDF]
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 Y. Kobayashi, Y. Ogra, K. Ishiwata, H. Takayama, N. Aimi, and K. T. Suzuki Selenosugars are key and urinary metabolites for selenium excretion within the required to low-toxic range PNAS, December 10, 2002; 99(25): 15932 - 15936. [Abstract] [Full Text] [PDF]
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K. A. Francesconi, R. Tanggaar, C. J. McKenzie, and W. Goessler Arsenic Metabolites in Human Urine after Ingestion of an Arsenosugar Clin. Chem., January 1, 2002; 48(1): 92 - 101. [Abstract] [Full Text] [PDF]
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J. Yoshinaga, A. Chatterjee, Y. Shibata, M. Morita, and J. S. Edmonds Human Urine Certified Reference Material for Arsenic Speciation Clin. Chem., November 1, 2000; 46(11): 1781 - 1786. [Abstract] [Full Text] [PDF]
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J. Feldmann, V. W-M. Lai, W. R. Cullen, M. Ma, X. Lu, and X. C. Le Sample Preparation and Storage Can Change Arsenic Speciation in Human Urine Clin. Chem., November 1, 1999; 45(11): 1988 - 1997. [Abstract] [Full Text] [PDF]
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