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Uranium(VI) Binding Forms in Selected Human Body Fluids: Thermodynamic Calculations versus Spectroscopic Measurements

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    Article

    Uranium(VI) Binding Forms in Selected Human Body Fluids: Thermodynamic Calculations versus Spectroscopic Measurements
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    † Helmholtz-Zentrum Dresden-Rossendorf (HZDR), Institute of Resource Ecology, Bautzner Landstraße 400, 01328 Dresden, Germany
    *Tel: +49 351 260 2306. Fax: +49 351 260 3553. E-mail: [email protected]
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    Chemical Research in Toxicology

    Cite this: Chem. Res. Toxicol. 2015, 28, 2, 238–247
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    https://doi.org/10.1021/tx5004084
    Published January 6, 2015
    Copyright © 2015 American Chemical Society
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    Abstract

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    Human exposure to uranium increasingly becomes a subject of interest in many scientific disciplines such as environmental medicine, toxicology, and radiation protection. Knowledge about uranium chemical binding forms (speciation) in human body fluids can be of great importance to understand not only its biokinetics but also its relevance in risk assessment and in designing decorporation therapy in the case of accidental overexposure. In this study, thermodynamic calculations of uranium speciation in relevant simulated and original body fluids were compared with spectroscopic data after ex-situ uranium addition. For the first time, experimental data on U(VI) speciation in body fluids (saliva, sweat, urine) was obtained by means of cryogenic time-resolved laser-induced fluorescence spectroscopy (cryo-TRLFS) at 153 K. By using the time dependency of fluorescence decay and the band positions of the emission spectra, various uranyl complexes were demonstrated in the studied samples. The variations of the body fluids in terms of chemical composition, pH, and ionic strength resulted in different binding forms of U(VI). The speciation of U(VI) in saliva and in urine was affected by the presence of bioorganic ligands, whereas in sweat, the distribution depends mainly on inorganic ligands. We also elucidated the role of biological buffers, i.e., phosphate (H2PO4–/HPO42–) on U(VI) distribution, and the system Ca2+/UO22+/PO43– was discussed in detail in both saliva and urine. The theoretical speciation calculations of the main U(VI) species in the investigated body fluids were significantly consistent with the spectroscopic data. Laser fluorescence spectroscopy showed success and reliability for direct determination of U(VI) in such biological matrices with the possibility for further improvement.

    Copyright © 2015 American Chemical Society

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    Supporting Information

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    Artificial body fluid preparation; elemental composition of original body fluids; thermodynamic stability constants for aqueous uranyl complexes that are used for speciation modeling in human body fluids; speciation of U(VI) in several artificial and human body fluids; pH dependent TRLFS measurements of U(VI) speciation in several artificial body fluids; luminescence decay curves and lifetimes for U(VI) spectra in the human body fluids under investigation; and time-resolved spectrum of U(VI) in human saliva (specimen SF) This material is available free of charge via the Internet at http://pubs.acs.org.

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    Cited By

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    This article is cited by 21 publications.

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    Chemical Research in Toxicology

    Cite this: Chem. Res. Toxicol. 2015, 28, 2, 238–247
    Click to copy citationCitation copied!
    https://doi.org/10.1021/tx5004084
    Published January 6, 2015
    Copyright © 2015 American Chemical Society
    Request reuse permissions

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