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Speciation and Bioavailability Measurements of Environmental Plutonium Using Diffusion in Thin Films
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Trace Uranium Partitioning in a Multiphase Nano-FeOOH System.

Martin E McBriarty1, Jennifer A Soltis1, Sebastien Kerisit1

  • 1Physical Sciences Division and ‡Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory , Richland, Washington 99352, United States.

Environmental Science & Technology
|April 14, 2017
PubMed
Summary

Extended X-ray absorption fine structure (EXAFS) analysis, enhanced by ab initio molecular dynamics (AIMD), precisely characterizes trace uranium in iron minerals. This method overcomes limitations in analyzing impurities in complex geological systems.

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Area of Science:

  • Geochemistry
  • Environmental Science
  • Materials Science
  • Spectroscopy

Background:

  • Characterizing trace elements in minerals is crucial for understanding contaminant interactions.
  • Traditional extended X-ray absorption fine structure (EXAFS) analysis faces limitations with trace impurities in heterogeneous systems.
  • Geochemical sequestration of actinides, like uranium, in iron (oxyhydr)oxides is environmentally significant.

Purpose of the Study:

  • To investigate the immobilization of trace uranium in nanophase iron (oxyhydr)oxides using a novel EXAFS analysis method.
  • To model the geochemical sequestration of radiotoxic actinides.
  • To overcome limitations in traditional EXAFS fitting for complex multiphase mineral systems.

Main Methods:

  • Employing ab initio molecular dynamics (AIMD)-informed extended X-ray absorption fine structure (EXAFS) analysis.
  • Investigating the reductive transformation of ferrihydrite in the presence of uranyl ions.
  • Utilizing atomically resolved transmission electron microscopy for validation.

Main Results:

  • Trace uranium preferentially incorporated into goethite (α-FeOOH) over lepidocrocite (γ-FeOOH) during ferrihydrite transformation, contrary to reaction conditions.
  • AIMD-informed EXAFS analysis successfully characterized uranium's local bonding environment and oxidation states.
  • This advanced method overcomes statistical limitations of traditional EXAFS fitting.

Conclusions:

  • AIMD-informed EXAFS analysis provides a powerful tool for detailed characterization of polyvalent impurities in complex mineral systems.
  • Understanding uranium immobilization in iron minerals is key for managing radiotoxic actinide contamination.
  • The study demonstrates a significant advancement in spectroscopic analysis for environmental geochemistry.