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Local structure and charge distribution in the UO(2)-U(4)O(9) system.

Steven D Conradson1, Dario Manara, Franck Wastin

  • 1Materials Science and Technology Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87544, USA. conradson@lanl.gov

Inorganic Chemistry
|October 27, 2004
PubMed
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X-ray absorption fine structure analysis of uranium dioxide (UO(2+x)) shows oxygen atoms form oxo groups, creating clusters. This differs from prior models and highlights unique UO(2+x) characteristics compared to plutonium dioxide (PuO(2+x)).

Area of Science:

  • Materials Science
  • Solid-State Chemistry
  • Nuclear Materials

Background:

  • Uranium dioxide (UO(2+x)) is a key nuclear material.
  • Previous models of UO(2+x) structure, based on neutron diffraction, proposed long U-O bonds and high coordination numbers.
  • Understanding the precise structure of UO(2+x) is crucial for nuclear fuel performance and waste management.

Purpose of the Study:

  • To elucidate the local atomic structure of UO(2+x) for x = 0-0.20.
  • To investigate the incorporation sites and bonding of adventitious oxygen atoms.
  • To compare the structural findings with previous models and related actinide oxides like PuO(2+x).

Main Methods:

  • X-ray absorption fine structure (XAFS) spectroscopy was used to analyze UO(2+x) samples.

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  • Spectra were collected for UO(2+x) with varying oxygen content (x = 0-0.20).
  • Analysis focused on determining U-O and U-U bond distances and coordination environments.

    • Main Results:

    • Adventitious oxygen atoms are incorporated as oxo groups (U-O distance of 1.74 Å), likely involving U(VI) species.
    • These oxo groups form clusters, leaving the primary UO(2) structure largely intact.
    • The U sublattice exhibits both ordered and disordered (glassy) regions, with distinct U-U distances.
    • Results contrast with neutron diffraction models, showing shorter U-oxo distances and no evidence of water coordination, unlike PuO(2+x).

    Conclusions:

    • The local structure of UO(2+x) is characterized by clustered oxo groups, challenging previous models.
    • UO(2+x) exhibits unique structural features compared to PuO(2+x), particularly regarding oxygen incorporation and hydration.
    • XAFS spectroscopy provides critical insights into the complex structure of non-stoichiometric uranium oxides.