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Interlink between solubility, structure, surface and thermodynamics in the ThO2(s, hyd)-H2O(l) system.

Christian Kiefer1, Thomas Neill1,2, Nese Cevirim-Papaioannou1

  • 1Institute for Nuclear Waste Disposal, Karlsruhe Institute of Technology, Karlsruhe, Germany.

Frontiers in Chemistry
|December 2, 2022
PubMed
Summary

Aging amorphous thorium dioxide (ThO2(am, hyd)) at 80°C increases particle size and crystallinity. Solubility decreases with aging, suggesting surface control, impacting thermodynamic properties of thorium dioxide solid phases.

Keywords:
solubilitystructuresurfacetemperaturethermodynamicsthorium

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Area of Science:

  • Geochemistry
  • Materials Science
  • Radiochemistry

Background:

  • Thorium dioxide (ThO2) is a key material in nuclear energy and research.
  • Understanding the aging behavior of amorphous thorium dioxide (ThO2(am, hyd)) is crucial for predicting its long-term stability and environmental impact.
  • The transformation of amorphous to crystalline phases influences solubility and thermodynamic properties.

Purpose of the Study:

  • To investigate the impact of temperature on the aging of freshly precipitated ThO2(am, hyd).
  • To characterize the structural and chemical changes in aged ThO2 solid phases.
  • To determine the solubility and thermodynamic properties of aged ThO2 solid phases and their relation to structure and surface properties.

Main Methods:

  • Undersaturation solubility experiments at 22°C.
  • Solid phase characterization using X-ray Diffraction (XRD), Extended X-ray Absorption Fine Structure (EXAFS), Thermogravimetric Differential Thermal Analysis (TG-DTA), and X-ray Photoelectron Spectroscopy (XPS).

Main Results:

  • Aging ThO2(am, hyd) at 80°C significantly increases particle size and crystallinity.
  • Aging reduces hydration water and hydroxide groups in the amorphous Th(IV) hydrous oxide.
  • Aged solid phases exhibit decreased solubility at 22°C, influenced by aging time and pH, suggesting surface-controlled dissolution.
  • Thermodynamic properties (log *K°s,0, ΔfG°m) were derived and discussed in relation to particle size.

Conclusions:

  • Aging transforms amorphous hydrous/hydroxide thorium dioxide into more stable crystalline oxides.
  • The solubility of ThO2(s, hyd) is controlled by its outermost surface, which is not fully characterized by the methods used.
  • The study provides insights into the interplay between solubility, structure, surface chemistry, and thermodynamics in the ThO2(s, hyd)-H2O(l) system.