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Methods of Ex Situ and In Situ Investigations of Structural Transformations: The Case of Crystallization of Metallic Glasses
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Disordered Crystal Structure and Anomalously High Solubility of Radium Carbonate.

Artem V Matyskin1, Burçak Ebin1, Stefan Allard1

  • 1Nuclear Chemistry and Industrial Materials Recycling Group, Energy and Materials Division, Department of Chemistry and Chemical Engineering, Chalmers University of Technology, Kemivägen 4, SE-41296 Gothenburg, Sweden.

Inorganic Chemistry
|July 21, 2023
PubMed
Summary
This summary is machine-generated.

Radium-226 carbonate was synthesized and characterized. Its higher solubility compared to witherite supports the disordered nature of the Ra-rich phase, applicable to pure RaCO3.

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Area of Science:

  • Radiochemistry
  • Solid-state chemistry
  • Geochemistry

Background:

  • Radium-226 (²²⁶Ra) is a key radioisotope in nuclear waste.
  • Understanding the solubility and structure of radium compounds is crucial for safe disposal.
  • Radium carbonate (RaCO₃) is expected to be a major solid phase in certain waste scenarios.

Purpose of the Study:

  • To synthesize and characterize radium-226 carbonate (RaCO₃).
  • To determine the solubility of RaCO₃ under varying conditions.
  • To provide structural insights into radium carbonate phases.

Main Methods:

  • Synthesis of radium-barium sulfate (²²⁶Ra₀.₇₆Ba₀.₂₄SO₄) at room temperature.
  • Characterization using X-ray powder diffraction (XRPD) and extended X-ray absorption fine structure (EXAFS).
  • Solubility studies conducted under- and oversaturation at 25.1 °C with varying ionic strengths.

Main Results:

  • Fractional crystallization yielded two phases: a major Ra-rich phase (Ra(Ba)CO₃) and a minor Ba-rich phase (Ba(Ra)CO₃).
  • The major Ra(Ba)CO₃ phase exhibits a disordered carbonate oxygen structure, confirmed by direct-space *ab initio* modeling.
  • The solubility product (log₁₀ *K*sp⁰) of Ra(Ba)CO₃ was determined to be -7.5(1), significantly higher than witherite (-8.56).
  • EXAFS data indicated radium is coordinated by nine oxygens with a mean Ra-O bond distance of 2.885(3) Å, yielding an ionic radius of 1.545(6) Å for Ra²⁺.

Conclusions:

  • The synthesized Ra-rich phase (Ra(Ba)CO₃) is significantly more soluble than witherite, consistent with its disordered structure.
  • The findings for Ra(Ba)CO₃ are applicable to pure RaCO₃, indicating higher mobility than previously assumed.
  • The determined ionic radius of Ra²⁺ and structural disorder are key factors influencing its geochemical behavior.