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Linking Solution Structures and Energetics: Thorium Nitrate Complexes.

S Skanthakumar1, Geng Bang Jin1, Jian Lin1

  • 1Chemical Sciences and Engineering Division, Argonne National Laboratory , 9700 S. Cass Avenue, Argonne, Illinois 60439, United States.

The Journal of Physical Chemistry. B
|August 18, 2017
PubMed
Summary
This summary is machine-generated.

Thorium speciation in acidic nitrate solutions was studied using X-ray scattering. Thorium forms bidentate nitrate complexes, influencing solution chemistry and precipitate structure.

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Area of Science:

  • Solution chemistry
  • Inorganic chemistry
  • Materials science

Background:

  • Understanding metal-ion speciation is crucial for predicting solution chemistry and solid precipitate formation.
  • Thorium's behavior in acidic media is relevant to nuclear fuel reprocessing and waste management.

Purpose of the Study:

  • To quantitatively probe thorium correlations with solvent and solute ions in acidic nitrate/perchlorate solutions.
  • To determine how metal-ion speciation impacts solution chemistry and solid precipitate composition/structure.
  • To gain predictive insights into thorium's interactions in aqueous systems.

Main Methods:

  • High-energy X-ray scattering (HEXS) was employed to obtain difference pair-distribution functions (dPDF).
  • Metrical fits of thorium coordination were performed as a function of nitrate concentration.
  • Molecular quantum chemical calculations were used to assess the relative stabilities of solid-state compounds.

Main Results:

  • A homoleptic thorium aqua ion with 10 water molecules in its first coordination shell was identified in perchloric acid.
  • Thorium exclusively forms bidentate nitrate complexes in acidic nitrate solutions.
  • Stability constants for thorium-nitrate complexes were calculated, correlating solution and solid-state structures.

Conclusions:

  • Bidentate nitrate complexation with thorium is consistent across solution and solid-state structures.
  • Accurate descriptions of complexed water are essential for predicting energetics of dissolved ions.
  • This study provides molecular-scale insights into thorium's behavior in aqueous solutions.