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A first phosphine oxide-based extractant with high Am/Cm selectivity.

P I Matveev1, N E Borisova, N G Andreadi

  • 1Department of Chemistry M.V. Lomonosov Moscow State University 1/3 Leninskie Gory, 119991 Moscow, Russia. Borisova.nataliya@gmail.com.

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|January 30, 2019
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Summary
This summary is machine-generated.

A novel phosphine oxide ligand selectively separates americium and curium (Am-Cm) and americium and europium (Am-Eu) in nitric acid. Selectivity arises from entropy-driven complexation and ligand cavity size differences, confirmed by DFT modeling.

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Area of Science:

  • Radiochemistry
  • Coordination Chemistry
  • Materials Science

Background:

  • Separation of trivalent actinides like Americium (Am), Curium (Cm), and Europium (Eu) is crucial for nuclear fuel reprocessing and waste management.
  • Developing selective ligands for these chemically similar elements remains a significant challenge in radiochemistry.

Purpose of the Study:

  • To synthesize and evaluate a new phosphine oxide ligand for selective separation of Am-Cm and Am-Eu pairs.
  • To elucidate the thermodynamic and structural factors governing the observed selectivity.

Main Methods:

  • Solvent extraction experiments were conducted in 0.1-3 M nitric acid to determine separation factors (SF).
  • Thermodynamic measurements (e.g., enthalpy and entropy changes) were performed to understand the driving forces for separation.
  • Density Functional Theory (DFT) modeling was employed to investigate the coordination complexes and metal-ligand interactions.

Main Results:

  • The phosphine oxide ligand exhibited high selectivity for the Am-Cm pair (SF = 2.9-3.5) and the Am-Eu pair (SF = 7.3-8.5).
  • Thermodynamic analysis indicated that the entropy factor predominantly contributes to the observed selectivity.
  • DFT calculations revealed differences in metal-nitrogen bond distances, with Curium (Cm) having larger distances than Americium (Am), leading to deeper insertion into the ligand's pseudo-cavity.

Conclusions:

  • The new phosphine oxide ligand shows promising selectivity for separating Am-Cm and Am-Eu, important for nuclear applications.
  • The selectivity is primarily governed by entropic contributions and specific ligand-metal interactions dictated by ion size.
  • DFT modeling provides valuable insights into the molecular-level mechanisms responsible for selective metal ion extraction.