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Metal ions can be separated from one another by complexation with organic ligands–the chelating agent– to form uncharged chelates. Here, the chelating agent must contain hydrophobic groups and behave as a weak acid, losing a proton to bind with the metal. Since most organic ligands used in this process are insoluble or undergo oxidation in the aqueous phase, the chelating agent is initially added to the organic phase and extracted into the aqueous phase. The metal-ligand complex is...
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Spectroscopic Study into Lanthanide Speciation in Deep Eutectic Solvents.

James T M Amphlett1, Yunu Lee1, Wonseok Yang1

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Deep eutectic solvents offer green alternatives for nuclear fuel recycling. Rare-earth element speciation in these solvents depends heavily on the hydrogen-bond donor, influencing their coordination and behavior.

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Area of Science:

  • Green Chemistry
  • Nuclear Fuel Cycle
  • Materials Science

Background:

  • Deep eutectic solvents (DES) are emerging as environmentally friendly alternatives for critical material recycling.
  • Understanding metal behavior in DES is crucial for optimizing recycling processes.
  • Limited knowledge exists on rare-earth element (REE) speciation within choline chloride-based DES.

Purpose of the Study:

  • To investigate the fundamental chemistry and speciation of rare-earth elements in choline chloride-based deep eutectic solvents.
  • To elucidate the influence of different hydrogen-bond donors on REE coordination and behavior.
  • To establish generalized coordination environments for REEs in various DES systems.

Main Methods:

  • Multi-technique spectroscopic analysis, including EXAFS, UV/vis absorption, and luminescence spectroscopy.
  • Systematic variation of hydrogen-bond donors (ethylene glycol, urea, lactic acid) in choline chloride-based DES.
  • Characterization of lanthanide (Ln³⁺) coordination environments and interactions.

Main Results:

  • REE speciation is highly sensitive to the choice of hydrogen-bond donor.
  • EXAFS data revealed specific coordination with ethylene glycol, urea, and lactic acid, with generalized coordination numbers [LnL₄₋₅], [LnL₇₋₁₀], and [LnL₅₋₆], respectively.
  • UV/vis and luminescence studies confirmed varying interactions and coordination geometries, indicating that Ln-Cl interactions are not dominant.

Conclusions:

  • The hydrogen-bond donor dictates the coordination environment and behavior of rare-earth elements in choline chloride-based DES.
  • Specific coordination geometries for Eu³⁺ were assigned based on the combined spectroscopic data.
  • These findings provide critical insights for the application of DES in nuclear fuel and critical material recycling.