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Accelerating Neodymium's First-Shell Dynamics toward Improved Metal Recovery.
Garima S Dobhal1, Cristina Pozo-Gonzalo2,3, Tiffany R Walsh
1Institute for Frontier Materials, Deakin University, Geelong, Victoria 3216, Australia.
The Journal of Physical Chemistry. B
|October 20, 2025
Summary
Trace water and specific phosphonium ionic liquids (ILs) enhance neodymium (Nd) electrodeposition by limiting Nd hydration and increasing ion mobility. This facilitates easier Nd metal recovery from secondary sources.
Area of Science:
- Materials Science
- Electrochemistry
- Computational Chemistry
Background:
- Growing demand for rare earth elements (REEs) necessitates efficient reclamation methods.
- Neodymium (Nd) electrodeposition using phosphonium ionic liquids (ILs) shows promise but lacks detailed mechanistic understanding.
- The role of water in Nd electrodeposition within ILs is not fully elucidated.
Purpose of the Study:
- To investigate the molecular-level mechanisms of neodymium (Nd) electrodeposition in phosphonium ionic liquids (ILs).
- To elucidate the influence of trace water concentrations on Nd ion coordination and solvation dynamics.
- To provide insights for optimizing REE recovery processes.
Main Methods:
- Force-field molecular dynamics (MD) simulations of neodymium salts in phosphonium ILs ([P666,14][TFSI] and [P1,444][TFSI]) with trace water.
- Ab initio MD simulations to validate coordination structures.
- Analysis of Nd3+ coordination, water participation, anion denticity, and solvation sphere dynamics.
Main Results:
- Identified dominant coordination structures of Nd3+ in the studied ILs.
- Observed increased participation of water in Nd3+ structures and broadened TFSI- denticity upon water addition.
- Demonstrated accelerated first-shell anion dynamics and limited Nd ion hydration with trace water and shorter alkyl chains.
Conclusions:
- Trace water, in conjunction with specific phosphonium ILs, favorably influences Nd electrodeposition conditions.
- Limited Nd hydration and enhanced solvation sphere dynamism are key factors for improved Nd deposition.
- Findings offer molecular-scale guidance for enhancing REE electrodeposition and recovery.
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