Data of research paper: Trade-off in Lithium Diffusivity and Transference in High Lithium Concentration Ternary Polymer Ionic Liquids

DOI:10.4121/0bd878cd-0d1d-420e-b424-aad2782cb616.v1
The DOI displayed above is for this specific version of this dataset, which is currently the latest. Newer versions may be published in the future. For a link that will always point to the latest version, please use
DOI: 10.4121/0bd878cd-0d1d-420e-b424-aad2782cb616

Datacite citation style

Weijers, Mark (2025): Data of research paper: Trade-off in Lithium Diffusivity and Transference in High Lithium Concentration Ternary Polymer Ionic Liquids . Version 1. 4TU.ResearchData. dataset. https://doi.org/10.4121/0bd878cd-0d1d-420e-b424-aad2782cb616.v1
Other citation styles (APA, Harvard, MLA, Vancouver, Chicago, IEEE) available at Datacite

Dataset

Data supporting findings of paper https://doi.org/10.1016/j.ssi.2025.116854


Highlights

A local optimum for lithium mobility in ternary IL/PIL/lithium salt is observed.

Lithium diffusion in ternary electrolyte system is analogous to ILE at low to moderate lithium salt concentrations.

A change from neutral pair to free lithium ion conductivity is observed at high lithium salt concentrations.


Abstract

For battery architectures that need a solid ion conductor with good contacting performance and high stability against electrochemical oxidation, polymerized ionic liquids (PIL) pose a valuable class of materials. The low conductivity of the binary PIL/ lithium salt system can be increased using a ternary ionic liquid acting as plasticiser. The conductive mechanism of the ternary system is however not fully understood. This work shows the shift in conduction mechanism for the ternary Li−/[1,3]PYR-/PDADMA-FSI system by increasing the lithium salt concentration and comparing the transfer mechanism to binary ionic liquid (IL) electrolyte analogues using pulsed field gradient (PFG) nuclear magnetic resonance (NMR), NMR relaxometry, Raman spectroscopy and electrochemical techniques. Two conducting regimes were found which show a strong trade-off between conductivity and transference number. In the low lithium salt regime (≤35 wt% LiFSI), cluster diffusion of aggregated lithium is the dominating mechanism leading to low transference numbers (0.04–0.15 at room temperature (RT)). The high salt regime (≥50 wt% LiFSI) shows diffusion through free lithium ion hopping transfer, which has a stronger dependence on temperature and yields higher transference numbers (0.31 at RT). Increasing lithium salt concentration shows an inverse linear correlation with conductivity. The electrochemical characteristics of ternary IL/PIL/lithium salt are shown to be highly tuneable by varying the lithium salt fraction, while it maintains excellent characteristics like processability, stability and mechanical function.

History

  • 2025-04-07 first online, published, posted

Publisher

4TU.ResearchData

Format

Spreadsheet / .xlsx, ASCII / .txt, Origin /.opju, MACCOR / (.digit), Image / .jpeg/.tiff, Verstastudio / .par, Powerpoint / .pptx

Organizations

TU Delft, faculty of Applied Sciences, department of Chemical Engineering

DATA

Files (6)