Abstract
The design of solid electrolyte composites for Li-ion batteries integrating polymers and organic ionic plastic crystals (OIPCs) requires an understanding of the synergy between their components to achieve the desired ionic conductivity. Here, we study composites between the OIPC hexamethylguanidinium bis(fluorosulfonyl)imide HMGFSI and polymers functionalised with the comonomer lithium 1-(3-(methacryloyloxy)propylsulfonyl)-1-(trifluoromethylsulfonyl)imide (LiMTFSI). These polymers have different macromolecular structures (i.e., homopolymers, copolymers, linear polymers, or polymer nanoparticles) and concentrations of lithium (Li). Characterisation of the composites by differential scanning calorimetry, X-ray diffraction, solid-state nuclear magnetic resonance spectroscopy, and electrochemical impedance spectroscopy showed that the composite containing large polymer nanoparticles with a low Li concentration had the highest ionic conductivity and structural disorder at low temperatures as well as a higher fraction of ions (i.e., Li+ and FSI−) that become highly dynamic. The role of the polymer nature and Li content in promoting interactions that led to different ion dynamics in the composites was discussed. Understanding the complex interplay between the composite components and the effect on properties such as thermal stability, structure and ion conduction, and dynamics assists in optimizing the overall performance of solid electrolyte composites.
| Original language | English |
|---|---|
| Pages (from-to) | 13447-13463 |
| Number of pages | 17 |
| Journal | Physical Chemistry Chemical Physics |
| Volume | 27 |
| Issue number | 25 |
| DOIs | |
| State | Published - May 26 2025 |
Funding
The Australian Research Council (ARC), through the ARC Centre of Excellence for Electromaterials Science (CE140100012) and the Industry Transformation Training Centre for Future Energy Technologies (storEnergy) IC180100049, is acknowledged for financial support of this work. L. P. has received funding from the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No. 797295. D. M. acknowledges financial support from the EU (IONBIKE 2.0 MSCA-SE), the Eusko Jaurlaritza (GV-IT1525-22) and the MINECO AEI (PID2020-119026GB-I00) is gratefully acknowledged. Synchrotron powder X-ray diffraction experiments were undertaken on the Powder Diffraction beamline proposal 19014 at the Australian Synchrotron, part of ANSTO. The Australian Research Council (ARC), through the ARC Centre of Excellence for Electromaterials Science (CE140100012) and the Industry Transformation Training Centre for Future Energy Technologies (storEnergy) IC180100049, is acknowledged for financial support of this work. L. P. has received funding from the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska–Curie grant agreement No. 797295. D. M. acknowledges financial support from the EU (IONBIKE 2.0 MSCA-SE), the Eusko Jaurlaritza (GV-IT1525-22) and the MINECO AEI (PID2020-119026GB-I00) is gratefully acknowledged. Synchrotron powder X-ray diffraction experiments were undertaken on the Powder Diffraction beamline proposal 19014 at the Australian Synchrotron, part of ANSTO.