Evaluating the Relationships between Molecular Interactions and Polymer Chain Dynamics across Phase Boundaries in Solid Polymer Electrolytes
Bibliographic record
Abstract
Fundamental studies on the structure–property relationships of solid polymer electrolytes (SPE) are required to further our understanding of the parameters impacting their ionic conductivity. This work investigates the interplay between molecular interactions and polymer chain dynamics of an electrolyte model system based on poly(ε-caprolactone)(PCL):LiTFSI across structural phase boundaries with salt concentrations varying from 0 to 65 wt %. To evaluate the thermodynamic behavior of PCL:LiTFSI and enable a clear overview of the phase environment of the system through the concentration range, construction of the phase diagram of PCL:LiTFSI is realized. Infrared (IR) spectroscopy experiments allowed probing of the polymer:salt molecular interactions. Spectroscopic identification of salt saturation at 27 wt % which corresponds to the beginning of a totally amorphous phase hints at the ideal concentration range to optimize ionic transport. Coordination thermodynamic parameters were evaluated through variable-temperature Fourier transformed infrared spectroscopy (FT-IR) experiments. Relationships between the free energy of coordination between the lithium ion and PCL and phase boundaries, as well as relationships between the change in coordination entropy and conductivity activation energy, were elucidated. Polymer chain dynamics was evaluated through oscillatory rheology. Relationships between the polymer terminal relaxation times and ionic conductivities identify an abnormal plasticization behavior at phase inversion (24 wt %). Finally, an integrated interpretation of molecular interactions, polymer chain dynamics, and phase environment of the PCL:LiTFSI and their relationship with ionic behavior is realized, highlighting the importance of each of these parameters.
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How this classification was reachedexpand
Full frame machine prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.
Distilled classifier scores by category (both heads)
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.001 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.001 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.001 | 0.000 |
Machine scores (provisional)
The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.
Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from itClassification
machine, unvalidatedMachine predicted; a candidate call from one source (direct Gemma or distilled Codex), not a consensus.
How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".