Transport anomalies emerging from strong correlation in ionic liquid electrolytes
| Autor: | Jake Christensen, Boris Kozinsky, Nicola Molinari, Craig Nathan P, Jonathan P. Mailoa |
|---|---|
| Rok vydání: | 2019 |
| Předmět: |
Battery (electricity)
Materials science Renewable Energy Sustainability and the Environment Energy Engineering and Power Technology Ionic bonding 02 engineering and technology Ideal solution Negative transference Electrolyte Conductivity 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences 0104 chemical sciences Molecular dynamics chemistry.chemical_compound chemistry Chemical physics Ionic liquid Electrical and Electronic Engineering Physical and Theoretical Chemistry 0210 nano-technology |
| Zdroj: | Journal of Power Sources. 428:27-36 |
| ISSN: | 0378-7753 |
| Popis: | Strong ionic interactions in concentrated ionic liquids is shown to result in significant correlations and deviations from ideal solution behavior. We use rigorous concentrated solution theory coupled with molecular dynamics simulations to compute and explain the unusual dependence of transport properties on cation concentration in the Na + - Pyr 13 + - FSI − ionic liquid electrolyte. When accounting for intra- and inter-species correlation, beyond the commonly used uncorrelated Nernst-Einstein equation, an anomalously low and even negative transference number emerges for x NaFSI lower than 0.2. With increasing concentration the transference number monotonically increases, approaching unity, while the total conductivity decreases as the system transitions to a state resembling a single-ion solid-state electrolyte. The degree of spatial ionic association is explored further by employing unsupervised single-linkage clustering algorithm. We emphasize that strong ion-ion coupling in the electrolyte significantly impacts the trade-off between key electrolyte transport properties, and consequently governs the power density of the battery. |
| Databáze: | OpenAIRE |
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