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Polymer electrolytes provide a safe solution for all-solid-state high energy density batteries. Materials that meet the simultaneous requirement of high ionic conductivity and high transference number remain a challenge, in particular for new battery chemistries beyond Lithium such as Na, K and Mg. Herein, we demonstrate the versatility of a polymeric ionic liquid (PolyIL) as a solid-state solvent to achieve this goal for both Na and K. Using molecular simulations, we predict and elucidate fast metal ion transport in PolyILs through a structural diffusion mechanism in a polymer-in-salt environment, facilitating a high transference number. Experimental validation of these computational designed Na and K polymer electrolytes gives high ionic conductivities of 1.010-3 S cm-1 at 80 oC and an exceptional Na+ transference number of ~0.57. Electrochemical cycling of a sodium anode also demonstrates an ultra-low overpotential of 40 mV and stable long term performance of more than 100 hours in a symmetric cell. PolyIL-based polymer-in-salt strategies for novel solid-state electrolytes thus offer a promising route to design high performance next generation sustainable battery chemistries.
Keywords
batteries, engery devices, polymer electrolytes
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This preprint is under consideration at a Nature Portfolio Journal. A preprint is a preliminary version of a manuscript that has not completed peer review at a journal. Research Square does not conduct peer review prior to posting preprints. The posting of a preprint on this server should not be interpreted as an endorsement of its validity or suitability for dissemination as established information or for guiding clinical practice.
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Article
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Complete author information
Appropriate declaration statements
Potential risks to human health
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CURRENT STATUS: Under Review
Version 1
Posted 25 May, 2021
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License:
This work is licensed under a CC BY 4.0 License. Read Full License
Polymer electrolytes provide a safe solution for all-solid-state high energy density batteries. Materials that meet the simultaneous requirement of high ionic conductivity and high transference number remain a challenge, in particular for new battery chemistries beyond Lithium such as Na, K and Mg. Herein, we demonstrate the versatility of a polymeric ionic liquid (PolyIL) as a solid-state solvent to achieve this goal for both Na and K. Using molecular simulations, we predict and elucidate fast metal ion transport in PolyILs through a structural diffusion mechanism in a polymer-in-salt environment, facilitating a high transference number. Experimental validation of these computational designed Na and K polymer electrolytes gives high ionic conductivities of 1.010-3 S cm-1 at 80 oC and an exceptional Na+ transference number of ~0.57. Electrochemical cycling of a sodium anode also demonstrates an ultra-low overpotential of 40 mV and stable long term performance of more than 100 hours in a symmetric cell. PolyIL-based polymer-in-salt strategies for novel solid-state electrolytes thus offer a promising route to design high performance next generation sustainable battery chemistries.
Figure 1
Figure 2
Figure 3
Figure 4
There is NO Competing Interest.
This is a list of supplementary files associated with this preprint. Click to download.
- SupplementaryInformation.docx
supplementary information
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