Journal
JOURNAL OF MATERIALS CHEMISTRY A
Volume 5, Issue 45, Pages 23844-23852Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c7ta08233a
Keywords
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Funding
- Australia-India Strategic Research Fund (AISRF)
- ARC [FL110100013, FL120100019]
- European Research Council through Starting Grant Innovative Polymers for Energy Storage (iPes) [306250]
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Polymerized ionic liquids or poly(ionic liquids) (polyILs) have been considered as promising hosts for fabrication of gel polymer electrolytes (GPEs) containing ionic liquids. In this work, a novel GPE based on a polyIL, poly(diallyldimethylammonium) bis(trifluoromethanesulfonyl) imide (PDADMA TFSI), and a high lithium-concentration phosphonium ionic liquid, trimethyl(isobutyl) phosphonium bis(fluorosulfonyl) imide (P111i4FSI), is prepared. The composition-dependent behaviour of the GPEs is investigated by differential scanning calorimetry (DSC), electrochemical impedance spectroscopy (EIS) and solid-state nuclear magnetic resonance (solid-state NMR). The effects of Al2O3 nano-particles on the polymer electrolyte properties are also discussed. It is shown that the introduction of high lithium-concentration ionic liquids into the polyIL can effectively decrease the glass transition temperature (T-g) of the resulting GPE, leading to improved ion dynamics and higher ionic conductivity. The Al2O3 nano-particles effectively enhanced the mechanical stability of the GPEs. Most importantly, although adding PDADMA TFSI to the ionic liquids decreases the diffusion coefficient of both Li+ and anions, a greater decrease in the anion diffusion is observed, resulting in a higher Li+ transport number (as evaluated by NMR) than that seen in the original ILs. Finally, a highly conductive free-standing GPE membrane is fabricated, and extremely stable lithium symmetrical cell performance is demonstrated.
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