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7548792 
Journal Article 
Gel–Polymer Electrolytes Based on Poly(Ionic Liquid)/Ionic Liquid Networks 
Sen, S; Goodwin, SE; Barbará, PV; Rance, GA; Wales, D; Cameron, JM; Sans, V; Mamlouk, M; Scott, K; Walsh, DA; , 
2020 
3 
1 
200-208 
WOS:000609249200022 
The use of electrically charged, polymerized ionic liquids (polylLs) offers opportunities for the development of gel-polymer electrolytes (GPEs), but the rational design of such systems is in its infancy. In this work, we compare the properties of polyIL/IL GPEs based on 1-butyl-3-(4-vinylbenzyl)imidazolium bis(trifluromethanesulfonyl)imide containing trapped ammonium-based protic ionic liquids (ILs) with an analogous series based on the electrically neutral host polymer 1-(4-vinylbenzyl)imidazole. The materials are synthesized by photo-polymerizing ionic and neutral monomers in the presence of diethylmethylammonium trifluoromethanesulfonate, [dema] [TfO], diethylmethylammonium trifluoroacetate, [dema][TFAc], and diethylmethylammonium bis[trifluoromethanesulfonyl]imide, [dema] [Tf2N], respectively. The resulting materials are characterized using electron microscopy, infrared spectroscopy, thermal analysis, Raman spectroscopy, and AC-impedance analysis. Spectroscopic analysis confirms that the ILs are distributed throughout the polymers, unless the GPE also contains poly(diallyldimethylammonium) bis[trifluoromethanesulfonyl] imide, when separation of the components occurs. The polyIL/IL GPEs are more electrochemically and thermally stable, and up to six times more conductive, than the materials based on the neutral host. As a proof-of-concept demonstration, we show that polyIL/IL gels can be 3D printed using readily available 3D-printing hardware.