In order to improve the multifunctionality of polymer composites for advanced applications a novel tri-composite material is presented based on the inclusion of MFI zeolite and the ionic liquid (IL) 1-butyl-3-methylimidazolium thiocyanate ([BMIM][SCN]) in an electroactive poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) polymer matrix. Tri-composites were produced by solvent casting with a relative overall filler content up to 40 wt.%. A compact film morphology is obtained, and the polymer degradation temperature and degree of crystallinity are independent on the filler content and type. On the other hand, the polymer crystalline phase depends on the presence of the IL but is independent of its content. Regarding the mechanical properties, it is observed that the IL has a plasticizing effect with a significant contribution to the reduction of the Young's modulus from 151 MPa for the pristine polymer to 92 MPa for the 30 wt.%/10 wt.% IL/MFI content sample. A high ionic conductivity value at room temperature of 3.9 × 10−5 S.cm−1 was obtained for the tri-composite with the highest IL content (30 wt.%/10 wt.% IL/MFI). The tri-composite system was studied as solid polymer electrolyte (SPE) for battery and bending actuator applications, demonstrating the multifunctionality of the material. The sample with the best cycling performance was observed for the highest MFI content (10 wt.%/30 wt.% IL/MFI) with a discharge capacity value of 110 mAh.g−1 and maintaining almost 80% of its initial capacity after 30 cycles at the C/10 rate. Regarding to the bending performance, the best bending actuation was detected for highest IL content (30 wt.%/10 wt.% IL/MFI), related to the ionic conductivity of the sample. Thus, it is demonstrated that the new tri-composite system, due to its tunable characteristics as a function of the relative IL and zeolite contents, is suitable for a next generation of multifunctional polymer composite materials for advanced applications.
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