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With the flourish of flexible and wearable electronics gadgets, the need for flexible power sources has become essential. The growth of this increasingly diverse range of devices boosted the necessity to develop materials for such flexible power sources such as secondary batteries, fuel cells, supercapacitors, sensors, dye-sensitized solar cells, etc. In that context, comprehensives studies on flexible conversion and energy storage devices have been released for other technologies such Li-ion standing out the importance of the research done lately in GPEs (gel polymer electrolytes) for energy conversion and storage. However, flexible zinc batteries have not received the attention they deserve within the flexible batteries field, which are destined to be one of the high rank players in the wearable devices future market. This review presents an extensive overview of the most notable or prominent gel polymeric materials, including biobased polymers, and zinc chemistries as well as its practical or functional implementation in flexible wearable devices. The ultimate aim is to highlight zinc-based batteries as power sources to fill a segment of the world flexible batteries future market.

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Gel Polymer Electrolytes (GPEs) composed by ZnTf2 salt, poly(vinylidene fluoride-co-hexafluoropropylene) (PVdF-HFP), and different ionic liquids are synthesized using n-methyl-2-pyrrolidone (NMP) as solvent. Three different imidazolium-based ionic liquids containing diverse cations and anions have been explored. Structural and electrical properties of the GPEs varying the ZnTf2 concentration are analyzed by ATR-FTIR, DSC, TG, and cyclic voltammetry. Free salt IL-GPEs present distinct behavior because they are influenced by the different IL cations and anions composition. However, inclusion of ZnTf2 salt inside the polymers provide GPEs with very similar characteristics, pointing out that ionic transport properties are principally caused by Zn2+ and triflate movement. Whatever the IL used, the presence of NMP solvent inside the polymer’s matrix turns out to be a key factor for improving the Zn2+ transport inside the GPE due to the interaction between Zn2+ cations and carbonyl groups of the NMP. High values of ionic conductivity, low activation energy values, and good voltammetric reversibility obtained regardless of the ionic liquid used enable these GPEs to be applied in Zn batteries. Capacities of 110–120 mAh·g−1 have been obtained for Zn/IL-GPE/MnO2 batteries discharged at −1 mA·cm−2.