An Ionic Liquid Supramolecular Gel Electrolyte with Unique Wide Operating Temperature Range Properties for Zinc-Ion Batteries

Zinc-ion batteries are promising candidates for large-scale energy storage. The side reactions of the hydrogen evolution reaction (HER) and zinc dendrite growth are major challenges for developing high-performance zinc-ion batteries. In this paper, a supramolecular gel electrolyte (BLO-ILZE) was self-assembled in an ionic liquid (EMIMBF4) with zinc tetrafluoroborate (Zn(BF4)2) on the separator in situ to obtain a gel electrolyte used in zinc-ion batteries. BLO-ILZE is demonstrated to significantly enhance conductivity over a broad temperature range between −70 and 100 °C. Interestingly, through testing and fitting, it is found that the supramolecular gel electrolyte satisfies the liquid state law over a wide temperature range, and even achieves high conductivity (2.12 mS cm−1) at −40 °C. It is equivalent to the conductivity of aqueous zinc-ion batteries (ZnSO4/H2O) at −10 °C, which is 2.33 mS cm−1. Moreover, the supramolecular gel electrolyte can effectively inhibit the HER, thus exhibiting a longer lifetime in Zn/Zn cells for 3470 h at 1 mA cm−2compared to the aqueous zinc-ion batteries with the Zn(BF4)2aqueous electrolyte (400 h at 1 mA cm−2). The assembled V2O5/BLO-ILZE/Zn full cells also showed cycling performance, with 5000 cycles at 0.5 mA g−1at room temperature, a capacity of 98%, and a coulombic efficiency of about 100%.