Electrolyte design principles for developing quasi-solid-state rechargeable halide-ion batteries.

Rechargeable halide-ion batteries (HIBs) are good candidates for large-scale due to their appealing energy density, low cost, and dendrite-free features. However, state-of-the-art electrolytes limit the HIBs' performance and cycle life. Here, via experimental measurements and modelling approach, we demonstrate that the dissolutions in the electrolyte of transition metal and elemental halogen from the positive electrode and discharge products from the negative electrode cause the HIBs failure. To circumvent these issues, we propose the combination of fluorinated low-polarity solvents with a gelation treatment to prevent dissolutions at the interphase, thus, improving the HIBs' performance. Using this approach, we develop a quasi-solid-state Cl-ion-conducting gel polymer electrolyte. This electrolyte is tested in a single-layer pouch cell configuration with an iron oxychloride-based positive electrode and a lithium metal negative electrode at 25 °C and 125 mA g. The pouch delivers an initial discharge capacity of 210 mAh g and a discharge capacity retention of almost 80% after 100 cycles. We also report assembly and testing of fluoride-ion and bromide-ion cells using quasi-solid-state halide-ion-conducting gel polymer electrolyte.