A Liquid Crystal Ionomer-Type Electrolyte toward Ordering-Induced Regulation for Highly Reversible Zinc Ion Battery

Novel electrolyte is being pursued toward exploring Zn chemistry in zinc ion batteries. Here, a fluorine-free liquid crystal (LC) ionomer-type zinc electrolyte is presented, achieving simultaneous regulated water activity and long-range ordering of conduction channels and SEI. Distinct from water network or local ordering in current advances, long-range ordering of layered water channels is realized. Via manipulating water activity, conductivities range from ≈0.34 to 15 mS cm⁻¹, and electrochemical window can be tuned from ≈2.3–4.3 V. The Zn|Zn symmetric cell with LC gel exhibits highly reversible Zn stripping/plating at 5 mA cm⁻² and 5 mAh cm⁻² for 800 h, with retained ordering of water channels. The capability of gel for inducing in situ formation of long-range ordered layer SEI associated with alkylbenzene sulfonate anion is uncovered. V₂O₅/Zn cell with the gel shows much improved cycling stability comparing to conventional zinc electrolytes, where the preserved structure of V₂O₅ is associated with the efficiently stabilized Zn anode by the gel. Via long-range ordering-induced regulation on ion transport, electrochemical stability, and interfacial reaction, the development of LC electrolyte provides a pathway toward advancing aqueous rechargeable batteries.