Gel Electrolytes With Regulated Ion Channels and Stabilized Zn Interfaces Enable Durable Flexible Zinc-Air Batteries

Flexible zinc-air batteries require gel electrolytes that simultaneously reconcile rapid ion transport, mechanical robustness, and stable Zn interfacial chemistry. Here, a trehalose-regulated L-PAT/PVA gel electrolyte is developed through hierarchical bulk-interface regulation. Hofmeister-induced PVA crystallization provides a mechanically reinforced framework, while trehalose-mediated competitive hydrogen bonding moderates excessive chain association, reconstructs the local hydration environment, and preserves continuous low-tortuosity ion-transport pathways. Simultaneously, sulfonate groups from L-carrageenan regulate the Zn/electrolyte interfacial microenvironment, homogenize local ionic flux, and direct Zn electrocrystallization toward the (002)-preferred orientation. DRT analysis further reveals suppressed slow-polarization contributions and more stable interfacial kinetics during cycling. The optimized electrolyte exhibits a tensile strength of 609 kPa, a fracture strain above 1200%, and an ionic conductivity of 154.5 mS cm^-1. The resulting flexible Zn-air battery delivers 77 mW cm^-2 peak power density, ≈200 mAh cm^-3 volumetric capacity, and stable cycling for 250 h at 1 mA cm^-2, while maintaining reliable operation from -15 C to 55°C and under mechanical deformation.