Double Network Gel Electrolyte with High Ionic Conductivity and Mechanical Strength for Zinc-Ion Batteries

Gel electrolytes hold promise for stabilizing zinc-ion batteries (ZIBs), but achieving both high ionic conductivity and strong mechanical properties remains challenging. This work presents a double network gel electrolyte based on poly(<i>N</i>-hydroxymethyl acrylamide) (PNMA) and sodium alginate (SA), overcoming this trade-off. The PNMA network provides mechanical strength and water retention, while the SA network facilitates rapid zinc-ion (Zn²⁺) diffusion through tailored solvation. This double network gel exhibits a tensile strength of up to 838 kPa, significantly higher than previous reports. The SA network provides ion channels for rapid transport of hydrated Zn²⁺, enhancing the ionic conductivity to a ground-breaking 33.1 mS cm^-1. This value is even higher than the liquid electrolytes. The growth of Zn dendrites is also suppressed due to the mechanical constraint and rapid ion conduction. In symmetrical cells, the PNMA/SA gel demonstrates exceptional cycling stability (>2000 h). Characterizations show this is because of reduced free water amount, hindering cathode material dissolution. The full cells with sodium vanadate cathode manifest a high capacity (364.8 mA h g^-1 at 0.5 A g^-1) and excellent capacity retention (83% after 2500 cycles at 10 A g^-1). This double network design offers a way to achieve high-performance and stable ZIBs.