The Polymer Society of Korea

Abstract

Zinc dendrites and side reactions limit the cycle life of aqueous Zn-metal batteries (AZMBs). In situ gel polymer electrolytes (GPEs) can mitigate these issues by forming robust interfaces, but conventional GPEs require initiators, crosslinkers, and harsh conditions, often yielding poor Zn²⁺ transport. Here, we report an initiator- and crosslinker-free in situ GPE that spontaneously forms at room temperature in air. Mixing zwitterionic monomers with Zn salt induces self-polymerization, resulting in a flexible, physically crosslinked network. This electrolyte ensures intimate interfacial contact and continuous Zn²⁺ ion conduction. Symmetric Zn cells show excellent cycling (>4100 h) and stable operation at –10 °C, outperforming conventional GPEs. Zn‖VO₂ full cells retain 95.6% capacity after 100 cycles. This sustainable, cost-effective strategy effectively addresses key AZMB challenges.