The Polymer Society of Korea

Abstract

Aqueous zinc metal batteries (AZMBs) suffer from dendrite formation and side reactions at the Zn anode, limiting cycle life and stability. In situ gel polymer electrolytes (GPEs) can mitigate these issues by forming robust electrode–electrolyte interfaces, but conventional GPEs require initiators and crosslinkers that generate byproducts and hinder Zn²⁺ conduction. Here, an initiator- and crosslinker-free GPE is developed that spontaneously polymerizes at room temperature in air via a Zinc salt-induced mechanism. Simply mixing zwitterionic monomer with Zinc salt induces spontaneous gelation, forming a flexible polymer network with tight electrode contact and continuous Zn²⁺ conduction pathways. Zn cells exhibit over 4100 h of stable cycling and retain 95.6% capacity after 100 cycles in Zn‖VO₂ full cells. This sustainable, scalable approach offers a practical solution to Zn-anode challenges and enables eco-friendly AZMBs for next-generation energy storage.