Ultrastable Zinc Anodes Enabled by Anti-Dehydration Ionic Liquid Polymer Electrolyte for Aqueous Zn Batteries

Abstract

The side reaction and dendrite of a zinc anode in an aqueous electrolyte represent a huge obstacle for the development of rechargeable aqueous Zn batteries. An electrolyte with confined water is recognized to fundamentally stabilize the zinc anode. This work proposes acetamide/zinc perchlorate hexahydrate (AA/ZPH) ionic liquid (IL)-polyacrylamide (PAM) polymer electrolytes, here defined as IL-PAM. The novel Zn²⁺-conducting IL is able to accommodate trace water and can achieve both high conductivity (15.02 mS cm^-1) and alleviation of side reactions (>90% reduction). Cross-linked PAM acts as the three-dimensional framework to suppress dendrites and obtain flexibility. As a result, the Zn anode with IL-PAM can cycle stably over 2000 h with a record highest cumulative capacity of 3000 mAh cm^-2 and well-preserved morphology. Based on IL-PAM, the flexible LFP|Zn hybrid batteries can be successfully assembled and operate normally in series and parallel conditions. Moreover, the low volatility of IL and binding forces exerted by the PAM network endues IL-PAM with an anti-dehydration property. In a 50 °C unsealed environment, the weight loss of IL-PAM is about two-fifths of PAM hydrogel and an aqueous electrolyte, and the corresponding hybrid battery with IL-PAM can also prolong a 4 times longer lifespan.