Polysaccharide hydrogel electrolytes with robust interfacial contact to electrodes for quasi-solid state flexible aqueous zinc ion batteries with efficient suppressing of dendrite growth

Abstract

Flexible aqueous zinc-ion batteries (AZIBs) require high conductive and adhesive hydrogel electrolytes. However, high adhesion tends to hinder ion conduction rate. Herein, we designed a water/glycerol binary solvent coordinating the hydrophilic polymers to reconstruct the water molecules' environment in the hydrogel. As a consequence, the interface adhesion strength between Zn and the hydrogel reached 3.0 kPa and the ionic conductivity was up to 16.8 mS cm^-1. In addition, inspired by the slurry electrode preparation method, we developed a simple blade coating technique using a non-Newtonian polysaccharide liquid solution to construct an ultra-thin hydrogel electrolyte in situ on the cathode. The thickness of the obtained hydrogel reached 70 μm, and the ultrathin flexible AZIBs were easily constructed by pasting a Zn anode directly on the adhesive hydrogel, showing the potential of flexible AZIBs scalable assembly. In addition, the Zn//Zn symmetrical cells with the hydrogel electrolyte provided stable cycling performance for over 400 h at 0.1 mA cm^-2 with suppressed dendrite growth. The assembled Zn//Polyaniline battery and Zn//V₂O₅ battery also exhibited excellent capacity retention after cycles. This work has realized the hydrogel electrolyte with high adhesion and conductivity, which has good adaptability to metal electrodes and opened up a new practical way for large-scale assembly of flexible energy storage devices.

Keywords: Adhesion; Flexible zinc ion battery; Hydrogel electrolyte; Scalable assembly; Suppressed dendrite growth.