Concurrently Improving both Mechanical and Electrochemical Performances of Quasi-Solid-State Electrical Double-Layer Capacitors by a Rational Design of Gel Polymer Electrolytes

Aqueous poly(vinyl alcohol) (PVA) gel electrolyte-based quasi-solid-state electrical double-layer capacitors (QSEDLCs) have been extensively investigated in the past ten years, but challenges remain to fabricate the PVA gel electrolyte possessing both superior mechanical and outstanding electrochemical performances. Herein, we develop a strategy to address this issue by a rational design of PVA gel electrolytes, based on a combination of the freeze-thaw (FT) method and sodium perchlorate (NaClO₄)-based water-in-salt (WIS) electrolyte. Our study demonstrates that either the FT method or the NaClO₄-based WIS electrolyte can improve both the mechanical performance of the PVA gel electrolyte by increasing the crystallization of PVA chains and the electrochemical performance of the PVA gel electrolyte-based QSEDLC by different mechanisms. In comparison with the conventional solvent evaporation method, this work provides an effective strategy to concurrently improve both the mechanical and electrochemical performances of aqueous QSEDLCs.