Decoupling of Mechanical Strength and Ionic Conductivity in Zwitterionic Elastomer Gel Electrolyte toward Safe...

Quasi-solid state electrolyte is one of the promising options for next generation batteries due to its superiority on safety and electrochemistry performance. However, the trade-off between the electrolyte swelling ratio and mechanical property of the quasi-solid state electrolyte significantly influences the battery performance. Herein, we design a nonswelling, solvent-adaptive polymer gel composed of oleophobic zwitterion poly(3-(1-vinyl-3-imidazolio)-propanesulfonate) and oleophilic elastomer poly(2-methoxyethyl acrylate) segments to retain high battery performance without sacrificing the mechanical property in lithium batteries. The as-designed gel can not only uptake enough electrolyte for a high ionic conductivity of 1.78 mS cm^-1 but also achieve excellent mechanical strength with compression stress at 90% strain (σ_0.9) reaching 5.8 MPa after long time soaking for battery safety due to its nonswelling property in ester electrolyte. Moreover, the as-prepared zwitterionic gel is beneficial to electrolyte salt dissociation, which further enhances the ionic conductivity and transference number of batteries. Consequently, the gel electrolyte can cycle for more than 500 h under a high current density of 3 mA cm^-2 on dendrite inhibition performance, and when assembled with LiFePO₄ as a cathode, the battery demonstrates a reversible specific capacity as high as 70 mAh g^-1 under a high current density of 5 C after 300 cycles. The rational designed solvophilic/solvophobic zwitterionic elastomers provide a guidance for engineering quasi-solid state electrolytes of different solvents with broad applications on flexible devices.