Abstract

The interfacial void and delamination between the hydrogel electrolyte and flexible electrode caused by the inconformal contact and weak adhesion lead to serious performance degradation of solid-state-sandwiched supercapacitors (SCs) upon repetitive deformation. Herein, we propose a hydrogel polymer electrolyte (HPE) engineering strategy for enhancing the interfacial adhesion (Γ) to achieve extremely durable SCs via the soft, tough, and self-adhesive HPE. Using a self-cross-linked poly(N-hydroxyethyl acrylamide)/H3PO4 (PHEAA/H3PO4) HPE as the model, the interfacial adhesion between HPE and polyaniline (PANI)-modified carbon cloth (CC) electrode (CC/PANI) reaches up to 556 J/m2, leading to excellent durability of electrochemical performance under long-term repetitive deformations. The as-assembled sandwiched SC retains 94.14 and 93.62% of initial capacitance after 180° bending and twisting for 100,000 cycles, respectively. Furthermore, benefiting from the addition of H3PO4, the flexible sandwiched SC displays excellent tolerance to low temperatures and delivers a capacitance retention of 98.03% after 180° bending for 10,000 cycles at -20 °C. This work highlights the importance of interfacial adhesion engineering for the design of extremely deformation-tolerable SCs.

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