While traditional three-layer structure supercapacitors are under mechanical manipulations, the high-stress region concentrates, inevitably causing persistent structural problems including interlayer slippage, crease formation, and delamination of the electrode–electrolyte interface. Toward this, an all-polymeric, all-elastic and non-laminated supercapacitor with high mechanical reliability and excellent electrochemical performance is developed. Specifically, a polypyrrole electrode layer is in situ integrated into a silk fibroin-based elastic supramolecular hydrogel film with extensive hydrogen and covalent bonds, where a non-laminate device is realized with structural elasticity at the device level. The non-laminate configuration can avoid slippage and delamination, while the elasticity can preclude crease formation. Furthermore, under more severe mechanical damage, the supercapacitors can restore the electrochemical performance through non-autonomous self-healing capabilities, where the supramolecular design of host–guest interactions in the hydrogel matrix results in a superior self-healing efficiency approaching ≈95.8% even after 30 cutting/healing cycles. The all-elastic supercapacitor delivers an areal capacitance of 0.37 F cm⁻² and a volumetric energy density of 0.082 mW h cm⁻³, which can well-maintain the specific capacitance even at −20 °C with over 85.2% retention after five cut/healing cycles.

中文翻译：

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自愈无皱超分子全聚合物超级电容器

传统的三层结构超级电容器在机械操作下，高应力区域集中，不可避免地会导致持续的结构问题，包括层间滑移、折痕形成和电极-电解质界面分层。为此，开发了一种具有高机械可靠性和优异电化学性能的全聚合物、全弹性、非层压超级电容器。具体来说，将聚吡咯电极层原位集成到具有广泛氢键和共价键的丝素蛋白基弹性超分子水凝胶薄膜中，在器件水平上实现具有结构弹性的非层压器件。非层压结构可以避免滑动和分层，而弹性可以防止折痕形成。此外，在更严重的机械损伤下，超级电容器可以通过非自主自愈能力恢复电化学性能，其中水凝胶基质中主客体相互作用的超分子设计导致优异的自愈效率接近约95.8％，甚至30 次切割/愈合循环后。全弹性超级电容器的面积电容为0.37 F cm ^-2，体积能量密度为0.082 mWh cm ^-3，即使在-20℃下也能很好地保持比电容，五次切割后比电容保持率超过85.2% /愈合周期。