Bioinspired Interfacial Strengthening Flexible Supercapacitors via Hierarchically Topological Interlocking Strategy

Flexible micro-supercapacitors (MSCs) featured with high storage capacity and mechanical stability are essential and indispensable for the development of wearable devices. Since the active materials physically deposited on the current collectors are rigid and will be desquamated under the mechanical cycling, the performance of flexible MSCs is still limited by the weak interfacial adhesions between materials and collectors. The effective strategy to strengthen the interfacial adhesion is one important key to achieve high-performance flexible MSCs. In this work, a flexible symmetrical micro-supercapacitor with a bioinspired hierarchically topological interlocking interfacial enhancement strategy was presented. Based on the high stability metal current collectors on the polyimide substrate, two-level 3D interlocking structures between the active materials and the current collectors were further utilized, which was inspired by the structures of a gecko's feet and a tree's roots in rock cracks, respectively. Through these 3D interlocking structures, the effective contact areas and the adhesion strengths of two interfaces, that is, the active material/current collectors and the current collector/substrate interfaces, are significantly enhanced. The energy density of the interfacial enhanced active carbon symmetrical MSC (IE SMSC) has been improved over 3 times in comparison with the in-plane active carbon SMSC (SMSC). The capacitance of IE SMSC can remain 92.9% even after 5000 cycles of bending treatment. Even more remarkable, the potential window of the IE SMSC can expand to 1.6 V in the aqueous electrolyte. The results show that the hierarchically topological interlocking strategy can not only ensure the mechanical stability of the flexible MSC but also improve its energy efficiency. Our strategy provides a new perspective for the study of flexible supercapacitors and various flexible devices to achieve high adhesion, high flexibility, and high electrical capacitive performance.