Dynamically Cross‐Linked, Self‐Healable, and Stretchable All‐Hydrogel Supercapacitor with Extraordinary Energy Density and Real‐Time Pressure Sensing

Wearable electronics with flexible, integrated, and self-powered multi-functions are becoming increasingly attractive, but their basic energy storage units are challenged in simultaneously high energy density, self-healing, and real-time sensing capability. To achieve this, a fully flexible and omni-healable all-hydrogel, that is dynamically crosslinked PVA@PANI hydrogel, is rationally designed and constructed via aniline/DMSO-emulsion-templated in situ freezing-polymerization strategy. The PVA@PANI sheet, not only possesses a honeycombed porous conductive mesh configuration with superior flexibility that provides numerous channels for unimpeded ions/electron transport and maximizes the utilization efficiency of pseudocapacitive PANI, but also can conform to complicated body surface, enabling effective detection and discrimination of body movements. As a consequence, the fabricated flexible PVA@PANI sheet electrode demonstrates an unprecedented specific capacitance (936.8 F g-1 ) and the assembled symmetric flexible all-solid-state supercapacitor delivers an extraordinary energy density of 40.98 Wh kg-1 , outperforming the previously highest-reported values of stretchable PVA@PANI hydrogel-based supercapacitors. What is more, such a flexible supercapacitor electrode enables precisely monitoring the full-range human activities in real-time, and fulfilling a quick response and excellent self-recovery. These outstanding flexible sensing and energy storage performances render this emerging PVA@PANI hydrogel highly promising for the next-generation wearable self-powered sensing electronics.