Photo‐Switchable Supercapacitors based on Photo‐Responsive Azopolymers: Enabling Dual‐Functionality in Tunable High Capacitance and Low Self‐Discharge

Abstract Stimuli‐responsive energy storage devices have attracted significant interest for their potential in next‐generation smart devices. Herein, the reversible photo‐switchable supercapacitors utilizing azobenzene‐containing polymer composite electrolytes are presented. Through the gel‐to‐sol transition triggered by light exposure, as proven using rheological analysis, these photo‐switchable electrolytes exhibit an impressive ionic conductivity modulation of 3206%. Owing to the reversible photo‐responsive physical properties, the photo‐switchable supercapacitors deliver a notable capacitance modulation of 105% with a rapid response time of 4 min. Additionally, the devices showed reduced self‐discharging properties under visible light exposure, highlighting their potential use in long‐term energy storage applications. The photo‐controllable and fast response features in this study create new possibilities for the development of multi‐functional energy storage devices.