Direct Ink Writing of Wearable Thermoresponsive Supercapacitors with rGO/CNT Composite Electrodes

Abstract Developing intelligent wearable energy storage devices that can endure harsh conditions is of interest for emerging applications in next‐generation electronics. Despite recent success in exploring functional materials for sophisticated self‐adaptivity in energy storage devices, it remains challenging to obtain both high reliability and superior performance. Herein, a novel method for fabricating micropatterned wearable thermoresponsive supercapacitors via direct ink writing (DIW) technique is reported. Thermal runaway of typical electrochemical storage devices with high power delivery capability can cause serious safety problems. The proposed temperature‐dependent structure works as self‐protection against the common thermal runaway issues of electrochemical energy storage devices. Such construction provides an automatic adjustment as high as 8 F g⁻¹ in specific capacitance, resulting in an overall heat reduction by up to 40%. The printing resolution of the electrodes (175 µm) is among the best in recently reported planar carbon‐based energy storage devices by DIW technique. Manufacturing‐related parameters such as time‐dependent printing speed and curing temperature are also investigated to fabricate this integrated design with varied materials and accuracy. This strategy shows tremendous promise for future intelligent energy storage devices.