Self-Assembly of Integrated Tubular Microsupercapacitors with Improved Electrochemical Performance and Self-Protective Function

Inspired by origami art, we demonstrate a tubular microsupercapacitor (TMSC) by self-assembling two-dimensional (2D) films into a “swiss roll” structure with greatly reduced footprint area. A polymeric framework consisting of swelling hydrogel and polyimide layers ensures excellent ion transport between poly(3,4-ethylenedioxythiophene) (PEDOT)-based electrodes and provides efficient self-protection of the TMSC against external compression up to about 30 MPa. Such TMSCs exhibit an areal capacitance of 82.5 mF cm–2 at 0.3 mA cm–2 with a potential window of 0.8 V, an energy density and power density of 7.73 μWh cm–2 and 17.8 mW cm–2 (0.3 and 45 mA cm–2), and an improved cycling stability with a capacitance retention up to 96.6% over 5000 cycles. Furthermore, as-fabricated TMSC arrays can be detached from their surface and transferred onto target substrates. The connection of devices in parallel/series greatly improves their capacity and voltage output. Overall, our prototype devices and fabrication methodology provide a promising route to create integratable microscale tubular energy storage devices with an efficient self-protection function and high performance for future miniaturized electronics.