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.