Three‐Dimensional Printed Mechanically Compliant Supercapacitor with Exceptional Areal Capacitance from a Self‐Healable Ink

Abstract

Abstract Known for its capability to architect tailored structures for the scaling of active materials in energy storage devices that cater for future electronics having stringent requirements on areal performance, 3D printing is receiving serious attention. However, lingering challenges originating from the notorious interfacial issue and weak component interaction restrain current devices from making a breakthrough in deliverable capacity and structural flexibility. In this work, the printed electrode delivers a record‐breaking electrical double layer (EDL) areal capacitance of 27.1 F cm −2 under an extremely large loading density of 134 mg cm −2 . This translates to a deliverable record‐high EDL energy density of 1.26 mWh cm −2 for device performance, which even rivals the highest value reported from highly loaded pseudocapacitors. The bespoke devices are enabled by a strategically formulated 3D printable ink that initiates efficient autonomous room‐temperature self‐healing and strong interplay between constituting ink components. These contribute to interlayer coalescing for eliminated interlayer resistance for a solid electrochemical performance and printed electrodes of great mechanical compliance. By tapping into the huge potential of 3D printing, this work lays a solid foundation on which flexible devices with customized geometry, functionality, and outstanding performance for a broad range of applications can be readily realized.