Aqueous Inks of Pristine Graphene for 3D Printed Microsupercapacitors with High Capacitance

Three-dimensional (3D) printing is gaining importance as a sustainable route for the fabrication of high-performance energy storage devices. It enables the streamlined manufacture of devices with programmable geometry at different length scales down to micron-sized dimensions. Miniaturized energy storage devices are fundamental components for on-chip technologies to enable energy autonomy. In this work, we demonstrate 3D printed microsupercapacitor electrodes from aqueous inks of pristine graphene without the need of high temperature processing and functional additives. With an intrinsic electrical conductivity of ∼1370 S m^-1 and rationally designed architectures, the symmetric microsupercapacitors exhibit an exceptional areal capacitance of 1.57 F cm^-2 at 2 mA cm^-2 which is retained over 72% after repeated voltage holding tests. The areal power density (0.968 mW cm^-2) and areal energy density (51.2 μWh cm^-2) outperform the ones of previously reported carbon-based supercapacitors which have been either 3D or inkjet printed. Moreover, a current collector-free interdigitated microsupercapacitor combined with a gel electrolyte provides electrochemical performance approaching the one of devices with liquid-like ion transport properties. Our studies provide a sustainable and low-cost approach to fabricate efficient energy storage devices with programmable geometry.