Scalable production of graphene inks via wet-jet milling exfoliation for screen-printed micro-supercapacitors

The miniaturization of energy storage units is pivotal for the development of next-generation portable electronic devices. Micro-supercapacitors (MSCs) hold a great potential to work as on-chip micro-power sources and energy storage units complementing batteries and energy harvester systems. The scalable production of supercapacitor materials with cost-effective and high-throughput processing methods is crucial for the widespread application of MSCs. Here, we report wet-jet milling exfoliation of graphite to scale-up the production of graphene as supercapacitor material. The formulation of aqueous/alcohol-based graphene inks allows metal-free, flexible MSCs to be screen-printed. These MSCs exhibit areal capacitance (Careal) values up to 1.324 mF cm-2 (5.296 mF cm-2 for a single electrode), corresponding to an outstanding volumetric capacitance (Cvol) of 0.490 F cm-3 (1.961 F cm-3 for a single electrode). The screen-printed MSCs can operate up to power density above 20 mW cm-2 at energy density of 0.064 uWh cm-2. The devices exhibit excellent cycling stability over charge-discharge cycling (10000 cycles), bending cycling (100 cycles at bending radius of 1 cm) and folding (up to angles of 180{\deg}). Moreover, ethylene vinyl acetate-encapsulated MSCs retain their electrochemical properties after a home-laundry cycle, providing waterproof and washable properties for prospective application in wearable electronics.