Sustainable graphene production for solution-processed microsupercapacitors and multipurpose flexible electronics

The growing demand for portable and wearable electronics, Internet of Things microdevices, and wireless sensor networks has led to the development of miniaturized energy storage devices, such as microsupercapacitors (mSCs). With excellent electrical conductivity and high surface area in a layered structure, graphene materials are ideal for mSCs, but current manufacturing methods still hinder their widespread integration. Here, we propose a sustainable approach for the rapid and eco-friendly production of few-layer graphene flakes based on the exfoliation of graphite in water by a combination of high-shear mixing and a high-pressure airless spray. An all-carbon composite paste with high electrical conductivity and tunable viscosity was designed to fabricate planar, interdigitated mSCs on polyethylene terephthalate (PET). The flexible, metal-free mSCs achieved a Coulombic efficiency close to 100%, with areal and volumetric capacitances of 6.16 mF cm−2 and 2.46 F cm−3, respectively. The maximum energy density exceeds 200 μWh cm−3 with 91.5% capacitance retention after 10000 galvanostatic charge[sbnd]discharge cycles. The mSCs retain the same performance when subjected to a wide bending range and can be easily modularized to adjust the voltage and capacitance outputs. Finally, high-performance coatings for electromagnetic interference shielding and wearable strain sensors are also fabricated to demonstrate the multipurpose applicability of the graphene-based paste.