A simple full-inkjet-printing technique is developed for the scalable fabrication of graphene-based microsupercapacitors (MSCs) on various substrates. High-performance graphene inks are formulated by integrating the electrochemically exfoliated graphene with a solvent exchange technique to reliably print graphene interdigitated electrodes with tunable geometry and "thickness. Along with the printed polyelectrolyte, poly(4-styrenesulfonic acid), the fully printed graphene-based MSCs attain the highest areal capacitance of similar to 0.7 mF/cm(2), substantially advancing the state-of-art of all-solid-state MSCs with printed graphene electrodes. The full printing solution enables scalable fabrication of MSCs and effective connection of them in parallel and/or in series at various scales. Remarkably, more than 100 devices have been connected to form large-scale MSC arrays as power banks on both silicon wafers and Kapton. Without any extra protection or encapsulation, the MSC arrays can be reliably charged up to 12 V and retain the performance even 8 months after fabrication.

The advance of miniaturized and low-power electronics has a striking impact on the development of energy storage devices with constantly tougher constraints in terms of form factor and performance. Microsupercapacitors (MSCs) are considered a potential solution to this problem, thanks to their compact device structure. Great efforts have been made to maximize their performance with new materials like graphene and to minimize their production cost with scalable fabrication processes. In this regard, we developed a full inkjet printing process for the production of all-graphene microsupercapacitors with electrodes based on electrochemically exfoliated graphene and an ultrathin solid-state electrolyte based on nano-graphene oxide. The devices exploit the high ionic conductivity of nano-graphene oxide coupled with the high electrical conductivity of graphene films, yielding areal capacitances of up to 313 mu F cm-2 at 5 mV s-1 and high power densities of up to 4 mW cm-3 with an overall device thickness of only 1 mu m.

Modern energy storage devices for portable and wearable technologies must fulfill a number of requirements, such as small size, flexibility, thinness, reliability, transparency, manufacturing simplicity and performance, in order to be competitive in an ever expanding market. To this end, a comprehensive inkjet printing process is developed for the scalable and low-cost fabrication of transparent and flexible micro-supercapacitors. These solid-state devices, with printed thin films of graphene flakes as interdigitated electrodes, exhibit excellent performance versus transparency (ranging from a single-electrode areal capacitance of 16 mu F cm(-2) at transmittance of 90% to a capacitance of 99 mu F cm(-2) at transmittance of 71%). Also, transparent and flexible devices are fabricated, showing negligible capacitance degradation during bending. The ease of manufacturing coupled with their great capacitive properties opens up new potential applications for energy storage devices ranging from portable solar cells to wearable sensors.

Significant research interest is being devoted to exploiting the properties of graphene but the difficult integration on various substrates limits its use. In this regard, we developed a transfer technique that allows the direct deposition of inkjet printed graphene devices on arbitrary substrates, even 3D objects and living plants. With this technique, we fabricated micro-supercapacitors, which exhibited good adhesion on almost all substrates and no performance degradation induced by the process. Specifically, the microsupercapacitor on an orchid leaf showed an areal capacitance as high as 441 mu F cm(-2) and a volumetric capacitance of 1.16 F cm(-3). This technique can boost the use of graphene in key technological applications, such as self powered epidermal electronics and environmental monitoring systems.