Fabricating 3D Macroscopic Graphene-Based Architectures with Outstanding Flexibility by the Novel Liquid Drop/Colloid Flocculation Approach for Energy Storage Applications

Inspired by "water ripples" in nature and the flocculation phenomenon in colloid chemistry, a novel liquid drop/colloid flocculation approach is developed to fabricate an extremely flexible and compressible 3D macroscopic graphene-based architecture (hydrogels or aerogels), via a new coagulation-induced self-assembly mechanism. This facile and universal technique can be achieved in a neutral, acidic, or basic coagulation bath, producing microsized hydrogels with various structures, such as mushroom, circle, disc shapes, etc. The method also allows us to introduce various guest materials in the graphene matrix using transition metal salts as the coagulating bath. A mushroom-shaped NiCo oxide/GS hybrid aerogel (diameter: 3 mm) is prepared as an example, with ultrathin NiCo oxide nanosheets in situ grown onto the surface of graphene. By employing as binder-free electrodes, these hybrid aerogels exhibit a specific capacitance of 858.3 F g^-1 at 2 A g^-1, as well as a good rate capability and cyclic stability. The asymmetric supercapacitor, assembling with the hybrid aerogels as cathode and graphene hydrogels as anode materials, could deliver an energy density of 21 Wh kg^-1 at power density of 4500 W kg^-1. The ease of synthesis and the feasibility of obtaining highly flexible aerogels with varied morphologies and compositions make this method a promising one for use in the field of biotechnology, electrochemistry, flexible electronics, and environment applications.