LAUSR

To push the energy density limit of supercapacitors (SCs), new electrode materials with hierarchical nano-micron pore architectures are strongly desired. Graphene hydrogels that consist of 3 D porous frameworks have received particular attention but their capacitance is limited by electrical double layer capacitance. In this work, we report the rational design and fabrication of a composite hydrogel of N-doped graphene (NG) that contains embedded Ni(OH)2 nanoplates that is cut conveniently into films to serve as positive electrodes for flexible asymmetric solid-state SCs with NG hydrogel films as negative electrodes. The use of high-power ultrasound leads to hierarchically porous micron-scale sheets that consist of a highly interconnected 3 D NG network in which Ni(OH)2 nanoplates are well dispersed, which avoids the stacking of NG, Ni(OH)2 , and their composites. The optimal SC device benefits from the compositional features and 3 D electrode architecture and has a high specific areal capacitance of 255 mF cm-2 at 1.0 mA cm-2 and a very stable, high output cell voltage of 1.45 V, which leads to an energy density of 80 μW h cm-2 even at a high power of 944 μW cm-2 , considerably higher than that reported for similar devices. The devices exhibit a high rate capability and only 8 % capacitance loss over 10 000 charging cycles as well as excellent flexibility with no clear performance degradation under strong bending.