Structurally-stable Mg-Co-Ni LDH grown on reduced graphene by ball-milling and ion-exchange for highly-stable asymmetric supercapacitor.

As an electrode for energy storage, the inherently poor conductivity of metal hydroxides (MHs) can be improved by in situ growth of MHs on conductive carbon based substrates so that their performances on energy storage could be enhanced to a high level. However, the incompatibility of hydrophilic component (metal hydroxides) and hydrophobic counterpart (carbon based materials) makes it difficult to be accomplished. Herein, we presented a scalable and easy-operated strategy by ball-milling combined with ion-exchange technique to grow Mg-Co-Ni LDH (layered double hydroxides) on reduced graphene, in which ball-milling was utilized to disperse the staring material of magnesium acetate on graphene oxide (GO) to obtain the composite of Mg(Ac)/GO. The composite can be in situ transformed to MgO/reduced grapheme (rG) by following heat treatment. While, the ion-exchange reaction could enables the in situ growth of Mg-Co-Ni LDHs on the reduced graphene. The derived products (denoted as Mg-Co-Ni LDH/rG-x) owns nanosheet morphology, surface area of 59-115 m/g, homogenous elements distribution. As electrode for supercapacitor, the maximum capacitance of 1204F/g@1.0 A/g was achieved and the corresponding asymmetric supercapacitor device shows a large energy density of 44.3 Wh/kg@800 W/kg. Particularly, a superlong cycling stability with 90.5% capacitance retention of the first cycle was attained after continuous charge/discharge for 20 000 cycles at current density of 5.0 A/g, promising great potential for practical energy storage application. The present strategy is simple and scalable that can be widely applied to the synthesis of various hydroxides/oxides or multi-component hydroxides/oxides on carbon substrates forming a composite structure, thus offers a great potential for broad application areas including catalysis, adsorption, energy storage, etc.