Three-Dimensional Framework of Graphene Nanomeshes Shell/Co₃O₄ Synthesized as Superior Bifunctional Electrocatalyst for Zinc–Air Batteries

The synthesis of durable and low-cost electrocatalyst is crucial but challenging. Here, we developed a one-pot pyrolysis approach toward the preparation of heteroatom-doped hierarchical porous three-dimensional (3D) graphene frameworks decorated with multilayer graphene shell-coated cobalt oxide nanocrystal. Large literal sheet size of graphene nanomeshes may stimulate rapid thermolysis with cobalt–oleate complex to form Co 3 O 4 nanocrystals and in situ growth of multilayer graphene coating co-doped by boron and nitrogen with controlling heating rate up to 600 °C. This new material worked as superior bifunctional electrocatalyst on oxygen reduction reaction and oxygen evolution reaction to commercial Pt/C with better onset potential/half-wave potentials, larger current density, better stability, and stronger methanol tolerance. The heteroatom co-doping into porous/curved graphene confined nanocrystals in 3D porous walls provided adequate accessibility of created catalytic active sites and ideal mass transport route for the excellent catalytic activity on redox reaction of oxygen. The synthesized material-based Zn–air battery further confirmed its superior electrolytic activity with high specific capacity and smaller overpotential. This one-pot pyrolysis method shows a great potential of scalable synthesis of high-performance practical electrocatalyst for metal–air batteries and fuel cells at a low cost.