Ni dispersed ultrathin carbon nanosheets as bi-functional oxygen electrocatalyst induced from graphite-like porous supramolecule

Excellent porosity and accessibility are key requirements during carbon-based materials design for energy conversion applications. Herein, a Ni-based porous supramolecular framework with graphite-like morphology (Ni-SOF) was rationally designed as a carbon precursor. Ultrathin carbon nanosheets dispersed with Ni nanoparticles and Ni-N_x sites (Ni@NiN_x-N-C) were obtained via in-situ exfoliation during pyrolysis. Due to the hetero-porous structure succeeding from Ni-SOF, the Ni@NiN_x-N-C catalyst showed outstanding bifunctional oxygen electrocatalytic activity with a narrow gap of 0.69 V between potential to deliver 10 mA cm⁻² oxygen evolution and half-wave potential of oxygen reduction reaction, which even surpassed the Pt/C + IrO₂ pair. Therefore, the corresponding zinc-air battery exhibited excellent power output and stability. The multiple Ni-based active sites, the unique 2D structure with a high graphitization degree and large specific surface area synergistically contributed to the excellent bifunctional electrocatalytic activity of Ni@NiN_x-N-C. This work provided a novel viewpoint for the development of carbon-based electrocatalyst.