Abstract

The rational design and fabrication of platinum group metal-free (PGM-free) electrocatalysts for oxygen reduction reaction (ORR) via economically feasible approach is essential for reducing the cost of fuel cells and metal-air batteries. Catalysts must have very high activity, and excellent mass diffusion of reactants. Herein, we display a high-performing dual-metal single atom catalyst (DM-SAC) composed of Fe and Ni SA active sites immobilized in porous carbon nanospheres (Fe/Ni-N-PCS), prepared via defects/vacancies anchoring strategy. The abundant and accessible edge-hosted Fe and Ni SA active sites can promote the adsorption/desorption behavior for ORR intermediates attributing to possible synergistic effects between dual-metal SA active sites. Thus, the as-developed Fe/Ni-N-PCS DM-SAC exhibits impressive ORR electrocatalytic performance in both alkaline (Eonset = 1.04 V, E1/2 = 0.9 V) and acid solutions (Eonset = 0.87 V, E1/2 = 0.71 V), and high stability, outperforming SACs with solo Fe-Nx or Ni-Nx active sites, and benchmark PGM. Fe/Ni-N-PCS also exhibits superior oxygen evolution reaction (OER) performance with low overpotential and long-term stability. Zn-air battery with Fe/Ni-N-PCS cathode yields encouraging performance, including working potential, peak power density, and the stability of charge and discharge cycles. Our synthesis method may promote the fabrication of other DM-SAC and the great promise in practical applications.

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