The development of nonprecious metal-based electrocatalysts with remarkable catalytic activity and long-cycling lifespan toward oxygen reduction reaction (ORR) and evolution reaction (OER) is especially important for rechargeable zinc-air batteries (ZABs). Herein, monodispersed Co 9 S 8 nanoparticles embedded in nitrogen-doped hierarchically porous hollow carbon spheres (Co 9 S 8 NPs/NHCS) are synthesized through a template-assisted strategy followed by a co-assembly, thermal annealing, and sulfurization process. Benefiting from larger specific surface area, hierarchically porous hollow structure, and carbon nanotubes self-growth, the obtained Co 9 S 8 NPs/NHCS-0.5 electro-catalyst exhibits decent performance for ORR (E 1/2 = 0.85 V) and OER (E 10 = 1.55 V). A rechargeable ZAB assembled using the Co 9 S 8 NPs/NHCS-0.5 as air cathode delivers a maximum power density of 116 mW cm À 2 , high open circuit voltage of 1.47 V, and good durability (no obvious voltage decay after 1200 cycles (200 hours)). Such a hierarchically porous hollow structure of Co 9 S 8 NPs/NHCS-0.5 provides a confined space shell and an interconnected hollow core to achieve outstanding bifunctional catalytic activity and cycling stability, which surpass the benchmark Pt/C-RuO 2 .
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