N- and O-doped hollow carbons constructed by self- and extrinsic activation for the oxygen reduction reaction and flexible zinc-air Batteries

Zinc-air batteries (ZAB), especially those assembled on flexible substrates, have attracted great research attention in electronics and wearable electronics. However, the air-cathode reaction-oxygen reduction reaction (ORR) has limited the development of ZAB technology. In this study, a hollow carbon catalyst, NOC-1000-1, was prepared by pyrolysis of a mixture of a N-enriched Zn/bispyrozolate-based metal-organic framework and urea to replace the labile Pt-based catalysts for ORR. The employment of sacrifical urea eliminated the requirement for complicated post-treatment compared to the template method. Combined with self-activation (Zn evaporation), the obtained carbon showed a micro- and mesopore-dominant hierarchical structure coexisting with some macropores. Moreover, the doped N and O species were also tailored in a preferable configuration for ORR by simply screening the pyrolysis conditions. Under the synergistic effect of the preferable N and O configurations and pore structure, the derived carbon catalyst displayed superior ORR activity of 0.977 V onset potential and 0.867 V half-wave potential; these values are slightly better than those of the 20% Pt/C benchmark catalyst (0.985 and 0.861 V, respectively). Flexible solid-state ZABs were further assembled by employing the derived carbon catalyst as an air-cathode, and they exhibited a higher peak power density of 100.92 mW cm −2 than a 20% Pt/C-RuO 2 battery as well as previously reported similar batteries and very high stability for up to 30 h. The flexible solid-state ZABs could drive a red light-emitting diode and run a 130-type motor for hours, which indicates their promising applications in real-world technologies. A metal-free hollow carbon with N and O doped in a preferable configuration has been prepared by self- and extrinsic activation, showing superior oxygen reduction reaction (ORR) activity and flexible zinc-air battery (ZAB) performance.