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

Abstract

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—RuO₂ 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.