<p>This study investigates the synergistic effects of pyrolysis temperature and sulfur doping on the structure and oxygen reduction reaction (ORR) performance of cobalt-based catalysts derived from metal–organic frameworks. Using thiourea as the sulfur source, a series of Co-NSC catalysts were synthesized at different temperatures (750–1050&#xa0;°C). The results demonstrate that sulfur doping effectively inhibits metal agglomeration by forming Co–S coordination bonds, while an optimal pyrolysis temperature (850&#xa0;°C) balances defect density, pore structure, and active-site distribution. Among all samples, Co-NSC-850 exhibits favorable ORR activity in alkaline medium, with a half-wave potential of 0.852&#xa0;V, an electron transfer number close to 4, and H<sub>2</sub>O<sub>2</sub> selectivity below 5%. When applied in zinc-air batteries, Co-NSC-850 delivers a power density of 254.22&#xa0;mW cm<sup>−2</sup>, a small charge–discharge gap (1.02&#xa0;V), a specific capacity of 809.18&#xa0;mAh g<sup>−1</sup>, and a cycle life of 220&#xa0;h, comparable to or better than commercial Pt/C. This work provides valuable insights for designing high-performance non-noble metal ORR catalysts through cooperative regulation of temperature and heteroatom doping.</p> Graphical abstract <p></p>

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Synergistic temperature and sulfur doping engineering of MOF‑derived Co‑N‑C catalysts for high‑performance zinc‑air batteries

  • Qing Hu,
  • Haiyi Wu,
  • Ling Shi,
  • Zhenhua Yao,
  • Fang Jin,
  • Maocong Hu

摘要

This study investigates the synergistic effects of pyrolysis temperature and sulfur doping on the structure and oxygen reduction reaction (ORR) performance of cobalt-based catalysts derived from metal–organic frameworks. Using thiourea as the sulfur source, a series of Co-NSC catalysts were synthesized at different temperatures (750–1050 °C). The results demonstrate that sulfur doping effectively inhibits metal agglomeration by forming Co–S coordination bonds, while an optimal pyrolysis temperature (850 °C) balances defect density, pore structure, and active-site distribution. Among all samples, Co-NSC-850 exhibits favorable ORR activity in alkaline medium, with a half-wave potential of 0.852 V, an electron transfer number close to 4, and H2O2 selectivity below 5%. When applied in zinc-air batteries, Co-NSC-850 delivers a power density of 254.22 mW cm−2, a small charge–discharge gap (1.02 V), a specific capacity of 809.18 mAh g−1, and a cycle life of 220 h, comparable to or better than commercial Pt/C. This work provides valuable insights for designing high-performance non-noble metal ORR catalysts through cooperative regulation of temperature and heteroatom doping.

Graphical abstract