Scholarlink

<p>Regulating the local coordination environment to break the inherent symmetry of Fe-N<sub>4</sub> active sites is a promising strategy for improving the catalytic performance of oxygen reduction reactions (ORR). However, achieving atomic-level control over heteroatom incorporation into specific coordination sites remains a formidable synthetic challenge. Herein, we report a novel pre-coordination strategy that employs a nitrogen-rich covalent triazine framework (Tri-COF) as a precursor to simultaneously construct Fe–N and Fe–S coordination motifs through sulffonation and subsequent metalation. The resulting asymmetric Fe-S-N<sub>3</sub> sites exhibit significantly higher ORR activity than conventional Fe-N<sub>4</sub>, achieving a half-wave potential of 0.92 V in alkaline media. Notably, the Fe-S-N<sub>3</sub>C catalyst delivers outstanding performance in Zn-air batteries, achieving a peak power density of 157.9 mW cm<sup>−2</sup> and exceptional long-term stability over 700 h. Density functional theory (DFT) calculations reveal that sulfur incorporation acts as an electronic modulator, inducing localized charge redistribution and downshifting the Fe d-band center. This electronic optimization weakens *OH adsorption, thereby accelerating the ORR kinetics. This work provides an effective strategy for precisely tailoring the atomic coordination microenvironment of single-atom catalysts to achieve superior electrocatalytic performance.</p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Pre-coordinated synthesis of asymmetric Fe-S-N3C atomic sites for efficient oxygen electroreduction

  • 期刊论文

  • 发表日期：

    2026年7月8日

查看全文
  • Yifan Huang,
  • Yuekai Wu,
  • Hao Zhuo,
  • Gang Zhang,
  • Ping Wu,
  • Ruxiang Shen,
  • Huixia Wu,
  • Fantao Kong,
  • Xiangzhi Cui

摘要

Regulating the local coordination environment to break the inherent symmetry of Fe-N4 active sites is a promising strategy for improving the catalytic performance of oxygen reduction reactions (ORR). However, achieving atomic-level control over heteroatom incorporation into specific coordination sites remains a formidable synthetic challenge. Herein, we report a novel pre-coordination strategy that employs a nitrogen-rich covalent triazine framework (Tri-COF) as a precursor to simultaneously construct Fe–N and Fe–S coordination motifs through sulffonation and subsequent metalation. The resulting asymmetric Fe-S-N3 sites exhibit significantly higher ORR activity than conventional Fe-N4, achieving a half-wave potential of 0.92 V in alkaline media. Notably, the Fe-S-N3C catalyst delivers outstanding performance in Zn-air batteries, achieving a peak power density of 157.9 mW cm−2 and exceptional long-term stability over 700 h. Density functional theory (DFT) calculations reveal that sulfur incorporation acts as an electronic modulator, inducing localized charge redistribution and downshifting the Fe d-band center. This electronic optimization weakens *OH adsorption, thereby accelerating the ORR kinetics. This work provides an effective strategy for precisely tailoring the atomic coordination microenvironment of single-atom catalysts to achieve superior electrocatalytic performance.