Atomically Dispersed FeN2P2 Motif with High Activity and Stability for Oxygen Reduction Reaction Over the Entire pH Range

Wendan Xue, Qixing Zhou, Xun Cui, Jiawei Zhang, Sijin Zuo, Fan Mo, Jiwei Jiang, Xuya Zhu, Zhiqun Lin

Research output: Contribution to journalArticlepeer-review

18 Scopus citations

Abstract

The past decade has witnessed the great potential of Fe-based single-atom electrocatalysis in catalyzing oxygen reduction reaction (ORR). However, it remains a grand challenge to substantially improve their intrinsic activity and long-term stability in acidic electrolytes. Herein, we report a facile chemical vapor deposition strategy, by which high-density Fe atoms (3.97 wt%) are coordinated with square-planar para-positioned nitrogen and phosphorus atoms in a hierarchical carbon framework. The as-crafted atomically dispersed Fe catalyst (denoted Fe-SA/PNC) manifests an outstanding activity towards ORR over the entire pH range. Specifically, the half-wave potential of 0.92 V, 0.83 V, and 0.86 V vs. reversible hydrogen electrode (RHE) are attained in alkaline, neutral, and acidic electrolytes, respectively, representing the high performance among reported catalysts to date. Furthermore, after 30,000 durability cycles, the Fe-SA/PNC remains to be stable with no visible performance decay when tested in 0.1 M KOH and 0.5 M H2SO4, and only a minor negative shift of 40 mV detected in 0.1 M HClO4, significantly outperforming commercial Pt/C counterpart. The coordination motif of Fe-SA/PNC is validated by density functional theory (DFT) calculations. This work provides atomic-level insight into improving the activity and stability of non-noble metal ORR catalysts, opening up an avenue to craft the desired single-atom electrocatalysts.

Original languageEnglish
Article numbere202307504
JournalAngewandte Chemie - International Edition
Volume62
Issue number41
DOIs
StatePublished - 9 Oct 2023

Bibliographical note

Publisher Copyright:
© 2023 Wiley-VCH GmbH.

Keywords

  • Non-Precious Metal
  • Oxygen Reduction Reaction
  • Phosphorus
  • Single-Atom Catalysts
  • Zinc-Air Battery

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