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

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...

Full description

Saved in:
Bibliographic Details
Published inAngewandte Chemie International Edition Vol. 62; no. 41
Main Authors Xue, Wendan, Zhou, Qixing, Cui, Xun, Zhang, Jiawei, Zuo, Sijin, Fan, Mo, Jiang, Jiwei, Zhu, Xuya, Lin, Zhiqun
Format Journal Article
LanguageEnglish
Published Weinheim Wiley Subscription Services, Inc 09.10.2023
EditionInternational ed. in English
Subjects
Catalysts
Chemical reduction
Chemical vapor deposition
Density functional theory
Durability
Electrocatalysts
Electrolytes
Noble metals
Oxygen reduction reactions
Phosphorus
Stability
Sulfuric acid
Online AccessGet full text

Cover

More Information
Summary: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.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202307504