Solid-state stepwise temperature-programmable synthesis of bioinspired Fe-N-C oxygen reduction electrocatalyst featuring Fe-N5 configuration

The bioinspired Fe-N-C features an asymmetric Fe-N5 configuration to produce active metal-oxygen intermediates by introducing axial N ligand into a symmetric Fe-N4 structure, enabling highly active oxygen reduction reaction (ORR). However, the artificial creation of active Fe-N5 configuration with a direct, facile and green method has been rarely developed yet, as current techniques involve complex processes and costly precursors. Herein, we advance a novel solid-state stepwise temperature-programmable (SST) route to directly produce bioinspired Fe-N5-C. We then demonstrate that such a Fe-N5-C exhibits a quite higher half-wave potential (0.92 V) with 22-fold faster ORR kinetics (15.6 mA·cm−2 @ 0.85 V) over that of the commercial Pt/C counterpart. Indeed, we perform density functional theory (DFT) to find that the Fe is discharged with an extra 0.1 e− through the axially coordinate N ligand, which significantly enhances the ability to activate O2 and enables an easier desorption of the crucial intermediate *OH on the Fe-N5 configuration over the conventional Fe-N4 structure. © 2025 Elsevier B.V., All rights reserved.

Авторы
Sang Wei 1 , Chaemchuen Somboon 1, 5 , Zhang Longyang 1 , Wang Zechen 1 , Li Xingchuan 1 , Nagasaka Cocoro Andrew 2 , Xiong Mo 3 , Ogiwara Naoki 2 , Chen Cheng 1, 4 , Wang Zhao 9 , Zhang Jian 10 , Verpoorť Francis Walter Cornelius 1, 7, 8 , Mu Shichun 1 , Kou Zongkui 1, 4 , Wang Tingting 6
Издательство
Tsinghua University Press
Номер выпуска
3
Язык
English
Статус
Published
Номер
94907245
Том
18
Год
2025
Организации
  • 1 State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan, China
  • 2 Department of Basic Sciences, The University of Tokyo, Tokyo, Japan
  • 3 School of Physics, Xi'an Jiaotong University, Xi'an, China
  • 4 Wuhan University of Technology, Wuhan, China
  • 5 Department of Chemical Engineering, Mahidol University, Nakhon Pathom, Thailand
  • 6 School of Mathematical and Physical Sciences, Wuhan Textile University, Wuhan, China
  • 7 Joint Institute of Chemical Research (FFMiEN), RUDN University, Moscow, Russian Federation
  • 8 Tomsk Polytechnic University, Tomsk, Russian Federation
  • 9 & Piezo-electric Materials and Devices, Hubei University, Wuhan, China
  • 10 School of Chemistry and Chemical Engineering, Hainan University, Haikou, China
Ключевые слова
Fe-N5 coordination; metal-air battery; oxygen reduction reaction (ORR); single atom catalysts; solvent-free synthesis
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