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Research Article

Simultaneous integration of Fe clusters and NiFe dual single atoms in nitrogen-doped carbon for oxygen reduction reaction

Jirong Bai1,2, Yuebin Lian1, Yaoyao Deng1, Mei Xiang1( ), Peng Xu1, Quanfa Zhou1, Yawen Tang2( ), Yaqiong Su3( )
Research Center of Secondary Resources and Environment, School of Chemical Engineering and Materials, Changzhou Institute of Technology, Changzhou 213022, China
Jiangsu Key Laboratory of New Power Batteries, School of Chemistry and Materials Science, Nanjing Normal University, Nanjing 210023, China
School of Chemistry, Engineering Research Center of Energy Storage Materials and Devices of Ministry of Education, National Innovation Platform (Center) for Industry-Education Integration of Energy Storage Technology, Xi’an Jiaotong University, Xi’an 710049, China
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Graphical Abstract

There is a strong electron exchange between NiFe dual single-atoms and the Fe clusters, which is conducive to breaking the symmetric electronic structure of Fe-N4, and the obtained FeNCs/NiFeSAs-NC catalyst shows low rate-determining step (RDS) energy barrier and high intrinsic oxygen reduction reaction (ORR) activity.

Abstract

Atomically-dispersed iron-based electrocatalysts are promising substitutes for noble metal electrocatalysts because of excellent performance in oxygen reduction reaction (ORR). Rationally modulating the local coordination environment of the Fe site and optimizing the binding energy of oxygen reduction intermediates are effective strategies to optimize ORR activity. Herein, we report a new method in which Ni is introduced to construct NiFe dual single atoms and iron nanoclusters loaded on the nitrogen-doped carbon with a highly porous structure. This design plays a synergistic role of dual single atoms and clusters, optimizes the 3d orbital and Fermi level of Fe, breaks the symmetrical structure of Fe-N4, and effectively improves the adsorption/desorption behavior of the oxygen-containing intermediates. Electrochemical tests show FeNCs/NiFeSAs-NC has an excellent intrinsic activity. Theoretical calculations show the oxygen-containing species on the Ni active site will move to the middle of NiFe (bridge site connection) after optimization and that the key step is OH desorption, with a reaction energy of 0.27 eV. The electron exchange between NiFe-N6 and Fe-cluster is very strong, further indicating the introduction of Ni species and Fe clusters has a regulatory effect on the electronic structure of Fe-N4.

Keywords

NiFe dual single atomsFe clustersOH* adsorption energyoxygen reduction reaction

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Nano Research
Volume 17 Issue 4,
April 2024
Pages 2291-2297
DOI: 10.1007/s12274-023-6038-7
Cite this article:
Bai J, Lian Y, Deng Y, et al. Simultaneous integration of Fe clusters and NiFe dual single atoms in nitrogen-doped carbon for oxygen reduction reaction. Nano Research, 2024, 17(4): 2291-2297. https://doi.org/10.1007/s12274-023-6038-7
Topics:
Oxygen reduction reaction

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Received: 02 July 2023
Revised: 19 July 2023
Accepted: 23 July 2023
Published: 18 August 2023
© Tsinghua University Press 2023
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