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Research Article | Open Access

Engineering of Fe d-band center in Fe3O4/CeO2 hetero-nanoparticles via orbital coupling for high-efficiency oxygen reduction electrocatalysis

Jiayi Liu1, Jingwen Yin1, Yingzi Lin1, Mingxin Pang1, Huan Pang3, Songtao Zhang4, Lin Xu1(), Jun Yang2(), Yawen Tang1()
Jiangsu Key Laboratory of New Power Batteries, Jiangsu Collaborative Innovation Center of Biomedical Functional Materials, School of Chemistry and Materials Science, Nanjing Normal University, Nanjing 210023, China
State Key Laboratory of Multiphase Complex Systems, Center of Mesoscience, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou 225009, China
Testing Center, Yangzhou University, Yangzhou 225009, China
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Benefiting from the engineered d-band center and unique structural design, the in-situ immobilization of Fe3O4/CeO2 hetero-nanoparticles onto N-doped carbon nanofibers demonstrates excellent oxygen reduction electrocatalytic activity and stability, and performs robust cycling stability.

Abstract

The deliberate engineering of the d-band center of metal site represents an effective strategy to boost the intrinsic electrocatalytic performance toward the oxygen reduction reaction (ORR). Herein, following a heterointerface-induced orbital coupling rationale, we report a judicious design of an efficient ORR electrocatalyst consisting of Fe3O4/CeO2 hetero-nanoparticles in-situ encased into N-doped carbon nanofibers (abbreviated as Fe3O4/CeO2@N-CNFs hereafter). The theoretic calculations uncover that the Fe3O4/CeO2 heterointerface-triggered orbital coupling can cause the down shift of the d-band center positions of Fe sites, which leads to the weakened chemisorption of oxygenated groups and lowered energy barrier for the potential-determining step, ultimately dramatically boosting the ORR intrinsic activity. As a consequence, the well-designed Fe3O4/CeO2@N-CNFs display admirable ORR activity with a half-wave potential of 0.84 V and outstanding structural/electrochemical stability in an alkaline electrolyte, surpassing the commercial Pt/C benchmark and a majority of recently reported Fe3O4-based electrocatalysts. More encouragingly, the Fe3O4/CeO2@N-CNFs-incorporated Zn-air battery outperforms the Pt/C-assembled counterpart with higher power density, larger energy density, and excellent cycling stability, serving as a competent candidate for ORR-involved renewable energy setups. This study offers an innovative approach for the rational manipulation of the d-band center and interfacial electron behavior of active sites toward the optimization of electrocatalytic performance.

Keywords

hetero-nanoparticleselectrospinninginterfacial engineeringorbital couplingoxygen reduction reaction

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Nano Research
Volume 18 Issue 1,
January 2025
Article number: 94907016
DOI: 10.26599/NR.2025.94907016
Cite this article:
Liu J, Yin J, Lin Y, et al. Engineering of Fe d-band center in Fe3O4/CeO2 hetero-nanoparticles via orbital coupling for high-efficiency oxygen reduction electrocatalysis. Nano Research, 2025, 18(1): 94907016. https://doi.org/10.26599/NR.2025.94907016
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