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Preparation of highly dispersed FeNx active sites for oxygen reduction reaction electrocatalyst by electrospinning and complexation

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Abstract

The development of high-efficiency oxygen reduction reaction (ORR) catalysts is crucial to the advancement of fuel cell technology. Herein, a flexible and free-standing carbon fiber membrane immobilized with atomically dispersed Fe-Nx@NC catalyst is synthesized via electrospinning methodology using suitable complexing agents. A major advantage of the newly designed intertwined fibers is that a highly open structure with abundant nanopores increases gas transportation, electrolyte infiltration, and electron transfer and exposes a high concentration of FeNx sites embedded in the carbon matrix. And Fe4N nanoparticles are generated during pyrolysis and dispersed on carbon fibers upon pyrolysis treatment at 800 °C and co-exist with numerous formed Fe–Nx moieties in the carbon matrix, being evidenced by using X-ray absorption and photoelectron spectroscopy. These factors contribute to excellent ORR activities of FeNx sites. As an ORR catalysts, the as-synthesized Fe-Nx@NC catalyst delivered a more positive half-wave potential of 0.90 V compared to commercial Pt/C. Based on the analyses of the scanning electron microscopy (SEM), the transmission electron microscopy (TEM), X-ray diffractometer (XRD), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy, combined with the density functional theory (DFT) calculations, the generation of FeNx active sites and the formation of the four-coordinate structure of Fe because of the existence of nitrogen-containing complexes were explained, and the catalyst also shows the higher onset potential and half-wave potential in electrochemical tests.

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Data Availability

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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Authors and Affiliations

  1. School of Chemical Engineering and Technology, Tianjin University, Tianjin, 300072, China

    Xuemeng Zhang, Xu Meng, Tao Liu & Wei Wang

  2. Forschungszentrum Jülich, IEK-9, 52425, Jülich, Germany

    Zigeng Liu

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Zhang, X., Meng, X., Liu, T. et al. Preparation of highly dispersed FeNx active sites for oxygen reduction reaction electrocatalyst by electrospinning and complexation. Ionics 29, 1089–1099 (2023). https://doi.org/10.1007/s11581-022-04861-4

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