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Fe2N nanoparticles boosting FeNx moieties for highly efficient oxygen reduction reaction in Fe-N-C porous catalyst

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Abstract

Replacing Pt-based electrocatalysts for the oxygen reduction reaction (ORR) with high performance and low-cost non-precious metal catalysts is crucial for the commercialization of fuel cells. Herein, we present a highly efficient Fe-N-C porous ORR electrocatalyst with FeNxmoieties promoted by Fe2N nanoparticles derived from Fe-doped zeolitic imidazolate framework. The best-performing Fe-N-C/HPC-NH3catalyst exhibits a superior ORR activity with an onset (E0) and half-wave (E1/2) potential of 0.945 and 0.803 V (RHE), respectively, which is comparable to those of the commercial Pt/C in acidic media. Probing and acid-leaching experiments prove that FeNx moieties play an important role in the ORR and the Fe2N can further improve the ORR activity. Density functional theory calculation reveals a synergistic effect that the existence of Fe2N weakens the adsorption of ORR intermediates on active sites and lowers the reaction free energy of the potential limiting step, thus facilitating the ORR. Both experimental evidence and theoretical analysis for the enhancement of ORR activity by Fe2N decoration in Fe-N-C catalyst might inspire a new strategy for rational design of high performance non-precious metal catalysts.

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Acknowledgements

The financial supports from the National Key Research and Development Program of China (No. 2017YFA0206500) and the National Natural Science Foundation of China (Nos. 21802161, 21673275, and 21533005) are greatly appreciated. We thank the HPC Platform of ShanghaiTech University for computing time.

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Authors and Affiliations

  1. Center for Energy Storage and Conversion, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, 201210, China

    Xiao Liu, Chi Chen, Liangliang Zou, Zhiqing Zou & Hui Yang

  2. University of the Chinese Academy of Sciences, Beijing, 100039, China

    Xiao Liu & Hong Liu

  3. School of Physical Science and Technology, ShanghaiTech University, Shanghai, 201210, China

    Hong Liu & Bo Yang

  4. Evergrande Neoenergy Technology Group, Shanghai, 201815, China

    Yuan Li & Qing Zhang

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  1. Xiao Liu
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  2. Hong Liu
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  5. Yuan Li
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Correspondence to Bo Yang or Hui Yang.

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Liu, X., Liu, H., Chen, C. et al. Fe2N nanoparticles boosting FeNx moieties for highly efficient oxygen reduction reaction in Fe-N-C porous catalyst. Nano Res. 12, 1651–1657 (2019). https://doi.org/10.1007/s12274-019-2415-7

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