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Research Article

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

Xiao Liu1,2, Hong Liu2,3, Chi Chen1, Liangliang Zou1, Yuan Li4, Qing Zhang4, Bo Yang3( ), Zhiqing Zou1, Hui Yang1( )
Center for Energy Storage and Conversion,Shanghai Advanced Research Institute, Chinese Academy of Sciences,Shanghai,201210,China;
,University of the Chinese Academy of Sciences,Beijing,100039,China;
School of Physical Science and Technology,ShanghaiTech University,Shanghai,201210,China;
Evergrande Neoenergy Technology Group,Shanghai,201815,China;
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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 FeNx moieties promoted by Fe2N nanoparticles derived from Fe-doped zeolitic imidazolate framework. The best-performing Fe-N-C/HPC-NH3 catalyst 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.

Keywords

non-precious metaloxygen reduction reactionFe2N nanoparticleFeNx moietyproton exchange membrane fuel cell

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Nano Research
Volume 12 Issue 7,
July 2019
Pages 1651-1657
DOI: 10.1007/s12274-019-2415-7
Cite this article:
Liu X, Liu H, Chen C, et al. Fe2N nanoparticles boosting FeNx moieties for highly efficient oxygen reduction reaction in Fe-N-C porous catalysts. Nano Research, 2019, 12(7): 1651-1657. https://doi.org/10.1007/s12274-019-2415-7
Topics:
Density functional theoryElectrocatalystsElectrolytic reduction Free energy Metal nanoparticlesOxygenPrecious metalsProton exchange membrane fuel cells (PEMFC) Reaction intermediates

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Received: 29 January 2019
Revised: 30 March 2019
Accepted: 10 April 2019
Published: 25 April 2019
© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2019
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