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The Role of Iron Nitrides in Fe-N-C Catalysis System towards Oxygen Reduction Reaction

Abstract

Fe-N-C series catalysts are always attractive for their high catalytic activity towards oxygen reduction reaction (ORR). However, they usually consist of various components such as iron nitrides, metallic iron, iron carbides, N-doped carbon and Fe-N4 moieties, leading to controversial contributions of these components to the catalysis of ORR, especially iron nitrides. In this work, to investigate the function of iron nitrides, FexN nanoparticles embedded in mesoporous N-doped carbon without Fe-N4 moieties are designed and constructed by a simple histidine-assisted method. Herein, the use of histidine can increase the N and Fe contents in the product. The obtained catalyst exhibits excellent ORR catalytic activity which is very close to that of the commercial Pt/C catalyst in alkaline electrolytes. Combining the catalytic activity, structural characterizations (especially from Mössbauer spectroscopy), and the results of DFT calculations for adsorption energies of oxygen on main surfaces of Fe2N including ε-Fe2N and ζ-Fe2N, it can be deduced that Fe2N NPs as active species make a contribution to the ORR catalysis, of which ε-FexN (x≤2.1) is more active than ζ-Fe2N. In addition, we find that there exists an obvious synergistic effect between Fe2N NPs and N-doped carbon, leading to the greatly enhanced ORR catalytic activity.

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Publication details

The article was accepted on 06 May 2017 and first published on 12 May 2017


Article type: Paper
DOI: 10.1039/C7NR01925D
Citation: Nanoscale, 2017, Accepted Manuscript
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    The Role of Iron Nitrides in Fe-N-C Catalysis System towards Oxygen Reduction Reaction

    M. Wang, Y. Yang, X. Liu, Z. Pu, Z. Kou, P. Zhu and S. Mu, Nanoscale, 2017, Accepted Manuscript , DOI: 10.1039/C7NR01925D

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