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Nano Research 2021, 14(1): 122-130 https://doi.org/10.1007/s12274-020-3054-8
Research Article | Issue | Published: 05 January 2021

Highly active sites of low spin FeⅡN4 species: The identification and the ORR performance

Show Author's Information Huizhu Cai1,  Bingbing Chen1,  Xiao Zhang1,  Yuchen Deng2,  Dequan Xiao3,  Ding Ma2( ),  Chuan Shi1( )
State Key Laboratory of Fine Chemicals, College of Chemical Engineering, Dalian University of Technology, Dalian 116024, China
College of Chemistry and Molecular Engineering and College of Engineering, Peking University, Beijing 100871, China
Center for Integrative Materials Discovery, Department of Chemistry and Chemical Engineering, University of New Haven, CT 06516, USA
Keywords:
oxygen reduction reaction, electrocatalysis, single sites of FeN4, structure-performance correlation
Topics:
AmmoniaCatalysis Electrolytic reduction Iron compoundsOxygen reduction reaction
Cite this article:
Cai H, Chen B, Zhang X, et al. Highly active sites of low spin FeⅡN4 species: The identification and the ORR performance. Nano Research, 2021, 14(1): 122-130. https://doi.org/10.1007/s12274-020-3054-8
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Abstract Full text Electronic supplementary material About this article

Over recent years, catalytic materials of Fe-N-C species have been recognized being active for oxygen reduction reaction (ORR). However, the identification of active site remains challenging as it generally involves a pyrolysis process and mixed components being obtained. Herein Fe3C/C and Fe2N/C samples were synthesized by temperature programmed reduction of Fe precursors in 15% CH4/H2 and pure NH3, respectively. By acid leaching of Fe2N/C sample, only single sites of FeN4 species were presented, providing an ideal model for identification of catalytic functions of the single sites of FeN4 in ORR. A correlation was conducted between the concentration of FeⅡN4 in low spin state by Mössbauer spectra and the kinetic current density at 0.8 V in alkaline media, and such a structure-performance correlation assures the catalytic roles of low spin FeⅡN4 species as highly active sites for the ORR.


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Electronic supplementary material
About this article

Highly active sites of low spin FeⅡN4 species: The identification and the ORR performance

Show Author's information Huizhu Cai1, Bingbing Chen1, Xiao Zhang1, Yuchen Deng2, Dequan Xiao3, Ding Ma2( ), Chuan Shi1( )
State Key Laboratory of Fine Chemicals, College of Chemical Engineering, Dalian University of Technology, Dalian 116024, China
College of Chemistry and Molecular Engineering and College of Engineering, Peking University, Beijing 100871, China
Center for Integrative Materials Discovery, Department of Chemistry and Chemical Engineering, University of New Haven, CT 06516, USA

Abstract

Over recent years, catalytic materials of Fe-N-C species have been recognized being active for oxygen reduction reaction (ORR). However, the identification of active site remains challenging as it generally involves a pyrolysis process and mixed components being obtained. Herein Fe3C/C and Fe2N/C samples were synthesized by temperature programmed reduction of Fe precursors in 15% CH4/H2 and pure NH3, respectively. By acid leaching of Fe2N/C sample, only single sites of FeN4 species were presented, providing an ideal model for identification of catalytic functions of the single sites of FeN4 in ORR. A correlation was conducted between the concentration of FeⅡN4 in low spin state by Mössbauer spectra and the kinetic current density at 0.8 V in alkaline media, and such a structure-performance correlation assures the catalytic roles of low spin FeⅡN4 species as highly active sites for the ORR.

Keywords: oxygen reduction reaction, electrocatalysis, single sites of FeN4, structure-performance correlation

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Acknowledgements

Publication history

Received: 24 May 2020
Revised: 12 August 2020
Accepted: 12 August 2020
Published: 05 January 2021
Issue date: January 2021

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature

Acknowledgements

The work was supported by the National Key R&D Program of China (No. 2017YFA0700103), the National Natural Science Foundation of China (Nos. 21932002, 21872014, 21707015, 21902018, and 21577013), the Postdoctoral Science Foundation of China (Nos. 2019T120210, 2018M641687) and the Natural Science Foundation of Liaoning Province (No. 2019-MS-053).

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