Research Article

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2021, 14(1): 122–130

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https://doi.org/10.1007/s12274-020-3054-8

Highly active sites of low spin FeN4 species: The identification and the ORR performance

Huizhu Cai1, Bingbing Chen1, Xiao Zhang1, Yuchen Deng2, Dequan Xiao3, Ding Ma2 (✉), and Chuan Shi1 (✉)

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1 State Key Laboratory of Fine Chemicals, College of Chemical Engineering, Dalian University of Technology, Dalian 116024, China
2 College of Chemistry and Molecular Engineering and College of Engineering, Peking University, Beijing 100871, China
3 Center for Integrative Materials Discovery, Department of Chemistry and Chemical Engineering, University of New Haven, CT 06516, USA

Keywords: single sites of FeN4, oxygen reduction reaction, structure-performance correlation, electrocatalysis
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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 Fe N4 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 Fe N4 species as highly active sites for the ORR.
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Highly active sites of low spin FeN4 species: The identification and the ORR performance. Nano Res. 2021, 14(1): 122–130 https://doi.org/10.1007/s12274-020-3054-8

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