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Fe(CN)5@PIL-derived N-doped porous carbon with FeCxNy active sites as a robust electrocatalyst for the oxygen reduction reaction

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Abstract

The synthesis and catalytic mechanism of new-type Fe–N co-doping catalysts are important topics for the research on fuel cells. Herein, we report the synthesis and oxygen reduction reaction (ORR) properties of a new Fe–N co-doping carbon composite using poly(ionic liquid)s and ferric salt as precursors. The structural characterizations revealed that the as-prepared material features ordered porous properties with a specific surface area of 719.1 m2 g−1, corresponding to FeCxNy/N-doped porous carbons (FeCxNy/N-PC). The electrochemical measurements indicated they show superior catalytic activity (Tafel slope of 70.8 mV dec−1 and E1/2 of 0.84 V), stability and high methanol tolerance compared to the commercial Pt/C catalyst. Furthermore, density functional theory calculations uncovered that the FeCxNy/N-PC composite catalyzes the ORR according to the four-electron associative mechanism with the free-energy barrier of 0.51 eV in the rate-determining formation of H2O. Interestingly, the electronic structure analysis demonstrated the FeCxNy particles serve as active sites and the synergistic effect of the Fe and N atoms of N-PC can promote the ORR performance.

Graphical abstract: Fe(CN)5@PIL-derived N-doped porous carbon with FeCxNy active sites as a robust electrocatalyst for the oxygen reduction reaction

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Publication details

The article was received on 15 Aug 2018, accepted on 02 Nov 2018 and first published on 07 Nov 2018


Article type: Paper
DOI: 10.1039/C8CY01694A
Citation: Catal. Sci. Technol., 2019, Advance Article
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    Fe(CN)5@PIL-derived N-doped porous carbon with FeCxNy active sites as a robust electrocatalyst for the oxygen reduction reaction

    S. Zhang, Y. Gao, S. Cheng, Y. Yan, S. Zhang, G. Zhuang, S. Deng, Z. Wei, X. Zhong and J. Wang, Catal. Sci. Technol., 2019, Advance Article , DOI: 10.1039/C8CY01694A

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