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Phosphorus-doped iron-nitrogen-carbon catalyst with penta-coordinated single atom sites for efficient oxygen reduction

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Abstract

Single-atomic Fe-N4 is the well-acknowledged active site in iron-nitrogen-carbon (Fe-N-C) material for oxygen reduction reaction (ORR). The adjusting of the electronic distribution of Fe-N4 is promising for further enhancing the performance of the Fe-N-C catalyst. Herein, a phosphorus (P)-doped Fe-N-C catalyst with penta-coordinated single atom sites (FeNPC) is reported for efficient oxygen reduction. Fe K-edge X-ray absorption spectroscopy (XAS) verifies the coordination environment of single Fe atom, while density functional theory (DFT) calculations reveal that the penta-coordination and neighboring doped P atoms can simultaneously change the electronic distribution of Fe-N4 and its adsorption strength of key intermediates, reducing the reaction-free energy of the potential-limiting step. Electrochemical tests validate the remarkable intrinsic ORR activity of FeNPC in alkaline media (a half-wave potential (E1/2) of 0.904 V vs. reversible hydrogen electrode (RHE) and limited current density (JL) of 6.23 mA·cm−2) and an enhanced ORR performance in neutral (E1/2 = 0.751 V, JL = 5.27 mA·cm−2) and acidic media (E1/2 = 0.735 V, JL = 5.82 mA·cm−2) with excellent stability, highlighting the benefits of optimizing the local environment of single-atomic Fe-N4.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 21875285, 22171288, and 22005340), the Key Research and Development Projects of Shandong Province (No. 2019JZZY010331), and the Natural Science Foundation of Shandong Province (No. ZR2020MB017).

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  1. Lili Fan and **aofei Wei contributed equally to this work.

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  1. School of Materials Science and Engineering, China University of Petroleum (East China), Qingdao, 266580, China

    Lili Fan, **aofei Wei, Xuting Li, Zhanning Liu, Shuo Liu, Zixi Kang, Fangna Dai, **aoqing Lu & Daofeng Sun

  2. College of Science, China University of Petroleum (East China), Qingdao, 266580, China

    Mengfei Li

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Fan, L., Wei, X., Li, X. et al. Phosphorus-doped iron-nitrogen-carbon catalyst with penta-coordinated single atom sites for efficient oxygen reduction. Nano Res. 16, 1810–1819 (2023). https://doi.org/10.1007/s12274-022-4939-5

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