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Phosphorus-doping activates carbon nanotubes for efficient electroreduction of nitrogen to ammonia

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Abstract

The electrochemical nitrogen reduction reaction (NRR) as an energy-efficient approach for ammonia synthesis is hampered by the low ammonia yield and ambiguous reaction mechanism. Herein, phosphorus-doped carbon nanotube (P-CNTs) is developed as an efficient metal-free electrocatalyst for NRR with a remarkable NH3 yield of 24.4 μg·h−1·mg−1cat. and partial current density of 0.61 mA·cm−2. Such superior activity is found to be from P doping and highly conjugated CNTs substrate. Experimental and theoretical investigations discover that the electron-deficient phosphorus sites with Lewis acidity should be genuine active sites and NRR on P-CNTs follows the distal pathway. These findings provide insightful understanding on NRR processes on P-CNTs, opening up opportunities for the rational design of highly-active cost-effective metal-free catalysts for electrochemical ammonia synthesis.

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Acknowledgements

We acknowledge the financial supports are from the National Key Research and Development Program of China (No. 2016YFB0101202), the National Natural Science Foundation of China (Nos. 91645123 and 21773263).

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Authors and Affiliations

  1. Beijing National Laboratory for Molecular Sciences (BNLMS), CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China

    Lu-Pan Yuan, Ze-Yuan Wu, Wen-Jie Jiang, Tang Tang, Shuai Niu & Jin-Song Hu

  2. University of Chinese Academy of Sciences, Beijing, 100049, China

    Lu-Pan Yuan, Ze-Yuan Wu, Tang Tang, Shuai Niu & Jin-Song Hu

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  1. Lu-Pan Yuan
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  2. Ze-Yuan Wu
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Yuan, LP., Wu, ZY., Jiang, WJ. et al. Phosphorus-doping activates carbon nanotubes for efficient electroreduction of nitrogen to ammonia. Nano Res. 13, 1376–1382 (2020). https://doi.org/10.1007/s12274-020-2637-8

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