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Mechanochemical route to fabricate an efficient nitrate reduction electrocatalyst

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Abstract

The electrochemical nitrate reduction reaction (NO3RR) to ammonia under ambient conditions is a promising approach for addressing elevated nitrate levels in water bodies, but the progress of this reaction is impeded by the complex series of chemical reactions involving electron and proton transfer and competing hydrogen evolution reaction. Therefore, it becomes imperative to develop an electro-catalyst that exhibits exceptional efficiency and remarkable selectivity for ammonia synthesis while maintaining long-term stability. Herein the magnetic biochar (Fe-C) has been synthesized by a two-step mechanochemical route after a pyrolysis treatment (450, 700, and 1000 °C), which not only significantly decreases the particle size, but also exposes more oxygen-rich functional groups on the surface, promoting the adsorption of nitrate and water and accelerating electron transfer to convert it into ammonia. Results showed that the catalyst (Fe-C-700) has an impressive NH3 production rate of 3.5 mol·h−1·gcat−1, high Faradaic efficiency of 88%, and current density of 0.37 A·cm−2 at 0.8 V vs. reversible hydrogen electrode (RHE). In-situ Fourier transform infrared spectroscopy (FTIR) is used to investigate the reaction intermediate and to monitor the reaction. The oxygen functionalities on the catalyst surface activate nitrate ions to form various intermediates (NO2, NO, NH2OH, and NH2) and reduce the rate determining step energy barrier (*NO3 → *NO2). This study presents a novel approach for the use of magnetic biochar as an electro-catalyst in NO3RR and opens the road for solving environmental and energy challenges.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 52072152 and 51802126), the Jiangsu University Jinshan Professor Fund, the Jiangsu Specially-Appointed Professor Fund, Open Fund from Guangxi Key Laboratory of Electrochemical Energy Materials, Zhenjiang “Jinshan Talents” Project 2021, China PostDoctoral Science Foundation (No. 2022M721372), “Doctor of Entrepreneurship and Innovation” in Jiangsu Province (No. JSSCBS20221197), the Postgraduate Research & Practice Innovation Program of Jiangsu Province (No. KYCX22_3645), the National Natural Science Foundation of China (No. 22208134), and Jiangsu Agricultural Science and Technology Innovation Fund (No. CX(21)1010).

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  1. Yunliang Liu and Zhiyu Zheng contributed equally to this work.

Authors and Affiliations

  1. Institute for Energy Research, School of Energy and Power Engineering, Jiangsu University, Zhenjiang, 212013, China

    Yunliang Liu, Sobia Jabeen, Naiyun Liu, Yixian Liu, Yuanyuan Cheng, Yaxi Li, Jingwen Yu, Xin Wu & Haitao Li

  2. Jiangsu Engineering Technology Research Center of Biomass Composites and Addictive Manufacturing, Institute of Agricultural Facilities and Equipment, Jiangsu Academy of Agricultural Sciences, Nanjing, 210014, China

    Zhiyu Zheng, Nina Yan & Lei Xu

  3. Key Laboratory for Protected Agricultural Engineering in the Middle and Lower Reaches of Yangtze River, Ministry of Agriculture and Rural Affairs, Nanjing, 210014, China

    Zhiyu Zheng, Nina Yan & Lei Xu

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  1. Yunliang Liu
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  8. Jingwen Yu
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  9. Xin Wu
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  10. Nina Yan
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  11. Lei Xu
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  12. Haitao Li
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Corresponding authors

Correspondence to Naiyun Liu, Nina Yan, Lei Xu or Haitao Li.

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Liu, Y., Zheng, Z., Jabeen, S. et al. Mechanochemical route to fabricate an efficient nitrate reduction electrocatalyst. Nano Res. (2024). https://doi.org/10.1007/s12274-024-6478-8

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  • DOI: https://doi.org/10.1007/s12274-024-6478-8

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