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Nano Research 2024, 17(6): 4889-4897 https://doi.org/10.1007/s12274-024-6478-8
Research Article | Issue | Published: 08 February 2024

Mechanochemical route to fabricate an efficient nitrate reduction electrocatalyst

Show Author's Information Yunliang Liu1,§,  Zhiyu Zheng2,3,§,  Sobia Jabeen1,  Naiyun Liu1( ),  Yixian Liu1,  Yuanyuan Cheng1,  Yaxi Li1,  Jingwen Yu1,  Xin Wu1,  Nina Yan2,3( ),  Lei Xu2,3( ),  Haitao Li1( )
Institute for Energy Research, School of Energy and Power Engineering, Jiangsu University, Zhenjiang 212013, China
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
Key Laboratory for Protected Agricultural Engineering in the Middle and Lower Reaches of Yangtze River, Ministry of Agriculture and Rural Affairs, Nanjing 210014, China

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

Keywords:
ammonia, electron transfer, nitrate, mechanochemical route, magnetic biochar
Topics:
CarbonElectrocatalystsElectrolytic reduction
Cite this article:
Liu Y, Zheng Z, Jabeen S, et al. Mechanochemical route to fabricate an efficient nitrate reduction electrocatalyst. Nano Research, 2024, 17(6): 4889-4897. https://doi.org/10.1007/s12274-024-6478-8
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Abstract Full text Electronic supplementary material About this article

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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Electronic supplementary material
About this article

Mechanochemical route to fabricate an efficient nitrate reduction electrocatalyst

Show Author's information Yunliang Liu1,§, Zhiyu Zheng2,3,§, Sobia Jabeen1, Naiyun Liu1( ), Yixian Liu1, Yuanyuan Cheng1, Yaxi Li1, Jingwen Yu1, Xin Wu1, Nina Yan2,3( ), Lei Xu2,3( ), Haitao Li1( )
Institute for Energy Research, School of Energy and Power Engineering, Jiangsu University, Zhenjiang 212013, China
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
Key Laboratory for Protected Agricultural Engineering in the Middle and Lower Reaches of Yangtze River, Ministry of Agriculture and Rural Affairs, Nanjing 210014, China

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

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.

Keywords: ammonia, electron transfer, nitrate, mechanochemical route, magnetic biochar

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Publication history
Copyright
Acknowledgements

Publication history

Received: 05 November 2023
Revised: 30 December 2023
Accepted: 09 January 2024
Published: 08 February 2024
Issue date: June 2024

Copyright

© Tsinghua University Press 2024

Acknowledgements

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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