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Research Article

Mechanochemical route to fabricate an efficient nitrate reduction electrocatalyst

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.

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Graphical Abstract

Magnetic-biochar was prepared by a two-step ball milling method for the electrocatalytic reduction of nitrate to ammonia. Mechanochemical force can effectively enhance the properties of biochar by reducing particle size, increasing surface area, and enriching oxygen-containing functional groups, thereby promoting water adsorption and facilitating the reduction of nitrate to ammonia.

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

mechanochemical routemagnetic biocharelectron transfernitrateammonia

Electronic Supplementary Material

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Nano Research
Volume 17 Issue 6,
June 2024
Pages 4889-4897
DOI: 10.1007/s12274-024-6478-8
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
Topics:
CarbonElectrocatalystsElectrolytic reduction

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Received: 05 November 2023
Revised: 30 December 2023
Accepted: 09 January 2024
Published: 08 February 2024
© Tsinghua University Press 2024
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