Mechanochemical route to fabricate an efficient nitrate reduction electrocatalyst  

作　　者：Yunliang Liu Zhiyu Zheng Sobia Jabeen Naiyun Liu Yixian Liu Yuanyuan Cheng Yaxi Li Jingwen Yu Xin Wu Nina Yan Lei Xu Haitao Li 

机构地区：[1]Institute for Energy Research,School of Energy and Power Engineering,Jiangsu University,Zhenjiang 212013,China [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 [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

出　　处：《Nano Research》2024年第6期4889-4897,共9页纳米研究（英文版）

基　　金：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);Jiangsu Agricultural Science and Technology Innovation Fund(No.CX(21)1010).

摘　　要：The electrochemical nitrate reduction reaction(NO_(3)RR)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℃),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 NH_(3)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(NO_(2),NO,NH_(2)OH,and NH_(2))and reduce the rate determining step energy barrier(*NO_(3)→*NO_(2)).This study presents a novel approach for the use of magnetic biochar as an electro-catalyst in NO_(3)RR and opens the road for solving environmental and energy challenges.

关 键 词：mechanochemical route magnetic biochar electron transfer NITRATE ammonia 

分 类 号：O64[理学—物理化学]