학술논문
Mechanochemical route to fabricate an efficient nitrate reduction electrocatalyst
Document Type
Original Paper
Author
Source
Nano Research. 17(6):4889-4897
Subject
Language
English
ISSN
1998-0124
1998-0000
1998-0000
Abstract
The electrochemical nitrate reduction reaction (NO3 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 °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, NH2 OH, 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 NO3 RR and opens the road for solving environmental and energy challenges.