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2024年6月27日,Elsevier 旗下top期刊《Journal of Colloid and Interface Science》(影响因子:9.4)在线发表了云南师范大学化学化工学院赵学教授最新研究成果《Self-supported iron-doped cobalt–copper oxide heterostructures for efficient electrocatalytic denitrification》。云南师范大学化学化工学院赵学、湖北文理学院湖北文理学院,低维光电材料与器件湖北省重点实验室周书星副教授和云南大学胡广志教授教授为共同通讯作者。
https://www.sciencedirect.com/science/article/abs/pii/S002197972401453X
Abstract
The electrocatalytic reduction of nitrate ions (NO3−) to nitrogen gas (N2) has emerged as an effective approach for mitigating nitrate pollution in water bodies. However, the development of efficient and highly selective cathode materials remains challenging. Conventional copper-based catalysts often exhibit low selectivity because they strongly adsorb oxygen. In this study, a straightforward solvothermal and pyrolysis method was used to grow iron-doped cobalt–copper oxide heterogeneous structures on copper foam surfaces (Fe–CoO/CuO@CF). Then, the effects of the applied potential, initial NO3− concentration, Cl− concentration, electrolyte pH, and different catalysts on the catalyst performance were investigated. Compared with recently reported congeners, Fe–CoO/CuO@CF is less expensive and exhibits outstanding activity for NO3− reduction. Meanwhile, under a cathode potential of − 1.31 V vs. Ag/AgCl, Fe–CoO/CuO@CF degrades 98.6 % of NO3− in 200 min. In addition, when employing a method inspired by NH4+ removal by breakpoint chlorination, N2 selectivity over Fe–CoO/CuO@CF was raised from 10 % without Cl− to 99.7 % when supplemented with Cl−. The catalyst demonstrated excellent cyclic stability, maintaining a high electrocatalytic activity for the conversion of NO3− to N2 gas over eleven cycles. Moreover, Fe–CoO/CuO@CF enabled 63.7 % removal of NO3− from wastewater (50 mg/L NO3−–N) prepared from natural water, with 100 % conversion to N2. Computational studies showed that iron doping decreased the free energy change of the intermediate of NO3− reduction reaction. This study provides an effective strategy for the electrochemical reduction of nitrate to nitrogen gas and offers good prospects for addressing nitrate pollution.
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