Electrochemical reduction of nitrate via Cu/Ni composite cathode paired with Ir-Ru/Ti anode: High efficiency and N2 selectivity

Electrochemical reduction of nitrate via Cu/Ni composite cathode paired with Ir-Ru/Ti anode: High efficiency and N2 selectivity
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通过 Cu/Ni 复合阴极与 Ir-Ru/Ti 阳极配对电化学还原硝酸盐:高效率和 N2 选择性

DOI:
10.1016/j.electacta.2018.08.154
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发表时间:
2018-11
影响因子:
6.6
通讯作者:
Fei Wang
Fei Wang
中科院分区:
材料科学2区
文献类型:
--
作者:
Yimei Zhang;Yalong Zhao;Zhuang Chen;Liqun Wang;Panpan Wu;Fei Wang

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针对水源地硝酸盐污染严重的问题,采用阴极电沉积法制备了Cu/Ni复合电极。通过扫描电子显微镜、能量色散谱和X射线衍射表征证实,Cu纳米颗粒成功沉积在泡沫镍表面,呈不规则球形结构,直径约为900 nm。在硝酸盐电还原实验中,Cu/Ni电极被用作阴极,与Ni泡沫电极(15.0%去除)相比,在60分钟内实现了几乎完全去除硝酸盐。线性扫描伏安法和电化学阻抗谱分析表明,催化活性中心的增加和电极电阻的降低是催化剂性能提高的主要原因。影响电解的参数,包括电流密度,Cl−浓度和溶液pH值进行了评估。结果表明:(a)增大电流密度有利于硝酸盐的去除,但降低了电子能量利用效率;(B)Cl−的存在对硝酸盐的去除略有阻碍,但对NH 4 +-N的去除有显著促进作用;(c)酸性条件不利于硝酸盐和总氮的去除。此外,重复使用实验的Cu/Ni电极超过8个周期进行。这表明Cu/Ni电极具有优异的稳定性,在8次循环中保持>95.0%的高去除效率。最后,提出了Cu/Ni阴极电还原去除硝酸盐的可能途径。
To address the severe nitrate contamination of water sources, a Cu/Ni bimetallic composite electrode was successfully prepared via cathodic electrodeposition method. Characterization by scanning electron microscopy, energy-dispersive spectroscopy, and X-ray diffraction confirmed that Cu nanoparticles were successfully deposited on the surface of Ni foam as irregular spherical structures with a diameters of 900 nm. The Cu/Ni electrode was applied as a cathode in nitrate electroreduction experiments, achieving nearly complete removal of nitrate within 60 min compared to a Ni foam electrode (15.0% removal). The improved performance was attributed to the dramatically increased catalytically active sites and the decreased resistance of the electrode, as shown by linear sweep voltammetry and electrochemical impedance spectroscopy analyses. The parameters influencing electrolysis, including current density, Cl−concentration, and solution pH were evaluated. It was concluded that (a) Increasing the current density favored nitrate removal, but reduced the electronic energy utilization efficiency; (b) Cl−presence hindered nitrate removal slightly, but facilitated NH4+-N removal significantly; (c) Acidic conditions were detrimental to nitrate and total nitrogen removal. Additionally, reusability experiments of the Cu/Ni electrode over eight cycles were performed. These indicated that the Cu/Ni electrode possessed excellent stability, maintaining a high removal efficiency of >95.0% over eight cycles. Finally, a possible removal pathway of nitrate electroreduction with the Cu/Ni cathode was proposed.
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