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用于高效电催化硝酸盐还原的三维铜纳米带阴极

A three-dimensional Cu nanobelt cathode for highly efficient electrocatalytic nitrate reduction.

作者信息

Wang Xiaodan, Zhu Mengqi, Zeng Guoshen, Liu Xun, Fang Chihhsiang, Li Chuanhao

机构信息

School of Environmental Science and Engineering and Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Sun Yat-sen University, Guangzhou 510006, China.

出版信息

Nanoscale. 2020 May 7;12(17):9385-9391. doi: 10.1039/c9nr10743f. Epub 2020 Mar 20.

Abstract

Water treatment techniques for destructive removal of nitrates by reducing them to harmless N have recently begun to emerge. In this study, we present a novel three-dimensional (3D) Cu nanobelt cathode for efficient electrochemical nitrate reduction. Upon an applied potential of -1.4 V vs. Ag/AgCl, the removal efficiency of nitrates by the 3D Cu nanobelt electrode reaches 100% at 60 min, compared to 2.6% for the Cu foam electrode under the same conditions. Based on the mass balance on nitrogen atoms, the major product is determined to be ammonia. In the simulated wastewater containing NaCl, the as-generated ammonia ions are simultaneously oxidized into harmless N by the in situ generated ClO ions from the Pt anode, resulting in the complete removal of inorganic nitrogen (nitrate, nitride and ammonia) from wastewater. The mechanism for the improvement of electrocatalytic activity is systematically investigated. Firstly, the large surface area of the 3D Cu nanobelt electrode facilitates the mass transfer of nitrates, resulting in accelerated electrochemical kinetics. Secondly, linear sweep voltammetry (LSV) and electrochemical impedance spectroscopy (EIS) measurements confirm that the 3D Cu nanobelt electrode exhibits improved charge transfer ability. Also, further investigations demonstrate that the 3D Cu nanobelt electrode preferentially reacts with nitrates, compared to the pristine Cu foam electrode readily reacting with the dissolved oxygen (DO) to generate HO. This study might expand the prospects of electrocatalytic techniques towards the destructive removal of inorganic nitrogen pollutants in wastewater.

摘要

通过将硝酸盐还原为无害的氮来进行破坏性去除的水处理技术最近已开始出现。在本研究中,我们展示了一种用于高效电化学硝酸盐还原的新型三维(3D)铜纳米带阴极。在相对于Ag/AgCl为 -1.4 V的外加电势下,3D铜纳米带电极在60分钟时对硝酸盐的去除效率达到100%,而在相同条件下铜泡沫电极的去除效率为2.6%。基于氮原子的质量平衡,确定主要产物为氨。在含有NaCl的模拟废水中,生成的氨离子同时被铂阳极原位生成的ClO离子氧化为无害的氮,从而实现废水中无机氮(硝酸盐、亚硝酸盐和氨)的完全去除。系统地研究了电催化活性提高的机制。首先,3D铜纳米带电极的大表面积促进了硝酸盐的传质,导致电化学动力学加速。其次,线性扫描伏安法(LSV)和电化学阻抗谱(EIS)测量证实3D铜纳米带电极表现出改善的电荷转移能力。此外,进一步的研究表明,与原始铜泡沫电极容易与溶解氧(DO)反应生成羟基相比,3D铜纳米带电极优先与硝酸盐反应。本研究可能会拓展电催化技术在废水无机氮污染物破坏性去除方面的前景。

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