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具有 pH 调节功能的单宁酸-Fe 配合物衍生物修饰电极用于电芬顿过程的环境修复。

Tannic acid-Fe complex derivative-modified electrode with pH regulating function for environmental remediation by electro-Fenton process.

机构信息

Collaborative Innovation Center of Atmospheric Environment and Equipment Technology, Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, School of Environmental Science and Engineering, Nanjing University of Information Science and Technology, Nanjing, 210044, PR China.

Collaborative Innovation Center of Atmospheric Environment and Equipment Technology, Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, School of Environmental Science and Engineering, Nanjing University of Information Science and Technology, Nanjing, 210044, PR China.

出版信息

Environ Res. 2022 Mar;204(Pt A):111994. doi: 10.1016/j.envres.2021.111994. Epub 2021 Sep 3.

Abstract

A heterogeneous electro-Fenton (hetero-EF) system can effectively broaden the applicable pH range, although the decreased electrogeneration efficiency of HO at elevated pH (especially neutral conditions) is unfavorable for the efficient removal of organic pollutants. Herein, a tannic acid-Fe complex derivative-modified carbon felt (TFD@CF) cathode was prepared for hetero-EF treatment of organic pollutants over a wide pH range. Interestingly, the as-prepared hetero-EF cathode could act as a pH regulator that acidified the solution over a wide pH range. As expected, the TFD@CF cathode exhibited excellent hetero-EF activity for the removal of diverse organic pollutants (such as methyl orange, methylene blue, sulfamerazine, bisphenol A and 2,4-dichlorophenoxyacetic acid) at neutral and even alkaline pH (removal efficiency >90 %). A total of 2.98 kWh kg COD with 83.2 % COD removal could be achieved by the TFD@CF cathode for the treatment of actual textile dyeing secondary wastewater. Electrochemical characterizations proved that the TFD@CF cathode had excellent electrochemical properties with improved electron transfer ability and a well-pronounced Fe(III) electroreductive response. Meanwhile, more acidic groups were newly generated during the electrochemical reaction (an increase of 30.1 %), thus dissociating more H into solution. The identification of reactive oxygen species suggested that OH and O could be responsible for the removal of organic pollutants in the TFD@CF EF system. These interesting findings may provide new insights into the design of multifunctional hetero-EF cathodes for the removal of refractory organic pollutants.

摘要

一种非均相电芬顿(hetero-EF)系统可以有效地拓宽适用的 pH 范围,尽管在较高 pH 下(尤其是中性条件下) HO 的电生成效率降低不利于有效去除有机污染物。本文中,制备了单宁酸-铁配合物衍生修饰的碳纤维毡(TFD@CF)阴极,用于在宽 pH 范围内进行非均相 EF 处理有机污染物。有趣的是,所制备的非均相 EF 阴极可以充当 pH 调节剂,在宽 pH 范围内使溶液酸化。正如预期的那样,TFD@CF 阴极在中性甚至碱性 pH 下对多种有机污染物(如甲基橙、亚甲基蓝、磺胺嘧啶、双酚 A 和 2,4-二氯苯氧乙酸)的去除表现出优异的非均相 EF 活性(去除效率>90%)。通过 TFD@CF 阴极处理实际纺织印染二级废水,可实现 2.98 kWh kg COD,COD 去除率为 83.2%。电化学特性证明 TFD@CF 阴极具有优异的电化学性能,提高了电子转移能力和明显的 Fe(III)电还原响应。同时,在电化学过程中会新生成更多的酸性基团(增加了 30.1%),从而将更多的 H 解离到溶液中。活性氧物种的鉴定表明,OH 和 O 可能是 TFD@CF EF 体系中去除有机污染物的原因。这些有趣的发现可能为设计用于去除难处理有机污染物的多功能非均相 EF 阴极提供新的思路。

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