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利用具有再生能力的流通式三维活性炭阴极电化学合成羟基自由基用于对硝基苯酚降解

Electrochemical Synthesis of HO for -nitrophenol Degradation Utilizing a Flow-through Three-dimensional Activated Carbon Cathode with Regeneration Capabilities.

作者信息

Compton Patrick, Dehkordi Nazli Rafei, Sarrouf Stephanie, Ehsan Muhammad Fahad, Alshawabkeh Akram N

机构信息

Department of Civil and Environmental Engineering, Northeastern University, Boston, MA, USA.

出版信息

Electrochim Acta. 2023 Feb 10;441. doi: 10.1016/j.electacta.2022.141798. Epub 2022 Dec 28.

Abstract

The growing ubiquity of recalcitrant organic contaminants in the aqueous environment poses risks to effective and efficient water treatment and reuse. A novel three-dimensional (3D) electrochemical flow-through reactor employing activated carbon (AC) encased in a stainless-steel (SS) mesh as a cathode is proposed for the removal and degradation of a model recalcitrant contaminant -nitrophenol (PNP), a toxic compound that is not easily biodegradable or naturally photolyzed, can accumulate and lead to adverse environmental health outcomes, and is one of the more frequently detected pollutants in the environment. As a stable 3D electrode, granular AC supported by a SS mesh frame as a cathode is hypothesized to 1) electrogenerate HO via a 2-electron oxygen reduction reaction on the AC surface, 2) initiate decomposition of this electrogenerated HO to form hydroxyl radicals on catalytic sites of the AC surface 3) remove PNP molecules from the waste stream via adsorption, and 4) co-locate the PNP contaminant on the carbon surface to allow for oxidation by formed hydroxyl radicals. Additionally, this design is utilized to electrochemically regenerate the AC within the cathode that is significantly saturated with PNP to allow for environmentally friendly and economic reuse of this material. Under flow conditions with optimized parameters, the 3D AC electrode is nearly 20% more effective than traditional adsorption in removing PNP. 30 grams of AC within the 3D electrode can remove 100% of the PNP compound and 92% of TOC under flow. The carbon within the 3D cathode can be electrochemically regenerated in the proposed flow system and design thereby increasing the adsorptive capacity by 60%. Moreover, in combination with continuous electrochemical treatment, the total PNP removal is enhanced by 115% over adsorption. It is anticipated this platform holds great promises to eliminate analogous contaminants as well as mixtures.

摘要

难降解有机污染物在水环境中日益普遍,给高效水处理及回用带来风险。本文提出一种新型三维(3D)电化学流通式反应器,该反应器采用包裹在不锈钢(SS)网中的活性炭(AC)作为阴极,用于去除和降解典型难降解污染物——硝基苯酚(PNP)。PNP是一种有毒化合物,不易生物降解或自然光解,会累积并导致不良环境健康后果,是环境中较常检测到的污染物之一。作为一种稳定的3D电极,由SS网框架支撑的颗粒状AC作为阴极,推测其作用如下:1)通过AC表面的双电子氧还原反应电生成HO;2)使电生成的HO在AC表面催化位点引发分解形成羟基自由基;3)通过吸附从废水中去除PNP分子;4)使PNP污染物共定位在碳表面,以便被形成的羟基自由基氧化。此外,该设计用于对阴极中被PNP显著饱和的AC进行电化学再生,以实现该材料的环境友好和经济回用。在优化参数的流动条件下,3D AC电极去除PNP的效率比传统吸附法高出近20%。3D电极内的30克AC在流动条件下可去除100%的PNP化合物和92%的总有机碳(TOC)。3D阴极内的碳可在所提出的流动系统和设计中进行电化学再生,从而使吸附容量提高60%。此外,结合连续电化学处理,PNP的总去除率比吸附法提高了115%。预计该平台在消除类似污染物及混合物方面具有巨大潜力。

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