Swiss-roll electrodes for efficient degradation of carbofuran by electrochemical advanced oxidation processes
Swiss-roll electrodes for efficient degradation of carbofuran by electrochemical advanced oxidation processes
复制标题
通过电化学高级氧化工艺有效降解克百威的瑞士卷电极
DOI：
10.1016/j.jece.2022.108801
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发表时间：
2022
影响因子：
7.7
通讯作者：
Ookawara Shinichi
中科院分区：
文献类型：
--
作者：
Zhang Bei;Hiramatsu Toshiya;Hamano Shinji;Fujii Manabu;Alalm Mohamed Gar;Yoshikawa Shiro;Matsumoto Hideyuki;Ookawara Shinichi
电化学高级氧化工艺(EAOPs)已被广泛用于降解新出现的污染物。然而，只有电极的组成得到了很好的研究，而对电极结构的研究却很少。这项工作开发了一种新的电极结构，沿着优化的阿基米德螺线滚动，形成了一个“瑞士卷”。通过改变电极结构和电化学氧化条件，考察了电极间距、电极面积和电流对电极性能的影响。电极间距的增加有利于过氧化氢的积累，但不利于克百威的阳极氧化。电极间距适中的EAOPs表现出电Fenton过程和阳极氧化过程对克百威的协同去除作用。通过改变电极面积和电流来优化电流密度。电流密度的增加促进了H_2O_2和·OH的生成，从而显著提高了电-Fenton法对克百威的去除效果。因此，建立了新的动力学模型，并用实验数据进行了验证，以描述电-Fenton和阳极氧化耦合反应。对转化产物的分析表明，·OH的连续产生加速了克百威和转化产物的裂解和开环。该反应堆在长期EAOPS中消耗的电能很低(34.4千瓦时/公斤)，在大规模应用中提供了性能和成本方面的有前途的解决方案。
Electrochemical advanced oxidation processes (EAOPs) have been extensively investigated for the degradation of emerging contaminants. However, only the composition of electrodes is well studied but less for the electrode configuration. This work developed a new configuration of electrodes rolled along the optimized Archimedes spirals shaping a “Swiss roll”. The effects of electrode distance, electrode area and current were investigated via regulating the electrode configuration and EAOPs conditions. The increasing electrode distance contributed to the H2O2accumulation but went against the anodic oxidation of carbofuran. The EAOPs with moderate electrode distance showed synergetic removal of carbofuran by electro-Fenton and anodic oxidation processes. The current density was optimized by changing electrode area and current. The increasing current density promoted the generation of H2O2and•OH, which could significantly improve the removal of carbofuran by electro-Fenton process. Accordingly, novel kinetic models were developed and validated with experimental data to describe the coupled electro-Fenton and anodic oxidation reactions. Examination of transformation products indicated that the continuous production of•OH accelerated the cleavage and ring-opening of carbofuran and transformation products. The reactor consumed low electrical energy (34.4 kWh/kg) in long-term EAOPs, providing promising solutions in terms of performance and cost in large-scale applications.