Square-wave pulsed potential driven electrocatalytic degradation of 4-chlorophenol using Fe-Ni/rGO/PPy@NF three dimensional electrode.

Journal of hazardous materials Pub Date : 2024-12-05 Epub Date: 2024-10-04 DOI:10.1016/j.jhazmat.2024.136054
Bei Ma, Bobing Lu, Hanyu Tang, Hui Wang, Zhaoyong Bian
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Abstract

To develop an energy-efficient system for the removal of chlorinated organic pollutants, Fe-Ni/reduced graphite oxide/polymerized polypyrrole@nickel foam was constructed as a catalytic cathode for pulsed electrocatalytic degradation, where cathode-catalyzed production of hydrogen radicals (H*) and hydroxyl radical (·OH) generated at the anode led to dechlorination of 4-chlorophenol (4-CP), and dechlorination products were mineralized and degraded under the action of·OH. When energy was continuously supplied to the reaction system in the constant potential mode, the 4-CP concentration near the electrode was insufficient, limiting the reaction rate. Conversely, in the square-wave pulsed potential mode, mass transfer limitations were mitigated, significantly enhancing reaction efficiency and reducing energy consumption. At -1.2 V (vs. Ag/AgCl), the 4-CP removal efficiency reached 93.79 % in the pulsed potential mode, surpassing the constant potential mode's performance of 81.40 %. The synergistic periodic oscillation of the potential, direct electron transfer, and catalytic generation of active free radicals in the pulsed potential mode reduced intermediate concentrations and increased 4-CP mineralization, while the degradation pathway remained unchanged. This research presents a method for the efficient treatment of chlorinated organic pollutants in water using pulsed electrocatalytic degradation.

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使用 Fe-Ni/rGO/PPy@NF 三维电极对 4-氯苯酚进行方波脉冲电位驱动电催化降解。
为了开发一种去除氯化有机污染物的高能效系统,构建了铁-镍/还原氧化石墨/聚合聚吡咯@镍泡沫作为脉冲电催化降解的催化阴极、在阴极催化下,阳极产生的氢自由基(H*)和羟自由基(-OH)导致 4-氯苯酚(4-CP)脱氯,脱氯产物在羟自由基的作用下矿化降解。在恒定电位模式下,当持续向反应系统提供能量时,电极附近的 4-CP 浓度不足,从而限制了反应速率。相反,在方波脉冲电位模式下,传质限制得到缓解,大大提高了反应效率并降低了能耗。在 -1.2 V 的电压下(相对于 Ag/AgCl),脉冲电位模式下的 4-CP 去除效率达到 93.79%,超过恒定电位模式下的 81.40%。在脉冲电位模式下,电位的周期性振荡、直接电子传递和活性自由基的催化生成协同作用,在降解途径保持不变的情况下,降低了中间体浓度,提高了 4-CP 的矿化度。这项研究提出了一种利用脉冲电催化降解高效处理水中氯化有机污染物的方法。
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