PEI/MWCNT修饰含铁电芬顿电极处理印染废水的研究

doi:10.13209/j.0479-8023.2017.111

摘要/Abstract

摘要：

以褐铁矿粉为铁源, 用聚乙烯亚胺/多壁碳纳米管(polyethylenimine/multi-walled carbon nanotube, PEI/ MWCNT)修饰石墨毡为外层, 制备含铁电芬顿阴极。PEI/MWCNT修饰层可使石墨毡电还原产生H₂O₂的能力增强: 在阴极电位为-0.95 V(vs. SCE)、曝气速率为200 mL/min的条件下, 90分钟反应器内H₂O₂的积累量为66.5±2.4 mg/L, 比普通石墨毡阴极提高56.8%。PEI/MWCNT修饰层具有较好的稳定性, 连续使用20个周期, 修饰石墨毡电还原产生H₂O₂的能力未发生明显变化。采用以制备电极为阴极的电芬顿体系处理橙Ⅱ染料模拟废水, 结果表明: 橙Ⅱ染料初始浓度为20 mg/L, 在近中性(初始pH为6~7)条件下, 60分钟内降解效率为96.8%; 制备电极具备一定稳定性, 可重复使用多次。最后对以制备电极为阴极的电芬顿体系处理实际印染废水的能力进行测试, 在近中性条件下电解2小时后, 废水色度去除率为91.7%, COD去除率为69.4%, 氨氮去除率为56.2%。

关键词: 电芬顿, MWCNT, 褐铁矿, 橙Ⅱ, 染料, 印染废水

Abstract:

An iron-doped (using limonite as the source of iron) cathode with PEI/MWCNT (polyethylenimine/ Multi- walled carbon nanotube) modified carbon felt outer layers was prepared for Electro-Fenton systems. PEI/MWCNT multi-layers could significantly increase the production of H₂O₂. The highest H₂O₂ accumulation was achieved up to 66.5 ± 2.4 mg/L at -0.95 V, neutral pH and 200 mL/min of aeration rate, which increased about 56.8% than the carbon felt at the same condition. The PEI/MWCNT multi-layers were stable enough that there was no obvious decrease in H₂O₂ accumulation after 20 recycles. This study tested the performance of the prepared cathode in treating the simulated dyeing wastewater. The results were as follows: Orange II with initial concentration of 20 mg/L at neutral pH (pH₀=6-7) was discolored completely after 60 min electrolysis process, and the decolorizing efficiency was up to 96.8%. In addition, the prepared cathode was stable enough and could be reused without catalytic activity decrease. This study also tested the performance of the prepared cathode in treating the actual dyeing wastewater. The chroma, COD and ammonia-nitrogen removal efficiency after 120 min electrolysis process were 91.7%, 69.4%, and 56.2% respectively.

Key words: Electron-Fenton, MWCNT, limonite, Orange Ⅱ, dye, dyeing wastewater

陶虎春, 石刚, 于太安, 李金龙, 李金波, 许楠. PEI/MWCNT修饰含铁电芬顿电极处理印染废水的研究[J]. 北京大学学报自然科学版, 2017, 53(5): 982-988.

Huchun TAO, Gang SHI, Taian YU, Jinlong Li, Jinbo LI, Nan XU. An Iron-doped Cathode with PEI/MWCNT Modified Carbon Felt Outer Layers for Dyeing Wastewater Treatment by Electro-Fenton System[J]. Acta Scientiarum Naturalium Universitatis Pekinensis, 2017, 53(5): 982-988.

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链接本文: https://xbna.pku.edu.cn/CN/10.13209/j.0479-8023.2017.111

https://xbna.pku.edu.cn/CN/Y2017/V53/I5/982

图/表 7

图1 电极制备过程示意图

Fig. 1 Schematic diagram of the prepared cathode

图2 实验装置示意图

Fig. 2 Schematic diagram of the experimental setup

图3 修饰石墨毡阴极与普通石墨毡阴极电还原生成H2O2能力对比

Fig. 3 Electro-generation of H2O2 by a carbon felt electrode assembling with PEI/MWCNT multilayer films

图4 普通石墨毡纤维表面 SEM 图像(a)、修饰石墨毡纤维表面 SEM 图像(b)、修饰石墨毡纤维表面高倍率 SEM 图像(c)以及普通石墨毡电极与PEI/MWCNT修饰石墨毡电极的启动电流对比(d)

Fig. 4 SEM image of carbon felt (a), SEM image of the PEI/MWCNT modified carbon felt at low (b), and high magnifications (c),and starting current of normal carbon felt and PEI/MWCNT modified carbon felt (d)

图5 不同阴极电化学体系对橙Ⅱ染料模拟废水的降解

Fig. 5 Degradation of Orange Ⅱ in different electrochemical systems by different cathode

图6 应用制备电极的电芬顿体系对橙Ⅱ染料模拟废水的连续7个批次处理

Fig. 6 Degradation of Orange II in Electro-Fenton system by the prepared cathode in 7 cycles

表1 实际废水电芬顿处理前后各项指标

Table 1 Parameters of dyeing wastewater before and after Electron-Fenton process

参数	处理前	处理后	去除率/%
色度	300	25	91.7
COD	425 mg/L	130 mg/L	69.4
氨氮	1.90 mg/L	0.44 mg/L	56.2

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