生物电芬顿系统在废水处理中的研究进展

doi:10.16085/j.issn.1000-6613.2022-2314

摘要/Abstract

摘要：

随着工业化进程加快，废水的类型和排放量日益增加，对自然环境和人类社会造成了严重危害，因此亟需开发经济高效的废水处理技术。生物电芬顿（BEF）系统是将生物电化学系统与芬顿氧化工艺耦合的水处理技术，其因高效、绿色、节能的特点而受到广泛关注。本文综述了BEF系统的基本原理，讨论了阳极和阴极性能的主要影响因素（微生物胞外电子传递过程、阳极材料、阴极材料、芬顿反应催化剂和系统运行条件），总结了BEF系统在各类废水（染料废水、制药废水、垃圾渗滤液、煤化工废水、养猪废水等）处理中的应用，最后指出BEF系统当前面临的挑战及未来的研究方向，包括开发高效的电极材料和催化剂、耦合其他水处理工艺、降低膜材料成本和开展中试研究等，旨在为BEF系统的进一步发展提供参考。

关键词: 生物电芬顿系统, 阳极性能, 阴极性能, 影响因素, 废水处理

Abstract:

With the acceleration of industrialization, the types and discharge of wastewater are increasing, which has caused serious harm to the natural environment and human society. Therefore, it is urgent to develop economical and efficient wastewater treatment technology. Bio-electro-Fenton (BEF) system is a water treatment technology which combines bioelectrochemical system with Fenton oxidation process. As a high efficiency, green and energy saving approach, BEF system is attracting a growing interest recently. Here, the work principle of BEF system was introduced. Main factors influencing the properties of anode and cathode were discussed, including the extracellular electron transport process of microorganisms, anode materials, cathode materials, catalysts of Fenton reaction and system operating conditions. The application of BEF system in various wastewater (dye wastewater, pharmaceutical wastewater, landfill leachate, coal chemical wastewater and swine wastewater) treatment was summarized. Finally, the current challenges and future research directions of BEF system were pointed out, including developing the efficient electrode materials and catalysts, coupling with other water treatment processes, reducing the cost of membrane materials and conducting pilot studies, in order to support its further development.

Key words: bio-electro-Fenton system, anode performance, cathode performance, influencing factors, wastewater treatment

中图分类号:

X703

武诗宇, 杜志平, 申婧, 李剑锋, 程芳琴, 赵华章. 生物电芬顿系统在废水处理中的研究进展[J]. 化工进展, 2023, 42(11): 5929-5942.

WU Shiyu, DU Zhiping, SHEN Jing, LI Jianfeng, CHENG Fangqin, ZHAO Huazhang. Treatment of wastewater by bio-electro-Fenton system: a review[J]. Chemical Industry and Engineering Progress, 2023, 42(11): 5929-5942.

图/表 10

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微生物	门	种	电子传递机质	参考文献
细菌	变形菌门	沼泽红假单胞菌	细胞接触传递	[12]
		嗜酸性氧化亚铁硫杆菌	细胞接触传递	[14]
		大肠埃希菌	电子传递中介体传递	[15]
		铜绿假单胞菌	电子传递中介体传递	[13]
		运动发酵单胞菌	细胞接触传递、电子传递中介体传递	[16]
		希瓦氏菌	细胞接触传递、纳米导线传递、电子传递中介体传递	[17-19]
		硫还原地杆菌	细胞接触传递、纳米导线传递	[20-21]
	厚壁菌门	丁酸梭菌	细胞接触传递	[22]
真菌	子囊菌门	异常汉逊酵母	细胞接触传递	[23]
		酿酒酵母菌	细胞接触传递、电子传递中介体传递	[24-25]
古菌	广古菌门	产甲烷菌	细胞接触传递、纳米导线传递	[26]

微生物	门	种	电子传递机质	参考文献
细菌	变形菌门	沼泽红假单胞菌	细胞接触传递	[12]
		嗜酸性氧化亚铁硫杆菌	细胞接触传递	[14]
		大肠埃希菌	电子传递中介体传递	[15]
		铜绿假单胞菌	电子传递中介体传递	[13]
		运动发酵单胞菌	细胞接触传递、电子传递中介体传递	[16]
		希瓦氏菌	细胞接触传递、纳米导线传递、电子传递中介体传递	[17-19]
		硫还原地杆菌	细胞接触传递、纳米导线传递	[20-21]
	厚壁菌门	丁酸梭菌	细胞接触传递	[22]
真菌	子囊菌门	异常汉逊酵母	细胞接触传递	[23]
		酿酒酵母菌	细胞接触传递、电子传递中介体传递	[24-25]
古菌	广古菌门	产甲烷菌	细胞接触传递、纳米导线传递	[26]

废水类型	阳极	阴极	催化剂	运行条件	污染物浓度	去除率	参考文献
染料废水
橙黄Ⅱ	碳毡	PPy/AQDS/碳毡	γ-FeOOH	pH=7，外部电阻1000Ω，曝气量100mL/min，γ-FeOOH 1g/L	0.2mmol/L	100%	[41]
橙黄Ⅱ	碳毡	碳纳米管/ γ-FeOOH		pH=7，外部电阻1000Ω	0.1mmol/L	100%	[58]
甲基橙	碳纸+ 颗粒活性炭	负载Pt碳纸+ 颗粒活性炭	FeSO₄·7H₂O	pH=3，外部电阻1000Ω，曝气量150mL/min，FeSO₄·7H₂O 0.05mol/L	300mg/L	86.39%	[40]
甲基橙	石墨纤维刷	Fe₂O₃/活性碳毡		pH=3，外部电阻100Ω，曝气量750mL/min	5mg/L	86.7%	[49]
罗丹明B	活性碳毡	Fe@Fe₂O₃/ 活性碳毡		pH=3，外部电阻120Ω，曝气量300mL/min	10mg/L	95.0%	[46]
橙G	碳刷	石墨板	Fe²⁺	pH=2，外部电阻10Ω，曝气量8mL/min，Fe²⁺ 0.01mol/L	400mg/L	99.6%	[59]
酸性橙7	碳布	碳毡	FeVO₄	pH=3，外部电阻1000Ω，FeVO₄ 12.5g/L	50mg/L	89%	[60]
酸性绿50 结晶紫	石墨棒	石墨棒	铁藻酸盐微珠	pH=2，外部电阻1000Ω，曝气量2L/min，铁藻酸盐微珠10g（铁浓度150mg/L）	10mg/L	94% 83%	[61]
亚甲基蓝	碳刷	石墨板	Fe²⁺	pH=3，外部电阻5Ω，曝气量10mL/min，Fe²⁺ 2mmol/L	50mg/L	100%	[62]
亚甲基蓝	碳刷	石墨板	Fe²⁺	pH=2，外加电压0.4V，曝气量350mL/min，Fe²⁺ 0.2mmol/L	20mg/L	99%	[63]
橙G						100%
甲苯胺蓝						98%
麦尔多拉蓝						99%
罗丹明B						100%
罗丹明6G						100%
雷马素蓝RR	葡萄糖氧化酶固定化碳毡	碳毡	FeSO₄·7H₂O	pH=3.5，外部电阻10Ω，FeSO₄·7H₂O 1.5g/L	50mg/L	COD 34%	[64]
含PPCPs废水
对硝基苯酚	碳毡	碳毡	废铁屑	pH=3，外部电阻1000Ω，废铁屑10g	1mmol/L	100%	[5]
对硝基苯酚	碳毡	碳毡	褐铁矿	pH=2，外部电阻300Ω，曝气量100mL/min，褐铁矿2.24g/L	0.25mmol/L	96%	[45]
磺胺甲𫫇唑诺氟沙星	碳毡	γ-FeOOH石墨烯聚丙烯酰胺碳化气凝胶		自然pH，外部电阻1000Ω	0.1mmol/L	97.4% 96.1%	[65]
土霉素	碳毡	FeCo/氧化石墨烯/碳毡		pH=7.2，外部电阻1000Ω，曝气量50mL/min	20mg/L	80.34%	[66]
四环素	碳毡	碳毡	Fe²⁺	pH=3，外部电阻250Ω，溶解氧≥8.4mg/L，Fe²⁺ 1mg/L	20mg/L	100%	[67]
17β-雌二醇 17α-乙炔基雌二醇	碳毡+ 颗粒石墨	Fe@Fe₂O₃/非催化碳毡		pH=3，外部电阻1000Ω，曝气量100mL/min	20μg/L 20μg/L	81% 56%	[68]
双酚A	石墨棒	石墨棒+ 石墨颗粒	FeSO₄·7H₂O	pH=3，外部电阻10Ω， FeSO₄·7H₂O 1.25mmol/L	1mg/L	75%	[69]
雌酮						100%
磺胺二甲基嘧啶						97%
三氯卡班						98%
扑热息痛	石墨毡	石墨板	FeSO₄·7H₂O	pH=2，外部电阻20Ω， FeSO₄·7H₂O 5mg/L	10mg/L	70%	[55]
含PPCPs废水
酮洛芬	碳刷	石墨板	FeSO₄·7H₂O	pH=2，外加电压0.5V，曝气量8mL/min，FeSO₄·7H₂O 5mmol/L	40μg/L	59%	[70]
双氯芬酸						87%
布洛芬						80%
萘普生						75%
美托洛尔	碳刷	石墨板	FeSO₄·7H₂O	pH=3，外加电压 0.2V，曝气量2mL/min，FeSO₄·7H₂O 0.2mmol/L	0.5mg/L	70.1%	[71]
垃圾渗滤液
垃圾渗滤液	碳布	nZVI@MAC/不锈钢网		pH=7.57，外部电阻1000Ω	COD 3520mg/L	83.8%	[50]
垃圾渗滤液	碳毡	磁黄铁矿负载石墨片		pH=2.7，外部电阻500Ω，曝气量8mL/min	COD 1022mg/L	78%	[72]
垃圾渗滤液	碳毡	碳毡	FeSO₄·7H₂O	pH=7.6，FeSO₄·7H₂O 60mg/L	COD (2152±624)mg/L	49.3%	[73]
其他类型废水
煤气化废水	碳毡	FeVO₄/碳毡		pH=7，外部电阻500Ω，曝气量100mL/min	COD 346mg/L	83.7%	[51]
苯胺废水	碳刷	石墨板	FeSO₄	pH=3，外加电压0.5V，曝气量16mL/min，FeSO₄ 10mmol/L	(4460±52)mg/L	97.1%	[54]
养猪废水	石墨棒+ 石墨颗粒	Fe@Fe₂O₃/非催化碳毡		pH=3，外部电阻100Ω，曝气量300mL/min	COD 1652mg/L	62.2%	[74]
中药废水	石墨板	Fe@Fe₂O₃/石墨		pH=3，外部电阻100Ω，曝气量300mL/min	COD (6183±309)mg/L	84.02%	[75]
含油废水	石墨毡	γ-FeOOH/石墨毡		pH=3，外部电阻500Ω，曝气量200mL/min，温度35℃	油浓度154mg/L	95.3%	[76]

废水类型	阳极	阴极	催化剂	运行条件	污染物浓度	去除率	参考文献
染料废水
橙黄Ⅱ	碳毡	PPy/AQDS/碳毡	γ-FeOOH	pH=7，外部电阻1000Ω，曝气量100mL/min，γ-FeOOH 1g/L	0.2mmol/L	100%	[41]
橙黄Ⅱ	碳毡	碳纳米管/ γ-FeOOH		pH=7，外部电阻1000Ω	0.1mmol/L	100%	[58]
甲基橙	碳纸+ 颗粒活性炭	负载Pt碳纸+ 颗粒活性炭	FeSO₄·7H₂O	pH=3，外部电阻1000Ω，曝气量150mL/min，FeSO₄·7H₂O 0.05mol/L	300mg/L	86.39%	[40]
甲基橙	石墨纤维刷	Fe₂O₃/活性碳毡		pH=3，外部电阻100Ω，曝气量750mL/min	5mg/L	86.7%	[49]
罗丹明B	活性碳毡	Fe@Fe₂O₃/ 活性碳毡		pH=3，外部电阻120Ω，曝气量300mL/min	10mg/L	95.0%	[46]
橙G	碳刷	石墨板	Fe²⁺	pH=2，外部电阻10Ω，曝气量8mL/min，Fe²⁺ 0.01mol/L	400mg/L	99.6%	[59]
酸性橙7	碳布	碳毡	FeVO₄	pH=3，外部电阻1000Ω，FeVO₄ 12.5g/L	50mg/L	89%	[60]
酸性绿50 结晶紫	石墨棒	石墨棒	铁藻酸盐微珠	pH=2，外部电阻1000Ω，曝气量2L/min，铁藻酸盐微珠10g（铁浓度150mg/L）	10mg/L	94% 83%	[61]
亚甲基蓝	碳刷	石墨板	Fe²⁺	pH=3，外部电阻5Ω，曝气量10mL/min，Fe²⁺ 2mmol/L	50mg/L	100%	[62]
亚甲基蓝	碳刷	石墨板	Fe²⁺	pH=2，外加电压0.4V，曝气量350mL/min，Fe²⁺ 0.2mmol/L	20mg/L	99%	[63]
橙G						100%
甲苯胺蓝						98%
麦尔多拉蓝						99%
罗丹明B						100%
罗丹明6G						100%
雷马素蓝RR	葡萄糖氧化酶固定化碳毡	碳毡	FeSO₄·7H₂O	pH=3.5，外部电阻10Ω，FeSO₄·7H₂O 1.5g/L	50mg/L	COD 34%	[64]
含PPCPs废水
对硝基苯酚	碳毡	碳毡	废铁屑	pH=3，外部电阻1000Ω，废铁屑10g	1mmol/L	100%	[5]
对硝基苯酚	碳毡	碳毡	褐铁矿	pH=2，外部电阻300Ω，曝气量100mL/min，褐铁矿2.24g/L	0.25mmol/L	96%	[45]
磺胺甲𫫇唑诺氟沙星	碳毡	γ-FeOOH石墨烯聚丙烯酰胺碳化气凝胶		自然pH，外部电阻1000Ω	0.1mmol/L	97.4% 96.1%	[65]
土霉素	碳毡	FeCo/氧化石墨烯/碳毡		pH=7.2，外部电阻1000Ω，曝气量50mL/min	20mg/L	80.34%	[66]
四环素	碳毡	碳毡	Fe²⁺	pH=3，外部电阻250Ω，溶解氧≥8.4mg/L，Fe²⁺ 1mg/L	20mg/L	100%	[67]
17β-雌二醇 17α-乙炔基雌二醇	碳毡+ 颗粒石墨	Fe@Fe₂O₃/非催化碳毡		pH=3，外部电阻1000Ω，曝气量100mL/min	20μg/L 20μg/L	81% 56%	[68]
双酚A	石墨棒	石墨棒+ 石墨颗粒	FeSO₄·7H₂O	pH=3，外部电阻10Ω， FeSO₄·7H₂O 1.25mmol/L	1mg/L	75%	[69]
雌酮						100%
磺胺二甲基嘧啶						97%
三氯卡班						98%
扑热息痛	石墨毡	石墨板	FeSO₄·7H₂O	pH=2，外部电阻20Ω， FeSO₄·7H₂O 5mg/L	10mg/L	70%	[55]
含PPCPs废水
酮洛芬	碳刷	石墨板	FeSO₄·7H₂O	pH=2，外加电压0.5V，曝气量8mL/min，FeSO₄·7H₂O 5mmol/L	40μg/L	59%	[70]
双氯芬酸						87%
布洛芬						80%
萘普生						75%
美托洛尔	碳刷	石墨板	FeSO₄·7H₂O	pH=3，外加电压 0.2V，曝气量2mL/min，FeSO₄·7H₂O 0.2mmol/L	0.5mg/L	70.1%	[71]
垃圾渗滤液
垃圾渗滤液	碳布	nZVI@MAC/不锈钢网		pH=7.57，外部电阻1000Ω	COD 3520mg/L	83.8%	[50]
垃圾渗滤液	碳毡	磁黄铁矿负载石墨片		pH=2.7，外部电阻500Ω，曝气量8mL/min	COD 1022mg/L	78%	[72]
垃圾渗滤液	碳毡	碳毡	FeSO₄·7H₂O	pH=7.6，FeSO₄·7H₂O 60mg/L	COD (2152±624)mg/L	49.3%	[73]
其他类型废水
煤气化废水	碳毡	FeVO₄/碳毡		pH=7，外部电阻500Ω，曝气量100mL/min	COD 346mg/L	83.7%	[51]
苯胺废水	碳刷	石墨板	FeSO₄	pH=3，外加电压0.5V，曝气量16mL/min，FeSO₄ 10mmol/L	(4460±52)mg/L	97.1%	[54]
养猪废水	石墨棒+ 石墨颗粒	Fe@Fe₂O₃/非催化碳毡		pH=3，外部电阻100Ω，曝气量300mL/min	COD 1652mg/L	62.2%	[74]
中药废水	石墨板	Fe@Fe₂O₃/石墨		pH=3，外部电阻100Ω，曝气量300mL/min	COD (6183±309)mg/L	84.02%	[75]
含油废水	石墨毡	γ-FeOOH/石墨毡		pH=3，外部电阻500Ω，曝气量200mL/min，温度35℃	油浓度154mg/L	95.3%	[76]

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