基于三维生物膜电极的难生化有机化工废水处理研究进展

doi:10.16085/j.issn.1000-6613.2023-1079

摘要/Abstract

摘要：

近年来，难降解有机化工污染物在自然水体中被广泛检出，对水生态环境和人体健康构成了严重威胁。生物膜电极技术因具备环境友好、去除效率高、适用范围广等优点，在难降解污染物处理领域应用前景日渐广阔。对此，介绍了三维生物膜电极（3D-BERs）反应器构建方法，阐述了三维生物膜电极对有机污染物的降解机理，分析了电化学催化氧化与电活性微生物（EAMs）的协同降解作用，从电子迁移强化角度解析了污染物强化降解机制，并概述了3D-BERs的构建方法与运行参数对反应器效率的影响。本文系统综述了3D-BERs在难生化有机化工废水处理领域中的应用与优势，提出了三维生物膜电极技术的发展前景和今后研究工作的重点方向，为难生化有机化工废水的高效处理提供新思路与技术选择。

关键词: 三维生物膜电极, 电活性微生物, 难生化有机化工废水, 电化学

Abstract:

Recently, refractory organic pollutants have been widely detected in natural water bodies, posing a serious threat to aquatic ecosystems and human health. The biofilm electrode technology is increasingly recognized as a promising approach in the field of recalcitrant pollutant treatment owing to its environmental friendliness, high removal efficiency, and wide applicability. In this study, a three-dimensional biofilm electrode reactors (3D-BERs) is constructed; the degradation mechanism of organic pollutants by 3D-BERs is elucidated; the synergistic degradation effect of electrochemical catalytic oxidation and electroactive microorganisms is analyzed; the enhanced degradation mechanism of pollutants is explicated from the perspective of electron migration; and the impact of construction methods and operational parameters of 3D-BERs on reactor efficiency is outlined. Furthermore, this study systematically reviews the application and advantages of 3D-BERs in treating refractory organic chemical wastewater, proposes the development prospects of 3D-BERs technology, and highlights the focus of future research efforts. Finally, this study aims to provide novel insights into the efficient treatment of recalcitrant organic chemical industrial wastewater to further promote the application and dissemination of biofilm electrode technology in the field of recalcitrant organic pollutant treatment.

Key words: three-dimensional biofilm electrode reactors (3D-BERs), electroactive microorganisms (EAMs), refractory organic chemical wastewater, electrochemical

中图分类号:

X783

王宝山, 陈晓杰, 赵培宇, 张许. 基于三维生物膜电极的难生化有机化工废水处理研究进展[J]. 化工进展, 2024, 43(6): 3359-3373.

WANG Baoshan, CHEN Xiaojie, ZHAO Peiyu, ZHANG Xu. Research progress on the treatment of refractory organic chemical wastewater using three-dimensional biofilm electrodes[J]. Chemical Industry and Engineering Progress, 2024, 43(6): 3359-3373.

图/表 8

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类型	门水平	属水平	环境	功能特点	参考文献
古菌	广古菌门（Euryarchaeota）	铁丸菌属（Ferroglobus）	阴极	可接收电子，在阴极产氢产甲烷	[38]
		地丸菌属（Geoglobus）
		火球菌属（Pyrococcus）
细菌	绿弯菌门（Chloroflexi）	SBR1031属（SBR1031）	阴极	可分泌紧密黏附的蛋白质，促进邻近细菌细胞的附着和聚集，在不利环境中获得抗性	[40]
	放线菌门（Actinobacteria）	微白霜菌属（Micropruina）	阳极	易适应抗生素环境；可在电场中参与木质素降解	[41-42]
	拟杆菌门（Bacteroidetes）	金黄杆菌属（Chryseobacterium）	阳极	对有毒污染物具有优异的耐受性，可降解多种有机物，同时富含胞外电子传递基因	[43]
	厚壁菌门（Firmicutes）	丹毒丝菌属（Erysipelothrix）	阴极	利用有机碳源进行生长繁殖并将硝酸盐还原为氮气	[11]
		食酸菌属（Acidovorax）	阳极	具有胞外电子传递能力的细菌，在微生物燃料电池中高度富集	[44]
		梭菌属（Clostridium）	两极	能够利用黄素或泛醌等介体将电子传递到阳极	[45]
	变形菌门（Proteobacteria）	寡养单胞菌属（Stenotrophomonas）	阳极	可生物降解许多环境化学物质如毒死蜱、咔唑等	[46]
		嗜甲基菌属（Methylophilus）	阳极	可降解多种有机化合物，如双氯芬酸、布洛芬	[47-48]
		假单胞菌属（Pseudomonas）	两极	可高效矿化多环芳烃	[49]
		动胶菌属（Zoogloea）	阳极	可降解表面活性剂和甲苯等有机污染物	[50]
		丛毛单胞菌属（Comamonas）	阳极	可降解抗生素，产电双重功能，对多种重金属具有较高的适应性	[43]
		陶厄氏菌属（Thauera）	阴极	可以利用氢和无机碳进行自养生长	[51]
		不动杆菌属（Acinetobacter）	阳极	是抗生素污染废水中的主要细菌属	[52]
		氢噬胞菌属（Hydrogenophaga）	阴极	典型的氢利用物种，可以利用氢作为电子供体，还具有降解复杂有机污染物的能力	[53-54]
		脱硫球茎菌属（Desulfobulbus）	阳极	可高效去除磺胺嘧啶、环丙沙星、磺胺甲𫫇唑等抗生素	[55]
		脱硫弧菌属（Desulfovibrio）	阳极	可参与降解四氢呋喃等环状有机物	[11]
		地杆菌属（Geobacter）	阳极	利用乙酸作为主要的发酵产物，可用于发电	[56]
		希瓦氏菌属（Shewanella）	阳极	可降解硝基苯等复杂有机物	[57]
		赫山单胞菌属（Herminiimonas）	阳极	具有抵抗有毒物质的能力，可对有机物实现矿化	[58]
真菌	子囊菌门（Ascomycota）	假丝酵母属（Candida）	阳极	可自身产电发挥与细菌相同功能	[38]
		克鲁维酵母属（Kluyveromyces）
		多型汉逊酵母菌属（Ogataea）
		路德类酵母菌属（Saccharomyces）
		毕赤酵母属（Scheffersomyces）
		芽生葡萄孢酵母属（Blastobotrys）

类型	门水平	属水平	环境	功能特点	参考文献
古菌	广古菌门（Euryarchaeota）	铁丸菌属（Ferroglobus）	阴极	可接收电子，在阴极产氢产甲烷	[38]
		地丸菌属（Geoglobus）
		火球菌属（Pyrococcus）
细菌	绿弯菌门（Chloroflexi）	SBR1031属（SBR1031）	阴极	可分泌紧密黏附的蛋白质，促进邻近细菌细胞的附着和聚集，在不利环境中获得抗性	[40]
	放线菌门（Actinobacteria）	微白霜菌属（Micropruina）	阳极	易适应抗生素环境；可在电场中参与木质素降解	[41-42]
	拟杆菌门（Bacteroidetes）	金黄杆菌属（Chryseobacterium）	阳极	对有毒污染物具有优异的耐受性，可降解多种有机物，同时富含胞外电子传递基因	[43]
	厚壁菌门（Firmicutes）	丹毒丝菌属（Erysipelothrix）	阴极	利用有机碳源进行生长繁殖并将硝酸盐还原为氮气	[11]
		食酸菌属（Acidovorax）	阳极	具有胞外电子传递能力的细菌，在微生物燃料电池中高度富集	[44]
		梭菌属（Clostridium）	两极	能够利用黄素或泛醌等介体将电子传递到阳极	[45]
	变形菌门（Proteobacteria）	寡养单胞菌属（Stenotrophomonas）	阳极	可生物降解许多环境化学物质如毒死蜱、咔唑等	[46]
		嗜甲基菌属（Methylophilus）	阳极	可降解多种有机化合物，如双氯芬酸、布洛芬	[47-48]
		假单胞菌属（Pseudomonas）	两极	可高效矿化多环芳烃	[49]
		动胶菌属（Zoogloea）	阳极	可降解表面活性剂和甲苯等有机污染物	[50]
		丛毛单胞菌属（Comamonas）	阳极	可降解抗生素，产电双重功能，对多种重金属具有较高的适应性	[43]
		陶厄氏菌属（Thauera）	阴极	可以利用氢和无机碳进行自养生长	[51]
		不动杆菌属（Acinetobacter）	阳极	是抗生素污染废水中的主要细菌属	[52]
		氢噬胞菌属（Hydrogenophaga）	阴极	典型的氢利用物种，可以利用氢作为电子供体，还具有降解复杂有机污染物的能力	[53-54]
		脱硫球茎菌属（Desulfobulbus）	阳极	可高效去除磺胺嘧啶、环丙沙星、磺胺甲𫫇唑等抗生素	[55]
		脱硫弧菌属（Desulfovibrio）	阳极	可参与降解四氢呋喃等环状有机物	[11]
		地杆菌属（Geobacter）	阳极	利用乙酸作为主要的发酵产物，可用于发电	[56]
		希瓦氏菌属（Shewanella）	阳极	可降解硝基苯等复杂有机物	[57]
		赫山单胞菌属（Herminiimonas）	阳极	具有抵抗有毒物质的能力，可对有机物实现矿化	[58]
真菌	子囊菌门（Ascomycota）	假丝酵母属（Candida）	阳极	可自身产电发挥与细菌相同功能	[38]
		克鲁维酵母属（Kluyveromyces）
		多型汉逊酵母菌属（Ogataea）
		路德类酵母菌属（Saccharomyces）
		毕赤酵母属（Scheffersomyces）
		芽生葡萄孢酵母属（Blastobotrys）

序号	类型	阳极	阴极	颗粒电极	其他参数	去除率	参考文献
1	垃圾渗滤液	RuO₂-IrO₂	不锈钢	柱状活性炭	J₀=60mA/cm²；C₀=2091mg/L； NH₄⁺-N=2531mg/L；pH=8.4；HRT=3h； D=4.8cm	COD_Cr=26.5%； NH₄⁺-N=81.1%	[88]
2	磺胺甲𫫇唑（SMX）、四环素（TC）	活性炭纤维/ 钛网	活性炭纤维/ 钛网	GAC+GR	V₀=0.8V；C₀=0.2mg/L；HRT=6h；T=28℃	SMX=88.9%~93.5%；TC=89.3%~95.6%	[89]
3	RBRX-3B	不锈钢网/ 活性炭纤维	钛网/ 活性炭纤维	GAC	V₀=2.5V；C₀=1000mg/L；HRT=24h； T=20℃；D=21cm	>90.0%	[90]
4	磺胺甲𫫇唑（SMX）	不锈钢网	钛网	GAC	V₀=1V；C₀=4000mg/L；HRT=2.5d； T=28℃±2℃；D=11cm	>99.3%	[91]
5	布洛芬	钛网	不锈钢孔板	赤泥	J₀=12.73A/m²；C₀=93.2μg/L±5.16μg/L； HRT=3.5h；T=28℃±2℃；pH=7.16±0.13； D=30cm	93.5%	[92]
6	焦化废水	钛网	RuO₂-IrO₂	GAC	V₀=8V；C₀=734mg/L；HRT=20h； pH=6.94；D=10cm	79.6%	[58]
7	四氢呋喃	Ti-IrO₂	钛网	聚氨酯海绵填料	V₀=10V；C₀=4190mg/L±585mg/L； HRT=24h；pH=6.9；D=15cm	95.9%±1.6%	[11]
8	焦化废水（中试）	Ti/RuO₂-IrO₂	Ti/RuO₂-IrO₂	GAC	V₀=8V；C₀=3160.56mg/L；HRT=6h； pH=10.09；D=28cm	94.4%	[93]
9	焦化废水	石墨棒	不锈钢网	GAC	I₀=20mA；C₀=497mg/L；NH₄⁺-N=418mg/L； HRT=10h；pH=8.99；D=5cm	COD_Cr=68.5%； NH₄⁺-N=99.0%	[9]
10	地塞米松（DEX）	钛板	钛板	聚苯胺负载活性炭	I₀=3mA；C₀=100μg/L；HRT=20h； pH=7.2±0.2；D=5cm	95.7%	[94]
11	高氯酸盐	石墨棒	钛网	活性炭纤维	I₀=20mA；C₀=10mg/L；HRT=48h；T=30℃±2℃；pH=7.4~8.4；D=2.5cm	98.2%	[95]
12	四溴双酚A	Ti/RuO₂-IrO₂	不锈钢板	GAC / 颗粒沸石	V₀=5V；C₀=20mg/L；HRT=2h；pH=8； D=10cm	95.0%	[22]
13	十二烷基硫酸钠（SDS）	石墨板	石墨板	石墨颗粒	I₀=1786~1796mA/m³；C₀=105mg/L±10mg/L； HRT=38.5h；pH=7.5~7.8；D=10cm	88.0%	[96]
14	甲硝唑（MNZ）混合含氮废水	石墨棒	活性炭纤维毡缠绕不锈钢	GAC和玻璃珠	I₀=1mA；C₀(MNZ)=10mg/L；NO₃^--N=35mg/L； HRT=6h；T=25℃±3℃；D=8cm	MNZ=94.4%； NO₃^--N=82.8%	[97]
15	水杨酸	不锈钢板	钛板	锂渣	I₀=0.25~0.40A；C₀=110.86μg/L；HRT=6h； T=20℃；pH=7.4~7.5；D=15cm	85.2%	[98]
16	罗丹明B	不锈钢板	钛板	钢渣	I₀=1.0A；C₀=10mg/L；HRT=3.5h； T=20℃±1℃；pH=7.3~7.4；D=8cm	91.7±1.3%	[50]
17	合成废水	碳板	碳板	陶粒	V₀=0.5V；C₀=250mg/L；HRT=6h； T=25℃±1℃；D=10cm	>90.0%	[99]
18	有机酸工业废水	碳棒	碳棒	MnO₂/TiO₂/ g-C₃N₄@ GAC	V₀=0.439V；C₀=6500mg/L；HRT=12h； pH=5~6	COD_Cr=98.0%	[20]
19	磺胺嘧啶（SDZ）、环丙沙星（CIP）	不锈钢丝网	不锈钢丝网	GAC	V₀=0.8V；C₀=2mg/L；HRT=36h；D=8cm	SDZ=99.1%； CIP=97.3%	[60]

序号	类型	阳极	阴极	颗粒电极	其他参数	去除率	参考文献
1	垃圾渗滤液	RuO₂-IrO₂	不锈钢	柱状活性炭	J₀=60mA/cm²；C₀=2091mg/L； NH₄⁺-N=2531mg/L；pH=8.4；HRT=3h； D=4.8cm	COD_Cr=26.5%； NH₄⁺-N=81.1%	[88]
2	磺胺甲𫫇唑（SMX）、四环素（TC）	活性炭纤维/ 钛网	活性炭纤维/ 钛网	GAC+GR	V₀=0.8V；C₀=0.2mg/L；HRT=6h；T=28℃	SMX=88.9%~93.5%；TC=89.3%~95.6%	[89]
3	RBRX-3B	不锈钢网/ 活性炭纤维	钛网/ 活性炭纤维	GAC	V₀=2.5V；C₀=1000mg/L；HRT=24h； T=20℃；D=21cm	>90.0%	[90]
4	磺胺甲𫫇唑（SMX）	不锈钢网	钛网	GAC	V₀=1V；C₀=4000mg/L；HRT=2.5d； T=28℃±2℃；D=11cm	>99.3%	[91]
5	布洛芬	钛网	不锈钢孔板	赤泥	J₀=12.73A/m²；C₀=93.2μg/L±5.16μg/L； HRT=3.5h；T=28℃±2℃；pH=7.16±0.13； D=30cm	93.5%	[92]
6	焦化废水	钛网	RuO₂-IrO₂	GAC	V₀=8V；C₀=734mg/L；HRT=20h； pH=6.94；D=10cm	79.6%	[58]
7	四氢呋喃	Ti-IrO₂	钛网	聚氨酯海绵填料	V₀=10V；C₀=4190mg/L±585mg/L； HRT=24h；pH=6.9；D=15cm	95.9%±1.6%	[11]
8	焦化废水（中试）	Ti/RuO₂-IrO₂	Ti/RuO₂-IrO₂	GAC	V₀=8V；C₀=3160.56mg/L；HRT=6h； pH=10.09；D=28cm	94.4%	[93]
9	焦化废水	石墨棒	不锈钢网	GAC	I₀=20mA；C₀=497mg/L；NH₄⁺-N=418mg/L； HRT=10h；pH=8.99；D=5cm	COD_Cr=68.5%； NH₄⁺-N=99.0%	[9]
10	地塞米松（DEX）	钛板	钛板	聚苯胺负载活性炭	I₀=3mA；C₀=100μg/L；HRT=20h； pH=7.2±0.2；D=5cm	95.7%	[94]
11	高氯酸盐	石墨棒	钛网	活性炭纤维	I₀=20mA；C₀=10mg/L；HRT=48h；T=30℃±2℃；pH=7.4~8.4；D=2.5cm	98.2%	[95]
12	四溴双酚A	Ti/RuO₂-IrO₂	不锈钢板	GAC / 颗粒沸石	V₀=5V；C₀=20mg/L；HRT=2h；pH=8； D=10cm	95.0%	[22]
13	十二烷基硫酸钠（SDS）	石墨板	石墨板	石墨颗粒	I₀=1786~1796mA/m³；C₀=105mg/L±10mg/L； HRT=38.5h；pH=7.5~7.8；D=10cm	88.0%	[96]
14	甲硝唑（MNZ）混合含氮废水	石墨棒	活性炭纤维毡缠绕不锈钢	GAC和玻璃珠	I₀=1mA；C₀(MNZ)=10mg/L；NO₃^--N=35mg/L； HRT=6h；T=25℃±3℃；D=8cm	MNZ=94.4%； NO₃^--N=82.8%	[97]
15	水杨酸	不锈钢板	钛板	锂渣	I₀=0.25~0.40A；C₀=110.86μg/L；HRT=6h； T=20℃；pH=7.4~7.5；D=15cm	85.2%	[98]
16	罗丹明B	不锈钢板	钛板	钢渣	I₀=1.0A；C₀=10mg/L；HRT=3.5h； T=20℃±1℃；pH=7.3~7.4；D=8cm	91.7±1.3%	[50]
17	合成废水	碳板	碳板	陶粒	V₀=0.5V；C₀=250mg/L；HRT=6h； T=25℃±1℃；D=10cm	>90.0%	[99]
18	有机酸工业废水	碳棒	碳棒	MnO₂/TiO₂/ g-C₃N₄@ GAC	V₀=0.439V；C₀=6500mg/L；HRT=12h； pH=5~6	COD_Cr=98.0%	[20]
19	磺胺嘧啶（SDZ）、环丙沙星（CIP）	不锈钢丝网	不锈钢丝网	GAC	V₀=0.8V；C₀=2mg/L；HRT=36h；D=8cm	SDZ=99.1%； CIP=97.3%	[60]

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