A critical review of bioelectrochemical system in the degradation of hydrophobic emerging contaminants

doi:10.16085/j.issn.1000-6613.2021-0106

Abstract

Abstract:

The transformation and degradation of hydrophobic emerging contaminants (HECs) has become research hot spots due to the characteristics of widespread distribution, persistence, and refractory of HECs. Bioelectrochemical system (BES) is a flourishing technology for the remediation of various contaminants and has been proven to efficiently transform and degrade HECs. In this work, the effect of BES operational factors on HECs removal performance was analyzed, the effectiveness of BES technology in treating various HECs’was evaluated, and the feasibility and superiority of integrating BES into traditional treating technologies, such as anaerobic digestion, Fenton, wetlands, and photocatalysis, were discussed as well. Besides, the prospective development of functional electrode materials, the mechanism of HECs’transformation and degradation, and the engineering applications of BES technology were proposed. This review is expected to provide theoretical and technical supports for future research and promote the BES technology closer to the practical application.

Key words: hydrophobic emerging contaminants, bioelectrochemical system, degradation, remediation, oxidation, reduction, coupling process

摘要：

疏水性新兴污染物（hydrophobic emerging contaminants，HECs）具有环境危害大、分布范围广和处理难度高等特点，利用生物电化学系统（bioelectrochemical system，BES）实现HECs的降解和脱毒是当前研究热点。本文综述了BES降解转化HECs的研究现状，分析了影响BES去除HECs效果的关键因素，着重介绍了BES降解转化不同类型HECs（包括药物类、个人护理品类、卤代烃类和抗生素及抗性基因类）的效能，然后回顾了BES与其他技术（传统厌氧工艺、芬顿、复合湿地及光催化等）结合协同降解HECs的最新进展，最后在功能电极材料设计研发、HECs降解去除与安全转化的理论研究及工程化应用等方面进行了总结和展望，以期对该领域的研究人员提供一定的理论参考和技术支持，从而推进生物电化学技术在疏水性新兴污染物降解领域的应用和发展。

关键词: 疏水性新兴污染物, 生物电化学系统, 降解, 修复, 氧化, 还原, 耦合工艺

CLC Number:

X505

ZHANG Qian, CUI Minhua, CHEN Lei, WU Ping, LIU He. A critical review of bioelectrochemical system in the degradation of hydrophobic emerging contaminants[J]. Chemical Industry and Engineering Progress, 2021, 40(12): 6846-6858.

张钤, 崔敏华, 陈蕾, 吴平, 刘和. 生物电化学技术降解疏水性新兴污染物的研究进展[J]. 化工进展, 2021, 40(12): 6846-6858.

Figures/Tables 7

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处理方法	具体工艺/试剂	污染物种类	去除效果	优点	缺点	参考文献
好氧生物降解	传统活性污泥法	佳乐麝香	73%~96%	降解、矿化程度高；成本低；降解产物毒性一般小于母体污染物	降解周期长；可降解污染物种类少、具有局限性	［9］
	膜生物反应器	双氯酚酸	60%~80%
	水解酸化-生物处理	环丙沙星	90%			［10］
厌氧生物降解	污泥厌氧消化	萘普生	80%
		麝香	50%~90%			［11］
		布洛芬	30%~60%
		卡马西平	无明显降解
化学氧化法	β-FeOOH/Al₂O₃	布洛芬	100%	降解/矿化程度高、效果稳定、反应过程容易控制	基建/运行成本高，二次污染重；中间降解产物生态毒性不稳定	［12］
化学氧化法	β-FeOOH/Al₂O₃	环丙沙星	100%			［12］
臭氧催化氧化	Mg₃Fe_0.5Al	双氯酚酸	73%			［13-17］
芬顿法	FeS₂	三氯生	90%			［15］
	Fe₃O₄	卡马西平布洛芬	86.26% 83.29%			［18］
	Fe₃O₄	萘啶酸	60%			［19］
电离辐射	⁶⁰Co（1.1KGy）	布洛芬	100%			［20］
	⁶⁰Co（2.0KGy）	双氯酚酸	100%			［21］
	⁶⁰Co（5.0KGy）	氯贝酸	100%			［22］
	⁶⁰Co（20Gy）	4-壬基酚	100%			［23］
吸附法	颗粒活性炭	双氯酚酸、三氯生布洛芬	10%~68%	系统简单，不形成有毒中间产物；处理方法成本基建及设备投资少，稳定性高，能耗低	污染物没有进一步降解转化，仍存在介质中	［24-25］
	粉状活性炭（PAC）	卡马西平	60%
	AmberliteXAD-4	双氯酚酸	92.80%
	磁性树脂W150	呋喃西林	180mg·g^-1
	矿物	双氯酚酸	37.5%~95.9%
膜分离法	微滤-颗粒活性炭-纳滤	疏水性PPCPs	45%~80%	操作简单，污染物去除率高，占用空间小	易造成膜孔隙堵塞污染	［26-27］
膜分离法	超滤-纳滤	磺胺甲唑、双氯芬酸	70%	操作简单，污染物去除率高，占用空间小	易造成膜孔隙堵塞污染	［26-27］

处理方法	具体工艺/试剂	污染物种类	去除效果	优点	缺点	参考文献
好氧生物降解	传统活性污泥法	佳乐麝香	73%~96%	降解、矿化程度高；成本低；降解产物毒性一般小于母体污染物	降解周期长；可降解污染物种类少、具有局限性	［9］
	膜生物反应器	双氯酚酸	60%~80%
	水解酸化-生物处理	环丙沙星	90%			［10］
厌氧生物降解	污泥厌氧消化	萘普生	80%
		麝香	50%~90%			［11］
		布洛芬	30%~60%
		卡马西平	无明显降解
化学氧化法	β-FeOOH/Al₂O₃	布洛芬	100%	降解/矿化程度高、效果稳定、反应过程容易控制	基建/运行成本高，二次污染重；中间降解产物生态毒性不稳定	［12］
化学氧化法	β-FeOOH/Al₂O₃	环丙沙星	100%			［12］
臭氧催化氧化	Mg₃Fe_0.5Al	双氯酚酸	73%			［13-17］
芬顿法	FeS₂	三氯生	90%			［15］
	Fe₃O₄	卡马西平布洛芬	86.26% 83.29%			［18］
	Fe₃O₄	萘啶酸	60%			［19］
电离辐射	⁶⁰Co（1.1KGy）	布洛芬	100%			［20］
	⁶⁰Co（2.0KGy）	双氯酚酸	100%			［21］
	⁶⁰Co（5.0KGy）	氯贝酸	100%			［22］
	⁶⁰Co（20Gy）	4-壬基酚	100%			［23］
吸附法	颗粒活性炭	双氯酚酸、三氯生布洛芬	10%~68%	系统简单，不形成有毒中间产物；处理方法成本基建及设备投资少，稳定性高，能耗低	污染物没有进一步降解转化，仍存在介质中	［24-25］
	粉状活性炭（PAC）	卡马西平	60%
	AmberliteXAD-4	双氯酚酸	92.80%
	磁性树脂W150	呋喃西林	180mg·g^-1
	矿物	双氯酚酸	37.5%~95.9%
膜分离法	微滤-颗粒活性炭-纳滤	疏水性PPCPs	45%~80%	操作简单，污染物去除率高，占用空间小	易造成膜孔隙堵塞污染	［26-27］
膜分离法	超滤-纳滤	磺胺甲唑、双氯芬酸	70%	操作简单，污染物去除率高，占用空间小	易造成膜孔隙堵塞污染	［26-27］

分类	名称	分子式	辛醇-水分配系数 lgK_ow	分子量	浓度水平/ng·L^-1	国家/地区
药品及个人护理用品	阿奇霉素^①	C₃₈H₇₂N₂O₁₂	4.02	749	47~82	加拿大^［39］
	克拉霉素^①	C₃₈H₆₉NO₁₃	3.16	748	89~231	加拿大^［40］
	双氯芬酸^②	C₁₄H₁₀Cl₂O₂	4.51	296	147~320	上海^［41］
	氯贝酸^①	C₁₀H₁₁ClO₃	2.57	214	7.4~51.3	上海^［42］
	布洛芬^②	C₁₃H₁₈O₂	3.97	206	480	意大利^［42］
	卡马西平^②	C₁₅H₁₂N₂O	2.47	236	0.1~8.5 44.6~118	北京^［43］长江流域
	三氯生^②	C₁₂H₇Cl₃O₂	4.71	289	5.74~105	东江^［44］
	三氯卡班^②	C₁₃H₉ClN₂O	4.90	315	4.11~71.8	东江^［44］
	萘普生^②	C₁₄H₁₄O₃	3.18	230	6.32~145	美国^［44］
	苯扎贝特	C₁₉H₂₀ClNO₄	4.25	362	72.1	美国^［45］
	氯霉素^②	C₁₁H₁₂Cl₂N₂O₅	1.14	323	93~1178	河北^［46］
	吲哚美辛^①	C₁₉H₁₆ClNO₄	4.27	358	83~979	长江流域^［47］
内分泌干扰物	邻苯二甲酸二（2-乙基）己酯	C₂₄H₃₈O₄	7.60	391	61	全国平均值^［46］
	酞酸二丁酯	C₁₆H₂₂O₄	4.50	278	284	长江上游^［46］
	双酚A^②	C₁₅H₁₆O₂	3.32	228	26.2	黄河口^［47］
	壬基酚	C₁₅H₂₄O	5.99	220	60~730	全国^［48］

分类	名称	分子式	辛醇-水分配系数 lgK_ow	分子量	浓度水平/ng·L^-1	国家/地区
药品及个人护理用品	阿奇霉素^①	C₃₈H₇₂N₂O₁₂	4.02	749	47~82	加拿大^［39］
	克拉霉素^①	C₃₈H₆₉NO₁₃	3.16	748	89~231	加拿大^［40］
	双氯芬酸^②	C₁₄H₁₀Cl₂O₂	4.51	296	147~320	上海^［41］
	氯贝酸^①	C₁₀H₁₁ClO₃	2.57	214	7.4~51.3	上海^［42］
	布洛芬^②	C₁₃H₁₈O₂	3.97	206	480	意大利^［42］
	卡马西平^②	C₁₅H₁₂N₂O	2.47	236	0.1~8.5 44.6~118	北京^［43］长江流域
	三氯生^②	C₁₂H₇Cl₃O₂	4.71	289	5.74~105	东江^［44］
	三氯卡班^②	C₁₃H₉ClN₂O	4.90	315	4.11~71.8	东江^［44］
	萘普生^②	C₁₄H₁₄O₃	3.18	230	6.32~145	美国^［44］
	苯扎贝特	C₁₉H₂₀ClNO₄	4.25	362	72.1	美国^［45］
	氯霉素^②	C₁₁H₁₂Cl₂N₂O₅	1.14	323	93~1178	河北^［46］
	吲哚美辛^①	C₁₉H₁₆ClNO₄	4.27	358	83~979	长江流域^［47］
内分泌干扰物	邻苯二甲酸二（2-乙基）己酯	C₂₄H₃₈O₄	7.60	391	61	全国平均值^［46］
	酞酸二丁酯	C₁₆H₂₂O₄	4.50	278	284	长江上游^［46］
	双酚A^②	C₁₅H₁₆O₂	3.32	228	26.2	黄河口^［47］
	壬基酚	C₁₅H₂₄O	5.99	220	60~730	全国^［48］

污染物种类	污染物名称	污染物浓度	反应装置类型	输出电压（MFC）	外加电压（MEC）	电极材料	降解周期	降解效率/%	参考文献
疏水性药品及个人护理用品	三氯生	10mg·L^-1	AD-MFC	（420±40）mV	—	碳毡（9×9cm²）	8天	100	［54］
	三氯生	1mg·L^-1	MFC	60mV	—	碳刷（5.9×6.9cm²）	48h	94	［55］
	氯霉素	50mg·L^-1	MFC	>50mV	—	碳毡（3×3cm²）	12h	84	［56］
	氯霉素	20mg·L^-1	电辅助厌氧系统	—	0~2V	石墨板	1天	53~88	［57］
	双氯芬酸	10mg·L^-1	CF-MFC	0.51V		Ru/Fe-碳毡	2天	76	［58］
卤代烃类化合物	对氯硝基苯	40~120mg·L^-1	BES	—	0.2~0.8V	碳刷（3×3cm²）	55h	>80	［59］
	二氯硝基苯	100mg·L^-1	MEC	—	1.5V	碳毡（200×70mm²）	24h	91	［60］
	多氯联苯	（20.2±4.0）mg·kg^-1	BES	—	1.5、2.2、3.0V	碳毡	24h	40~60	［61］
	2，4-二氯酚	100mg·L^-1	BES	—	保持恒电流密度50mA/cm²	Pd/MWNTs气体扩散电极	2h	>79	［62］
	对氟硝基苯	0.4mmol·L^-1	BES	—	0~1.4V	石墨电极	10h	0～100	［63］
	对硝基酚	0.93~6.77mol·m^-3·d^-1	UASB–BES	—	1.2V	碳毡（5×3cm²）	9h	100	［64］