可见光催化降解水中卤代有机污染物的研究进展

doi:10.16085/j.issn.1000-6613.2022-1049

摘要/Abstract

摘要：

卤代有机污染物（HOCs）在水环境中检出频率高达45%，由于其具有毒性大、持久性强和易累积等特点，该类污染物引发的环境问题已引起越来越多的关注。可见光催化技术具有高效太阳能利用率、强选择性及反应条件温和、处理费用低等优点，对于降解水中HOCs具有独特的处理优势，因此近年来被广泛研究。本文梳理了可见光催化降解水中HOCs的核心脱卤机制，包括氧化脱卤、还原脱卤和水解脱卤，在脱卤机制的基础上汇总了三大类主流催化剂的脱卤贡献率，主要包括金属基光催化剂、碳基光催化剂及其他新型光催化剂三类光催化材料。基于可见光作用下降解水中HOCs的应用案例分析，探讨了光催化反应过程中的主要影响因素是溶液pH、催化剂用量及反应温度等。可见光催化降解去除效率高是本技术的核心优势，但由于催化剂的成本高和选择性差导致了其无法大规模应用，未来可见光催化材料设计应向成本低廉、精准匹配污染物从而实现高选择性的方向改进。

关键词: 光化学, 催化剂, 降解, 卤代有机污染物, 光催化效率, 材料改性

Abstract:

Halogenated organic contaminants (HOCs) are frequently detected in water with 45% detection frequency. These contaminants have attracted world-wide attention due to their high toxicity, strong persistence and easy accumulation. Visible-light photocatalysis shows advantages in HOCs contaminated wastewater treatment due to the high efficiency and selectivity, low cost and processing condition restrictions. Therefore, visible-light photocatalysis technology as practicable approach for refractory wastewater treatment have been studied extensively. We firstly introduce the primary mechanisms of visible photocatalytic degradation of HOCs in water, including oxidative dehalogenation, reductive dehalogenation and hydrolytic dehalogenation, then summarize the dehalogenation contribution of the three mainstream catalysts on the basis of their dehalogenation mechanisms, namely metal-based photocatalysts, carbon-based photocatalysts and other new photocatalytic materials. Based on the application case analysis, the main influencing factors for the photocatalytic reaction are discussed, such as solution pH, catalyst dosage and reaction temperature. The high degradation efficiency is the primary advantage of this technology, but the high cost and poor selectivity of the catalysts prevent its large-scale application. In the future, the design of visible photocatalytic materials shall be improved in the direction of low cost and precise matching of pollutants to achieve high selectivity.

Key words: photochemistry, catalyzer, degradation, halogenated organic contaminants, photocatalytic efficiency, material modification

中图分类号:

刘怡璇, 林跃朝, 马伟芳. 可见光催化降解水中卤代有机污染物的研究进展[J]. 化工进展, 2022, 41(S1): 571-579.

LIU Yixuan, LIN Yuechao, MA Weifang. Research progress on degradation of halogenated organic contaminants in water by visible light photocatalysis[J]. Chemical Industry and Engineering Progress, 2022, 41(S1): 571-579.

图/表 4

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溯源地	HOCs名称	污染物检出浓度 /ng·L^-1	参考文献
太湖生态保护引领区	有机氯农药	22.03～166.24	［4］
北江中上游地表水	多氯联苯	0.81～287.5	［5］
洞庭湖及入湖河流	多氯联苯	0.077～10	［6］
北京玉渊潭水体	多溴联苯醚	3.45～11.89	［7］
贵州草海湖泊水体	全氟化合物	3.17～16.33	［8］
千岛湖（新安江水库）	全氟化合物	1.70～6.21	［9］
沱江流域	全氟/多氟化合物	12.5～3789	［10］
渤海湾天津滨海区	多溴联苯醚	43.8～94.3	［11］
白洋淀水体	有机氯农药	0.05～24.01	［12］
汕尾近岸水体	有机氯农药	0.26～6.77	［13］

溯源地	HOCs名称	污染物检出浓度 /ng·L^-1	参考文献
太湖生态保护引领区	有机氯农药	22.03～166.24	［4］
北江中上游地表水	多氯联苯	0.81～287.5	［5］
洞庭湖及入湖河流	多氯联苯	0.077～10	［6］
北京玉渊潭水体	多溴联苯醚	3.45～11.89	［7］
贵州草海湖泊水体	全氟化合物	3.17～16.33	［8］
千岛湖（新安江水库）	全氟化合物	1.70～6.21	［9］
沱江流域	全氟/多氟化合物	12.5～3789	［10］
渤海湾天津滨海区	多溴联苯醚	43.8～94.3	［11］
白洋淀水体	有机氯农药	0.05～24.01	［12］
汕尾近岸水体	有机氯农药	0.26～6.77	［13］

类别	名称	光源/波长	HOCs种类	HOCs浓度 /mol·L^-1	反应时间/h	降解效率/%	参考文献
金属基光催化剂	Pd/TiO₂	300W氙灯/＞400nm	4-溴代二苯	2×10^-5	0.5	100	［20］
	(BiO)₄CO₃(OH)₂/Bi₂O₂CO₃	300W氙灯/＞365nm	4-氯苯酚	3.8×10^-5	2	80	［21］
	Bi/Bi₂WO₆	300W氙灯/＞420nm	五氯酚钠	3.5×10^-5	5	90	［22］
	Fe₃O₄/TiO₂	125W汞灯/400~600nm	2，4-二氯苯酚	3.1×10^-4	0.8	92	［23］
	AgI/ TiO₂	300W氙灯/＞400nm	十溴联苯醚	1×10^-5	1	93	［24］
	TiO₂/Cu₂O	300W氙灯/400~770nm	四溴联苯醚	1×10^-5	2	95	［25］
	Bi₅O₇I/ZnO	500W氙灯/＞420nm	全氟辛酸	2.4×10^-6	6	91	［26］
碳基光催化剂	Ni-g-C₃N₄	300W氙灯/＞420nm	四溴联苯醚	—	24	94.5	［27］
	Pd/HR-g- C₃N₄	300W氙灯/＞400nm	六溴环十二烷	1.6×10^-6	1	92.6	［28］
	C/g-C₃N₄	1000W氙灯/＞400nm	三溴甲烷	4×10^-6	1	51.8	［29］
	Pd /g-C₃N₄	300W氙灯/＞400nm	四溴二苯醚	—	2	100	［30］
	Fe₃O₄-g-C₃N₄	300W氙灯/＞400nm	多溴二苯醚	1×10^-5	2.5	100	［31］
	PTH/SWNT	LED灯/420nm	溴苯腈	6×10^-5	16	99	［32］
其他新型光催化剂	COFs/PTH	LED灯/420nm	单溴联苯醚	3.3×10^-6	24	85	［33］
	COF-JLU22	LED灯/520nm	苯基溴	2.7×10^-4	6	85	［34］
	PTBC-por COF	150W氙灯/400~780nm	2-溴苯乙酮	4×10^-5	2	82	［35］
	陶瓷BCN	LED灯/420nm	4-溴联苯	3.3×10^-5	30	95	［36］

类别	名称	光源/波长	HOCs种类	HOCs浓度 /mol·L^-1	反应时间/h	降解效率/%	参考文献
金属基光催化剂	Pd/TiO₂	300W氙灯/＞400nm	4-溴代二苯	2×10^-5	0.5	100	［20］
	(BiO)₄CO₃(OH)₂/Bi₂O₂CO₃	300W氙灯/＞365nm	4-氯苯酚	3.8×10^-5	2	80	［21］
	Bi/Bi₂WO₆	300W氙灯/＞420nm	五氯酚钠	3.5×10^-5	5	90	［22］
	Fe₃O₄/TiO₂	125W汞灯/400~600nm	2，4-二氯苯酚	3.1×10^-4	0.8	92	［23］
	AgI/ TiO₂	300W氙灯/＞400nm	十溴联苯醚	1×10^-5	1	93	［24］
	TiO₂/Cu₂O	300W氙灯/400~770nm	四溴联苯醚	1×10^-5	2	95	［25］
	Bi₅O₇I/ZnO	500W氙灯/＞420nm	全氟辛酸	2.4×10^-6	6	91	［26］
碳基光催化剂	Ni-g-C₃N₄	300W氙灯/＞420nm	四溴联苯醚	—	24	94.5	［27］
	Pd/HR-g- C₃N₄	300W氙灯/＞400nm	六溴环十二烷	1.6×10^-6	1	92.6	［28］
	C/g-C₃N₄	1000W氙灯/＞400nm	三溴甲烷	4×10^-6	1	51.8	［29］
	Pd /g-C₃N₄	300W氙灯/＞400nm	四溴二苯醚	—	2	100	［30］
	Fe₃O₄-g-C₃N₄	300W氙灯/＞400nm	多溴二苯醚	1×10^-5	2.5	100	［31］
	PTH/SWNT	LED灯/420nm	溴苯腈	6×10^-5	16	99	［32］
其他新型光催化剂	COFs/PTH	LED灯/420nm	单溴联苯醚	3.3×10^-6	24	85	［33］
	COF-JLU22	LED灯/520nm	苯基溴	2.7×10^-4	6	85	［34］
	PTBC-por COF	150W氙灯/400~780nm	2-溴苯乙酮	4×10^-5	2	82	［35］
	陶瓷BCN	LED灯/420nm	4-溴联苯	3.3×10^-5	30	95	［36］

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