基于紫外线的高级氧化或高级还原技术降解水中全氟或多氟烷基化合物

doi:10.16085/j.issn.1000-6613.2023-1013

化工进展 ›› 2024, Vol. 43 ›› Issue (8): 4587-4600.DOI: 10.16085/j.issn.1000-6613.2023-1013

• 资源与环境化工 • 上一篇

基于紫外线的高级氧化或高级还原技术降解水中全氟或多氟烷基化合物

张茜¹(), 李皓芯¹, 张天阳²^,³, 李子富¹, 孙文俊⁴, 敖秀玮¹()

^1.北京科技大学能源与环境工程学院，北京 100083
^2.同济大学环境科学与工程学院，上海 200092
^3.水利部长三角城镇供水节水及水环境治理重点实验室，上海 200092
^4.清华大学环境学院，北京 100084

收稿日期:2023-06-20 修回日期:2023-09-25 出版日期:2024-08-15 发布日期:2024-09-02
通讯作者: 敖秀玮
作者简介:张茜（1999—），女，硕士研究生，研究方向为紫外线高级氧化技术去除水中新污染物。E-mail：zx877592915@163.com。
基金资助:
国家自然科学基金(52270020);中央高校基本科研业务费项目(06500211)

Degradation of per- and polyfluoroalkyl substances in water by UV-based advanced oxidation or advanced reduction processes

ZHANG Xi¹(), LI Haoxin¹, ZHANG Tianyang²^,³, LI Zifu¹, SUN Wenjun⁴, AO Xiuwei¹()

^1.School of Energy and Environmental Engineering, University of Science and Technology Beijing, Beijing 100083, China
^2.College of Environmental Science & Engineering, Tongji University, Shanghai 200092, China
^3.Key Laboratory of Urban Water Supply, Water Saving and Water Environment Governance in the Yangtze River Delta of Ministry of Water Resources, Shanghai 200092, China
^4.School of Environment, Tsinghua University, Beijing 100084, China

Received:2023-06-20 Revised:2023-09-25 Online:2024-08-15 Published:2024-09-02
Contact: AO Xiuwei

摘要/Abstract

摘要：

全氟或多氟烷基化合物（PFASs）是一类具有难降解性、生物蓄积性和潜在毒性的持久性有机污染物，广泛存在于各类环境介质中。水环境是PFASs最重要的归趋之一，然而水处理常规技术难以去除PFASs，近年来，基于紫外线的高级氧化或高级还原技术在PFASs的降解中表现出巨大的发展潜力和良好的应用前景。本文针对目前对于直接紫外光降解、紫外高级氧化技术和紫外高级还原技术降解PFASs的相关研究，重点从降解机理（包括活性物种产生机理和反应机理）、降解效率（包括降解率和脱氟率）和影响因素（包括光波长、pH、溶解氧、无机离子和腐殖酸等）三个维度对比了不同反应体系下PFASs的去除效能，并总结了基于紫外线的高级氧化或高级还原技术应用于去除实际水体中PFASs时需克服的难点，以期为该类技术在PFASs降解方面的发展提供参考。

关键词: 全氟或多氟烷基化合物, 光化学, 高级氧化技术, 自由基, 高级还原技术, 降解率, 脱氟率

Abstract:

Per- and polyfluoroalkyl substances (PFASs) are a class of persistent organic pollutants that exhibit high resistance to degradation, bioaccumulation, and potential toxicity. They are widely present in various environmental media, and the aqueous environment is one of the most significant fates for PFASs. However, conventional water treatment technologies struggle to remove PFASs. In recent years, advanced oxidation processes (AOPs) or advanced reduction processes (ARPs) based on ultraviolet (UV) light have shown great potential and promising prospects for the removal of PFASs. According to the latest research on the degradation of PFASs by direct UV photodegradation, UV-AOPs and UV-ARPs, this article focused on the degradation mechanism, degradation efficiency and influencing factors of different reaction systems. Among them, the degradation mechanism included active species generation mechanism and reaction mechanism; the degradation efficiency included degradation rate and defluorination rate; and the influencing factors included light wavelength, pH, dissolved oxygen, inorganic ions and humic acid. Finally, the difficulties to be overcome were proposed when UV-AOPs or UV-ARPs were applied to the removal of PFASs in real water bodies, aiming to provide thinking for its future development.

Key words: per- and polyfluoroalkyl substances, photochemistry, advanced oxidation processes, radical, advanced reduction processes, degradation rate, defluorination rate

中图分类号:

张茜, 李皓芯, 张天阳, 李子富, 孙文俊, 敖秀玮. 基于紫外线的高级氧化或高级还原技术降解水中全氟或多氟烷基化合物[J]. 化工进展, 2024, 43(8): 4587-4600.

ZHANG Xi, LI Haoxin, ZHANG Tianyang, LI Zifu, SUN Wenjun, AO Xiuwei. Degradation of per- and polyfluoroalkyl substances in water by UV-based advanced oxidation or advanced reduction processes[J]. Chemical Industry and Engineering Progress, 2024, 43(8): 4587-4600.

图/表 8

表1 紫外线直接光解PFASs的研究总结

化合物	光波长/nm	灯功率/W	反应时间/h	降解率/%	脱氟率/%	参考文献
PFOA	254	200	72	89.5	33	[27]
PFOA	185	20	3	87	21	[23]
PFOA	254	23	2	9	—	[26]
PFOA	185	23	2	87	25	[26]
PFOA	185	15	2	61.7	17.1	[25]
PFOS	185	23	12	8	—	[28]
PFOS（水溶液）	254	32	24	8	—	[21]
PFOS（碱性2-丙醇溶液）	254	32	24	76	—	[21]
6∶2 FTUCA	254	—	2	<7	—	[22]

表2 PFOS和PFOA主要理化性质

性质	PFOS	PFOA
CAS号	176-23-1	335-67-1
物理状态（室温、标准大气压）	白色粉末	白色粉末/蜡状白色固体
分子式	CF₃(CF₂)₇SO₃H	CF₃(CF₂)₆COOH
分子量	500.130	414.068
蒸气压/Pa	3.31×10^-4（20℃）	4.21（25℃）
水中溶解度/g·L^-1	0.57	3.3
pK_a	3.27	2.5
半衰期（水中，25℃）/年	>41	>92

表3 均相UV-AOPs去除PFASs的研究总结

化合物	光波长/nm	灯功率/W	反应时间/h	UV-AOPs	降解率/%	脱氟率/%	参考文献
PFOA	254	24	24	UV/H₂O₂	19.7	6.8	[33]
PFOA	254	400	12	UV/H₂O₂（HCO₃^-共存）	100	82.3	[34]
PFOA	254	28	4	UV/O₃	27.1	10.6	[35]
PFASs	185/254	300	20min	UV/O₃	95	—	[36]
PFOA	220~460	200	2	UV/Na₂S₂O₈	99.1	—	[37]
PFOA	220~460	200	12	UV/Na₂S₂O₈	—	73.8	[37]
OBS	254	—	5	UV/Na₂S₂O₈	100	27.6	[38]
PFBA	254~400	1000	5	UV/Na₂S₂O₈	88.0	39.6	[39]
PFOA	254	23	2	UV/NaIO₄	70	17	[26]
PFOA	185	23	2	UV/NaIO₄	60	13	[26]
PFOA	254	15	2	UV/NaIO₄（通O₂）	47	12.5	[40]
PFOA	254	15	2	UV/NaIO₄（通N₂）	69	17	[40]
PFOA	254	24	30min	UV/NaClO	6	—	[41]

表4 非均相UV-AOPs去除PFASs的研究总结

化合物	光波长/nm	灯功率/W	反应时间	UV-AOPs	降解率/%	脱氟率/%	参考文献
GenX	230~300	15	48h	UV/TiO₂	37	2.8	[32]
PFOA	310~400	500	6h	UV/TiO₂	30	—	[42]
PFOA	254	400	12h	UV/Cu-TiO₂	91	19	[43]
PFASs	185/254	300	20min	UV/O₃	95	—	[36]
PFOA	365	125	7h	UV/TiO₂	31.3	3.3	[44]
				UV/Ag-TiO₂	57.7	8.7
				UV/Pd-TiO₂	94.2	25.9
				UV/Pt-TiO₂	100	34.8
PFOA	200~600	150	8h	UV/TiO₂-rGO	86	30	[45]
PFOA	365	24	30min	UV/BN/TiO₂	100	—	[46]
PFOA	365	24	60min	UV/BN/TiO₂	—	>50	[46]
PFOA	254	32	4h	UV/In₂O₃-300℃	100	35	[47]
PFOA	254	32	4h	UV/In₂O₃-400℃	100	38	[47]
PFOA	185	14	65min	UV/纳米针状β-Ga₂O₃	100	—	[48]
PFOA	254	50	90min	UV/纳米棒状β-Ga₂O₃	98.8	56.2	[49]
PFOA	254	32	90min	UV/Ga₂O₃/PMS	100	—	[50]
PFOA	185	32	60min	UV/Ga₂O₃/PMS	100	—	[50]
PFOA	254	200	60min	UV/In-Ga₂O₃	100	—	[51]
5∶3 FTCA	365	—	3d	UV/ZnO	96	14.9	[52]
PFOA	254	—	4h	UV/ZnO-rGO/Na₂S₂O₈/O₃	99.2	60	[53]
PFOA	185/254	8	4h	UV/H₃PW₁₂O₄₀/BMS	—	52.6	[54]
PFOA	365	500	40min	UV/{0 1 0}-BiOCl	100	—	[55]
PFOA	365	500	4h	UV/{0 1 0}-BiOCl	—	41	[55]
PFOA	254	500	6h	UV/BiOCl/Zn-Al水滑石（BHZA）	94	—	[56]
GenX	254	—	4h	UV/Bi/TnTs@AC	70.0	42.7	[55]
PFOA	254	10	12h	UV/BiOCl	100	59.3	[57]

图1 PFOS和PFOA在UV/PDS体系中的降解机理[60]

图2 PFOA在UV/IO4-体系中的降解机理[60]

表5 UV-ARPs去除PFASs的研究总结

化合物	光波长 /nm	灯功率 /W	反应时间/h	UV-AOPs	降解率 /%	脱氟率 /%	参考文献
GenX	254	—	2	UV/SO $3 2 -$	100	—	[88]
GenX	254	—	6	UV/SO $3 2 -$	—	90	[88]
PFOA	254	10	1	UV/SO $3 2 -$	100	—	[89]
PFOA	254	10	24	UV/SO $3 2 -$	—	88.5	[89]
PFOA	254	250	10min	UV/SO $3 2 -$	100	45.7	[90]
PFOS	185	10	4	UV/SO $3 2 -$	97.3	68.5	[91]
PFOS	254	10	4	UV/SO $3 2 -$	85.8	64.6	[91]
PFOS	185	—	3	UV/SO $3 2 -$	—	53.5	[92]
PFOS	254	—	3	UV/SO $3 2 -$	—	40.2	[92]
F-53B	254	—	1min	UV/SO $3 2 -$	99	—	[93]
F-53B	254	—	8	UV/SO $3 2 -$	—	90	[93]
PFOA	254	15	6	UV/I^-	93.9	76.8	[94]
PFOS	254	14	1.5	UV/I^-（HA共存）	86.0	55.6	[95]
PFOA	254	14	1.5	UV/I^-	67.5	23.5	[96]
PFOS	254	36	8	UV/IAA	95	—	[97]
PFOA	254	36	2	UV/DIHA	95	51	[98]
PFOS	254	14	0.5	UV/NTA	45.1	18.6	[99]
PFOS	254	14	10	UV/NTA	85.4	46.8	[99]

表5 UV-ARPs去除PFASs的研究总结

化合物	光波长 /nm	灯功率 /W	反应时间/h	UV-AOPs	降解率 /%	脱氟率 /%	参考文献
GenX	254	—	2	UV/SO $3 2 -$	100	—	[88]
GenX	254	—	6	UV/SO $3 2 -$	—	90	[88]
PFOA	254	10	1	UV/SO $3 2 -$	100	—	[89]
PFOA	254	10	24	UV/SO $3 2 -$	—	88.5	[89]
PFOA	254	250	10min	UV/SO $3 2 -$	100	45.7	[90]
PFOS	185	10	4	UV/SO $3 2 -$	97.3	68.5	[91]
PFOS	254	10	4	UV/SO $3 2 -$	85.8	64.6	[91]
PFOS	185	—	3	UV/SO $3 2 -$	—	53.5	[92]
PFOS	254	—	3	UV/SO $3 2 -$	—	40.2	[92]
F-53B	254	—	1min	UV/SO $3 2 -$	99	—	[93]
F-53B	254	—	8	UV/SO $3 2 -$	—	90	[93]
PFOA	254	15	6	UV/I^-	93.9	76.8	[94]
PFOS	254	14	1.5	UV/I^-（HA共存）	86.0	55.6	[95]
PFOA	254	14	1.5	UV/I^-	67.5	23.5	[96]
PFOS	254	36	8	UV/IAA	95	—	[97]
PFOA	254	36	2	UV/DIHA	95	51	[98]
PFOS	254	14	0.5	UV/NTA	45.1	18.6	[99]
PFOS	254	14	10	UV/NTA	85.4	46.8	[99]

图3 PFASs在UV/SO32-体系中的降解机理[60]

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基于紫外线的高级氧化或高级还原技术降解水中全氟或多氟烷基化合物

Degradation of per- and polyfluoroalkyl substances in water by UV-based advanced oxidation or advanced reduction processes

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