过硫酸盐高级氧化降解水体中有机污染物研究进展

doi:10.16085/j.issn.1000-6613.2018-1576

化工进展 ›› 2019, Vol. 38 ›› Issue (05): 2461-2470.DOI: 10.16085/j.issn.1000-6613.2018-1576

过硫酸盐高级氧化降解水体中有机污染物研究进展

黄智辉^1,^2,³(),纪志永^1,^2,³(),陈希^2,³,郭小甫^2,³,王士钊^2,³,袁俊生^1,^2,³

1. 河北工业大学化工学院，化工节能过程集成与资源利用国家-地方联合工程实验室，天津 300130
2. 河北工业大学化工学院，海水资源高效利用化工技术教育部工程研究中心，天津 300130
3. 河北省现代海洋化工技术协同创新中心，天津 300130

收稿日期:2018-08-01 修回日期:2018-10-22 出版日期:2019-05-05 发布日期:2019-05-05
通讯作者: 纪志永
作者简介:黄智辉（1993—），男，博士研究生，研究方向为环境化学。E-mall：<email>cmhzh@163.com</email>。
基金资助:
国家重点研发计划(2016YFB0600504);河北省研究生创新资助项目(CXZZSS2017042)

Degradation of organic pollutants in water by persulfate advanced oxidation

Zhihui HUANG^1,^2,³(),Zhiyong JI^1,^2,³(),Xi CHEN^2,³,Xiaofu GUO^2,³,Shizhao WANG^2,³,Junsheng YUAN^1,^2,³

1. National-Local Joint Engineering Laboratory of Chemical Energy Saving Process Integration and Resource Utilization, School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin 300130, China
2. Engineering Research Center of Seawater Utilization of Ministry of Education, School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin 300130, China
3. Hebei Collaborative Innovation Center of Modern Marine Chemical Technology, Tianjin 300130, China

Received:2018-08-01 Revised:2018-10-22 Online:2019-05-05 Published:2019-05-05
Contact: Zhiyong JI

摘要/Abstract

摘要：

基于硫酸根自由基（sulfate radical，SO₄ ^-·）氧化原理的活化过硫酸盐（persulfate，PS）氧化法是近年来高级氧化工艺（advanced oxidation process，AOP）的研究热点，以经济、高效、环境友好、安全稳定的优势在水处理、环境保护等领域开辟了新的思路。此前，学者们发现过硫酸盐高级氧化根据活化反应条件（如温度、光照、pH、过渡金属及催化剂等）的不同，会产生不同的自由基参与氧化反应，对降解结果也会产生不同程度的影响。本文根据相关自由基氧化机理，从产生硫酸根自由基的单一氧化、复杂活化体系硫酸根自由基与其他自由基复合氧化以及强化降解等方面，分析了近几年国内外学者对过硫酸盐降解典型有机污染物的研究及在催化剂开发方面所做的工作，指出了许多新颖的过硫酸盐活化手段及其降解效果与不足，并就未来的发展进行了展望，以期为过硫酸盐氧化法未来更好地发展和应用探索出路。

关键词: 活化过硫酸盐, 高级氧化, 硫酸根自由基, 羟基自由基, 有机污染物

Abstract:

Activated persulfate (PS) oxidation based on the oxidation principle of sulfate radical (SO₄ ^-·) is a hot research topic of advanced oxidation process (AOP) in recent years. Since activated persulfate oxidation is economical, efficient, environmentally friendly, safe and stable, it gives out new countermeasures in water treatment, environmental protection and other fields. Previously, scholars found that the activated persulfate oxidation had different free radicals involved in the oxidation reaction with different reaction conditions such as pH, catalysts, which lead to varying degrees of influence in degradation results. Based on the relevant radical oxidation mechanism, including single oxidation with sulfate radical, synergistic oxidation with sulfate radical and the other enhanced catalytic activation, the domestic and foreign scholars’ research on the degradation of typical organic pollutants by persulfate was analyzed. Besides, the work on catalyst development was studied, and many novel activated methods of persulfate and its degradation effect and deficiency were pointed out. Furthermore, the way out for better development and application of persulfate oxidation method in the future was explored.

Key words: activated persulfate, advanced oxidation process, sulfate radical, hydroxyl radical, organic pollutants

中图分类号:

黄智辉, 纪志永, 陈希, 郭小甫, 王士钊, 袁俊生. 过硫酸盐高级氧化降解水体中有机污染物研究进展[J]. 化工进展, 2019, 38(05): 2461-2470.

Zhihui HUANG, Zhiyong JI, Xi CHEN, Xiaofu GUO, Shizhao WANG, Junsheng YUAN. Degradation of organic pollutants in water by persulfate advanced oxidation[J]. Chemical Industry and Engineering Progress, 2019, 38(05): 2461-2470.

图/表 1

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污染物	活化手段	氧化剂/ 污染物（摩尔比）	反应时间 /min	去除率/%	初始 pH	最适pH	pH范围	主要氧化物质	文献
norfloxacin	磁性纳米粒子	66.67	60	90	4	4,6.7	4,6.7,9	SO₄ ^-·,·OH	[39]
chloramphenicol	UV	33.33	120	79.8	3	3	3～11	SO₄ ^-·	[24]
tetracycline	magnetic Ag/AgCl/zeolite	22.22	120	100	3.5	3.5	3.5～7.5	SO₄ ^-·,·O₂ ^-	[45]
tetracycline	AC@Fe₃O₄	441.18	240	99.8	3	3	3～7	SO₄ ^-·	[57]
sulfaclozine	UV/TiO₃	100	60	99	7,11	11	7,11	SO₄ ^-·,·OH	[38]
sulfaclozine	UV	200	60	80	7,11	7,11	7,11	SO₄ ^-·,·OH	[38]
sulfaclozine	太阳光	200	60	84	7			SO₄ ^-·,·OH	[38]
sulfaclozine	Fe(Ⅱ)	200	60	60	7			SO₄ ^-·,·OH	[38]
cefixime	UV/zeolite-TiO₂	1818.18	40	59	7			SO₄ ^-·,·OH	[46]
phenazopyridine	UV/zeolite-TiO₂	106.38	30	70	7			SO₄ ^-·,·OH	[46]
reactive black 5	UV/zeolite-TiO₂	2000	40	92	7			SO₄ ^-·,·OH	[46]
acid orange 7	Vis/MIL-53(Fe)	40	50	99	3	3	3,6,7,9	SO₄ ^-·,·OH	[41]
orange G	WMF/Fe⁰	10	8	98	3	3	3～10	SO₄ ^-·	[16]
caffeine	WMF/Fe⁰	25	50	98	7			SO₄ ^-·	[16]
4-nitrophenol	WMF/Fe⁰	25	60	96	7			SO₄ ^-·	[16]
benzotriazole	WMF/Fe⁰	25	80	90	7			SO₄ ^-·	[16]
diuron	WMF/Fe⁰	25	30	92	7			SO₄ ^-·	[16]
naphthol blue black	超声	259.03	20	92	6			SO₄ ^-·	[47]
rhodamine B	超声/FeSO₄	1300	6	99	3	3	3～11	SO₄ ^-·,·OH	[36]
amaranth	二茂铁	12.21	60	99	5	3～6	3～11	SO₄ ^-·	[23]
2,4,4'-trichlorobiphenyl	V₂O₃	256.41	240	100	5.9	5.9	5.9,7.4,8.4	SO₄ ^-·	[40]
perfluorooctanoic acid	铁改性硅藻土	12500	360	50	12	12	3,9,12	SO₄ ^-·,·O₂ ^-	[60]
perfluorooctanoic acid	UV	100	360	83.3	4			SO₄ ^-·	[27]
decabromodiphenyl ether	Fe(Ⅱ)	19183.40	360	53	3	3	3～9	SO₄ ^-·	[48]
decabromodiphenyl ether	热	23979.25	360	53.8	5	5	3～9	SO₄ ^-·	[54]
p-chloroaniline	黄铁矿(FeS₂)	5	60	100	3	3	3～11	SO₄ ^-·,·OH,·O₂ ^-	[44]
triclosan	热	5	48	100	3	3,5	3～11	SO₄ ^-·	[51]
4-tert-butylphenol	正方针铁矿	20	120	90	4.7	无影响		SO₄ ^-·,·O₂ ^-	[21]
4-tert-butylphenol	水铁矿	20	300	60	4.7	3.2	3.2～8	SO₄ ^-·,·O₂ ^-	[21]
4-tert-butylphenol	Fe(Ⅲ)	20	180	62	2.4	2.4	2.4～5	SO₄ ^-·,·O₂ ^-	[21]
EDTA	UV	60	40	100	2	2,4,6,8	2,4,6,8,10	SO₄ ^-·	[10]
triton X-45	Al⁰	73.61	90	100	3			SO₄ ^-·,·OH	[48]
bisphenol A	零价铁	28.54	60	100	5			SO₄ ^-·	[17]
phenol	纳米金刚石	30.58	20	100	11	11	2～11	SO₄ ^-·,·OH	[59]

污染物	活化手段	氧化剂/ 污染物（摩尔比）	反应时间 /min	去除率/%	初始 pH	最适pH	pH范围	主要氧化物质	文献
norfloxacin	磁性纳米粒子	66.67	60	90	4	4,6.7	4,6.7,9	SO₄ ^-·,·OH	[39]
chloramphenicol	UV	33.33	120	79.8	3	3	3～11	SO₄ ^-·	[24]
tetracycline	magnetic Ag/AgCl/zeolite	22.22	120	100	3.5	3.5	3.5～7.5	SO₄ ^-·,·O₂ ^-	[45]
tetracycline	AC@Fe₃O₄	441.18	240	99.8	3	3	3～7	SO₄ ^-·	[57]
sulfaclozine	UV/TiO₃	100	60	99	7,11	11	7,11	SO₄ ^-·,·OH	[38]
sulfaclozine	UV	200	60	80	7,11	7,11	7,11	SO₄ ^-·,·OH	[38]
sulfaclozine	太阳光	200	60	84	7			SO₄ ^-·,·OH	[38]
sulfaclozine	Fe(Ⅱ)	200	60	60	7			SO₄ ^-·,·OH	[38]
cefixime	UV/zeolite-TiO₂	1818.18	40	59	7			SO₄ ^-·,·OH	[46]
phenazopyridine	UV/zeolite-TiO₂	106.38	30	70	7			SO₄ ^-·,·OH	[46]
reactive black 5	UV/zeolite-TiO₂	2000	40	92	7			SO₄ ^-·,·OH	[46]
acid orange 7	Vis/MIL-53(Fe)	40	50	99	3	3	3,6,7,9	SO₄ ^-·,·OH	[41]
orange G	WMF/Fe⁰	10	8	98	3	3	3～10	SO₄ ^-·	[16]
caffeine	WMF/Fe⁰	25	50	98	7			SO₄ ^-·	[16]
4-nitrophenol	WMF/Fe⁰	25	60	96	7			SO₄ ^-·	[16]
benzotriazole	WMF/Fe⁰	25	80	90	7			SO₄ ^-·	[16]
diuron	WMF/Fe⁰	25	30	92	7			SO₄ ^-·	[16]
naphthol blue black	超声	259.03	20	92	6			SO₄ ^-·	[47]
rhodamine B	超声/FeSO₄	1300	6	99	3	3	3～11	SO₄ ^-·,·OH	[36]
amaranth	二茂铁	12.21	60	99	5	3～6	3～11	SO₄ ^-·	[23]
2,4,4'-trichlorobiphenyl	V₂O₃	256.41	240	100	5.9	5.9	5.9,7.4,8.4	SO₄ ^-·	[40]
perfluorooctanoic acid	铁改性硅藻土	12500	360	50	12	12	3,9,12	SO₄ ^-·,·O₂ ^-	[60]
perfluorooctanoic acid	UV	100	360	83.3	4			SO₄ ^-·	[27]
decabromodiphenyl ether	Fe(Ⅱ)	19183.40	360	53	3	3	3～9	SO₄ ^-·	[48]
decabromodiphenyl ether	热	23979.25	360	53.8	5	5	3～9	SO₄ ^-·	[54]
p-chloroaniline	黄铁矿(FeS₂)	5	60	100	3	3	3～11	SO₄ ^-·,·OH,·O₂ ^-	[44]
triclosan	热	5	48	100	3	3,5	3～11	SO₄ ^-·	[51]
4-tert-butylphenol	正方针铁矿	20	120	90	4.7	无影响		SO₄ ^-·,·O₂ ^-	[21]
4-tert-butylphenol	水铁矿	20	300	60	4.7	3.2	3.2～8	SO₄ ^-·,·O₂ ^-	[21]
4-tert-butylphenol	Fe(Ⅲ)	20	180	62	2.4	2.4	2.4～5	SO₄ ^-·,·O₂ ^-	[21]
EDTA	UV	60	40	100	2	2,4,6,8	2,4,6,8,10	SO₄ ^-·	[10]
triton X-45	Al⁰	73.61	90	100	3			SO₄ ^-·,·OH	[48]
bisphenol A	零价铁	28.54	60	100	5			SO₄ ^-·	[17]
phenol	纳米金刚石	30.58	20	100	11	11	2～11	SO₄ ^-·,·OH	[59]

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过硫酸盐高级氧化降解水体中有机污染物研究进展

Degradation of organic pollutants in water by persulfate advanced oxidation

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