活化过氧乙酸技术降解环境有机污染物的研究进展

王辉锋; 郭艳菲; 郭壮; 黄意涵; 徐东耀; 魏健

doi:10.12153/j.issn.1674-991X.20230056

活化过氧乙酸技术降解环境有机污染物的研究进展

doi: 10.12153/j.issn.1674-991X.20230056

王辉锋^{1, 3,},
郭艳菲^{1, 4, ,},
郭壮^{1, 2},
黄意涵^{2, 5},
徐东耀⁴,
魏健^{1, 2, ,}

1.
环境基准与风险评估国家重点实验室, 中国环境科学研究院
2.
中国环境科学研究院水生态环境研究所
3.
中国环境科学研究院环境工程技术有限公司
4.
中国矿业大学(北京)化学与环境工程学院
5.
华北电力大学(北京)环境科学与工程学院

基金项目: 中央级公益性科研院所基本科研专项（2022YSKY-65）

详细信息

作者简介:
王辉锋（1978—），男，高级工程师，博士，主要从事水污染治理技术研究，13311307830@126.com

通讯作者:
郭艳菲（1988—），女，博士研究生，研究方向为水污染控制技术，guoyanfeide@163.com

魏健（1983—），男，副研究员，博士，主要从事流域水污染治理与管理研究，weijian0911@163.com

中图分类号: X703
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- 被引次数: 0
出版历程
- 收稿日期: 2023-01-27
- 网络出版日期: 2023-11-24

Research progress on the degradation of environmental organic pollutants by activated peracetic acid technology

WANG Huifeng^{1, 3
,},
GUO Yanfei^{1, 4
, ,},
GUO Zhuang^{1, 2},
HUANG Yihan^{2, 5},
XU Dongyao⁴,
WEI Jian^{1, 2
, ,}

1.
State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences
2.
Institute of Water Ecology and Environment, Chinese Research Academy of Environmental Sciences
3.
Chinese Research Academy of Environmental Sciences Environmental Technology & Engineering Co., Ltd.
4.
College of Chemical and Environmental Engineering, China University of Mining and Technology (Beijing)
5.
College of Environmental Sciences and Engineering, North China Electric Power University (Beijing)

摘要

摘要:
近年来，以抗生素、内分泌干扰物等为代表的新污染物在环境中被频繁检出，对生态系统和人类健康构成潜在风险，高效稳定的有机污染物控制技术研发是当前环境领域的研究热点。以活化过氧乙酸的高级氧化技术为研究对象，对过渡金属、碳材料及其复合材料活化过氧乙酸的效果及其降解有机污染物的机制进行系统论述，重点探讨反应过程中的自由基（有机自由基、羟基自由基）和非自由基（单线态氧、高价金属氧物种、电子转移和表面络合的复合物）降解机制，总结了活化过氧乙酸技术在废水、土壤或沉积物、地下水等环境介质中对污染物的降解效果。提出了未来研究重点，即开发高效稳定的活化过氧乙酸催化剂，加强活化过氧乙酸技术在土壤和沉积物中降解有机污染物机制的探索，深入联合其他处理技术的应用研究。
- 过氧乙酸(PAA) /
- 过渡金属 /
- 碳材料 /
- 复合材料 /
- 降解机制
Abstract:
The frequent detection of emerging contaminants poses a potential risk to ecosystems and human health, such as antibiotics and endocrine disruptors in the environment in recent years. The research and development of efficient and stable organic pollutant control technology is a research hotspot in the current environmental field. Taking the advanced oxidation technology of activated peracetic acid (PAA) as the research example, the effectiveness of activated PAA through transition metals, carbon materials and their composites, and their degradation mechanism of organics were discussed, with emphasis on the degradation mechanism of free radicals (organic radicals, hydroxyl radicals) and non-radicals (singlet oxygen, high-valent metal-Oxo species, electron transfer and surface complexes). In addition, the application effect of activated PAA in wastewater, soil or sediments, groundwater, and other environmental media for the degradation of organic pollutants was summarized. Finally, future research focuses were proposed, including developing the catalysts of activated PAA with efficiency and stability, strengthening the mechanism exploration of activated PAA to degrade organic pollutants in soil and sediment, and deepening the application studies of combined treatment technologies.
- peracetic acid (PAA) /
- transition metals /
- carbon materials /
- composite materials /
- degrading mechanism

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图 1 2000—2022年Web of Science中关于PAA的发文量

Figure 1. Number of papers published on PAA in Web of Science in 2000-2022

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图 2 基于PAA的高级氧化技术降解有机污染物的机制

Figure 2. Degradation mechanisms of organic pollutants by PAA-based AOPs

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图 3 过渡金属活化PAA降解有机污染物的自由基机制

Figure 3. Free radical mechanism of transition-metal activated PAA for degradation of organic pollutants

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图 4 基于PAA的高级氧化技术降解有机污染物的非自由基机制

Figure 4. Non-free radical mechanism of organic pollutants by PAA-based AOPs

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表 1 均相过渡金属活化PAA降解有机污染物的效能

Table 1. Effectiveness of homogeneous transition-metal activated PAA to degrade organic pollutants

活化PAA的催化剂	降解的有机污染物		反应条件	降解率/%	数据来源
活化PAA的催化剂	名称	浓度/(µmol/L)	反应条件	降解率/%	数据来源
Fe(Ⅱ)	亚甲基蓝、萘普生、双酚A	15	催化剂浓度为100 μmol/L，PAA浓度为 100 μmol/L， pH为3.0，温度为22 ℃，时间为10 min	89.4、98.2、87.7	文献[13]
Co(Ⅱ)	卡马西平	15	催化剂浓度为10 μmol/L，PAA浓度为100 μmol/L， pH为7.1，温度为22 ℃，时间为30 min	97.7	文献[15]
Fe(Ⅱ)	双氯芬酸	1	催化剂浓度为5 mg/L，PAA浓度为100 μmol/L， pH为7.0，温度为25 ℃，时间为1 min	80	文献[16]
Fe(Ⅵ)	卡马西平	10	催化剂浓度为200 μmol/L，PAA浓度为100 μmol/L， pH为9.0，温度为(25±1)℃，时间为1 min	100	文献[17]
Cu²⁺强化UV	双氯芬酸	1	催化剂浓度为5 μmol/L，PAA浓度为50 μmol/L， pH为7.0，时间为20 min	96	文献[18]
Cu(Ⅱ)协同热	双氯芬酸	5	催化剂浓度为10 μmol/L，PAA浓度为0.55 mmol/L， pH为8，温度为60 °C，时间为13 min	100	文献[19]
FeCl₃	罗丹明B	50¹⁾	催化剂浓度为50 mg/L，PAA浓度为50 mg/L， pH为3.0，时间为10 min	99.9	文献[20]
1)单位为mg/L。

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表 2 非均相过渡金属活化PAA降解有机污染物的效能

Table 2. Effectiveness of heterogeneous transition-metal activated PAA to degrade organic pollutants

活化PAA的催化剂	降解的有机污染物		反应条件	降解率/%	数据来源
活化PAA的催化剂	名称	浓度/(µmol/L)	反应条件	降解率/%	数据来源
S-Fe⁰	磺胺二甲嘧啶	5^1）	催化剂浓度为20 mg/L，PAA浓度为100 µmol/L，pH为4.0，时间为60 min	86.5	文献[21]
FeS	SMX	10	催化剂浓度为25 mg/L，PAA浓度为100 µmol/L，pH为7.0，时间为10 min	93.08	文献[22]
零价铜	双氯芬酸	1	催化剂浓度为0.5 g/L，PAA浓度为100 µmol/L，pH为3.0，温度为25 ℃，时间为40 min	95.5	文献[23]
纳米CuO	卡马西平	4.23	催化剂浓度为40 mg/L，PAA浓度为0.52 mmol/L，pH为7.0，时间为30 min	87	文献[24]
CuFeS₂	甲硝唑	10^1）	催化剂浓度为4 g/L，PAA浓度为460 µmol/L，pH为3.0，时间为30 min	83.92	文献[25]
Co₃O₄	橙G	50	催化剂浓度为 0.1 g/L，PAA浓度为0.5 mmol/L，pH为7.0，时间为90 min	100	文献[26]
FeCo₂O₄	SMX	10	催化剂浓度为0.1 g/L，PAA浓度为100 µmol/L，pH为7.0，温度为25 ℃，时间为60 min	97	文献[28]
Co_1.1Mn_1.9O₄	SMX	10	催化剂浓度为25 mg/L，PAA浓度为0.26 mmol/L，pH为7.0，温度为20 ℃，时间为7 min	100	文献[29]
CoFe₂O₄	罗丹明B	20 ^1）	催化剂浓度为 0.5 g/L，PAA浓度为0.8 mmol/L，pH为7.0，时间为10 min	95	文献[30]
零价钴	SMX	5	催化剂浓度为0.1 g/L，PAA浓度为50 µmol/L，pH为7.0，时间为10 min	99.4	文献[31]
零价钴	罗丹明B	20 ^1）	催化剂浓度为0.1 g/L，PAA浓度为0.8 mmol/L，pH为7.0，时间为3 min	98.3	文献[32]
LaCoO₃	SMX	50	催化剂浓度为20 mg/L，PAA浓度为0.66 mmol/L，pH为7.0，温度为25 ℃，时间为60 min	100	文献[33]
1)单位为mg/L。

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表 3 碳材料活化PAA降解有机污染物的效果

Table 3. Effectiveness of carbon material activated PAA to degrade organic pollutants

活化PAA的催化剂	降解的有机污染物		反应条件	降解率/%	数据来源
活化PAA的催化剂	名称	浓度/(μmol/L)	反应条件	降解率/%	数据来源
活性炭纤维	活性艳红 X-3B	50	催化剂浓度为2 g/L，PAA浓度为5 mmol/L， pH=7.0，温度为25 ℃，时间为45 min	97	文献[4]
氮掺杂还原石墨烯	SMX	150	催化剂浓度为0.5 g/L，PAA浓度为1 mmol/L， pH为3.0，温度为25 ℃，时间为60 min	96	文献[34]
氮掺杂氧化石墨烯	苯酚	1^1）	催化剂浓度为30 mg/L，PAA浓度为25 mg/L， pH为7.0，时间为60 min	100	文献[35]
剩余污泥制备碳基材料	4-氯苯酚	5^1）	催化剂浓度为25 mg/L，PAA浓度为6 mmol/L， pH为7.0，时间为90 min	91.2	文献[36]
花生壳基生物炭	乙酰氨基酚	100	催化剂浓度为0.2 g/L，PAA浓度为4 mmol/L， pH为5.0，时间为20 min	92.8	文献[37]
碳化聚苯胺	苯酚	10	催化剂浓度为25 mg/L，PAA浓度为0.1 mmol/L， pH为7.0，时间为60 min	96	文献[38]
热改性活性炭	SMX	79	催化剂浓度为50 mg/L，PAA浓度为0.26 mmol/L， pH为7.0，时间为90 min	99.4	文献[39]
碳纳米管	偶氮染料	20^1）	催化剂浓度为0.1 g/L，PAA浓度为0.02 g/L， pH为7.0，时间为180 min	≥90	文献[40]
氧化还原石墨烯	SMX	10	催化剂浓度为0.1 g/L，PAA浓度为100 μmol/L， pH为5，温度为(25±2)℃，时间为5 min	95	文献[41]
1)单位为mg/L。

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表 4 复合材料活化PAA降解有机污染物的效果

Table 4. Effectiveness of composite materials activated PAA to degrade organic pollutants

活化PAA的催化剂	降解的有机污染物		反应条件	降解率/%	数据来源
活化PAA的催化剂	名称	浓度/(μmol/L)	反应条件	降解率/%	数据来源
Fe负载生物质炭	酸性橙色染料	143	催化剂浓度为0.3 g/L，PAA浓度为1.144 mol/L， pH为7.0，时间为25 min	93.3	文献[42]
Fe₂O₃改性蒙脱石	2,4-二氯苯酚	100¹⁾	催化剂浓度为1 g/L，PAA浓度为0.02 mol/L， pH为7.0，温度为25 ℃，时间为210 min	70	文献[43]
CoFe₂S₄-CN	罗丹明B	40	催化剂浓度为20 mg/L，PAA浓度为1 mmol/L， pH为6.5，温度为25 ℃，时间为60 min	99.1	文献[44]
Co@微米零价铁	SMX	20	催化剂浓度为0.1 g/L，PAA浓度为200 µmol/L， pH为7.0，时间为30 min	96	文献[45]
RuO₂/MWCNTs	SMX	50	催化剂浓度为0.2 g/L，PAA浓度为1 mmol/L， pH为7，时间为15 min	100	文献[46]
金属有机骨架（ZIF）-67	磺胺氯哒嗪	10	催化剂浓度为0.05 g/L，PAA浓度为50 µmol/L， pH为7.0，温度为25 ℃，时间为3 min	100	文献[47]
CoFe₂O₄/CuO	SMX	10	催化剂浓度为20 mg/L，PAA浓度为200 µmol/L， pH为7.0，温度为31 ℃，时间为10 min	92	文献[48]
氮化碳负载FeCo₂S₄	罗丹明B	40	PAA浓度为1 mmol/L，pH为6.5，温度为25 ℃，时间为60 min	100	文献[49]
混合Fe(Ⅱ)/Fe(Ⅲ)价态 MIL-53(Fe)	对硝基苯酚	20¹⁾	催化剂浓度为20 mg/L，PAA浓度为5 mol/L， pH为7.0，温度为20 ℃，时间为120 min	100	文献[50]
CoFe₂O₄@木质素衍生生物质炭	SMX	10¹⁾	催化剂浓度为0.1 g/L，PAA浓度为550 µmol/L， pH 为7.0，温度为25 ℃，时间为60 min	95.8	文献[51]
1)单位为mg/L。

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表 5 活化过氧乙酸技术在降解废水有机污染物的应用

Table 5. Application of activated PAA technology to degrade organic pollutants in wastewater

降解的有机污染物			PAA浓度/ (mmol/L)	活化剂		pH	活性物种	去除率/%	数据来源
类型	名称	浓度/(µmol/L)	PAA浓度/ (mmol/L)	种类	剂量	pH	活性物种	去除率/%	数据来源
酚类有机物	苯酚	10	0.4	Co(Ⅱ)	0.01 mmol/L	7.0	CH₃C(O)OO·	74.1（10 min）	文献[58]
	对硝基苯酚	20¹⁾	5 000	混合Fe(Ⅱ)/Fe(Ⅲ) 价态MIL-53(Fe)	20 mg/L	7	·OH	100（120 min）	文献[50]
	苯酚	10	0.1	碳化聚苯胺	25 mg/L	7	¹O₂	96（60 min）	文献[38]
染料	亚甲蓝	31.26	3.6	电化学（EC）	铂片和石墨板电极，电解液Na₂NO₃浓度为0.45 g/L；电流密度为10 mA/cm²	3	·OH、CH₃C(O)O·和 CH₃C(O)OO·	93.99（120 min）	文献[59]
	橙G	50	0.5	Co₃O₄	100 mg/L	7	CH₃C(O)O·和 CH₃C(O)OO·	100（90 min）	文献[26]
	偶氮染料	20¹⁾	20¹⁾	碳纳米管	100 mg/L	7	未提及	>90（180 min）	文献[40]
药物	卡马西平	4.23	0.52	纳米CuO	40 mg/L	7.0	CH₃C(O)OO·	87（30 min）	文献[24]
	土霉素	≤10.86	0.066	UV	波长为254 nm, 照射剂量为0~223.2 mJ/cm²	7.1	·OH	100（45 min）	文献[60]
	诺氟沙星	6.26	0.131	中压紫外线 (MPUV)	波长为200~300 nm，照射剂量为0~500 mJ/cm²	9	·OH、·O₂^-和¹O₂	96.60（50 min）	文献[61]
	三氯生	1	1	UV-Fe²⁺	Fe²⁺浓度为0.56 mg/L，波长为254 nm，光强度为0.24 mW/cm²	3.5	·OH、CH₃C(O)O·和CH₃C(O)OO·	100（20 min）	文献[62]
	磺胺二甲嘧啶	35.93	0.1	UV/Fe⁰	Fe⁰浓度为0.1 g/L，波长为254 nm，紫外灯功率为6 W	4	·OH、CH₃C(O)O·和CH₃C(O)OO·	85（60 min）	文献[63]
	SMX	5	0.2	热	60 ℃	7	CH₃C(O)O·和CH₃C(O)OO·	86（25 min）	文献[9]
	SMX	5	400	Fe²⁺-沸石	800 mg/L	7	·OH	100（50 min）	文献[11]
	SMX	50	0.66	LaCoO₃	20 mg/L	7	CH₃C(O)O·和 CH₃C(O)OO·	100（60 min）	文献[33]
	SMX	10	0.55	CoFe₂O₄@生物质炭	100 mg/L	7.0±0.2	CH₃C(O)O·和CH₃C(O)OO·	95.8（60 min）	文献[51]
注：本表所列均为降解反应的最佳条件。1)单位为mg/L。

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表 6 活化过氧乙酸技术在降解土壤和沉积物中有机污染物的应用

Table 6. Application of activated PAA technology to degrade organic pollutants in soil and sediment

降解的有机污染物			氧化剂	土壤/沉积物基本情况	pH	影响去除效果的因素	去除效果
类型	名称	浓度	氧化剂	土壤/沉积物基本情况	pH	影响去除效果的因素	去除效果
湖泊沉积物^[64]	α-甲基萘	10~25 mmol/kg	去离子水、乙酸、H₂O₂溶液体积比为1:1:1的混合物	总有机碳含量为2.1%~ 12.8%，表面积为3.2~ 22.0 m²/g	7.49~7.67	沉积物的表面积和有机碳含量	24 h，沙质沉积物和粉质黏土沉积物中α-甲基萘的去除率分别为70%和100%
湖泊沉积物^[65]	苯并[a]芘	10~25 mmol/kg	H₂O₂、乙酸、去离子水体积比为1:1:1的混合物	沉积物Ⅰ，大部分颗粒粒径<75 μm，有机碳含量为12.6%，表面积为14.0 m²/g；沉积物Ⅱ，沙质类型，大部分颗粒粒径为75~850 μm，有机碳含量为0.5%，表面积为1.2 m²/g	约7	沉积物的粒径、表面积和有机碳含量	24 h，苯并[a]芘的去除率均为100%，其中，沉积物Ⅰ中的反应速率为沉积物Ⅱ的1.5倍
超级基金污染场地(Superfund)^[66]	多环芳烃(PAHs)	密歇根湖西南海岸的污染土壤（Bedford LT）和Bedford LT10号场地的PAH浓度分别为500~ 1 000、2 000~ 3 000 mg/kg	H₂O₂、乙酸、去离子水体积比为3:5:7或3:3:9的混合物	Bedford LT 10和Bedford LT土壤的含水量分别为25%和18.5%，TOC浓度分别为11%和18.5%，pH分别为7.09和7.04	约7	沉积物的表面积和有机碳含量	24 h，Bedford LT 的14种PAHs几乎完全降解； Bedford LT10号未观察到14种PAHs的降解
沙质和粉质黏土沉积物^[67]	α-甲基萘和苯并[a]芘	α-甲基萘或苯并[a]芘浓度为500 mg/kg	H₂O₂、乙酸、去离子水体积比为2:5:8的混合物	沙质沉积物，颗粒粒径>150 μm；粉质黏土，颗粒粒径为75~150 μm，总有机碳浓度分别为0.5%和1.4%	约7	沉积物粒径和有机碳含量	24 h，α-甲基萘的去除率为90%；苯并[a]芘的去除率为90%

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参考文献(68)

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活化过氧乙酸技术降解环境有机污染物的研究进展

doi: 10.12153/j.issn.1674-991X.20230056

作者简介:
王辉锋（1978—），男，高级工程师，博士，主要从事水污染治理技术研究，13311307830@126.com

通讯作者:
郭艳菲（1988—），女，博士研究生，研究方向为水污染控制技术，guoyanfeide@163.com

魏健（1983—），男，副研究员，博士，主要从事流域水污染治理与管理研究，weijian0911@163.com

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Research progress on the degradation of environmental organic pollutants by activated peracetic acid technology

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活化过氧乙酸技术降解环境有机污染物的研究进展

doi: 10.12153/j.issn.1674-991X.20230056

作者简介: 王辉锋（1978—），男，高级工程师，博士，主要从事水污染治理技术研究，13311307830@126.com

通讯作者: 郭艳菲（1988—），女，博士研究生，研究方向为水污染控制技术，guoyanfeide@163.com 魏健（1983—），男，副研究员，博士，主要从事流域水污染治理与管理研究，weijian0911@163.com

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Research progress on the degradation of environmental organic pollutants by activated peracetic acid technology

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作者简介:
王辉锋（1978—），男，高级工程师，博士，主要从事水污染治理技术研究，13311307830@126.com

通讯作者:
郭艳菲（1988—），女，博士研究生，研究方向为水污染控制技术，guoyanfeide@163.com

魏健（1983—），男，副研究员，博士，主要从事流域水污染治理与管理研究，weijian0911@163.com