基于过硫酸盐活化的高级氧化技术处理水中磺胺类药物研究进展

刘诗月; 彭向天; 马瑞瑞; 曾萍; 李娟; 朱幸运

doi:10.12153/j.issn.1674-991X.20230529

基于过硫酸盐活化的高级氧化技术处理水中磺胺类药物研究进展

doi: 10.12153/j.issn.1674-991X.20230529

刘诗月^1,,
彭向天^{1, 2, 3},
马瑞瑞^{2, 3},
曾萍^{2, 3},
李娟^{2, 3, ,},
朱幸运¹

1.
沈阳工业大学
2.
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
3.
中国环境科学研究院水生态环境研究所

基金项目: 中央级公益性科研院所基本科研业务费专项（2022YSKY-63）；国家重点研发计划项目(2022YFC3203301)；江西省华赣环境集团有限公司开放课题（HGKF-2020-01）

详细信息

作者简介:
刘诗月（1990—），女，讲师，博士，主要研究方向为水污染治理、碳排放管理，liushiyue@sut.edu.cn

通讯作者:
李娟（1988—），女，助理研究员，博士，主要研究方向为有毒有害物污染控制技术，lij2007@126.com

中图分类号: X703
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出版历程
- 收稿日期: 2023-07-17
- 录用日期: 2023-12-29
- 修回日期: 2023-10-22

Research progress of advanced oxidation technology based on persulfate activation for the treatment of sulfonamides in water

LIU Shiyue^1
,,
Peng Xiangtian^{1, 2, 3},
MA Ruirui^{2, 3},
ZENG Ping^{2, 3},
LI Juan^{2, 3
, ,},
ZHU Xingyun¹

1.
Shenyang University of Technology
2.
State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences
3.
Institute of Water Environment, Chinese Research Academy of Environmental Sciences

摘要

摘要:
磺胺类药物（SAs）是水中最常被检出的抗生素之一，传统的生物处理无法对其有效降解，研发高效降解SAs的技术具有现实意义。近年来，通过活化过硫酸盐（persulfate，PS）产生硫酸根自由基（$\mathrm{SO}_4^{-}\cdot $）的高级氧化技术受到了广泛关注。聚焦于PS的各种活化方法，包括热活化、紫外活化、金属离子及金属氧化物活化、碳材料活化、金属-有机骨架材料活化等，分析了不同活化方法可能的活化机理和优缺点，综述了基于过硫酸盐活化的高级氧化技术（PS-AOPs）在SAs降解中的应用，阐述了PS-AOPs降解SAs的机制。结果表明：活化PS的机制是通过活化方法使其分子结构中的O—O键断裂，从而使PS分解形成$\mathrm{SO}_4^{-}\cdot $或其他活性物质，活化方法决定了PS-AOPs降解SAs的效率。SAs的降解途径分为自由基途径与非自由基途径，其中自由基途径主要包括苯胺部分氧化、磺酰胺基团及相邻位点（C—NH—SO₂—C）的裂解等，非自由基途径包括电子传递、表面活化、单线态氧（¹O₂）作用等。最后，提出未来研究重点应在开发稳定高效活化PS的催化剂以及使用多种处理技术协同作用基础上，加强对SAs降解机制以及含SAs实际废水的研究。
- 磺胺类药物(SAs) /
- 过硫酸盐(PS) /
- 活化 /
- 硫酸根自由基 /
- 羟基自由基
Abstract:
Sulfonamide drugs (SAs) are one of the most frequently detected antibiotics in water, traditional biological treatment cannot effectively degrade sulfonamides, and thus the development of technology for efficient degradation of SAs has practical significance. In recent years, the advanced oxidation processes that generate sulfate radicals ($\mathrm{SO}_4^{-}\cdot $) by activating persulfate (PS) have received widespread attention. Various methods for the activation of PS were focused on, including thermal, ultraviolet light, metal ion and metal oxides, carbon materials and MOFs activation and so on; and their possible activation mechanisms, advantages and disadvantages were summarized. The application of advanced oxidation processes based on persulfate activation (PS-AOPs) in the degradation of sulfonamides was reviewed and the mechanism of degradation of SAs by PS-AOPs was summarized. The results showed that the activation mechanism of PS was to break O—O bond in the molecular structure, which led to the decomposition of PS to form $\mathrm{SO}_4^{-}\cdot $ or other active substances. The efficiency of PS-AOPs in degrading SAs was determined by the activation method. The degradation pathways of SAs were divided into free radical and non-free radical pathways, in which the free radical pathways mainly included partial oxidation of aniline, cleavage of sulfonamide groups and adjacent sites (${\mathrm{C—NH—}}{\mathrm{SO}}_2—{\mathrm{C}} $), and the non-free radical pathways included electron transfer, surface activation, and the role of single linear oxygen (¹O₂). Finally, it was suggested that the future research focus should be on the development of catalysts for stable and efficient activation of PS, as well as the synergistic effect of multiple treatment technologies. Meanwhile, research on the mechanism of SAs degradation and the actual wastewater containing SAs should be strengthened.
- sulfonamides(SAs) /
- persulfates(PS) /
- activation /
- sulfate radicals /
- hydroxyl radicals

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图 1 金属离子和金属氧化物对PDS和PMS的活化机理^[24]

Figure 1. Activation mechanism of metal ions and metal oxide for PDS and PMS

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图 2 SAs的苯胺转化途径

Figure 2. Aniline degradation pathways of SAs

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图 3 SAs原子编号

Figure 3. Atom numbering of SAs

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表 1 PMS和PDS的基本特征

Table 1. Basic features of PMS and PDS

氧化剂	化学式	结构式	分子量	溶解度/（g/L）	氧化还原电位/V	O—O键键长/Å	O—O键键能/（kJ/mol）
PMS	HSO₅		114.07	>250	1.82	1.453	140~213.3
PDS	H₂S₂O₈		194.13	>520	2.01	1.497	140

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表 2 热活化PS降解SAs的条件与效果

Table 2. Conditions and effects of thermally activated persulfate for the degradation of SAs

SAs类别	SAs浓度/ (μmol/L)	氧化剂及浓度/(mmol/L)	温度/℃	pH	反应时间/h	去除率/%
SMX^[13]	30	PDS，2	50	7	8	50
SIX^[13]	30	PDS，2	50	7	8	100
STZ^[13]	30	PDS，2	50	7	8	100
SD^[14]	30	PDS，2	60	7	6	100
SMR^[14]	30	PDS，2	50	9	2	86
SMX^[15]	39	PDS，4	70	9.5	1	93

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表 3 紫外活化PS降解SAs的条件与效果

Table 3. Conditions and effects of UV-activated PS for the degradation of SAs

SAs类别	SAs浓度/ (μmol/L)	氧化剂及浓度/ (mmol/L)	紫外线功率/W	紫外线波长/nm	pH	反应时间/min	去除率/%
SD^[21]	3.9	PDS，0.18	28	254		10	99.8
SMX^[22]	20	PDS，1	10	254	3	60	100
SMZ^[18]	53	PDS，0.44	15	254	7	60	100
SMZ^[19]	20	PDS，0.2	15	254	6.5	45	96.5
SMX^[20]	100	PDS，2	46		7	5	接近100

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表 4 金属离子及其氧化物活化PS降解SAs的条件与效果

Table 4. Conditions and effects of metal ions and metal oxide-activated PS for the degradation of SAs

SAs类别	SAs浓度/(μmol/L)	氧化剂及浓度/(mmol/L)	催化剂	pH	反应时间/min	去除率/%
SMX^[25]	10	PMS，0.1	Co²⁺	3	30	62.3
SMR^[26]	100	PDS，0.4	Ag⁺	3	240	85
SMX^[27]	63047	PDS，1 849 656	Fe²⁺	3	30	57.3
SD^[28]	8	PMS，0.033	CuFeO₂RCs	6.8	24	接近100
SMX^[29]	39	PMS，0.65	CoFe₂O₄	7	10	91
SMM^[30]	64	PDS，0.9	Fe₃O₄	6	180	88
SDM^[30]	64	PDS，100	Fe₃O₄	7	180	99.8
SMX^[31]	6	PDS，0.14	α-Fe₂O₃	6.8	180	接近100

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表 5 碳材料活化PS降解SAs的条件与效果

Table 5. Conditions and effects of carbon material-activated PS for the degradation of SAs

SAs类别	催化剂	催化剂浓度/(g/L)	氧化剂及浓度/ (mmol/L)	pH	掺杂类型	去除率/%
SMX^[36]	活性炭	0.1	PMS，0.5	7.2		91.2
SMX^[37]	活性炭		PMS，5			95
SMX^[38]	生物炭	0.05	PMS，4		氮	接近100
SMX^[39]	生物炭	0.1	PDS，0.5	10	氮、硫	68.8
SCP^[41]	氧化还原石墨烯（RGO）	0.2	PDS，7.39		氮	100
SMX^[42]	碳纳米管（CNTs）	0.1	PMS，1	7	Fe₃C	100
SMX^[43]	石墨烯	0.5	PMS，800	3.4	氮	91.7
SMX^[44]	石墨烯	0.05	PMS，1	6	N	99.9

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表 6 MOFs材料活化PS降解SAs的条件与效果

Table 6. Conditions and effects of MOFs-activated PS for the degradation of SAs

SAs类别	催化剂	催化剂浓度/(g/L)	氧化剂及浓度/(mmol/L)	pH	改性类型	去除率/%
SMZ^[49]	MIL-10（Cr）	0.15	PDS，10	6.0		80
SMX^[50]	MIL/PDA	0.1	PDS，4			79.2
SMX^[51]	Fe-MOFs-2	1	PDS，3.7	3	调节剂	91.95
SMT^[52]	DMOFS	0.1	PMS，1	10	高温碳化	提高1.8倍
SMX^[53]	MnOx@NC	0.05	PMS，0.55	5.2	氮掺杂、碳化	72.9
SMX^[54]	Co-NC-C	0.1	PMS，0.74	7	碳化	接近100
SMX^[55]	CuFe₂O₄/Fe₂O₃	0.2	PMS，6	3.4	双金属、碳化	99.7

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表 7 PS-AOPs在降解SAs过程中的主要活性物种

Table 7. Main active species in the degradation of SAs by PS-AOPs

SAs类别	氧化剂	活化方法	起主要作用的活性氧剂
SMX^[28]	PMS	CoFe₂O₄	·OH、¹O₂
SMX^[38]	PMS	氮掺杂碳材料	$\mathrm{SO}_4^{-}\cdot $、¹O₂
SMZ^[48]	PDS	MIL-101（Cr）	$\mathrm{SO}_4^{-}\cdot $
SMX^[53]	PMS	MOFs衍生碳材料	$\mathrm{SO}_4^{-}\cdot $、¹O₂、$\mathrm{O}_2^{-} \cdot$

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