电絮凝活化过单硫酸盐降解磺胺甲<inline-graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="1005-829X-2022-42-7-80/C9D9C857-C4DA-40a6-8305-02565BE64140-F502c.jpg"> </inline-graphic>唑

doi:10.19965/j.cnki.iwt.2021-1022

摘要/Abstract

摘要：

采用电絮凝（EC）/过单硫酸盐（PMS）体系降解磺胺甲唑（SMX），考察了电流、PMS和SMX浓度及反应初始pH对SMX降解的影响，比较了不同电流条件下的电化学能耗，并基于猝灭实验，分析了反应过程中存在的活性物种。结果表明：在SMX质量浓度为1 mg/L、初始pH=7、PMS浓度为20 μmol/L、电流为10 mA的条件下，6 min内EC/PMS体系对SMX降解率可达97.8%，较同等条件下单一Fe²⁺体系、电絮凝体系和Fe²⁺活化PMS体系的SMX的降解率有大幅提高；在一定范围内随着电流和PMS浓度增大，SMX降解率增大，但是电流超过40 mA或PMS浓度超过20 μmol/L均会抑制SMX的降解；在降解率基本持平时，10 mA电流条件下电解6 min，电化学能耗为9.65×10^-4 kW·h/m³，远小于40 mA电流条件下电解2 min的能耗（3.74×10^-3 kW·h/m³）；EC/PMS体系对pH有较好的适应性，当初始pH为3~9时，SMX均能被有效降解；SMX初始浓度的增加会降低SMX降解率，但SMX降解总量会增加；自由基猝灭实验表明，活化过程中的主要活性物种为硫酸根自由基和羟基自由基，且硫酸根自由基所占比例较大。

关键词: 电絮凝, 活化, 过硫酸盐, 磺胺甲唑

Abstract:

The electroflocculation（EC）/permonosulfate（PMS） system was used to degrade sulfamethoxazole （SMX）. The effects of current，PMS and SMX concentrations and initial pH on the degradation of SMX were investigated. The electrochemical energy consumption was compared under different current conditions，and the active species present in the reaction process were analyzed based on the quenching experiment. The results showed that the degradation rate of SMX could reach 97.8% within 6 min by EC/PMS system under the conditions of the initial SMX mass concentrations of 1 mg/L，the initial pH=7，the PMS dosage of 20 μmol/L，and the current of 10 mA. Compared with the single Fe²⁺ system，electroflocculation system and PMS/Fe²⁺ system under the same conditions，the EC/PMS system had a higher degradation rate of SMX. The degradation rate of SMX increased with the increased of current and PMS concentration within a certain range，but the degradation of SMX was inhibited by the current exceeding 40 mA or the PMS concentration exceeding 20 μmol/L. When the degradation rate was basically the same，under the condition of 10 mA current for 6 min，the electrochemical energy consumption was 9.65×10^-4 kW·h/m³，which was much less than the energy consumption （3.74×10^-3 kW·h /m³） of 2 min at 40 mA current. EC/PMS system had better adaptability to pH，when the initial pH was 3-9，SMX could be effectively degraded. An increase in the initial concentration of SMX decreased the rate of SMX degradation，but the total amount of SMX degradation increased. The free radical quenching experiments showed that the main active species in the activation process were sulfate radicals and hydroxyl radicals，and sulfate radicals accounted for a large proportion.

Key words: electroflocculation, activation, persulfate, sulfamethoxazole

中图分类号:

刘晓艳, 詹焕, 叶中伟, 谢世伟, 王松林. 电絮凝活化过单硫酸盐降解磺胺甲唑[J]. 工业水处理, 2022, 42(7): 80-86.

Xiaoyan LIU, Huan ZHAN, Zhongwei YE, Shiwei XIE, Songlin WANG. Degradation of sulfamethoxazole by electroflocculation activated permonosulfate[J]. Industrial Water Treatment, 2022, 42(7): 80-86.

https://www.iwt.cn/CN/Y2022/V42/I7/80

图/表 10

图1 实验装置示意

Fig. 1 Schematic diagram of the experimental device

图2 不同体系下SMX的降解效率

Fig. 2 Degradation efficiency of SMX in different systems

图3 电流对EC/PMS体系降解SMX的影响

Fig. 3 The effect of current on the degradation of SMX in EC/PMS system

表1 10 mA和40 mA电流下降解率基本持平时能耗比较

Table 1 Comparison of energy consumption when the degradation rate was basically the same under the current of 10 mA and 40 mA

电流/mA	电解时间/min	降解率/%	E _EO/（kW·h·m^-3）
10	6	97.8	9.65×10^-4
40	2	97.3	3.74×10^-3

图4 PMS浓度对EC/PMS体系降解SMX的影响

Fig. 4 The effect of PMS concentration on the degradation of SMX in the EC/PMS system

图5 初始pH对EC/PMS体系降解SMX的影响

Fig. 5 The effect of initial pH on the degradation of SMX in the EC/PMS system

图6 初始SMX质量浓度对EC/PMS体系降解SMX的影响

Fig. 6 The effect of initial SMX mass concentration on the degradation of SMX in the EC/PMS system

表2 不同SMX质量浓度下SMX的降解总量

Table 2 Total degradation of SMX under different SMX mass concentrations

初始SMX质量浓度/（mg·L^-1）	0.5	1	2	4
降解总量/mg	0.245	0.489	0.799	0.976

图7 猝灭剂对SMX降解的影响

Fig.7 The effect of quencher on the degradation of SMX

图8 EC/PMS体系降解SMX的机理示意

Fig. 8 Schematic diagram of the mechanism of degradation of SMX in EC/PMS system

参考文献 20

1	陈姗，许凡，张玮，等. 磺胺类抗生素污染现状及其环境行为的研究进展［J］. 环境化学，2019，38（7）：1557-1569. doi:10.7524/j.issn.0254-6108.2018091901
	CHEN Shan， XU Fan， ZHANG Wei，et al. Research progress in pollution situation and environmental behavior of Sulfonamides［J］. Environmental Chemistry，2019，38（7）：1557-1569. doi:10.7524/j.issn.0254-6108.2018091901
2	KOVALAKOVA P， CIZMAS L， MCDONALD T J，et al. Occurrence and toxicity of antibiotics in the aquatic environment：A review［J］. Chemosphere，2020，251：126351. doi:10.1016/j.chemosphere.2020.126351
3	银仁莉. 过硫酸盐的非自由基氧化降解磺胺抗生素的效能及机制［D］. 哈尔滨：哈尔滨工业大学，2019. doi:10.1016/j.cej.2018.09.184
	YIN Renli. Performance and mechanism of sulfonamides degradation by the nonradical oxidation of persulfates［D］. Harbin：Harbin Institute of Technology，2019. doi:10.1016/j.cej.2018.09.184
4	赵富强，高会，张克玉，等. 中国典型河流水域抗生素的赋存状况及风险评估研究［J］. 环境污染与防治，2021，43（1）：94-102.
	ZHAO Fuqiang， GAO Hui， ZHANG Keyu，et al. Occurrence and risk assessment of antibiotics in typical river basins in China［J］. Environmental Pollution & Control，2021，43（1）：94-102.
5	WU Yao， GUO Jing， HAN Yijie，et al. Insights into the mechanism of persulfate activated by rice straw biochar for the degradation of aniline［J］. Chemosphere，2018，200：373-379. . doi:10.1016/j.chemosphere.2018.02.110
6	GIANNAKIS S， LIN K Y A， GHANBARI F. A review of the recent advances on the treatment of industrial wastewaters by sulfate radical-based advanced oxidation processes（SR-AOPs）［J］. Chemical Engineering Journal，2021，406：127083. doi:10.1016/j.cej.2020.127083
7	DING Xinxin， GUTIERREZ L， CROUE J P，et al. Hydroxyl and sulfate radical-based oxidation of RhB dye in UV/H₂O₂ and UV/persulfate systems：Kinetics，mechanisms，and comparison［J］. Chemosphere，2020，253：126655. doi:10.1016/j.chemosphere.2020.126655
8	李红州，沈国宸，耿金菊，等. 联合活化过硫酸盐及其去除污水中污染物研究进展［J］. 工业水处理，2021，41（6）：66-76. doi:10.11894/iwt.2021-0255
	LI Hongzhou， SHEN Guochen， GENG Jinju，et al. Joint activation of persulfate and its removal of pollutants in wastewater：Progresses and perspective［J］. Industrial Water Treatment，2021，41（6）：66-76. doi:10.11894/iwt.2021-0255
9	OH W D， DONG Zhili， LIM T T. Generation of sulfate radical through heterogeneous catalysis for organic contaminants removal：Current development，challenges and prospects［J］. Applied Catalysis B：Environmental，2016，194：169-201. doi:10.1016/j.apcatb.2016.04.003
10	ZHANG Botao， ZHANG Yang， TENG Yanguo，et al. Sulfate radical and its application in decontamination technologies［J］. Critical Reviews in Environmental Science and Technology，2015，45（16）：1756-1800. doi:10.1080/10643389.2014.970681
11	米记茹，田立平，刘丽丽，等. 过硫酸盐活化方法的研究进展［J］. 工业水处理，2020，40（7）：12-17.
	MI Jiru， TIAN Liping， LIU Lili，et al. Research progress on persulfate activation method［J］. Industrial Water Treatment，2020，40（7）：12-17.
12	WANG Songlin， XU Wenxin， WU Junfeng，et al. Improved sulfamethoxazole degradation by the addition of MoS₂ into the Fe²⁺/peroxymonosulfate process［J］. Separation and Purification Technology，2020，235：116170. doi:10.1016/j.seppur.2019.116170
13	RADJENOVIC J， SEDLAK D L. Challenges and opportunities for electrochemical processes as next-generation technologies for the treatment of contaminated water［J］. Environmental Science & Technology，2015，49（19）：11292-11302. doi:10.1021/acs.est.5b02414
14	PEREIRA L A， DE LIMA ALMEIDA D A， COUTO A B，et al. Titanium dioxide/oxidized carbon fiber electrodes electrochemically produced and their influences on Brilliant Green dye degradation［J］. Materials Research Bulletin，2020，122：110642. doi:10.1016/j.materresbull.2019.110642
15	XU Xiangrong， LI Xiangzhong. Degradation of azo dye Orange G in aqueous solutions by persulfate with ferrous ion［J］. Separation and Purification Technology，2010，72（1）：105-111. doi:10.1016/j.seppur.2010.01.012
16	SHI Xingdong， LI Yitao， ZHANG Zhi，et al. Enhancement of ciprofloxacin degradation in the Fe（Ⅱ）/peroxymonosulfate system by protocatechuic acid over a wide initial pH range［J］. Chemical Engineering Journal，2019，372：1113-1121. doi:10.1016/j.cej.2019.04.195
17	DO S H， JO J H， JO Y H，et al. Application of a peroxymonosulfate/cobalt〔PMS/Co（Ⅱ）〕 system to treat diesel-contaminated soil［J］. Chemosphere，2009，77（8）：1127-1131. doi:10.1016/j.chemosphere.2009.08.061
18	谢欣卓，钟金魁，李静，等. 四氧化三铁负载纳米零价铁类Fenton法降解水中磺胺甲唑［J］. 中国环境科学，DOI：10.19674/j.cnki.issn1000-6923.20220314.014 .
	XIE xinzhuo， ZHONG jinkui， LI Jing，et al. Degradation of sulfamethoxazole in water by Fenton-like process using ferriferrous oxide supported nanometer zero-valent iron［J］. China Environmental Science，DOI：10.19674/j.cnki.issn1000-6923.20220314.014 .
19	YU Yaqun， JI Yuefei， LU Junhe，et al. Degradation of sulfamethoxazole by Co₃O₄-palygorskite composites activated peroxymonosulfate oxidation［J］. Chemical Engineering Journal，2021，406：126759. doi:10.1016/j.cej.2020.126759
20	LUO Lianshun， WU Di， DAI Dejun，et al. Synergistic effects of persistent free radicals and visible radiation on peroxymonosulfate activation by ferric citrate for the decomposition of organic contaminants［J］. Applied Catalysis B：Environmental，2017，205：404-411. doi:10.1016/j.apcatb.2016.12.060

[1]	徐浩, 张凡, 于鑫, 陈红, 薛罡. 铁铜微电解-Fenton联合工艺去除磺胺甲唑和卡马西平[J]. 工业水处理, 2025, 45(3): 55-64.
[2]	傅翔宇, 李亚峰, 刘奕含, 崔可清, 王玲萍. 磷酸三丁酯改性生物炭活化PMS降解双酚A的效能[J]. 工业水处理, 2025, 45(1): 87-93.
[3]	倪宽, 山晓莉, 戚栋, 李强, 张文军. 商混站污水的双铝电极电絮凝研究[J]. 工业水处理, 2025, 45(1): 123-130.
[4]	张磊, 张进, 闫新龙. 多孔Ni/Co水滑石活化过硫酸盐降解磺胺甲唑研究[J]. 工业水处理, 2024, 44(8): 162-170.
[5]	赵杰, 吴俊峰, 窦艳艳, VIKTOROVICH Fedorov Svyatoslav, 王现丽, 刘彪, 朱新锋, 毛艳丽, 高宏斌. 单原子活化过硫酸盐降解有机污染物研究进展[J]. 工业水处理, 2024, 44(7): 38-46.
[6]	谢亮, 石姝彤, 郑帅, 吴隽玮, 孙鑫格, 张琦, 杨萍萍, 曾玉彬. 高温超稠油采出水的电絮凝实验及机理分析[J]. 工业水处理, 2024, 44(6): 101-110.
[7]	柴瑾, 白雪, 张祉瑶, 胡敏, 石娟, 金鹏康. 顺丁烯二酸活化过硫酸盐降解染料有机物研究[J]. 工业水处理, 2024, 44(6): 151-157.
[8]	苗艳晖, 王振磊, 张婷婷, 赵云良, 温通. 机械力活化方解石复合硫酸亚铁去除水中镉/砷复合污染研究[J]. 工业水处理, 2024, 44(5): 80-87.
[9]	刘楚楚, 金春姬, 孙楠, 高孟春. 阴极阳极协同电催化降解高硫酸盐废水中活性染料[J]. 工业水处理, 2024, 44(4): 127-137.
[10]	张静, 张彦平, 裴佳华, 贾小赛, 李一兵, 吕宁. 铁基污泥炭活化过硫酸盐调理剩余污泥脱水的效能和机理研究[J]. 工业水处理, 2024, 44(3): 142-151.
[11]	黄艳, 邢波, 晏伟, 杨郭, 范凤艳, 张华芳, 汤鲲彪. 钢渣/氮掺杂改性活性炭催化过硫酸盐降解罗丹明B[J]. 工业水处理, 2024, 44(2): 147-156.
[12]	辛浩洋, 李家俊. 磺胺甲唑对生物除磷性能的影响及机制[J]. 工业水处理, 2024, 44(2): 79-86.
[13]	高璐瑶, 刘邦海, 代鑫, 陈景光, 金春姬. 碱改性污泥生物炭活化过氧乙酸降解磺胺甲唑[J]. 工业水处理, 2024, 44(11): 132-141.
[14]	范秀磊, 王申鹏, 张舒, 纪伟, 崔月, 孔熙哲, 吕博文. 铜改性生物炭的制备及催化过硫酸盐去除水体中四环素的研究[J]. 工业水处理, 2024, 44(10): 133-142.
[15]	陈用泷, 方伟, 李思阳, 骆其金, 谢刚, 吴泽璇, 王艺霖, 黎京士. 响应面法优化零价铁活化过硫酸盐处理酱香型白酒废水[J]. 工业水处理, 2024, 44(1): 119-125.

选择文件类型/文献管理软件名称

选择包含的内容

电絮凝活化过单硫酸盐降解磺胺甲唑

Degradation of sulfamethoxazole by electroflocculation activated permonosulfate

RichHTML

PDF

可视化

被引次数

摘要/Abstract

引用本文

使用本文

图/表 10

参考文献 20

相关文章 15

编辑推荐

Metrics

本文评价

模态框（Modal）标题

选择文件类型/文献管理软件名称

选择包含的内容

电絮凝活化过单硫酸盐降解磺胺甲 唑

Degradation of sulfamethoxazole by electroflocculation activated permonosulfate

RichHTML

PDF

可视化

被引次数

摘要/Abstract

引用本文

使用本文

图/表 10

参考文献 20

相关文章 15

编辑推荐

Metrics

本文评价

电絮凝活化过单硫酸盐降解磺胺甲唑