Fe<sub>3</sub>O<sub>4</sub>活化过硫酸盐体系同步去除诺氟沙星和铅

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摘要采用Fe₃O₄活化过硫酸盐（PS）同步去除水中的NOR （诺氟沙星）和Pb （II）.探讨了Fe₃O₄投加量、PS浓度、初始pH值和Pb （II）浓度对NOR降解的影响.结果表明，NOR的降解符合伪一级反应动力学，在温度为30℃、NOR初始浓度为5.0mg/L、Pb （II）浓度为1.0mg/L、Fe₃O₄投加量为2.0g/L、PS浓度为1.5mmol/L、初始pH值为7.0的条件下，反应120min后，NOR降解率达90.2%，Pb （II）去除率为99.5%.自由基淬灭实验证实，硫酸根自由基（SO₄^-·）是NOR降解的主要自由基.通过LC-MS分析结果推测了NOR可能的降解路径和中间产物.Fe₃O₄活化PS高级氧化工艺可作为一种同步去除有机污染物和重金属的工艺.

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	苏冰琴
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	权晓慧
	李瑞
	芮创学

关键词 ：诺氟沙星, 铅, Fe₃O₄磁性纳米颗粒, 过硫酸盐, 同步去除

Abstract：This study employed the advanced oxidation process of persulfate, activated with Fe₃O₄ magnetic nanoparticles (Fe₃O₄/PS), for simultaneous removal of NOR (norfloxacin) and Pb(II) in wastewater. The effects of Fe₃O₄ dosage, PS concentration, initial pH value and Pb(II) concentration on the degradation of NOR were investigated. Experimental results indicated that the degradation of NOR followed the pseudo-first-order kinetics. The degradation of NOR and the removal of Pb(II) reached to 90.2% and 99.5%, respectively, under the reaction conditions of temperature of 30℃, initial NOR concentration of 5.0mg/L, Fe₃O₄ dosage of 2.0g/L, PS concentration of 1.5mmol/L, initial pH value of 7.0, and reaction time of 120minutes. Free radical quenching experiments confirmed that SO₄^-· was the dominant free radical in the degradation of NOR. The possible degradation pathways and intermediate products of NOR were inferred using LC-MS. This study indicated that the Fe₃O₄-activated PS oxidation process could be served as a novel technique for the simultaneous removal of organic pollutants and heavy metals.

Key words： NOR(norfloxacin) Pb(II) Fe₃O₄ magnetic nanoparticles persulfate simultaneous removal

收稿日期: 2021-07-09

PACS:

X703.1

基金资助:国家自然科学基金资助项目（22008167）；山西省自然科学基金资助项目（201801D121274）；国家大学生创新创业项目（202010112010）

通讯作者: 苏冰琴,副教授,subingqin@tyut.edu.cn E-mail: subingqin@tyut.edu.cn

作者简介: 苏冰琴(1972-),女,山西忻州人,副教授,博士,主要从事水污染控制理论与技术的研究.发表论文20余篇.

引用本文:

苏冰琴, 刘一清, 林昱廷, 王健, 权晓慧, 李瑞, 芮创学. Fe₃O₄活化过硫酸盐体系同步去除诺氟沙星和铅[J]. 中国环境科学, 2022, 42(2): 717-727. SU Bing-qin, LIU Yi-qing, LIN Yu-ting, WANG Jian, QUAN Xiao-hui, LI Rui, RUI Chuang-xue. Simultaneous removal of norfloxacin and Pb(II) via Fe₃O₄-activated persulfate oxidation. CHINA ENVIRONMENTAL SCIENCECE, 2022, 42(2): 717-727.

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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2022/V42/I2/717

[1]	Yang Z, Jia S Y, Zhang T T, et al. How heavy metals impact on ﬂocculation of combined pollution of heavy metals-antibiotics:A comparative study[J]. Separation & Purification Technology, 2015, 149:398-406.
[2]	Wu D, Pan B, Wu M, et al. Coadsorption of Cu and sulfamethoxazole on hydroxylized and graphitized carbon nanotubes[J]. Science of The Total Environment, 2012,427:247-252.
[3]	张建强,黄雯,陈佼,等.羊粪生物炭对水体中诺氟沙星的吸附特性[J]. 环境科学学报, 2017,37(9):3398-3408. Zhang J Q, Huang W, Chen J, et al. Adsorption characteristics of norfloxacin in aqueous solution by sheep manure biochar[J]. Acta Scientiae Circumstantiae, 2017,37(9):3398-3408.
[4]	王盈霏,王枫亮,黎杰华,等.介孔氮化碳光催化降解诺氟沙星的动力学机制[J]. 中国环境科学, 2018,38(4):1346-1355. Wang Y F, Wang F L, Li J H, et al. Photocatalytic degradation kinetics and mechanism of norfloxacin using mesoporous g-C3N4 under visible-light irradiation[J]. China Environmental Science, 2018,38(4):1346-1355.
[5]	魏红,史京转,李佳霖,等.超声、过硫酸钾协同去除水中诺氟沙星的效果[J]. 环境科学, 2015,36(11):4121-4126. Wei H, Shi J Z, Li J L, et al. Norfloxacin solution degradation under ultrasound' potassium persulfate collaborative system[J]. Environmental Science, 2015,36(11):4121-4126.
[6]	Brown E E, Gerrentsen P, Pollock B, et al. Psychiatric benefits of lithium in water supplies may be due to protection from the neurotoxicity of lead exposure[J]. Medical Hypotheses, 2018,115:94-102.
[7]	李佳凡,姚竞芳,顾佳媛,等.黄浦江铅的人体健康水质基准研究[J]. 环境科学学报, 2018,38(12):4840-4847. Li J F, Yao J F, Gu J Y, et al. Human health-based water quality criteria of lead in Huangpu River[J]. Acta Scientiae Circumstantiate, 2018,38(12):4840-4847.
[8]	Tan F, Sun D, Gao J, et al. Preparation of molecularly imprinted polymer nanoparticles for selective removal of fluoroquinolone antibiotics in aqueous solution[J]. Journal of Hazardous Materials, 2013,(244):750-757.
[9]	Yang X, Flowers R C, Weinberg H S, et al. Occurrence and removal of pharmaceuticals and personal care products (PPCPs) in an advanced wastewater reclamation plant[J]. Water Research, 2011,45(16):5218-5228.
[10]	Rakhshandehroo G R, Salari M, Nikoo M R. Optimization of degradation of ciprofloxacin antibiotic and assessment of degradation products using full factorial experimental design by Fenton Homogenous process[J]. Global Nest Journal, 2018,20(2):324-332.
[11]	Paul T, Miller P L, Strathmann T J. Visible-light-mediated TiO2 photocatalysis of fluoroquinolone antibacterial agents[J]. Environmental Science & Technology, 2007,41(13):4720-4727.
[12]	汪婷,高滢,金晓英,等.纳米四氧化三铁同步去除水中的Pb(II)和Cr(III)离子[J]. 环境工程学报, 2013,7(9):3476-3482. Wang T, Gao Y, Jin X Y, et al. Simultaneous removal of Pb(II) and Cr(III) from wastewater by magnetite nanoparticles[J]. Chinese Journal of Environmental Engineering, 2013,7(9):3476-3482.
[13]	周爱娟,赵玉珏,刘芝宏,等.Fe(II)活化过硫酸盐处理喹啉工艺参数优化及生物毒性[J]. 中国环境科学, 2020,40(11):4795-4803. Zhou A J, Zhao Y J, Liu Z H, et al. Accelerated quinoline removal by Fe(II) -activated persulfate:parameters optimization and biological detoxification analysis[J]. China Environmental Science, 2020,40(11):4795-4803.
[14]	张饮江,相元泉,鲁仙,等.零价铁激活过硫酸盐降解水中铬黑T特性[J]. 中国环境科学, 2020,40(2):191-198. Zhang Y J, Xiang Y Q, Lu Xian, et al. Characteristics on the Eriochrome black T(EBT) degradation in aquatics by Fe/persulfate system[J]. China Environmental Science, 2020,40(2):191-198.
[15]	刘美琴,宋秀兰.Fe2+激活过硫酸盐耦合活性炭深度处理焦化废水[J]. 中国环境科学, 2018,38(4):1377-1384. Liu M Q, Song X L. Fe2+activated persulfate coupled with activated carbon for advanced treatment of coking wastewater[J]. China Environment Science, 2018,38(4):1377-1384.
[16]	佘月城,董正玉,吴丽颖,等.MnFe2O4活化过一硫酸盐降解废水中LAS[J]. 中国环境科学, 2019,39(8):3323-3331. She Y C, Dong Z Y, Wu L Y, et al. Degradation of LAS in wastewater by peroxymonosulfate activated by MnFe2O4[J]. China Environmental Science, 2019,39(8):3323-3331.
[17]	Potakis N, Frontistis Z, Antonopoulou M, et al. Oxidation of bisphenol A in water by heat-activated persulfate[J]. Journal of Environmental Management, 2016,195(2):125-132.
[18]	Xu L Y, Zhou X, Wang G L. Catalytic degradation of acid red B in the system of ultrasound/peroxymonosulfate/Fe3O4[J]. Separation and Purification Technology, 2021,276:119417.
[19]	Lu X, Shao Y, Gao N, et al. Degradation of diclofenac by UV-activated persulfate process:Kinetic studies, degradation pathways and toxicity assessments[J]. Ecotoxicology and Environmental Safety, 2017,141:139-147.
[20]	Dominguez C M, Rodriguez V, Montero E, et al. Abatement of dichloromethane using persulfate activated by alkali:A kinetic study[J]. Separation and Purification Technology, 2020,241:11667.
[21]	黄智辉,纪志永,陈希,等.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(5):402-411. Huang Z H, Ji Z Y, Chen X, et al. Degradation of organic pollutants in water by persulfate advanced oxidation[J]. Chemical Industry and Engineering Progress, 2019,38(5):402-411.
[22]	Mona Kohantorabi, Gholamreza Moussavi, Paula Oulego, et al. Radical-based degradation of sulfamethoxazole via UVA/PMS -assisted photocatalysis, driven by magnetically separable Fe3O4@CeO2@BiOI nanospheres[J]. Separation and Purification Technology, 2021,267:118665.
[23]	苏冰琴,林昱廷,宋秀兰,等.磁性纳米Fe3O4活化过一硫酸盐降解三氯生性能[J]. 中国给水排水, 2021,37(15):89-94,101. Su B Q, Lin Y T, Song X L, et al. Degradation of triclosan in water by magnetic nanoscale Fe3O4 activated peroxymonosulfate[J]. China Water & Wastewater, 2021,37(15):89-94,101.
[24]	张丽娜,钟华,张俊涛,等.热,碱和Fe3O4激活过硫酸钠降解二恶烷的对比研究[J]. 中国环境科学, 2017,37(10):3741-3747. Zhang L N, Zhong H, Zhang J T, et al. A comparative study on activation of persulfate by heat, base and Fe3O4 for degradation of 1,4-dioxane[J]. China Environmental Science, 2017,37(10):3741-3747.
[25]	刘一清,苏冰琴,陶艳,等.磁性纳米Fe3O4活化过硫酸盐降解水中磺胺甲恶唑[J]. 环境工程学报, 2020,14(9):2515-2526. Liu Y Q, Su B Q, Tao Y, et al. Degradation of sulfamethoxazole in water by magnetic nano-Fe3O4 activated persulfate[J]. Chinese Journal of Environmental Engineering, 2020,14(9):2515-2526.
[26]	Liu D, Zhang L, Li M K, et al. Magnetic Fe3O4-PS-polyacetylene composite microspheres showing chirality derived from helical substituted polyacetylene[J]. Micromole Rapid Common, 2012,33(8):672-677.
[27]	Kelly Peeters, Gaetane Lespes, Tea Zulian, et al. The fate of iron nanoparticles in environmental waters treated with nanoscale zero-valent iron, FeONPs and Fe3O4NPs[J]. Water Research, 2016,94:315-327.
[28]	Niu H, Di Z, Zhang S, et al. Humic acid coated Fe3O4 magnetic nanoparticles as highly efficient Fenton-like catalyst for complete mineralization of sulfathiazole[J]. Journal of Hazard Materials, 2011, 190:559-565.
[29]	Sun S P, Lemley A T. p-Nitrophenol degradation by a heterogeneous Fenton-like reaction on nano-magnetite:Process optimization, kinetics, and degradation pathways[J]. Journal of Molecular Catalysis A, 2011,349:71-79.
[30]	SadaVenkateswarlu, Bhajanthri NateshKumar, BobbalaPrathima, et al. A novel green synthesis of Fe3O4 magnetic nanorods using Punica Granatum rind extract and its application for removal of Pb(II) from aqueous environment[J]. Arabian Journal of Chemistry, 2019,12(4):588-596.
[31]	Guo S Z, Duan N, Dan Z G, et al. g-C3N4 modified magnetic Fe3O4 adsorbent:Preparation, characterization, and performance of Zn(II), Pb(II) and Cd(II) removal from aqueous solution[J]. Journal of Molecular Liquids, 2018,258(15):225-234.
[32]	Tang X, Hashmi M Z, Zeng B, et al. Application of iron-activated persulfate oxidation for the degradation of PCBs in soil[J]. Chemical Engineering Journal, 2015,279:673-680.
[33]	Moussav G, Momeninejad H, Shekoohiyan S, et al. Oxidation of acetaminophen in the contaminated water using UVC/S2O82- process in a cylindrical photoreactor:Efficiency and kinetics of degradation and mineralization[J]. Separation & Purification Technology, 2017, 181:132-138.
[34]	刘洪位,郭洪光,付垚,等.硫酸根自由基降解诺氟沙星动力学因子优化分析[J]. 水处理技术, 2016,42(3):27-31,42. Liu H W, Guo H G, Fu Y, et al. Optimal analysis for kinetics factors on the degradation of norfloxacin using sulfate radical[J]. Technology of Water Treatment, 2016,42(3):27-31,42.
[35]	Gong H, Chu W. Photodegradation of sulfamethoxazole with a recyclable catalyst[J]. Industrial & Engineering Chemistry Research, 2015,54(51):12763-12769.
[36]	Wang S, Wang J. Radiation-induced degradation of sulfamethoxazole in the presence of various inorganic anions[J]. Chemical Engineering Journal, 2018,351:688-696.
[37]	张君.活性炭纤维催化过一硫酸氢盐降解水中的酸性橙7[D]. 青岛:中国海洋大学, 2014. Zhang J. Activated carbon fiber catalyzed peroxymonosulfate oxidation of acid orange 7 in aqueous solution[D]. Qingdao:China Ocean University, 2014.
[38]	Tan C Q, Gao N Y, Deng Y, et al. Radical induced degradation of acetaminophen with Fe3O4 magnetic nanoparticles as heterogeneous activator of peroxymonosulfate[J]. Journal of Hazardous Materials, 2014,276:452-460.
[39]	Dong H R, Deng J M, Xie Y K, et al. Stabilization of nanoscale zero-valent iron (nZVI) with modified biochar for Cr(VI) removal from aqueous solution[J]. Journal of Hazardous Materials, 2017,332:79-86.