CoFe2O4增强超声/H2O2降解环丙沙星

史京转, 魏红, 周孝德, 程小莉, 李克斌. CoFe2O4增强超声/H2O2降解环丙沙星[J]. 环境化学, 2018, 37(10): 2237-2246. doi: 10.7524/j.issn.0254-6108.2018030401
引用本文: 史京转, 魏红, 周孝德, 程小莉, 李克斌. CoFe2O4增强超声/H2O2降解环丙沙星[J]. 环境化学, 2018, 37(10): 2237-2246. doi: 10.7524/j.issn.0254-6108.2018030401
SHI Jingzhuan, WEI Hong, ZHOU Xiaode, CHENG Xiaoli, LI Kebin. Enhanced ultrasonic/H2O2 degradation of ciprofloxacin using CoFe2O4[J]. Environmental Chemistry, 2018, 37(10): 2237-2246. doi: 10.7524/j.issn.0254-6108.2018030401
Citation: SHI Jingzhuan, WEI Hong, ZHOU Xiaode, CHENG Xiaoli, LI Kebin. Enhanced ultrasonic/H2O2 degradation of ciprofloxacin using CoFe2O4[J]. Environmental Chemistry, 2018, 37(10): 2237-2246. doi: 10.7524/j.issn.0254-6108.2018030401

CoFe2O4增强超声/H2O2降解环丙沙星

  • 基金项目:

    陕西省自然科学基金(2017JM5082),陕西省水利科技项目(2013slkj-07)和环境工程国家重点学科培育学科项目(106-5X1204)资助.

Enhanced ultrasonic/H2O2 degradation of ciprofloxacin using CoFe2O4

  • Fund Project: Supported by the Province Natural Science Foundation of Shaanxi(2017JM5082), the Province Water Conservancy Science and Technology of Shaanxi(2013slkj-07) and the National Key Subject Cultivation Subject Project of Environmental Engineering (106-5X1204).
  • 摘要: 实验合成磁性CoFe2O4,采用X射线衍射仪(XRD)、扫描电镜(SEM)和X射线能谱仪(EDS)对其进行表征,研究其催化超声/H2O2(US/H2O2)降解环丙沙星的效果和机理.实验考察了CoFe2O4和H2O2添加浓度、初始pH值、不同形态氮、氯离子等因素对环丙沙星降解效果的影响.并以大肠杆菌为指示菌种,分析了CoFe2O4催化US/H2O2降解环丙沙星过程中抑菌性的变化.结果表明,CoFe2O4能够有效增强US/H2O2降解环丙沙星,CoFe2O4和H2O2浓度分别为0.04 g·L-1和1.0 mmol·L-1、pH=3.0、反应60 min环丙沙星的降解率达到85.26%;与NH4+相比,NO3-促进环丙沙星的降解,NO2-和Cl-不同程度抑制环丙沙星的降解.自由基抑制结果表明,CoFe2O4增强US/H2O2降解环丙沙星主要在于·OH的生成.CoFe2O4稳定性结果表明,5次反复实验后,环丙沙星60 min的降解率仅降低了4%左右,催化剂的重复利用性较高.琼脂扩散实验表明,CoFe2O4在催化US/H2O2降解环丙沙星的同时,CoFe2O4/US/H2O2体系能够完全去除其对大肠杆菌的抑菌性.
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  • [1] TONG L, LI P, WANG Y X, et al. Analysis of veterinary antibiotic residues in swine wastewater and environmental water samples using optimized SPE-LC/MS/MS[J]. Chemosphere, 2009, 74(8):1090-1097.
    [2] NAKATA H, KANNAN K, JONES P D, et al. Determination of fluoroquinolone antibiotics in wastewater effluents by liquid chromatography -mass spectrometry and fluorescence detection[J]. Chemosphere, 2005, 58(6):759-766.
    [3] PENG X Z, TAN J H, TANG C M, et al. Multiresidue determination of fluoroquinolone, sulfonamide, trimethoprim, and chloramphenicol antibiotics in urban waters in China[J]. Environmental Toxicology and Chemistry, 2008, 27(1):73-79.
    [4] STURINI M, SPELTINI A, PRETALI L, et al. Solid-phase extraction and HPLC determination of fluoroquinolones in surface waters[J]. Journal of Separation Science, 2009, 32(17):3020-3028.
    [5] SARA R M, SARA C, ELISABET M, et al. Occurrence of antibiotics and antibiotic resistance genes in hospital and urban wastewaters and their impact on the receiving river[J]. Water Research, 2015, 69:234-242.
    [6] 孙晓君, 冯玉杰, 蔡伟民,等. 废水中难降解有机物的高级氧化技术[J]. 化工环保, 2001, 21(5):264-269.

    SUN X J, FENG Y J, CAI W M, et al. Advanced oxidation processes for refractory organic pollutants in wastewater[J]. Environmental Protection of Chemical Industry, 2001, 21(5):264-269(in Chinese).

    [7] 宋孟珂. 高级氧化技术处理废水中药品与个人护理用品的研究[D].新乡:河南师范大学硕士论文,2011. SONG M K. Research on the degradation of PPCPs in water by advanced oxidation technologies(AOTs)[D]. Xinxiang:Master's thesis of Henan Normal University, 2011(in Chinese).
    [8] 吕春玲, 王莹, 刘强,等. UV/Fenton混凝法对浮选废水预处理研究[J]. 黄金, 2015, 36(4):75-77.

    LV C L, WANG Y, LIU Q, et al. Experimental study on the pre-treatment of flotation wastewater by UV/Fenton oxidation-coagulation process[J]. Gold, 2015, 36(4):75-77(in Chinese).

    [9] RAHMANI H, GHOLAMI H, MAHVI A.H, et al. Tinidazole removal from aqueous solution by sonolysis in the presence of hydrogen peroxide[J]. Bulletin of Environmental Contamination and Toxicology, 2014, 92(3):341-346.
    [10] WANG X K, WANG Y N, LI D J,et al. Degradation of tetracycline in water by ultrasonic irradiation[J]. Water Sciense &Technology, 2013, 67(4):715-721.
    [11] WEI H, HU D, SU J, et al. Intensification of Fe3O4 magnetic nanoparticles on levofloxacin sono-degradation under a US/H2O2 system[J]. Chinese Journal of Chemical Engineering, 2015, 23:296-302.
    [12] 张中杰, 王旭, 邱士鑫,等.磁性埃洛石对水溶液中盐酸土霉素的吸附[J]. 环境工程学报, 2013, 7(10):3921-3926.

    ZhANG Z J,WANG X,QIU S X,et al. Adsorption of oxytetracycline hydrochloride in aqueous solutions by magnetic halloysite composites[J]. Chinese Journal of Environmental Engineering, 2013, 7(10):3921-3926(in Chinese).

    [13] 伊玉. 可回收磁性材料CoFe2O4/GO催化PMS降解染料废水的性能研究[D].上海:东华大学硕士学位论文, 2014. YI Y. The Research on the degradation of dye wastewater using PMS activated by CoFe2O4 immobilized on GO[D]. Shanghai:Donghua University Master's Dissertation, 2014

    (in Chinese).

    [14] GUO X J, LI H R, ZHAO S G, et al. Fast degradation of acid orange Ⅱ by bicarbonate-activated hydrogen peroxide with a magnetic S-modified CoFe2O4 catalyst[J]. Journal of the Taiwan Institute of Chemical Engineers, 2015, 55:90-100.
    [15] 马楠, 刘华波, 谢鑫源,等. 天然矿物负载Fe/Co催化H2O2氧化降解阳离子红3R[J]. 环境科学, 2015, 36(2):576-583.

    MA N, LIU H B, XIE X Y, et al. Oxidation of cationic red 3R in water with H2O2 catalyzed by mineral loaded with Fe/Co[J]. Environmental Science, 2015, 36(2):576-583(in Chinese).

    [16] 魏红, 杨虹, 赵琳,等. 粉煤灰增强超声/H2O2降解左氧氟沙星的实验研究[J]. 中国环境科学, 2014, 34(4):889-895.

    WEI H, YANG H, ZHAO L, et al. Enhancement of levofloxacin degradation in US/H2O2 system by addition of fly ash[J]. China Environmental Science, 2014, 34(4):889-895(in Chinese).

    [17] BEGG J D, ZAVARIN M, KERSTING A B, et al. Plutonium desorption from mineral surfaces at environmental concentrations of hydrogen peroxide[J]. Environmental Science& Technology, 2014, 48(11):6201-6210.
    [18] SPANNRING P, PRAT I, COSTAS M,et al. Fe(6-Me-PyTACN)-catalyzed, one-pot oxidative cleavage of methyl oleate and oleic acid into carboxylic acids with H2O2 and NaIO4[J]. Catalysis Science&Technology, 2014, 4(3):708-716.
    [19] LU X F, YANG L, BIAN X J, et al. Rapid, microwave-assisted, and one-pot synthesis of magnetic palladium-CoFe2O4-graphene composite nanosheets and their applications as recyclable catalysts[J]. Particle & Particle Systems Characterization, 2014, 31(2):245-251.
    [20]
    [21] ANDERSSON A. S, THOMAS J. O, et al. The source of first-cycle capacity loss in LiFePO4[J]. Journal of Power Sources, 2001, 97/98(1/2):498-502.
    [22] 王彦斌, 赵红颖, 赵国华,等. 基于铁化合物的异相Fenton催化氧化技术[J]. 化学进展, 2013, 25(8):1246-1259.

    WANG Y B, ZHAO H Y, ZHAO G H, et al. Iron compounded -based heterogeneous Fenton catalytic oxidation technology[J]. Progress in Chemistry, 2013, 25(8):1246-1259(in Chinese).

    [23] 陆天宇, 周培国, 张楠,等. 以凹凸棒土为载体的非均相Fenton催化剂处理苯酚废水研究[J]. 环境污染与防治, 2018, 40(2):155-160.

    LU T Y, ZHOU P G, ZHANG N, et al. Research on treatment of phenol wastewater by attapulgite heterogeneous Fenton catalysts[J].Environmental Pollution & Control, 2018, 40(2):155-160(in Chinese).

    [24] 吴大清, 刁桂仪,等. 含铁矿物的表面催化氧化作用及其环境意义[J]. 矿物岩石, 2003, 23(4):11-14.

    WU D Q, DIAO G Y, et al. The surface catalyzed oxidation of iron-bearing minerals and their environmental significations[J]. J Mineralogy Petrology, 2003, 23(4):11-14(in Chinese).

    [25] 孔青青, 张祥丹, 李富华,等. 不同形态氮对水环境中氯贝酸光降解的影响[J]. 中国环境科学, 2017, 37(2):584-591.

    KONG Q Q,ZHANG X D,LI F H, et al. Effect of different forms of nitrogen on the photodegradation of clofibric acid in water environment[J]. China Environmental Science, 2017, 37(2):584-591(in Chinese).

    [26] 何占伟, 刘国光, 刘海津,等. 水体中不同形态氮对环丙沙星溶液光降解影响[J]. 环境科学学报, 2011, 31(11):2409-2415.

    HE Z W, LIU G G, LIU H J, et al. The effect of different nitrogen forms on the photo-degradation of ciprofloxacin in water[J]. Acta Scientiae Circumstantiae, 2011, 31(11):2409-2415.(in Chinese).

    [27] ZHANG X X, LI R P, JIA M K, et al. Degradation of ciprofloxacin in aqueous bismuth oxybromide(BIOBr) suspensions under visible light irradiation:a direct hole oxidation pathway[J].Chemical Engineering Journal, 2015, 274:290-297.
    [28] 孙猛, 李娟, 徐勤勤,等. 超声波对垃圾渗滤液COD和氨氮去除的研究[J]. 中国农学通报, 2010, 26(18):347-352.

    SUN M, LI J, XU Q Q, et al. The research of removing COD and NH3-N in landfill leachate by using ultrasonic[J]. Chinese Agricultural Science Bulletin, 2010,26(18):347-352(in Chinese).

    [29] 尚会建, 周艳丽, 赵彦,等. 活性炭催化臭氧氧化处理低浓度氨氮废水[J]. 化工环保, 2012, 32(5):405-408.

    SHANG H J,ZHOU Y L,ZHAO Y, et al.Treatment of low-concentration ammonia nitrogen wastewater by catalytic ozonation process with activated carbon[J].Environmental Protection of Chemical Industry, 2012,32(5):405-408(in Chinese).

    [30] 彭人勇, 陈康康, 李艳琳,等. 超声吹脱处理印染废水中氨氮的研究[J]. 环境科学与技术, 2010, 33(10):166-168

    ,204. PENG R Y, CHEN K K, LI Y L, et al. Removal of ammonia nitrogen in dyeing wastewater by ultrasonic stripping[J]. Environmental Science & Technology, 2010,33(10):166-168,204(in Chinese).

    [31] 伊玉, 李洁冰, 王倩,等. 无机盐离子对CoFe2O4/GO催化PMS氧化降解酸性橙Ⅱ的影响[J]. 广东化工, 2014, 41(13):10-11.

    YI Y, LI J B, WANG Q, et al. The effects of inorganic ions on the CoFe2O4/GO catalytic oxidation orange Ⅱ by PMS[J]. Guangdong Chemical Industry, 2014,41(13):10-11(in Chinese).

    [32] 朱锡忠, 王泉源, 胡建强,等. 微波协同CuFeO2类Fenton反应降解橙黄G的研究[J]. 广州化工, 2017, 45(11):110-113

    ,138. ZHU X Z, WANG Q Y, HU J Q, et al. Degradation of orange G by microwave coupled with Fenton-like reaction using CuFeO2 as catalysis[J]. Guangzhou Chemical Industry,2017,45(11):110-113,138(in Chinese).

    [33] 赵莹, 任月明, 张慧玉,等. Go/CoFe2O4催化过硫酸盐降解邻苯二甲酸二丁酯效能[J]. 哈尔滨工业大学学报, 2017, 49(8):31-36.

    ZHAO Y, REN Y M, ZHANG H Y, et al. Efficiency of dibutyl phthalate degradation by Go/CoFe2O4 catalytic oxidation of peroxymonosulfate[J]. Journal of Harbin Institute of Technology, 2017,49(8):31-36(in Chinese).

    [34] SHEN L L, MITSCHER L A, SHARMA P N, et al. Mechanism of inhibition of DNA gyrase by quinolone antibacterials:A cooperative drug-DNA binding model[J]. Biochemistry, 1989, 28(9):3886-3894.
    [35] 魏红, 杨虹, 李克斌,等. CCl4增强超声降解环丙沙星的效果及路径解析[J]. 高校化学工程学报, 2015, 29(3):703-708.

    WEI H, YANG H, LI K B, et al. The enhanced effect of ciprofloxacin sonochemical degradation by adding CCl4 and its degradation pathways[J]. Journal of Chemical Engineering of Chinese Universities, 2015, 29(3):703-708(in Chinese).

    [36] TIAS P, MICHAEL C. D, TIMOTHY J. S, et al. Photolytic and photocatalytic decomposition of aqueous ciprofloxacin:Transformation products and residual antibacterial activity[J]. Water Research, 2010, 44(10):3121-3132.
    [37] 魏红, 史京转, 杨虹,等. CCl4强化超声降解诺氟沙星的效果和抗菌性分析[J]. 环境化学, 2015, 34(5):884-890.

    WEI H,SHI J Z, YANG H, et al. Degradation and antibacterial activity analysis of norfloxacin under CCl4-enhanced ultrasound irradiation process[J]. Environmental Chemistry,2015,34(5):884-890(in Chinese).

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  • 收稿日期:  2018-03-04
  • 刊出日期:  2018-10-15
史京转, 魏红, 周孝德, 程小莉, 李克斌. CoFe2O4增强超声/H2O2降解环丙沙星[J]. 环境化学, 2018, 37(10): 2237-2246. doi: 10.7524/j.issn.0254-6108.2018030401
引用本文: 史京转, 魏红, 周孝德, 程小莉, 李克斌. CoFe2O4增强超声/H2O2降解环丙沙星[J]. 环境化学, 2018, 37(10): 2237-2246. doi: 10.7524/j.issn.0254-6108.2018030401
SHI Jingzhuan, WEI Hong, ZHOU Xiaode, CHENG Xiaoli, LI Kebin. Enhanced ultrasonic/H2O2 degradation of ciprofloxacin using CoFe2O4[J]. Environmental Chemistry, 2018, 37(10): 2237-2246. doi: 10.7524/j.issn.0254-6108.2018030401
Citation: SHI Jingzhuan, WEI Hong, ZHOU Xiaode, CHENG Xiaoli, LI Kebin. Enhanced ultrasonic/H2O2 degradation of ciprofloxacin using CoFe2O4[J]. Environmental Chemistry, 2018, 37(10): 2237-2246. doi: 10.7524/j.issn.0254-6108.2018030401

CoFe2O4增强超声/H2O2降解环丙沙星

  • 1.  西安理工大学, 省部共建西北旱区生态水利国家重点实验室, 西安, 710048;
  • 2.  西北大学化学与材料科学学院, 合成与天然功能分子化学教育部重点实验室, 西安, 710069;
  • 3.  渭南市环境科学研究所, 渭南, 714000
基金项目:

陕西省自然科学基金(2017JM5082),陕西省水利科技项目(2013slkj-07)和环境工程国家重点学科培育学科项目(106-5X1204)资助.

摘要: 实验合成磁性CoFe2O4,采用X射线衍射仪(XRD)、扫描电镜(SEM)和X射线能谱仪(EDS)对其进行表征,研究其催化超声/H2O2(US/H2O2)降解环丙沙星的效果和机理.实验考察了CoFe2O4和H2O2添加浓度、初始pH值、不同形态氮、氯离子等因素对环丙沙星降解效果的影响.并以大肠杆菌为指示菌种,分析了CoFe2O4催化US/H2O2降解环丙沙星过程中抑菌性的变化.结果表明,CoFe2O4能够有效增强US/H2O2降解环丙沙星,CoFe2O4和H2O2浓度分别为0.04 g·L-1和1.0 mmol·L-1、pH=3.0、反应60 min环丙沙星的降解率达到85.26%;与NH4+相比,NO3-促进环丙沙星的降解,NO2-和Cl-不同程度抑制环丙沙星的降解.自由基抑制结果表明,CoFe2O4增强US/H2O2降解环丙沙星主要在于·OH的生成.CoFe2O4稳定性结果表明,5次反复实验后,环丙沙星60 min的降解率仅降低了4%左右,催化剂的重复利用性较高.琼脂扩散实验表明,CoFe2O4在催化US/H2O2降解环丙沙星的同时,CoFe2O4/US/H2O2体系能够完全去除其对大肠杆菌的抑菌性.

English Abstract

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