不同形态洛美沙星在高岭土上的吸附特性
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摘要
本研究采用批实验方法探究了不同形态洛美沙星(LOM)在高岭土上的吸附特性。LOM吸附动力学结果符合准二级反应动力学方程,吸附等温数据可用Langmuir方程很好地拟合。随着溶液pH值增大,洛美沙星吸附量先增大后减小,且pH值在洛美沙星pK_(a1)与pK_(a2)间吸附量达到最大。不同形态LOM在高岭土上的吸附量排序为LOM~±>LOM~+>LOM~-。溶液离子强度和无机阳离子种类对LOM~+在高岭土上的吸附影响十分微弱,但均明显抑制了LOM~±的吸附,且离子强度越大,抑制作用越明显。不同无机阳离子抑制程度排序为Mg~(2+)>Ca~(2+)>K~+>Na~+。LOM~+在高岭土上的吸附机理主要是内层络合和阳离子交换;LOM~±在高岭土上的吸附机理主要是阳离子交换、氢键作用和静电引力作用;LOM~-与高岭土表面存在较大静电斥力,导致吸附量很小,可能是外层表面络合引起少量的吸附。
We carried out batch experiments to investigate the sorption characteristics of different forms of lomefloxacin(LOM)on kaolinite.Sorption kinetics were pseudo-second-order,and all equilibrium data could be well described by the Langmuir equation.As solution pH increased,the amount of LOM sorption increased first and then decreased.Maximum sorption was achieved at pH values between pK_(a1)and pK_(a2)of LOM.The sorption capacity of different forms of LOM on kaolinite ranked as LOM~±>LOM~+>LOM~-.The ionic strength of LOM solution and inorganic cations had little effect on LOM~+sorption,but both factors significantly inhibited LOM~±sorption.The sorption capacity of LOM~±decreased with increasing ionic strength,and the inhibition potency of different inorganic cations was in the order of Mg~(2+)>Ca~(2+)>K~+>Na~+.The sorption mechanisms were mainly inner-sphere complexation and cation exchange for LOM~+or cation exchange,hydrogen bonding and electrostatic attraction for LOM~±on kaolinite.LOM~-sorption on kaolinite is very small due to strong repulsive electrostatic effect;the small sorption may resulted from outer-sphere surface complexation.
We carried out batch experiments to investigate the sorption characteristics of different forms of lomefloxacin(LOM)on kaolinite.Sorption kinetics were pseudo-second-order,and all equilibrium data could be well described by the Langmuir equation.As solution pH increased,the amount of LOM sorption increased first and then decreased.Maximum sorption was achieved at pH values between pK_(a1)and pK_(a2)of LOM.The sorption capacity of different forms of LOM on kaolinite ranked as LOM~±>LOM~+>LOM~-.The ionic strength of LOM solution and inorganic cations had little effect on LOM~+sorption,but both factors significantly inhibited LOM~±sorption.The sorption capacity of LOM~±decreased with increasing ionic strength,and the inhibition potency of different inorganic cations was in the order of Mg~(2+)>Ca~(2+)>K~+>Na~+.The sorption mechanisms were mainly inner-sphere complexation and cation exchange for LOM~+or cation exchange,hydrogen bonding and electrostatic attraction for LOM~±on kaolinite.LOM~-sorption on kaolinite is very small due to strong repulsive electrostatic effect;the small sorption may resulted from outer-sphere surface complexation.
引文
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[15] LI Z H,HONG H L,LIAO L B,et al.A mechanistic study of ciprofloxacin removal by kaolinite[J].Colloids and Surfaces B:Biointerfaces,2011,88(1):339-344.
[16] WANG P,ZHANG D,ZHANG H,et al.Impact of concentration and species of sulfamethoxazole and ofloxacin on their adsorption kinetics on sediments[J].Chemosphere,2017,175:123-129.
[17] LI Z H,SCHULZ L,ACKLEY C,et al.Adsorption of tetracycline on kaolinite with pH-dependent surface charges[J].Journal of Colloid and Interface Science,2010,351(1):254-260.
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[20] QIN X P,LIU F,WANG G C,et al.Modeling of levofloxacin adsorption to goethite and the competition with phosphate[J].Chemosphere,2014,111:283-290.
[21] CHASSA A W,OHNO T,HIGGINS S R,et al.Chemical force spectroscopy evidence supporting the layer-by-layer model of organic matter binding to iron(oxy)hydroxide mineral surfaces[J].Environmental Science and Technology,2015,49(16):9733-9741.
[22] GOYNE K W,CHOROVER J,KUBICKI J D,et al.Sorption of the antibiotic ofloxacin to mesoporous and nonporous alumina and silica[J].Journal of Colloid and Interface Science,2005,283(1):160-170.
[23]高鹏,莫测辉,李彦文,等.高岭土对喹诺酮类抗生素吸附特性的初步研究[J].环境科学,2011,32(6):1740-1744.
[24] URBANIAK B,KOKOT Z J.Analysis of the factors that significantly influence the stability of fluoroquinolone-metal complexes[J].Analytica Chimica Acta,2009,647(1):54-59.
[25] ROSS D L,RILEY C M.Physicochemical properties of the fluoroquinolone antimicrobials.III.Complexation of lomefloxacin with various metal ions and the effect of metal ion complexation on aqueous solubility[J].International Journal of Pharmaceutics,1992,87(1/2/3):203-213.
[26] SAGDINC S,BAYARI S.Spectroscopic studies on the interaction of ofloxacin with metals[J].Journal of Molecular Structure,2004,691(1):107-113.
[27]全瑶,毕二平.不同形态的氧氟沙星在凹凸棒土上的吸附特征[J].高等学校化学学报,2017,38(4):622-630.
[28] PARK H R,CHUNG K Y,LEE H C,et al.Ionization and divalent cation complexation of quinolone antibiotics in aqueous solution[J].Bulletin of the Korean Chemical Society,2000,21(9):849-854.
[29] KUTZNER S,SCHAFFER M,LICHA T,et al.Sorption of organic cations onto silica surfaces over a wide concentration range of competing electrolytes[J].Journal of Colloid and Interface Science,2016,484:229-236.
[2] KRESSE H,BELSEY M J,ROVINI H.The antibacterial drugs market[J].Nature Reviews Drug Discovery,2007,6(1):19-20.
[3]刘克.MgCl2/SiO2复合载体的活化处理研究[J].广东化工,2013,40(10):29-31.
[4] CHEN G L,LI M,LIU X.Fluoroquinolone antibacterial agent contaminants in soil/groundwater:a literature review of sources,fate,and occurrence[J].Water Air and Soil Pollution,2015,226(12):418.
[5] RIAZ L,MAHMOOD T,KHALID A,et al.Fluoroquinolones(FQs)in the environment:a review on their abundance,sorption and toxicity in soil[J].Chemosphere,2017,191:704-720.
[6] YAN W,HU S,JING C Y.Enrofloxacin sorption on smectite clays:effects of pH,cations,and humic acid[J].Journal of Colloid and Interface Science,2012,372(1):141-147.
[7]齐会勉,吕亮,乔显亮.抗生素在土壤中的吸附行为研究进展[J].土壤,2009,41(5):703-708.
[8] ZHANG J H,LU M Y,WAN J,et al.Effects of pH,dissolved humic acid and Cu2+on the adsorption of norfloxacin on montmorillonite-biochar composite derived from wheat straw[J].Biochemical Engineering Journal,2018,130:104-112.
[9] LI Y D,BI E P,CHEN H H.Sorption behavior of ofloxacin to kaolinite:effects of pH,ionic strength,and Cu(II)[J].Water Air and Soil Pollution,2017,228(1):46.
[10] YAN W,ZHANG J F,JING C Y.Adsorption of enrofloxacin on montmorillonite:two-dimensional correlation ATR/FTIR spectroscopy study[J].Journal of Colloid and Interface Science,2013,390(1):196-203.
[11] GU C,KARTHIKEYAN K G.Sorption of the antimicrobial ciprofloxacin to aluminum and iron hydrous oxides[J].Environmental Science and Technology,2005,39(23):66-73.
[12]吴沙沙.可溶性腐殖酸对典型黏土矿物吸附诺氟沙星的影响研究[D].北京:中国地质大学(北京),2014.
[13]吴林.蒙脱土和高岭土对吉非罗齐的吸附特征及影响因素研究[D].北京:中国地质大学(北京),2015.
[14] APPEL C,MA L Q,RHUE R D,et al.Point of zero charge determination in soils and minerals via traditional methods and detection of electroacoustic mobility[J].Geoderma,2003,113(1):77-93.
[15] LI Z H,HONG H L,LIAO L B,et al.A mechanistic study of ciprofloxacin removal by kaolinite[J].Colloids and Surfaces B:Biointerfaces,2011,88(1):339-344.
[16] WANG P,ZHANG D,ZHANG H,et al.Impact of concentration and species of sulfamethoxazole and ofloxacin on their adsorption kinetics on sediments[J].Chemosphere,2017,175:123-129.
[17] LI Z H,SCHULZ L,ACKLEY C,et al.Adsorption of tetracycline on kaolinite with pH-dependent surface charges[J].Journal of Colloid and Interface Science,2010,351(1):254-260.
[18] CARRASQUILLO A J,BRULAND G L,MACKAY A A,et al.Sorption of ciprofloxacin and oxytetracycline zwitterions to soils and soil minerals:influence of compound structure[J].Environmental Science and Technology,2008,42(20):7634-7642.
[19] QIN X P,LIU F,WANG G C,et al.Adsorption of levofloxacin onto goethite:effects of pH,calcium and phosphate[J].Colloids and Surfaces B:Biointerfaces,2014,116(14):591-596.
[20] QIN X P,LIU F,WANG G C,et al.Modeling of levofloxacin adsorption to goethite and the competition with phosphate[J].Chemosphere,2014,111:283-290.
[21] CHASSA A W,OHNO T,HIGGINS S R,et al.Chemical force spectroscopy evidence supporting the layer-by-layer model of organic matter binding to iron(oxy)hydroxide mineral surfaces[J].Environmental Science and Technology,2015,49(16):9733-9741.
[22] GOYNE K W,CHOROVER J,KUBICKI J D,et al.Sorption of the antibiotic ofloxacin to mesoporous and nonporous alumina and silica[J].Journal of Colloid and Interface Science,2005,283(1):160-170.
[23]高鹏,莫测辉,李彦文,等.高岭土对喹诺酮类抗生素吸附特性的初步研究[J].环境科学,2011,32(6):1740-1744.
[24] URBANIAK B,KOKOT Z J.Analysis of the factors that significantly influence the stability of fluoroquinolone-metal complexes[J].Analytica Chimica Acta,2009,647(1):54-59.
[25] ROSS D L,RILEY C M.Physicochemical properties of the fluoroquinolone antimicrobials.III.Complexation of lomefloxacin with various metal ions and the effect of metal ion complexation on aqueous solubility[J].International Journal of Pharmaceutics,1992,87(1/2/3):203-213.
[26] SAGDINC S,BAYARI S.Spectroscopic studies on the interaction of ofloxacin with metals[J].Journal of Molecular Structure,2004,691(1):107-113.
[27]全瑶,毕二平.不同形态的氧氟沙星在凹凸棒土上的吸附特征[J].高等学校化学学报,2017,38(4):622-630.
[28] PARK H R,CHUNG K Y,LEE H C,et al.Ionization and divalent cation complexation of quinolone antibiotics in aqueous solution[J].Bulletin of the Korean Chemical Society,2000,21(9):849-854.
[29] KUTZNER S,SCHAFFER M,LICHA T,et al.Sorption of organic cations onto silica surfaces over a wide concentration range of competing electrolytes[J].Journal of Colloid and Interface Science,2016,484:229-236.
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