左氧氟沙星在针铁矿上的吸附：磷酸盐和腐殖酸的影响
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摘要
抗生素是环境中重要的新型污染物，而针铁矿是包气带中分布最广的铁氧化物，其对抗生素的吸附行为是重要的环境过程。本文主要研究了左氧氟沙星（LEV）在针铁矿上的吸附过程，讨论了pH、Ca2+、磷酸盐和天然有机物（NOM）的影响，同时也研究了不同来源NOM与针铁矿的相互作用，结果表明：
（1）由于针铁矿表面电荷的不对称性和吸附过程中对H+的消耗，LEV在针铁矿上的吸附量（0.034μmol/m2）在pH6附近达到最大，吸附曲线在最大吸附量（pH6）两边是不对称的。
（2）Ca2+的存在会明显抑制LEV在针铁矿上的吸附。这是因为溶液中Ca2+与LEV形成了稳定的络合物（CaH2L3+），由于静电作用和溶液中游离态LEV浓度的降低，导致吸附量降低。
（3）在单体系（LEV-针铁矿，磷酸盐-针铁矿）中，吸附数据都能够较好地利用电荷分布多位络合（CD-MUSIC）模型进行模拟。在复合体系中，磷酸盐会极大地抑制LEV在针铁矿上的吸附，而LEV对磷酸盐的吸附几乎没有影响。静电竞争作用是LEV和磷酸盐在针铁矿上竞争吸附的主要机理。
（4）腐殖酸（HA）在针铁矿上的吸附量在5min内就能接近平衡吸附量（0.51mg C/m2），大分子量的HA主要被针铁矿吸附，低pH有利于针铁矿对HA的吸附。针铁矿与HA之间的作用机理除了静电吸引作用外，还可能存在专属吸附和疏水作用等其他作用。
（5）不同来源的NOM都不同程度地促进了LEV在针铁矿上的吸附。LEV的吸附曲线符合Langmuir和CD-MUSIC的线性可加模型。计算得出的LEV与NOM的结合常数（log K）与NOM的摩尔吸光系数（SUVA）呈现非常好的正相关关系，而与E2/E3、羧基含量和极性呈负相关关系。因此，NOM的SUVA的大小能够反映NOM对LEV的吸附能力。疏水作用和-作用是LEV等抗生素在（矿物结合态的）NOM上吸附的主要机理。
In the environment, antibiotics are a group of new organic contaminants. In thevadose zone, their adsorption on a kind of common iron mineral goethite is veryimportant. In this study, effects of pH, Ca2+, phosphate, and natural organic matter(NOM) on levofloxacin (LEV) adsorption to goethite were investigated, and theinteractions between NOM and goethite were also studied. The results from our studyindicated that:
(1) The adsorbed amount of LEV to goethite reached its maximum (0.034μmol/m2)at pH values around6, and then decreased when pH was lower or higher than thisrange. The LEV adsorption envelope was asymmetric on the two sides of themaximum adsorption around pH6. This was because to a large extent of theasymmetric charge change on goethite surface and the consumption of protons duringthe adsorption of LEV to goethite
(2) In the presence of Ca2+, a decrease in adsorption was observed, because theCa-LEV complexes (CaH2L3+) was formed in solutions, which would cause theelectrostatic interactions and the decrease in free LEV in solutions.
(3) Adsorption of LEV (or phosphate) to goethite in single systems was wellpredicted using the CD-MUSIC (Charge Distribution Multi-Site Complexation)model. In the binary systems, the presence of phosphate decreased LEV adsorption togoethite significantly over the whole pH range. Electrostatic competition was themain reason for the competition of LEV and phosphate to goethite surface in thebinary systems.
(4) The amount of humic acid (HA) adsorbed to goethite was near its equilibriumvalue (0.51mg C/m2) in5min. HA with high molecular weight was mainly adsorbed.More HA was adsorbed to goethite at low pH. Specific adsorption and hydrophobicinteraction might also involved during the interactions between HA and goethitebesides electrostatic attraction.
(5) The presence of nine types of NOM samples increased the adsorption of LEV over the whole pH range. The adsorption envelops were well fitted to the linearadditive model which applies the CD-MUSIC model to simulate LEV adsorption togoethite and the Langmuir model to simulate LEV adsorption to NOM. The optimizedstability constants (log K) for LEV adsorption to NOM were significantly andpositively correlated with Specific UV absorbance (SUVA) values of NOM, andnegatively correlated with E2/E3values, carboxyl contents, and the polarity of NOM.H-bond and cationic complexation are probably not that important in the LEVadsorption process to NOM. Hydrophobic interactions and-interactions wereproposed as the major mechanisms in the adsorption of LEV to (mineral-complexed)NOM.
（1）由于针铁矿表面电荷的不对称性和吸附过程中对H+的消耗，LEV在针铁矿上的吸附量（0.034μmol/m2）在pH6附近达到最大，吸附曲线在最大吸附量（pH6）两边是不对称的。
（2）Ca2+的存在会明显抑制LEV在针铁矿上的吸附。这是因为溶液中Ca2+与LEV形成了稳定的络合物（CaH2L3+），由于静电作用和溶液中游离态LEV浓度的降低，导致吸附量降低。
（3）在单体系（LEV-针铁矿，磷酸盐-针铁矿）中，吸附数据都能够较好地利用电荷分布多位络合（CD-MUSIC）模型进行模拟。在复合体系中，磷酸盐会极大地抑制LEV在针铁矿上的吸附，而LEV对磷酸盐的吸附几乎没有影响。静电竞争作用是LEV和磷酸盐在针铁矿上竞争吸附的主要机理。
（4）腐殖酸（HA）在针铁矿上的吸附量在5min内就能接近平衡吸附量（0.51mg C/m2），大分子量的HA主要被针铁矿吸附，低pH有利于针铁矿对HA的吸附。针铁矿与HA之间的作用机理除了静电吸引作用外，还可能存在专属吸附和疏水作用等其他作用。
（5）不同来源的NOM都不同程度地促进了LEV在针铁矿上的吸附。LEV的吸附曲线符合Langmuir和CD-MUSIC的线性可加模型。计算得出的LEV与NOM的结合常数（log K）与NOM的摩尔吸光系数（SUVA）呈现非常好的正相关关系，而与E2/E3、羧基含量和极性呈负相关关系。因此，NOM的SUVA的大小能够反映NOM对LEV的吸附能力。疏水作用和-作用是LEV等抗生素在（矿物结合态的）NOM上吸附的主要机理。
In the environment, antibiotics are a group of new organic contaminants. In thevadose zone, their adsorption on a kind of common iron mineral goethite is veryimportant. In this study, effects of pH, Ca2+, phosphate, and natural organic matter(NOM) on levofloxacin (LEV) adsorption to goethite were investigated, and theinteractions between NOM and goethite were also studied. The results from our studyindicated that:
(1) The adsorbed amount of LEV to goethite reached its maximum (0.034μmol/m2)at pH values around6, and then decreased when pH was lower or higher than thisrange. The LEV adsorption envelope was asymmetric on the two sides of themaximum adsorption around pH6. This was because to a large extent of theasymmetric charge change on goethite surface and the consumption of protons duringthe adsorption of LEV to goethite
(2) In the presence of Ca2+, a decrease in adsorption was observed, because theCa-LEV complexes (CaH2L3+) was formed in solutions, which would cause theelectrostatic interactions and the decrease in free LEV in solutions.
(3) Adsorption of LEV (or phosphate) to goethite in single systems was wellpredicted using the CD-MUSIC (Charge Distribution Multi-Site Complexation)model. In the binary systems, the presence of phosphate decreased LEV adsorption togoethite significantly over the whole pH range. Electrostatic competition was themain reason for the competition of LEV and phosphate to goethite surface in thebinary systems.
(4) The amount of humic acid (HA) adsorbed to goethite was near its equilibriumvalue (0.51mg C/m2) in5min. HA with high molecular weight was mainly adsorbed.More HA was adsorbed to goethite at low pH. Specific adsorption and hydrophobicinteraction might also involved during the interactions between HA and goethitebesides electrostatic attraction.
(5) The presence of nine types of NOM samples increased the adsorption of LEV over the whole pH range. The adsorption envelops were well fitted to the linearadditive model which applies the CD-MUSIC model to simulate LEV adsorption togoethite and the Langmuir model to simulate LEV adsorption to NOM. The optimizedstability constants (log K) for LEV adsorption to NOM were significantly andpositively correlated with Specific UV absorbance (SUVA) values of NOM, andnegatively correlated with E2/E3values, carboxyl contents, and the polarity of NOM.H-bond and cationic complexation are probably not that important in the LEVadsorption process to NOM. Hydrophobic interactions and-interactions wereproposed as the major mechanisms in the adsorption of LEV to (mineral-complexed)NOM.
引文
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