滨湖底泥对2种喹诺酮类抗生素的吸附作用研究
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摘要
吸附-解吸是环境中抗生素发生迁移转化的重要过程。文章研究选择鄱阳湖滨湖底泥,采用批平衡实验法进行2种喹诺酮类抗生素的底泥吸附-解吸实验,并考察了pH、阳离子种类及阳离子浓度等因素对吸附的影响。结果表明,底泥对2种喹诺酮类抗生素的吸附过程符合拟二级动力学方程(R~2>0.99)。在298 K下,Langmuir模型能够更好地描述底泥对2种抗生素的等温吸附行为,底泥对CIP和ENR的最大吸附容量Q_m分别为15.289 0 mg/g和8.649 6 mg/g。底泥对2种抗生素在pH 3～9时均具有较好的吸附率,其中pH=5时其吸附率均达90%以上。底泥对2种抗生素的吸附-解吸行为受到水环境中Ca~(2+)的明显影响。研究表明,2种喹诺酮类抗生素在鄱阳湖滨湖底泥中具有较好的吸附作用,但考虑鄱阳湖流域水环境中以Ca~(2+)为主的常量阳离子的存在,则底泥对2种抗生素的平衡吸附率为40%～50%。研究可为喹诺酮类抗生素在鄱阳湖水环境中的环境行为及归趋研究提供科学依据。
Adsorption-desorption is an important process for the migration and transformation of antibiotics in the environment. In this study, sediments from the lakeside of Poyang Lake were selected, and the sediment adsorption-desorption experiments of two quinolone antibiotics were carried out by batch equilibrium experiments. The effects of pH, cation species and cation concentrations on adsorption were investigated. The results showed that the adsorption process of the two quinolone antibiotics by the sediment was consistent with the pseudo-second-order kinetic equation.(R~2>0.99). At 298 K, the Langmuir model can describe the isothermal adsorption behavior of the two antibiotics. The maximum adsorption capacities Qmof the sediment for ciprofloxacin(CIP) and enrofloxacin(ENR) were 15.289 0 mg/g and 8.649 6 mg/g, respectively. CIP and ENR were well adsorbed in pH 3～9 by the sediment, and the adsorption rates of CIP and ENR were both above 90% at p H 5. The presence of Ca~(2+) in water environment had a significant influence on the adsorption-desorption behavior of two quinolone antibiotics. This study showed that the two quinolone antibiotics had good adsorption in the sediment from the shore of Poyang Lake, but considering the presence of constant cations such as Ca~(2+) in the water environment, the equilibrium adsorption rate was 40%～50%. This study provided a scientific basis for the environmental behavior and fate research of quinolone antibiotics in the water environment of Poyang Lake region.
Adsorption-desorption is an important process for the migration and transformation of antibiotics in the environment. In this study, sediments from the lakeside of Poyang Lake were selected, and the sediment adsorption-desorption experiments of two quinolone antibiotics were carried out by batch equilibrium experiments. The effects of pH, cation species and cation concentrations on adsorption were investigated. The results showed that the adsorption process of the two quinolone antibiotics by the sediment was consistent with the pseudo-second-order kinetic equation.(R~2>0.99). At 298 K, the Langmuir model can describe the isothermal adsorption behavior of the two antibiotics. The maximum adsorption capacities Qmof the sediment for ciprofloxacin(CIP) and enrofloxacin(ENR) were 15.289 0 mg/g and 8.649 6 mg/g, respectively. CIP and ENR were well adsorbed in pH 3～9 by the sediment, and the adsorption rates of CIP and ENR were both above 90% at p H 5. The presence of Ca~(2+) in water environment had a significant influence on the adsorption-desorption behavior of two quinolone antibiotics. This study showed that the two quinolone antibiotics had good adsorption in the sediment from the shore of Poyang Lake, but considering the presence of constant cations such as Ca~(2+) in the water environment, the equilibrium adsorption rate was 40%～50%. This study provided a scientific basis for the environmental behavior and fate research of quinolone antibiotics in the water environment of Poyang Lake region.
引文
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[10]Tuc Q D,Elodie M G,Pierre L,et al.Fate of antibiotics from hospital and domestic sources in a sewage network[J].Science of the Total Environment,2016,575:758-766.
[11]Yang J F,Ying G G,Zhao J L,et al.Simultaneous determination of four classes of antibiotics in sediments of the Pearl Rivers using RRLC-MS/MS[J].Science of the Total Environment,2010,408(16):3424-3432.
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[16]徐颖,王飞,王祺,等.磺胺类抗生素在辽西河流沉积物中吸附行为研究[J].地球与环境,2016,44(2):199-203.Xu Ying,Wang Fei,Wang Qi,et al.The adsorption behaviors of sulfanilamide antibiotics in western Liaoning River sediment[J].Earth and Environment,2016,44(2):199-203.
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[19]黎园,赵纯,邓慧萍.2种孔径沸石分子筛对水中土霉素的去除研究[J].环境科学,2010,31(4):990-995.Li Yuan,Zhao Chun,Deng Huiping.Oxytetracycline removal in aqueous by two kinds of zeolites with different bore diameters[J].Environmental Science,2010,31(4):990-995.
[20]Zhu X D,Liu Y C,Qian F,et al.Preparation of magnetic porous carbon from waste hydrochar by simultaneous activation and magnetization for tetracycline removal[J].Bioresource Technology,2014,154:209-214.
[21]吴亦潇,李爱民,汪的华,等.一种纳米级不定形碳对水中四环素的吸附研究[J].环境科学,2015,36(1):426-429.Wu Yixiao,Li Aimin,Wang Dihua,et al.Removal of tetracycline by a kind of nano-sized amorphous carbon[J].Environmental Science,2015,36(1):426-429.
[22]李仕友,欧阳成炜,伍随意,等.L-谷氨酸功能化氧化石墨烯制备及其对铀的吸附研究[J].安全与环境学报,2019,19(1):231-238.Li Shiyou,Ouyang Chengwei,Wu Suiyi,et al.Adsorptive function for uranium by the L-glutamic acid-functionalized graphene oxide[J].Journal of Safety and Environment,2019,19(1):231-238.
[23]王富民,马秀兰,边炜涛,等.湖库底泥对环丙沙星吸附特性的研究[J].水土保持学报,2016,30(2):312-316.Wang Fumin,Ma Xiulan,Bian Weitao,et al.The adsorption characteristic of reservoir sediment to ciprofloxacin[J].Journal of Soil and Water Conservation,2016,30(2):312-316.
[24]边炜涛.抗生素环丙沙星在苏打盐碱土中吸附解吸特性的研究[D].长春:吉林农业大学,2017.Bian Weitao.Study on Adsorption and Desorption Characteristics of Antibiotic Ciprofloxacin in Soda Saline-Alkali Soil[D].Changchun:Jilin Agricultural University,2017.
[25]任艳婷.水环境中不同粒径高岭土吸附喹诺酮类抗生素的特征分析[D].天津:天津大学,2016.Ren Yanting.Characteristics of Adsorption of Quinolones Antibiotics with Different Particle Sizes Kaolin in Water Environment[D].Tianjin:Tianjin University,2016.
[26]Wu Q F,Li Z H,Hong H.Influence of types and charges of exchangeable cations on ciprofloxacin sorption by montmorillonite[J].Journal of Wuhan University of Technology:Materials Science Edition,2012,27(3):516-522.
[27]王增双.煤矸石及其改性产品对抗生素吸附特性的研究[D].太原:太原理工大学,2017.Wang Zengshuang.Study on the Adsorption Characteristics of Antibiotics to Coal Gangue and Its Modified Products[D].Taiyuan:Taiyuan University of Technology,2017.
[28]冯冬燕.石墨烯基碳纳米材料对类金属和抗生素吸附特性研究[D].苏州:苏州科技学院,2014.Feng Dongyan,Study of Adsorption Properties for Metalloid and Antibiotic with Graphene Based Carbon Nanomaterials[D].Suzhou:Suzhou University of Science and Technology,2014.
[29]李美兰,邓月华,孙成,等.强力霉素在凹凸棒土上的吸附行为[J].环境化学,2012,31(4):457-463.Li Meilan,Deng Yuehua,Sun Cheng,et al.Adsorption of doxycycline on attapulgite[J].Environmental Chemistry,2012,31(4):457-463.
[30]武庭瑄,周敏,郭宏栋,等.四环素在黄土中的吸附行为[J].环境科学学报,2008,28(11):2311-2314.Wu Tingxuan,Zhou Min,Guo Hongdong,et al.Adsorption of tetracycline on loess soils[J].Acta Scientia Circumstantiae,2008,28(11):2311-2314.
[31]张全军,于秀波,钱建鑫,等.鄱阳湖南矶湿地优势植物群落及土壤有机质和营养元素分布特征[J].生态学报,2012,32(12):3656-3669.Zhang Quanjun,Yu Xiubo,Qian Jianxin,et al.Distribution characteristics of plant communities and soil organic matter and main nutrients in Nanji wetland of Poyang Lake[J].Acta Ecologico Sinica,2012,32(12):3656-3669.
[32]易文利,王圣瑞,杨苏文,等.长江中下游浅水湖泊沉积物腐殖质组分赋存特征[J].湖泊科学,2011,23(1):21-28.Yi Wenli,Wang Shengrui,Yang Suwen,et al.Humus distribution and forms in the sediments from shallow Iakes in the middle and lower reaches of the Yangtze River[J].Journal of Lake Science,2011,23(1):21-28.
[33]Ding H,Wu Y,Zou B,et al.Simultaneous removal and degradation characteristics of sulfonamide,tetracycline,and quinolone antibiotics by laccase-mediated oxidation coupled with soil adsorption[J].Journal of Hazardous Materials,2016,307:350-358.
[34]徐颖,王祺,苏墨,等.磺胺抗生素在河流沉积物中的吸附特性研究[J].安全与环境学报,2016,16(2):278-283.Xu Ying,Wang Qi,Su Mo,et al.Adsorption characteristics of sulfa antibiotics in the river sediments[J].Journal of Safety&Environment,2016,16(2):278-283.
[35]胡春华.鄱阳湖水环境特征及演化趋势研究[D].南昌:南昌大学,2010.Hu Chunhua.Study on Water Environment Characteristics and Evolution Trend of Poyang Lake[D].Nanchang:Nanchang University,2010.
[2]Sarmah A K,Meyer M T,Boxall A B.A global perspective on the use,sales,exposure pathways,occurrence,fate and effects of veterinary antibiotics(VAs)in the environment[J].Chemosphere,2006,65(5):725-759.
[3]高品.典型抗生素和抗药性基因在污水处理系统中的归趋及迁移分布规律[D].上海:东华大学,2011.Gao Pin.Fate,Transport and Distribution of Typical Antibiotics and Antibiotic Resistance Genes in Sewage Treatment System[D].Shanghai:Donghua University,2011.
[4]Zhang Q Q,Ying G G,Pan C G,et al.Comprehensive evaluation of antibiotics emission and fate in the river basins of China:source analysis,multimedia modeling,and linkage to bacterial resistance[J].Environmental Science and Technology,2015,49(11):67-72.
[5]章强,辛琦,朱静敏,等.中国主要水域抗生素污染现状及其生态环境效应研究进展[J].环境化学,2014,3307:1075-1083.Zhang Qiang,Xin Qi,Zhu Jingmin,et al.The antibiotic contaminations in the main water bodies in China and the associated environmental and human health impacts[J].Environmental Chemistry,2014,3307:1075-1083.
[6]Zou S C,Xu W H,Zhang R J,et al.Occurrence and distribution of antibiotics in coastal water of the Bohai Bay,China:impacts of river discharge and aquaculture activities[J].Environmental Pollution,2011,159(10):2913-2920.
[7]Jiang H Y,Zhang D D,Xiao S C,et al.Occurrence and sources of antibiotics and their metabolites in river water,WWTPs,and swine wastewater in Jiulongjiang River basin,south China[J].Environmental Science&Pollution Research,2013,20(12):9075-9083.
[8]Zhao S N,Liu X H,Cheng D M,et al.Temporal-spatial variation and partitioning prediction of antibiotics in surface water and sediments from the intertidal zones of the Yellow River Delta,China[J].Science of the Total Environment,2016,569/570:1350-1358.
[9]李嘉,张瑞杰,王润梅,等.小清河流域抗生素污染分布特征与生态风险评估[J].农业环境科学学报,2016,35(7):1384-1391.Li Jia,Zhang Ruijie,Wang Runmei,et al.Distribution characteristics and ecological risk assessment of antibiotic pollution in Xiaoqing River watershed[J].Journal of Agro-environment Science,2016,35(7):1384-1391.
[10]Tuc Q D,Elodie M G,Pierre L,et al.Fate of antibiotics from hospital and domestic sources in a sewage network[J].Science of the Total Environment,2016,575:758-766.
[11]Yang J F,Ying G G,Zhao J L,et al.Simultaneous determination of four classes of antibiotics in sediments of the Pearl Rivers using RRLC-MS/MS[J].Science of the Total Environment,2010,408(16):3424-3432.
[12]葛林科.水中溶解性物质对氯霉素类和氟喹诺酮类抗生素光降解的影响[D].大连:大连理工大学,2009.Ge Linke.Effects of Aqueous Dissolved Matter on Photodegradation of Phenicol and Fluoroquinolone Antibiotics[D].Dalian:Dalian University of Technology,2009.
[13]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.Gao Peng,Mo Cehui,Li Yanwen,et al.Preliminary study on the adsorption of quinolones to kaolin[J].Environmental Science,2011,32(6):1740-1744.
[14]王富民.环丙沙星和恩诺沙星在湖库底泥和土壤中吸附-解吸特性研究[D].长春:吉林农业大学,2016.Wang Fumin.Adsorption-Desorption Characteristics Research of Ciprofloxacin and Enrofloxacin in Sediment and Soil[D].Changchun:Jilin Agricultural University,2016.
[15]苏畅.碳纳米管对磺胺类抗生素在底泥中迁移的影响研究[D].长沙:湖南大学,2016.Su Chang.Impact of Carbon Nanotubes on the Mobility of Sulfonamide Antibiotics in Sediment[D].Changsha:Hunan University,2016.
[16]徐颖,王飞,王祺,等.磺胺类抗生素在辽西河流沉积物中吸附行为研究[J].地球与环境,2016,44(2):199-203.Xu Ying,Wang Fei,Wang Qi,et al.The adsorption behaviors of sulfanilamide antibiotics in western Liaoning River sediment[J].Earth and Environment,2016,44(2):199-203.
[17]Ding H,Wu Y,Zhang W,et al.Occurrence,distribution,and risk assessment of antibiotics in the surface water of Poyang Lake,the largest freshwater lake in China[J].Chemosphere,2017,184:137-147.
[18]Conkle J L,Lattao C,White J R,et al.Competitive sorption and desorption behavior for three fluoroquinolone antibiotics in a wastewater treatment wetland soil[J].Chemosphere,2010,80(11):1353-1359.
[19]黎园,赵纯,邓慧萍.2种孔径沸石分子筛对水中土霉素的去除研究[J].环境科学,2010,31(4):990-995.Li Yuan,Zhao Chun,Deng Huiping.Oxytetracycline removal in aqueous by two kinds of zeolites with different bore diameters[J].Environmental Science,2010,31(4):990-995.
[20]Zhu X D,Liu Y C,Qian F,et al.Preparation of magnetic porous carbon from waste hydrochar by simultaneous activation and magnetization for tetracycline removal[J].Bioresource Technology,2014,154:209-214.
[21]吴亦潇,李爱民,汪的华,等.一种纳米级不定形碳对水中四环素的吸附研究[J].环境科学,2015,36(1):426-429.Wu Yixiao,Li Aimin,Wang Dihua,et al.Removal of tetracycline by a kind of nano-sized amorphous carbon[J].Environmental Science,2015,36(1):426-429.
[22]李仕友,欧阳成炜,伍随意,等.L-谷氨酸功能化氧化石墨烯制备及其对铀的吸附研究[J].安全与环境学报,2019,19(1):231-238.Li Shiyou,Ouyang Chengwei,Wu Suiyi,et al.Adsorptive function for uranium by the L-glutamic acid-functionalized graphene oxide[J].Journal of Safety and Environment,2019,19(1):231-238.
[23]王富民,马秀兰,边炜涛,等.湖库底泥对环丙沙星吸附特性的研究[J].水土保持学报,2016,30(2):312-316.Wang Fumin,Ma Xiulan,Bian Weitao,et al.The adsorption characteristic of reservoir sediment to ciprofloxacin[J].Journal of Soil and Water Conservation,2016,30(2):312-316.
[24]边炜涛.抗生素环丙沙星在苏打盐碱土中吸附解吸特性的研究[D].长春:吉林农业大学,2017.Bian Weitao.Study on Adsorption and Desorption Characteristics of Antibiotic Ciprofloxacin in Soda Saline-Alkali Soil[D].Changchun:Jilin Agricultural University,2017.
[25]任艳婷.水环境中不同粒径高岭土吸附喹诺酮类抗生素的特征分析[D].天津:天津大学,2016.Ren Yanting.Characteristics of Adsorption of Quinolones Antibiotics with Different Particle Sizes Kaolin in Water Environment[D].Tianjin:Tianjin University,2016.
[26]Wu Q F,Li Z H,Hong H.Influence of types and charges of exchangeable cations on ciprofloxacin sorption by montmorillonite[J].Journal of Wuhan University of Technology:Materials Science Edition,2012,27(3):516-522.
[27]王增双.煤矸石及其改性产品对抗生素吸附特性的研究[D].太原:太原理工大学,2017.Wang Zengshuang.Study on the Adsorption Characteristics of Antibiotics to Coal Gangue and Its Modified Products[D].Taiyuan:Taiyuan University of Technology,2017.
[28]冯冬燕.石墨烯基碳纳米材料对类金属和抗生素吸附特性研究[D].苏州:苏州科技学院,2014.Feng Dongyan,Study of Adsorption Properties for Metalloid and Antibiotic with Graphene Based Carbon Nanomaterials[D].Suzhou:Suzhou University of Science and Technology,2014.
[29]李美兰,邓月华,孙成,等.强力霉素在凹凸棒土上的吸附行为[J].环境化学,2012,31(4):457-463.Li Meilan,Deng Yuehua,Sun Cheng,et al.Adsorption of doxycycline on attapulgite[J].Environmental Chemistry,2012,31(4):457-463.
[30]武庭瑄,周敏,郭宏栋,等.四环素在黄土中的吸附行为[J].环境科学学报,2008,28(11):2311-2314.Wu Tingxuan,Zhou Min,Guo Hongdong,et al.Adsorption of tetracycline on loess soils[J].Acta Scientia Circumstantiae,2008,28(11):2311-2314.
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