环丙沙星在黄土中的吸附机制及影响因素

摘要
图/表
参考文献(34)
相关文章 (15)

全文: PDF (497 KB) HTML (1 KB)
输出: BibTeX | EndNote (RIS)

摘要

为了解兽药抗生素在西北黄土中的吸附行为及机制，以环丙沙星（Ciprfloxacin，CIP）为目标污染物，采用批平衡实验法研究其在黄土中的吸附动力学、吸附热力学、pH值和粒径等影响因素.结果表明：环丙沙星在黄土中的吸附可分为两个阶段，6h内表现为快速吸附，6~10h表现为慢速吸附，10h后吸附达到平衡；环丙沙星在黄土中的吸附动力学过程较符合准二级吸附动力学模型，吸附速率受颗粒内部扩散和外部液膜扩散共同影响；吸附热力学过程较符合Freundlich等温吸附模型，且吸附等温线符合L-型，表明黄土对环丙沙星的吸附受溶液中溶质和水分子共同作用影响；焓变ΔH^θ、熵变ΔS^θ和吉布斯自由能ΔG^θ均<0，表明黄土对环丙沙星的吸附是混乱度减少的自发进行的放热反应；pH=5时黄土对环丙沙星的吸附量最大，pH值为2~5时，黄土对环丙沙星的吸附量随pH值升高呈上升趋势，pH>5时，黄土对环丙沙星的吸附量随pH值升高呈下降趋势，表明强酸和碱性环境均不利于吸附；吸附量与黄土粒径呈反比，与初始浓度呈正比.由实验结果推断黄土对环丙沙星的吸附主要与有机质含量有关，主要吸附机制为环丙沙星分子中氨基的阳离子交换作用.

	服务

	把本文推荐给朋友
	加入我的书架
	加入引用管理器
	E-mail Alert
	RSS
	作者相关文章
	蒋煜峰
	温红
	张前
	刘兰兰
	原陇苗
	付雪

关键词 ：黄土, 环丙沙星, 吸附动力学, 吸附热力学, 影响因素

Abstract：

In order to study the adsorption behavior and mechanism of veterinary antibiotics on the loess of Northwest China, ciprofloxacin was selected as the target pollutant, and batch equilibrium method was conducted to investigate its adsorption kinetics, adsorption thermodynamics, and influencing fators, such as pH values and particle sizes, on the adsorption process. Results showed that the adsorption of ciprofloxacin on loess can be divided into two stages:fast adsorption stage (0~6h) and slow adsorption stage (6~10h), and adsorption equilibrium was reached after 10 hours. The adsorption processes fitted well with the pseudo-second-order adsorption kinetics model, and the adsorption rate was controlled by both the internal diffusion of particles and the external diffusion of liquid membrane. The adsorption thermodynamics process was in accordance with the Freundlich model, and the isotherm adsorption was belonged to L-type, which means the adsorption behaviour was affected by the interaction of solute and water molecules in solution. The changes of Enthalpy (ΔH^θ), Entropy (ΔS^θ) and Gibbs free energy (ΔG^θ) were all less than 0, indicated that the adsorption was a spontaneous exothermic reaction with a decrease of chaotic degree. The maximum adsorption amount of ciprofloxacin on loess was obtained at 5 of pH value, and the adsorption of ciprofloxacin on loess increased with the increase of pH value from 2 to 5. While, the adsorption of ciprofloxacin on loess decreased with the increase of pH value beyond 5, thus, strong acid and alkaline environment were unfavorable to adsorption. The adsorption amount of ciprofloxacin on loess was inversely proportional to the size of loess, and was proportional to the initial concentration as well. According to the experimental results, it was inferred that the adsorption of ciprofloxacin on loess was mainly related to the content of organic matter, and the adsorption mechanism was dominated by the cation exchange of amino groups in ciprofloxacin molecule.

Key words： loess ciprofloxacin kinetic adsorption thermodynamic adsorption influencing factors

收稿日期: 2019-04-03

PACS:

X131.3

基金资助:

国家自然科学基金资助项目（21966020，41772147）；兰州交通大学百名青年优秀人才培养计划基金

通讯作者: 蒋煜峰 E-mail: jiangyf7712@126.com

作者简介: 蒋煜峰(1977-),男,甘肃张掖人,博士,教授,主要从事土壤环境化学、土壤污染控制等相关研究工作.发表论文70余篇.

引用本文:

蒋煜峰, 温红, 张前, 刘兰兰, 原陇苗, 付雪. 环丙沙星在黄土中的吸附机制及影响因素[J]. 中国环境科学, 2019, 39(10): 4262-4269. JIANG Yu-feng, WEN Hong, ZHANG Qian, LIU Lan-lan, YUAN Long-miao, FU Xue. Adsorption mechanism and influencing factors of ciprofloxacin on loess. CHINA ENVIRONMENTAL SCIENCECE, 2019, 39(10): 4262-4269.

链接本文:

http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2019/V39/I10/4262

[1]	Chen H, Gao B, Li H, et al. Effects of pH and ionic strength on sulfamethoxazole and ciprofloxacin transport in saturated porous media[J]. Contam.Hydrol, 2011,126(1/2):29-36.
[2]	Zahra M, Bei Y, Catherine N. Adsorption of ciprofloxacin from water by pretreated oat hulls:Equilibrium, kinetic, and thermodynamic studies[J]. Industrial Crops and Products, 2019,127:237-250.
[3]	Everts S S, Berlin C. Drugs in the environment[J]. Chemical & Engineering News, 2010,88:23-24.
[4]	Soren T B. Pharmaceutical antibiotic compounds in soils-a review[J]. Journal of P1ant Nutrition and Soil Science, 2003,166:145-167.
[5]	Beatriz A, José L T, Miguel E, et al. Persistence and availability of veterinary antibiotics in soil and soil-manure systems[J]. Science of the Total Environment, 2018,643:1562-1570.
[6]	Alonso J J S, Kori N E, Melian-Martel N, et al.Removal of ciprofloxacin from seawater by reverse osmosis[J]. Journal of Environmental Management, 2018,217:337-345.
[7]	Martínez-Carballo E, González-Barreiro C, Scharf S, et al. Environmental monitoring study of selected veterinary antibiotics in animal manure and soils in Austria[J]. Environmental Pollution, 2007, 148:1-10.
[8]	Farzin N, Shahram N, Noorizadeh H. Enhanced adsorption and catalytic oxidation of ciprofloxacin by an Ag/AgCl@N-doped activated carbon composite[J]. Phys. Chem. Solids, 2018,114:36-44.
[9]	Wang S, Wang H. Adsorption behavior of antibiotic in soil environment:a critical review[J]..Frontiers of Environmental Science & Engineering, 2015,9:565-574.
[10]	孙红文,张闻.疏水性有机污染物在土壤/沉积物中的赋存状态研究[J]. 环境化学, 2011,30(1):231-241. Sun H W, Zhang W. Existing state of hydrophobic organic compounds in soil sand sediments[J]. Environmental Chemistry, 2011,30(1):231-241.
[11]	Andriamalala A, Vieublé-Gonod L, Dumeny V, et al. Fate of sulfamethoxazole, its main metabolite N-ac-sulfamethoxazole and ciprofloxacin in agricultural soils amended or not by organic waste products[J]. Chemosphere, 2018,191:607-615.
[12]	Li M F, Liu Y G, Liu S B, et al. Performance of magnetic graphene oxide/diethylenetriaminepentaacetic acid nanocomposite for the tetracycline and ciprofloxacin adsorption in single and binary systems[J]. Colloid Interface Science, 2018,521:150-159.
[13]	朱菁菁,任晓雅,汤琳,等.典型土壤改良剂对污染物生物可利用性的影响[J]. 哈尔滨工业大学学报, 2019,2-23:1-11. Zhu J J, Ren X Y, Tang L, et al. Effect of typical soil amendments on bioavailability of pollutants[J]. Journal of Harbin Institute of Technology, 2019,2-23:1-11.
[14]	Tolls J. Sorption of veterinary pharmaceuticals in soi:review[J]. Environmental Science & Technology, 2001,35(17):3397-3406.
[15]	Kumar K, Gupta S C, Chander Y, et al. Antibiotic use in agriculture and its impact on the terrestrial environment[J]. Advances in Agronomy, 2005,87:1-54.
[16]	王冲,罗义,毛大庆.土壤环境中抗生素的来源、转归、生态风险以及消减对策[J]. 环境化学, 2014,33(1):19-29. Wang C, Luo Y, Mao D Q. Sources, fate, ecological risks and mitigation strategies of antibiotics in the soil environment[J]. Environmental Chemistry, 2014,33(1):19-29.
[17]	Zhang H C, Huang C H. Adsorption and oxidation of fluoroquinolone antibacterial agents and structurally related amines with goethite[J]. Chemosphere, 2007,66(8):1502-1512.
[18]	蒋煜峰,刘兰兰,原陇苗,等.秸秆焚烧物对黄土吸附五氯酚的影响研究[J]. 中国环境科学, 2018,38(5):1826-1836. Jiang Y F, Liu L L, Yuan L M, et al. Adsorption of PCP onto loess soil affected by adding corn burning residual[J]. China Environmental Science, 2018,38(5):1826-1836.
[19]	蒋煜峰,Uwamungu Jean Yves,孙航,等.添加小麦秸秆生物炭对黄土吸附苯甲腈的影响[J]. 中国环境科学, 2016,36(5):1506-1513. Jiang Y F, Uwamungu J Y, Sun H, et al. Effect of wheat-waste Biochar on the adsorption behavior of benzonitrile ontoloess soil[J]. China Environmental Science, 2016,36(5):1506-1513.
[20]	Pignatello J J, Xing B. Mechanisms of slow sorption of organic chemicals to natural particles[J]. Environmental Science & Technology, 1995,30(1):1-11.
[21]	蒋煜峰.黄土中典型有机污染物的吸附行为[M]. 北京:中国水利水电出版社, 2016. Jiang Y F. Adsorption behavior of typical organic pollutants in loess[M]. Beijing:China Water Resources and Hydropower Publishing House, 2016.
[22]	Jiang Y F, Sun H, Yves U J, et al. Impact of biochar produced from post-harvest residue on the adsorption behavior of diesel oil on loess soil[J]. Environmental Geochemistry and Health, 2016,38(1):243-253.
[23]	崔皓,王淑平.环丙沙星在潮土中的吸附特性[J]. 环境科学, 2012,33(8):2895-2900. Cui H, Wang S P. Adsorption characteristics of ciprofloxacin in ustic cambosols[J]. Environmental Science, 2012,33(8):2895-2900.
[24]	Rakhshaee R, Khosravi M, Ganji M T. Kinetic modeling and thermodynamic study to remove Pb(II), Cd(II), Ni(II) and Zn (II) from aqueous solution using dead and living Azolla filiculoides[J]. Journal of Hazardous Materials, 2006,134(1-3):120-129.
[25]	彭小明.介孔碳材料制备及对两类典型有机污染物的吸附性能研究[D]. 南京:东南大学, 2015. Peng X M. Preparation of mesoporous carbon materials and adsorption properties of two typical organic pollutants[D]. Nanjing:Southeast University, 2015.
[26]	朱利中.土壤有机污染物界面吸附及调控行为[M]. 北京:科学出版社, 2015. Zhu L Z. Interfacial adsorption and regulation behavior of soil organic pollutants[M]. Beijing:Science Press, 2015.
[27]	Brozni?, Milin D, ?edomila. Effects of Temperature on sorption-desorption processes of imidacloprid in soils of croatian coastal regions[J]. Journal of Environmental Science and Health. Part B:Pesticides, Food Contaminants, and Agricultural Wastes, 2012,47(8):779-794.
[28]	Kiran I, Akart, Özcan A S, et al. Biosorption kinetics and isotherm of Acid Red 57by dried Cephalos-porium aphidicola cells from aqueous solution[J]. Biochemical Engineering Journal, 2006,31:197-203.
[29]	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 P, Mo C H, Li Y W, et al. Preliminary study on the adsorption of quinolones to kaolin[J]. Environmental Science, 2011,32(6):1740-1744.
[30]	谭印月,徐坚,顾雪元,等.环丙沙星在黑土及其组分中的吸附行为及铜和钙的影响[J]. 农业环境科学学报, 2015,34(12):2287-2294. Tan Y Y, Xu J, Gu X Y, et al. Soil components and Cu2+ and Ca2+ effects on ciprofloxac in adsorption by black soil[J]. Journal of Agricultural Environmental Science, 2015,34(12):2287-2294.
[31]	Weber W J J R, Huang W. A distributed reactivity model for sorption by soil and sediments.4. Intraparticle heterogeneity and phase distribution relationships under nonequilibrium conditions[J]. Environmental Science & Technology, 1996,30:881-888.
[32]	王蕊.塿土剖面土壤团聚体有机碳及养分状况研究[D]. 杨凌:西北农林科技大学, 2018. Wang R. Study on organic carbon and nutrient status of soil aggregates in lou soil profile[D]. Yangling:Northwest University of Agriculture and Forestry Science and Technology, 2018.
[33]	Delle Site A. Factors affecting sorption of organic compounds in natural sorbent/water systems and sorption coefficients for selected pollutants, a review[J]. American Institute of Physics, 2001,30:187-251.
[34]	Vasudevan D, Bruland G L, Torrance B S, et al. pH-dependent ciprofloxacin sorption to soils:interaction mechanisms and soil factors influencing sorption[J]. Geoderma, 2009,151(3/4):68-76.