Effect of pH and cations on co-transport of ciprofloxacin and soil colloids
LIU Xiao-wen1, SHAO Ming-yan2, XU Shao-hui1, LIN Qing1
1. College of Environmental Science and Engineering, Qingdao University, Qingdao 266071, China; 2. Qingdao Geo-Engineering Surveying Institute(Qingdao Geological Exploration Development Bureau), Qingdao 266101, China
Abstract：Soil colloids play an important role in the transport and transformation of antibiotics in underground environments, but the transport forms of antibiotics in dissolved and colloidal states have not been fully studied. The co-transport characteristics of ciprofloxacin (CIP) and brown soil colloids under different pH and cationic conditions were studied by static adsorption and column experiments. The results showed that CIP transport was inhibited by brown soil colloids at pH 4.0. At pH 7.0 and 9.0, soil colloids had no significant effect on CIP transport, but some CIP was transported in the colloidal form. Compared with pH, cations (Na+/Ca2+) had more significant effects on the co-transport of CIP and soil colloids. Except for low NaCl concentration (0.001mol/L), CIP transport was inhibited by large amounts of deposited colloids on the quartz sand. With the increase of ionic strength and cationic valence, the inhibition effect weakened due to the decreased adsorption capacity of CIP on brown soil colloids. Under 0.01mol/L NaCl, CIP was activated with the release of soil colloids as the ionic strength in bulk solution decreased, but this phenomenon did not occur under CaCl2, which can be explained by the DLVO theory and straining effect. In addition, CIP inhibited the transport of brown soil colloids under all tested conditions due to the increased surface charge heterogeneity and aggregation of colloids. Our findings demonstrated that the mobility of soil colloids and their adsorption capacity jointly determined the influence of colloids on CIP transport, and the antibiotic transport form not just the total amount should be carefully considered as assessing the potential environmental risks of antibiotics.
刘晓雯, 邵明艳, 徐绍辉, 林青. pH值和阳离子对环丙沙星与土壤胶体共运移的影响[J]. 中国环境科学, 2023, 43(9): 4768-4779.
LIU Xiao-wen, SHAO Ming-yan, XU Shao-hui, LIN Qing. Effect of pH and cations on co-transport of ciprofloxacin and soil colloids. CHINA ENVIRONMENTAL SCIENCECE, 2023, 43(9): 4768-4779.
邹高龙,刘志文,董洁平,等.环丙沙星在污水处理过程中的迁移转化及对污水生物处理的影响[J]. 环境科学学报, 2019,39(2):308-317. Zou G L, Liu Z W, Dong J P, et al. 2019.The transformation of ciprofloxacin in wastewater treatment and its impact on wastewater treatment[J]. Acta Scientiae Circumstantiae, 2019,39(2):308-317.
[2]
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. 2009,151:68-76.
[3]
张晶晶,陈娟,王沛芳,等.中国典型湖泊四大类抗生素污染特征[J]. 中国环境科学, 2021,41(9):4271-4283. Zhang J J, Chen J, Wang P F, et al. Characteristics of four types of antibiotic pollution in typical lakes in China[J]. China Environmental Science, 2021,41(9):4271-4283.
[4]
成玉婷,吴小莲,向垒,等.广州市典型有机蔬菜基地土壤中磺胺类抗生素污染特征及风险评价[J]. 中国环境科学, 2017,37(3):1154-1161. Cheng Y T, Wu X L, Xiang L, et al. Distribution and risk assessment of sulfonamide antibiotics in soil from organic vegetable farms in Guangzhou[J]. China Environmental Science, 2017,37(3):1154-1161.
[5]
杨唐,惠晓亮,王振兴,等.污水处理厂生物气溶胶抗生素抗性污染特征[J]. 中国环境科学, 2022,42(12):5626-5632. Yang T, Hui X L, Wang Z X, et al. Pollution characteristics of bioaerosol antibiotic resistance in sewage treatment plants[J]. China Environmental Science, 2022,42(12):5626-5632.
[6]
Chen H, Gao B, Yang L Y, et al. Montmorillonite enhanced ciprofloxacin transport in saturated porous media with sorbed ciprofloxacin showing antibiotic activity[J]. Journal of Contaminant Hydrology, 2015,173:1-7.
[7]
Zhang H, Lu T, Zhang R, et al. Effects of clay colloids on ciprofloxacin transport in saturated quartz sand porous media under different solution chemistry conditions[J]. Ecotoxicology and Environmental Safety, 2020,199:110754.
[8]
Chen H, Ma L Q, Gao B, et al. Influence of Cu and Ca cations on ciprofloxacin transport in saturated porous media[J]. Journal of Hazardous Materials, 2013,262:805-811.
[9]
Cuprys A, Pulicharla R, Brar S K, et al. Fluoroquinolones metal complexation and its environmental impacts[J]. Coordination Chemistry Reviews, 2018,376:46-61.
[10]
Petosa A R, Jaisi D P, Quevedo I R, et al. Aggregation and deposition of engineered nanomaterials in aquatic environments:role of physicochemical interactions[J]. Environmental Science & Technology, 2010,44(17):6532-6549.
[11]
Torkzaban S, Bradford S A, Vanderzalm J L, et al. Colloid release and clogging in porous media:Effects of solution ionic strength and flow velocity[J]. Journal of Contaminant Hydrology, 2015,181:161-171.
[12]
Sasidharan S, Torkzaban S, Bradford S A, et al. Coupled effects of hydrodynamic and solution chemistry on long-term nanoparticle transport and deposition in saturated porous media[J]. Colloids and Surfaces A:Physicochemical and Engineering Aspects, 2014,457:169-179.
[13]
冯桐桐,杨雯,刘克思,等.离子强度和腐植酸对高岭土协同磺胺二甲基嘧啶迁移的影响[J]. 农业环境科学学报, 2017,36(9):1804-1810. Feng T T, Yang W, Liu K S, et al. Effect of ionic strength and humic acid on the collaborative transport of kaolinite and sulfamethazine[J]. Journal of Agro-Environment Science, 2017,36(9):1804-1810.
[14]
Yang W, Feng T, Flury M, et al. Effect of sulfamethazine on surface characteristics of biochar colloids and its implications for transport in porous media. Environmental[J]. Environmental Pollution, 2019,113482.
[15]
Aguzzi C, Cerezo P, Viseras C, et al. Use of clays as drug delivery systems:Possibilities and limitations[J]. Applied Clay Science, 2007, 36:22-36.
[16]
Jiang W T, Chang P H, Wang Y S, et al. Removal of ciprofloxacin from water by birnessite[J]. Journal of Hazardous Materials, 2013:250-251,362-369.
[17]
Zrnčić M, Babić S, Mutavdžić Pavlović D. Determination of thermodynamic pKa values of pharmaceuticals from five different groups using capillary electrophoresis[J]. Journal of Separation Science, 2015,38(7):1232-1239.
[18]
孟秀.不同离子强度和pH下黏土类胶体和典型抗生素协同运移的机理研究[D]. 青岛:青岛大学, 2021. Meng X. Study on the mechanism of cooperative migration of clay-like colloid and typical antibiotics under different ionic strength and pH[D]. Qingdao:Qingdao University, 2011.
[19]
褚灵阳.纳米羟基磷灰石及其携带重金属铜在石英砂柱中迁移研究[D]. 合肥:安徽农业大学, 2011. Chu L Y. Study on the migration of nano-hydroxyapatite and its heavy metal copper in quartz sand column[D]. Hefei:Anhui Agricultural University, 2011.
[20]
Cheng D, Liao P, Yuan S. Effects of ionic strength and cationic type on humic acid facilitated transport of tetracycline in porous media[J]. Chemical Engineering Journal, 2016,284:389-394.
[21]
陈燕娜,吴鸣,程洲,等.典型微塑料对环丙沙星在多孔介质运移的影响[J]. 农业环境科学学报, 2021,40(2):400-407. Chen Y N, Wu M, Cheng Z et al. Effects of typical microplastics on migration of ciprofloxacin in porous media[J]. Journal of Agro-Environment Science, 2021,40(2):400-407.
[22]
Chen J, Xu Y, Zheng Z, et al. The mechanisms involved into the inhibitory effects of ionic liquids chemistry on adsorption performance of ciprofloxacin onto inorganic minerals[J]. Colloids and Surfaces A:Physicochemical and Engineering Aspects, 2022,648,129422.
[23]
Wang C J, Li Z, Jiang W T. Adsorption of ciprofloxacin on 2:1dioctahedral clay minerals[J]. Applied Clay Science, 2011,53:723-728.
[24]
黄翔峰,熊永娇,彭开铭,等.金属离子络合对抗生素去除特性的影响研究进展[J]. 环境化学, 2016,35(1):133-140. Huang X F, Xiong Y J, Peng K M, et al. The progress of antibiotics removal performance under the complexion effect of metal ions[J]. Environmental Chemistry, 2016,35(1):133-140.
[25]
Wu Q, Li Z, Hong H, et al. Adsorption and intercalation of ciprofloxacin on montmorillonite[J]. Applied Clay Science, 2010, 50:204-211.
[26]
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, 2018,191:704-720.
[27]
赵凌曦,侯万国.固-液界面吸附中的固体浓度效应[C]//中国化学会第十四届胶体与界面化学会议论文摘要集-第5分会:胶体与界面化学中的理论问题, 2013:21-22. Zhao L X, Hou W G. Effect of solid concentration on solid-liquid interface adsorption[C]//Abstracts of the 14th Colloidal and Interfacial Chemistry Conference of the Chinese Chemical Society-Session 5:Theoretical problems in colloid and interfacial chemistry[C]. 2013,21-22.
[28]
Chen H, Gao B, Li H, et al. Effects of pH and ionic strength on sulfamethoxazole and ciprofloxacin transport in saturated porous media[J]. Journal of Contaminant Hydrology, 2011,126:29-36.
[29]
Peng X, Lam F L Y, Wang Y, et al. Adsorption behavior and mechanisms of Ciprofloxacin from aqueous solution by ordered mesoporous carbon and bamboo-based carbon[J]. Journal of Colloid and Interface Science, 2015,460:349-360.
[30]
Li Z, Hong H, Liao L, et al. A mechanistic study of ciprofloxacin removal by kaolinite[J]. Colloids and Surfaces B:Biointerfaces, 2011, 88:339-344.
[31]
Dong S, Gao B, Sun Y, et al. Transport of sulfacetamide and levofloxacin in granular porous media under various conditions:Experimental observations and model simulations[J]. Science of The Total Environment, 2016,573:1630-1637.
[32]
李兵,李航,朱华玲,等.不同pH条件下黄壤胶体凝聚的动态光散射研究[J]. 土壤学报, 2013,50(1):89-95. Li B, Li H, Zhu H L, et al. Study on dynamic light scattering of yellow soil colloid condensation under different pH conditions[J]. Acta pedologica sinica, 2013,50(1):89-95.
[33]
Bradford S A, Yates S R, Bettahar M, et al. Physical factors affecting the transport and fate of colloids in saturated porous media[J]. Water Resources Research, 2002,38(12):61-63.
[34]
Shen C, Wu L, Zhang S, et al. Heteroaggregation of microparticles with nanoparticles changes the chemical reversibility of the microparticles' attachment to planar surfaces[J]. Journal of Colloid and Interface Science, 2014,421:103-113.
[35]
Bradford S A, Torkzaban S. Colloid interaction energies for physically and chemically heterogeneous porous media[J]. Langmuir, 2013,29:3668-3676.
[36]
Sibley S D, Pedersen J A. Interaction of the macrolide antimicrobial clarithromycin with dissolved humic acid[J]. Environmental Science & Technology, 2008,42(2):422-428.
[37]
Genç N, Dogan E C. Adsorption kinetics of the antibiotic ciprofloxacin on bentonite, activated carbon, zeolite, and pumice[J]. Desalination and Water Treatment, 2015,53:785-793.
[38]
Celis R, Adelino M A, Hermosín M C, et al. Montmorillonite-chitosan bionanocomposites as adsorbents of the herbicide clopyralid in aqueous solution and soil water suspensions[J]. Journal of Hazardous Materials, 2012:209-210,67-76.
[39]
孙凯璇,向令,孙占学,等.典型抗生素在多孔介质中迁移特性的对比研究[J]. 环境科学学报, 2020,40(5):1786-1797. Sun K X, Xiang L, Sun Z X, et al. Comparing the transport behavior of typical sulfonamides and fluoroquinolones in granular porous media[J]. Acta Scientiae Circumstantiae, 2020,40(5):1786-1797.
[40]
Lv X Y, Sun Y Y, Ji R, et al. Physicochemical factors controlling the retention and transport of perfluorooctanoic acid (PFOA) in saturated sand and limestone porous media[J]. Water Research, 2018,141:251-258.
[41]
Xie W H, Shiu W Y, Mackay D. A review of the effect of salts on the sol-ubility of organic compounds in seawater[J]. Marine Environmental Research, 1997,44:429-444.
[42]
胡俊栋,沈亚婷,王学军.离子强度、pH对土壤胶体释放、分配沉积行为的影响[J]. 生态环境学报, 2009,18(2):629-637. Hu J D, Shen Y T, Wang X J. Effects of ionic strength and pH on soil colloid release, distribution and deposition behavior[J]. Ecology and Environment, 2009,18(2):629-637.
[43]
吕雪艳,姚遥,孙媛媛,等.离子强度及pH对不同类型土壤中胶体释放的影响[J]. 农业环境科学学报, 2014,33(7):1358-1365. Lv X Y, Yao Y, Sun Y Y, et al. Effects of ionic strength and pH on colloidal release in different soil types[J]. Journal of Agro-Environment Science, 2014,33(7):1358-1365.
[44]
Fang J, Xu M J, Wang D J, et al. Modeling the transport of TiO2nanoparticle aggregates in saturated and unsaturated granular media:effects of ionic strength and pH[J]. Water Research, 2013,47:1399-1408.
