Skip to main content
SpringerLink
Log in

Different co-transport forms of ciprofloxacin with montmorillonite colloids in porous media as affected by pH and cations

  • Soils, Sec 2 • Global Change, Environmental Risk Assessment, Sustainable Land Use • Research Article
  • Published:
Journal of Soils and Sediments Aims and scope Submit manuscript

Abstract

Purpose

Continuous release of antibiotics into the environment poses a potential threat to human and animal health. The existing forms of antibiotics in soil and groundwater determine their fate, transport, and ecological risks. However, antibiotic transport forms (dissolved and colloidal) as affected by mineral colloids have not been well investigated to date.

Methods

Ciprofloxacin (CIP), one of the most frequently detected fluoroquinolones (FQs), and montmorillonite, ubiquitous in soil and groundwater, were chosen as the representative antibiotic and colloid. The co-transport forms of CIP with montmorillonite colloids under different pH and cations were systematically investigated in saturated quartz sand porous media. Additionally, solute (TSM) and colloid (TKRSM) transport models were used to simulate CIP and colloid transport and further reveal their co-transport mechanisms.

Results

More than 50% of recovered CIP was transported in colloidal form under different pH conditions due to the high adsorption capacity of montmorillonite colloids for CIP. However, in terms of the total amount, massive deposited colloids inhibited CIP transport under acidic conditions, resulting in 17.21% less CIP recovered. Conversely, under neutral and alkaline conditions, montmorillonite colloids slightly promoted the transport of CIP mainly owing to enhanced desorption. Compared with pH, cations (Na+/Ca2+) have more effects on CIP co-transport with colloids. At a low NaCl concentration, mobile colloids enhanced CIP transport. However, CIP was mainly transported in dissolved form and inhibited by immobile colloids with the recovery rates decreasing by 39.58%, 32.66%, and 21.78%, respectively, at 0.01 M Na+, 0.001 M Ca2+, and 0.01 M Ca2+. With the increasing ionic strength and valence, the inhibitory effect weakened. Notably, CIP was remobilized with the release of colloids under NaCl solution, whereas not under CaCl2 solution, which could be explained by DLVO theory and straining effect.

Conclusions

Colloid mobility and their sorption capacity jointly determined their impact on antibiotic transport, and the form, not just the total amount, should be considered carefully when evaluating the potential environmental risk of antibiotics.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6

Similar content being viewed by others

Availability of data and materials

All data generated or analyzed during this study are included in this published article (and its supplementary information files).

References

  • Aguzzi C, Cerezo P, Viseras C, Caramella C (2007) Use of clays as drug delivery systems: possibilities and limitations. Appl Clay Sci 36(1–3):22–36

    Article  CAS  Google Scholar 

  • Aristilde L, Sposito G (2008) Molecular modeling of metal complexation by a fluoroquinolone antibiotic. Environ Toxicol Chem 27(11):2304–2310

    Article  CAS  PubMed  Google Scholar 

  • Arya V, Philip L (2016) Adsorption of pharmaceuticals in water using Fe3O4 coated polymer clay composite. Micropor Mesopor Mat 232:273–280

    Article  CAS  Google Scholar 

  • Ashworth DJ, Ibekwe AM, Men Y, Ferreira JFS (2023) Dissemination of antibiotics through the wastewater–soil–plant–earthworm continuum. Sci Total Environ 858:159841

    Article  ADS  CAS  PubMed  Google Scholar 

  • Babakhani P, Bridge J, Doong R, Phenrat T (2017) Continuum-based models and concepts for the transport of nanoparticles in saturated porous media: a state- of-the-science review. Adv Colloid Interfac 246:75–104

    Article  CAS  Google Scholar 

  • Berhane TM, Levy J, Krekeler MPS, Danielson ND (2016) Adsorption of bisphenol A and ciprofloxacin by palygorskite-montmorillonite: effect of granule size, solution chemistry and temperature. Appl Clay Sci 132–133:518–527

    Article  Google Scholar 

  • Bradford SA, Torkzaban S (2013) Colloid interaction energies for physically and chemically heterogeneous porous media. Langmuir 29:3668–3676

    Article  CAS  PubMed  Google Scholar 

  • Bradford SA, Yates SR, Bettahar M, Simunek J (2002) Physical factors affecting the transport and fate of colloids in saturated porous media. Water Resour Res 38(12):1327

    Article  ADS  Google Scholar 

  • Bradford SA, Simunek J, Bettahar M, Van Genuchten MTh, Yates SR (2003) Modeling colloid attachment, straining, and exclusion in saturated porous media. Environ Sci Technol 37(10):2242–2250

    Article  ADS  CAS  PubMed  Google Scholar 

  • Bradford SA, Torkzaban S, Walker SL (2007) Coupling of physical and chemical mechanisms of colloid straining in saturated porous media. Water Res 41:3012–3024

    Article  CAS  PubMed  Google Scholar 

  • Brandt KK, Amézquita A, Backhaus T, Boxall A, Coors A, Heberer T, Lawrence JR, Lazorchak J, Schönfeld J, Snape JR, Zhu YG, Topp E (2015) Ecotoxicological assessment of antibiotics: a call for improved consideration of microorganisms. Environ Int 85:189–205

    Article  CAS  PubMed  Google Scholar 

  • Chen H, Ma LQ, Gao B, Gu C (2013) Influence of Cu and Ca cations on ciprofloxacin transport in saturated porous media. J Hazard Mat 262:805–811

    Article  CAS  Google Scholar 

  • Chen H, Gao B, Yang LY, Ma LQ (2015) Montmorillonite enhanced ciprofloxacin transport in saturated porous media with sorbed ciprofloxacin showing antibiotic activity. J Contam Hydrol 173:1–7

    Article  CAS  PubMed  Google Scholar 

  • Chen J, Xu Y, Zheng Z, Wei Q, Farooq U, Lu T, Chen W, Qi Z (2022) The mechanisms involved into the inhibitory effects of ionic liquids chemistry on adsorption performance of ciprofloxacin onto inorganic minerals. Colloids Surface A 648:129422

    Article  CAS  Google Scholar 

  • Chotpantarat S, Kiatvarangkul N (2018) Facilitated transport of cadmium with montmorillonite KSF colloids under different pH conditions in water-saturated sand columns: experiment and transport modeling. Water Res 146:216–231

    Article  CAS  PubMed  Google Scholar 

  • Cui S, Qi Y, Zhu Q, Wang C, Sun H (2023) A review of the influence of soil minerals and organic matter on the migration and transformation of sulfonamides. Sci Total Environ 861:160584

    Article  ADS  CAS  PubMed  Google Scholar 

  • Cuprys A, Pulicharla R, Brar SK, Drogui P, Verma M, Surampalli RY (2018) Fluoroquinolones metal complexation and its environmental impacts. Coordin Chem Rev 376:46–61

    Article  CAS  Google Scholar 

  • Dong Z, Zhang W, Qiu Y, Yang Z, Wang J, Zhang Y (2019) Cotransport of nanoplastics (NPs) with fullerene (C60) in saturated sand: Effect of NPs/C60 ratio and seawater salinity. Water Res 148:469–478

    Article  CAS  PubMed  Google Scholar 

  • Duan W, Wang N, Xiao W, Zhao Y, Zheng Y (2018) Ciprofloxacin adsorption onto different micro-structured tourmaline, halloysite and biotite. J Mol Liq 269:874–881

    Article  CAS  Google Scholar 

  • French RA, Jacobson AR, Kim B, Isley SL, Penn RL, Baveye PC (2009) Influence of ionic strength, pH, and cation valence on aggregation kinetics of titanium dioxide nanoparticles. Environ Sci Technol 43(5):1354–1359

    Article  ADS  CAS  PubMed  Google Scholar 

  • Gomes MP, Brito JCM, Carvalho Carneiro MML, Cunha MRR, Garcia QS, Figueredo CC (2018) Responses of the nitrogen-fixing aquatic fern Azolla to water contaminated with ciprofloxacin: impacts on biofertilization. Environ Pollut 232:293–299

    Article  CAS  PubMed  Google Scholar 

  • Gu C, Karthikeyan KG (2005) Sorption of the antimicrobial ciprofloxacin to aluminum and iron hydrous oxides. Environ Sci Technol 39(23):9166–9173

    Article  ADS  CAS  PubMed  Google Scholar 

  • Huang X, Xiong Y, Peng K, Lu L, Liu J (2016) The progress of antibiotics removal performance under the complexion effect of metal ions. J Environ Chem 35(1):133–140 (in Chinese)

  • Igwegbe CA, Oba SN, Aniagor CO, Adeniyi AG, Ighalo JO (2021) Adsorption of ciprofloxacin from water: a comprehensive review. J Ind Eng Chem 93:57–77

    Article  CAS  Google Scholar 

  • Jiang WT, Chang PH, Wang YS, Tsai Y, Jean JS, Li Z, Krukowski K (2013) Removal of ciprofloxacin from water by birnessite. J Hazard Mat 250–251:362–369

    Article  Google Scholar 

  • Lin Q, Li B, Liu X, Zhang B, Xu S (2022) Insights into sorption and leaching behavior of sulfadiazine in soil as affected by humic acid. J Soil Sediment 22(3):809–817

    Article  CAS  Google Scholar 

  • Lyu J, Yang L, Zhang L, Ye B, Wang L (2020) Antibiotics in soil and water in China–a systematic review and source analysis. Environ Pollut 266:115147

    Article  PubMed  Google Scholar 

  • Ma J, Guo H, Lei M, Wan X, Zhang H, Feng X (2016) Blocking effect of colloids on arsenate adsorption during co-transport through saturated sand columns. Environ Pollut 213:638–647

    Article  CAS  PubMed  Google Scholar 

  • Ma N, Tong L, Li Y, Yang C, Tan Q, He J (2022) Distribution of antibiotics in lake water-groundwater - Sediment system in Chenhu Lake area. Environ Res 204:112343

    Article  CAS  PubMed  Google Scholar 

  • Meng Y, Liu W, Fiedler H, Zhang J, Wei X, Liu X, Peng M, Zhang T (2021) Fate and risk assessment of emerging contaminants in reclaimed water production processes. Front Env Sci Eng 15(5):104

    Article  CAS  Google Scholar 

  • Molnar IL, Johnson WP, Gerhard JI, Willson CS, O’Carroll DM (2015) Predicting colloid transport through saturated porous media: a critical review. Water Resour Res 51(9):6804–6845

    Article  ADS  Google Scholar 

  • Pan M, Chu LM (2017) Transfer of antibiotics from wastewater or animal manure to soil and dedible crops. Environ Pollut 231:829–836

    Article  CAS  PubMed  Google Scholar 

  • Pang L, Close ME, Noonan MJ, Flintoft MJ, Brink PVD (2005) Heavy metals in the environment a laboratory study of bacteria-facilitated cadmium transport in alluvial gravel aquifer media. J Environ Qual 34:237–247

    Article  CAS  PubMed  Google Scholar 

  • Petosa AR, Jaisi DP, Quevedo IR, Elimelech M, Tufenkji N (2010) Aggregation and deposition of engineered nanomaterials in aquatic environments: role of physicochemical interactions. Environ Sci Technol 44(17):6532–6549

    Article  ADS  CAS  PubMed  Google Scholar 

  • Pino-Otín MR, Ferrando N, Ballestero D, Langa E, Roig FJ, Terrado EM (2022) Impact of eight widely consumed antibiotics on the growth and physiological profile of natural soil microbial communities. Chemosphere 305:135473

    Article  PubMed  Google Scholar 

  • Riaz L, Mahmood T, Khalid A, Rashid A, Siddique MBA, Kamal A, Coyne MS (2018) Fluoroquinolones (FQs) in the environment: a review on their abundance, sorption and toxicity in soil. Chemosphere 191:704–720

    Article  ADS  CAS  PubMed  Google Scholar 

  • Roca Jalil ME, Baschini M, Sapag K (2015) Influence of pH and antibiotic solubility on the removal of ciprofloxacin from aqueous media using montmorillonite. Appl Clay Sci 114:69–76

    Article  CAS  Google Scholar 

  • Sasidharan S, Torkzaban S, Bradford SA, Dillon PJ, Cook PG (2014) Coupled effects of hydrodynamic and solution chemistry on long-term nanoparticle transport and deposition in saturated porous media. Colloid Surface A 457:169–179

    Article  CAS  Google Scholar 

  • Shen C, Wu L, Zhang S, Ye H, Li B, Huang Y (2014) Heteroaggregation of microparticles with nanoparticles changes the chemical reversibility of the microparticles’ attachment to planar surfaces. J Colloid Interface Sci 421:103–113

    Article  ADS  CAS  PubMed  PubMed Central  Google Scholar 

  • Shen CY, Bradford SA, Li TT, Li BG, Huang YF (2018) Can nanoscale surface charge heterogeneity really explain colloid detachment from primary minima upon reduction of solution ionic strength? J Nanopart Res 20(6):165

    Article  Google Scholar 

  • Sun Y, Pan D, Wei X, Xian D, Wang P, Hou J, Xu Z, Liu C, Wu W (2020) Insight into the stability and correlated transport of kaolinite colloid: effect of pH, electrolytes and humic substances. Environ Pollut 266:115189

    Article  CAS  PubMed  Google Scholar 

  • Tolls J (2001) Sorption of veterinary pharmaceuticals in soils: a review. Environ Sci Technol 35(17):3397–3406

    Article  ADS  CAS  PubMed  Google Scholar 

  • Torkzaban S, Kim HN, Simunek J, Bradford SA (2010) Hysteresis of colloid retention and release in saturated porous media during transients in solution chemistry. Environ Sci Technol 44(5):1662–1669

    Article  ADS  CAS  PubMed  Google Scholar 

  • Torkzaban S, Bradford SA, Vanderzalm JL, Patterson BM, Harris B, Prommer H (2015) Colloid release and clogging in porous media: effects of solution ionic strength and flow velocity. J Contam Hydrol 181:161–171

    Article  CAS  PubMed  Google Scholar 

  • Vasudevan D, Bruland GL, Torrance BS, Upchurch VG, MacKay AA (2009) pH-dependent ciprofloxacin sorption to soils: interaction mechanisms and soil factors influencing sorption. Geoderma 151:68–76

    Article  ADS  CAS  Google Scholar 

  • Voice TC, Weber WJ (1985) Sorbent concentration effects in liquid/solid portioning. Environ Sci Technol 19:789–796

    Article  ADS  CAS  PubMed  Google Scholar 

  • Wang S, Wang H (2015) Adsorption behavior of antibiotic in soil environment: a critical review. Front Env Sci Eng 9(4):565–574

    Article  MathSciNet  CAS  Google Scholar 

  • Wang CJ, Li Z, Jiang WT (2011) Adsorption of ciprofloxacin on 2:1 dioctahedral clay minerals. Appl Clay Sci 53:723–728

    Article  CAS  Google Scholar 

  • Wang Y, Bradford SA, Shang JY (2020) Release of colloidal biochar during transient chemical conditions: The humic acid effect. Environ Pollut 260:114068

  • Wu Q, Li Z, Hong H, Yin K, Tie L (2010) Adsorption and intercalation of ciprofloxacin on montmorillonite. Appl Clay Sci 50:204–211

    Article  CAS  Google Scholar 

  • Wu Q, Li Z, Hong H, Li R, Jiang WT (2013) Desorption of ciprofloxacin from clay mineral surfaces. Water Res 47:259–268

    Article  CAS  PubMed  Google Scholar 

  • Wu M, Zhao S, Jing R, Shao Y, Liu X, Lv F, Hu X, Zhang Q, Meng Z, Liu A (2019) Competitive adsorption of antibiotic tetracycline and ciprofloxacin on montmorillonite. Appl Clay Sci 180:105175

    Article  CAS  Google Scholar 

  • Yang W, Feng T, Flury M, Li B, Shang J (2020) Effect of sulfamethazine on surface characteristics of biochar colloids and its implications for transport in porous media. Environ Pollut 256:113482

    Article  CAS  PubMed  Google Scholar 

  • Yin Z, Lin Q, Xu S (2021) Using hydrochemical signatures to characterize the long-period evolution of groundwater information in the Dagu River Basin. China Front Eviron Sci Eng 15(5):105

    CAS  Google Scholar 

  • Zhang H, Lu T, Zhang R, Wang M, Krishnan S, Liu S, Zhou Y, Li D, Qi Z (2020) Effects of clay colloids on ciprofloxacin transport in saturated quartz sand porous media under different solution chemistry conditions. Ecotox Environ Safe 199:110754

    Article  CAS  Google Scholar 

  • Zhang H, Zhao F, Xia M, Wang F (2021) Microscopic adsorption mechanism of montmorillonite for common ciprofloxacin emerging contaminant: molecular dynamics simulation and multiwfn wave function analysis. Colloid Surface A 614:126186

    Article  CAS  Google Scholar 

  • Zhao LX, Hou WG (2012) The effect of sorbent concentration on the partition coefficient of pollutants between aqueous and particulate phases. Colloid Surface A 396:29–34

    Article  ADS  CAS  Google Scholar 

  • Zhao W, Guo Y, Lu S, Yan P, Sui Q (2016) Recent advances in pharmaceuticals and personal care products in the surface water and sediments in China. Front Env Sci Eng 10(6):2

    Article  Google Scholar 

  • Zhao F, Yang L, Tang J, Fang L, Yu X, Li M, Chen L (2023) Urbanization–land-use interactions predict antibiotic contamination in soil across urban–rural gradients. Sci Total Environ 867:161493

    Article  ADS  CAS  PubMed  Google Scholar 

  • Zou Y, Zheng W (2013) Modeling manure colloid-facilitated transport of the weakly hydrophobic antibiotic florfenicol in saturated soil columns. Environ Sci Technol 47:5185–5192

    Article  ADS  CAS  PubMed  Google Scholar 

Download references

Funding

This work was financially supported by the National Natural Science Foundation of China (No. 41807010) and the Natural Science Foundation of Shandong Province (ZR2023MD043).

Author information

Authors and Affiliations

  1. Department of Environmental Science and Engineering, Qingdao University, Qingdao, 266071, China

    Qing Lin, Jiaqi Gong, Xiaowen Liu, Shuhua Ji & Shaohui Xu

Authors
  1. Qing Lin
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Jiaqi Gong
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Xiaowen Liu
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Shuhua Ji
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Shaohui Xu
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

QL designed the study and wrote the manuscript; JQG conducted the data analysis of sorption and transport experiments; XWL conducted sorption and transport experiments; SHJ conducted the modeling; and SHX provided advice on the design of the research and reviewed the manuscript. All authors read and approved the final manuscript.

Corresponding author

Correspondence to Qing Lin.

Ethics declarations

Ethics approval and consent to participate

Not applicable.

Consent for publication

Not applicable.

Competing interests

The authors declare no competing interests.

Additional information

Responsible editor: Mohammad Valipour

Publisher's Note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary Information

Below is the link to the electronic supplementary material.

Supplementary file1 (DOCX 1031 KB)

Rights and permissions

Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Lin, Q., Gong, J., Liu, X. et al. Different co-transport forms of ciprofloxacin with montmorillonite colloids in porous media as affected by pH and cations. J Soils Sediments 24, 1124–1138 (2024). https://doi.org/10.1007/s11368-024-03716-x

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11368-024-03716-x

Keywords

Search

Navigation