Transport of citrate-coated silver nanoparticles in saturated porous media

  • Myunghee Lim
  • Gukhwa Hwang
  • Sujin Bae
  • Min-Hee Jang
  • Sowon Choi
  • Hyunjung KimEmail author
  • Yu Sik HwangEmail author
Original Paper


In this study, the influences of physical and chemical factors [e.g., ionic strength (IS), pH, and flow rate] on the fate and transport of citrate-coated silver nanoparticles (AgNPs) were investigated through experiments using saturated columns. For the transport behavior of AgNPs under various conditions, retardation was confirmed with an increase in ionic strength (IS) while early elution developed with an increase in pH and flow rate. These transport experiment outcomes were simulated through Hydrus-1D, and the observed breakthrough curves were confirmed to have a significant correlation with the fitted results. Interestingly, the AgNPs and quartz sand used in this study showed a negative charge in the investigated experimental conditions. Although the reaction between AgNPs and quartz sand was expected to be unfavorable, AgNPs were observed to have been deposited onto the sand surface during the column test. To clarify the mechanism of the deposition of AgNPs even in unfavorable conditions, the interaction energy profiles were calculated based on the Derjaguin–Landau–Verwey–Overbeek (DLVO) theory. From the results, unfavorable interactions were expected in the NP–NP and NP–sand interactions in every condition. It was concluded that the deposition of AgNPs onto the sand surface under the unfavorable conditions in this study was mainly because of the physical roughness of the sand surface. Moreover, this hypothesis was supported by the zone of influence calculation in accordance with IS, the interpretation results of the fractional sand surface coverage in accordance with concentration changes of AgNPs, and series column tests.


Nanoparticles Transport Deposition Surface roughness 



This study was supported by the research project for site-specific risk assessment funded by the Korea Institute of Toxicology (KIT). This work was also supported by Korea Environment Industry & Technology Institute (KEITI) through The Chemical Accident Prevention Technology Development Project, funded by Korea Ministry of Environment (MOE) (2018001970001).


  1. Bai, C., Eskridge, K. M., & Li, Y. (2013). Analysis of the fate and transport of nC60 nanoparticles in the subsurface using response surface methodology. Journal of Contaminant Hydrology, 152, 60–69.CrossRefGoogle Scholar
  2. Bendersky, M., & Davis, J. M. (2011). DLVO interaction of colloidal particles with topographically and chemically heterogeneous surfaces. Journal of Colloid and Interface Science, 353, 87–97.CrossRefGoogle Scholar
  3. Bergström, L. (1997). Hamaker constants of inorganic materials. Advances in Colloid and Interface Science, 70, 125–169.CrossRefGoogle Scholar
  4. Bradford, S. A., Yates, S. R., Bettahar, M., & Simunek, J. (2002). Physical factors affecting the transport and fate of colloids in saturated porous media. Water Resources Research, 38, 1327.CrossRefGoogle Scholar
  5. Brunetti, G., Donner, E., Laera, G., Sekine, R., Scheckel, K. G., Khaksar, M., et al. (2015). Fate of zinc and silver engineered nanoparticles in sewerage networks. Water Research, 77, 72–84.CrossRefGoogle Scholar
  6. Cai, L., Tong, M., Wang, X., & Kim, H. (2014). Influence of clay particles on the transport and retention of titanium dioxide nanoparticles in quartz sand. Environmental Science and Technology, 48, 7323–7332.CrossRefGoogle Scholar
  7. Camesano, T. A., Unice, K. M., & Logan, B. E. (1999). Blocking and ripening of colloids in porous media and their implications for bacterial transport. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 160, 291–307.CrossRefGoogle Scholar
  8. Chowdhury, I., Hong, Y., Honda, R. J., & Walker, S. L. (2011). Mechanisms of TiO2 nanoparticle transport in porous media: Role of solution chemistry, nanoparticle concentration, and flowrate. Journal of Colloid and Interface Science, 360, 548–555.CrossRefGoogle Scholar
  9. Choy, C. C., Wazne, M., & Meng, X. (2008). Application of an empirical transport model to simulate retention of nanocrystalline titanium dioxide in sand columns. Chemosphere, 71, 1794–1801.CrossRefGoogle Scholar
  10. Cullen, E., O’Carroll, D. M., Yanful, E. K., & Sleep, B. (2010). Simulation of the subsurface mobility of carbon nanoparticles at the field scale. Advances in Water Resources, 33, 361–371.CrossRefGoogle Scholar
  11. Duffadar, R. D., & Davis, J. M. (2007). Interaction of micrometer-scale particles with nanotextured surfaces in shear flow. Journal of Colloid and Interface Science, 308(1), 20–29.CrossRefGoogle Scholar
  12. El Badawy, A. M., Aly Hassan, A., Scheckel, K. G., Suidan, M. T., & Tolaymat, T. M. (2013). Key factors controlling the transport of silver nanoparticles in porous media. Environmental Science and Technology, 47, 4039–4045.CrossRefGoogle Scholar
  13. Gliga, A. R., Skoglund, S., Wallinder, I. O., Fadeel, B., & Karlsson, H. L. (2014). Size-dependent cytotoxicity of silver nanoparticles in human lung cells: the role of cellular uptake, agglomeration and Ag release. Particle and Fibre Toxicology, 11, 11.CrossRefGoogle Scholar
  14. Gregory, J. (1981). Approximate expressions for retarded van der Waals interaction. Journal of Colloid and Interface Science, 83, 138–145.CrossRefGoogle Scholar
  15. Han, Y., Hwang, G., Kim, D., Bradford, S. A., Lee, B., Eom, I., et al. (2016). Transport, retention, and long-term release behavior of ZnO nanoparticle aggregates in saturated quartz sand: Role of solution pH and biofilm coating. Water Research, 90, 247–257.CrossRefGoogle Scholar
  16. Han, Y., & Kim, H. (2012). Surface modification of calcium carbonate with cationic polymer and their dispersibility. Materials Transactions, 53, 2195–2199.CrossRefGoogle Scholar
  17. Haznedaroglu, B., Kim, H., Bradford, S., & Walker, S. (2009). Relative transport behavior of Escherichia coli O157: H7 and Salmonella enterica serovar pullorum in packed bed column systems: Influence of solution chemistry and cell concentration. Environmental Science and Technology, 43, 1838–1844.CrossRefGoogle Scholar
  18. Hwang, G., Gomez-Flores, A., Bradford, S. A., Choi, S., Jo, E., Kim, S. B., et al. (2018). Analysis of stability behavior of carbon black nanoparticles in ecotoxicological media: Hydrophobic and steric effects. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 554, 306–316.CrossRefGoogle Scholar
  19. Jaisi, D. P., Saleh, N. B., Blake, R. E., & Elimelech, M. (2008). Transport of single-walled carbon nanotubes in porous media: Filtration mechanisms and reversibility. Environmental Science and Technology, 42, 8317–8323.CrossRefGoogle Scholar
  20. Jiang, X., Tong, M., Lu, R., & Kim, H. (2012). Transport and deposition of ZnO nanoparticles in saturated porous media. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 401, 29–37.CrossRefGoogle Scholar
  21. Kang, J. K., Yi, I. G., Park, J. A., Kim, S. B., Kim, H., Han, Y., et al. (2015). Transport of carboxyl-functionalized carbon black nanoparticles in saturated porous media: Column experiments and model analyses. Journal of Contaminant Hydrology, 177, 194–205.CrossRefGoogle Scholar
  22. Kiser, M., Westerhoff, P., Benn, T., Wang, Y., Perez-Rivera, J., & Hristovski, K. (2009). Titanium nanomaterial removal and release from wastewater treatment plants. Environmental Science and Technology, 43, 6757–6763.CrossRefGoogle Scholar
  23. Kosmulski, M., Eriksson, P., Brancewicz, C., & Rosenholm, J. B. (2000). Zeta potentials of monodispersed, spherical silica particles in mixed solvents as a function of cesium chloride concentration. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 162, 37–48.CrossRefGoogle Scholar
  24. Kuhnen, F., Barmettler, K., Bhattacharjee, S., Elimelech, M., & Kretzschmar, R. (2000). Transport of iron oxide colloids in packed quartz sand media: monolayer and multilayer deposition. Journal of Colloid and Interface Science, 231, 32–41.CrossRefGoogle Scholar
  25. Li, L., Hartmann, G., Doblinger, M., & Schuster, M. (2013). Quantification of nanoscale silver particles removal and release from municipal wastewater treatment plants in Germany. Environmental Science and Technology, 47, 7317–7323.CrossRefGoogle Scholar
  26. Li, M., He, L., Zhang, M., Liu, X., Tong, M., & Kim, H. (2019). Cotransport and deposition of iron oxides with different sized-plastic particles in saturated quartz sand. Environmental Science and Technology, 53, 3547–3557.CrossRefGoogle Scholar
  27. Li, Y., Wang, Y., Pennell, K. D., & Abriola, L. M. (2008). Investigation of the transport and deposition of fullerene (C60) nanoparticles in quartz sands under varying flow conditions. Environmental Science and Technology, 42, 7174–7180.CrossRefGoogle Scholar
  28. Li, X., Zhang, P., Lin, C., & Johnson, W. P. (2005). Role of hydrodynamic drag on microsphere deposition and re-entrainment in porous media under unfavorable conditions. Environmental Science and Technology, 39, 4012–4020.CrossRefGoogle Scholar
  29. Liang, Y., Bradford, S. A., Simunek, J., Vereecken, H., & Klumpp, E. (2013). Sensitivity of the transport and retention of stabilized silver nanoparticles to physicochemical factors. Water Research, 47, 2572–2582.CrossRefGoogle Scholar
  30. Lim, M., Bae, S., Lee, Y.-J., Lee, S.-K., & Hwang, Y. S. (2013). Aggregation behavior of silver and TiO2 nanoparticles in aqueous environment. Journal of Korean Society of Water and Wastewater, 27, 571–579.CrossRefGoogle Scholar
  31. Lin, S., Cheng, Y., Bobcombe, Y., L. Jones, K., Liu, J., & Wiesner, M. R. (2011). Deposition of silver nanoparticles in geochemically heterogeneous porous media: predicting affinity from surface composition analysis. Environmental Science and Technology, 45, 5209–5215.CrossRefGoogle Scholar
  32. Lin, D., Tian, X., Wu, F., & Xing, B. (2010). Fate and transport of engineered nanomaterials in the environment. Journal of Environmental Quality, 39, 1896–1908.CrossRefGoogle Scholar
  33. Makselon, J., Zhou, D., Engelhardt, I., Jacques, D., & Klumpp, E. (2017). Experimental and numerical investigations of silver nanoparticle transport under variable flow and ionic strength in soil. Environmental Science and Technology, 51(4), 2096–2104.CrossRefGoogle Scholar
  34. Mattison, N. T., O’Carroll, D. M., Kerry Rowe, R., & Petersen, E. J. (2011). Impact of porous media grain size on the transport of multi-walled carbon nanotubes. Environmental Science and Technology, 45, 9765–9775.CrossRefGoogle Scholar
  35. Phenrat, T., Kim, H.-J., Fagerlund, F., Illangasekare, T., & Lowry, G. V. (2010). Empirical correlations to estimate agglomerate size and deposition during injection of a polyelectrolyte-modified Fe0 nanoparticle at high particle concentration in saturated sand. Journal of Contaminant Hydrology, 118, 152–164.CrossRefGoogle Scholar
  36. Quevedo, I. R., & Tufenkji, N. (2012). Mobility of functionalized quantum dots and a model polystyrene nanoparticle in saturated quartz sand and loamy sand. Environmental Science and Technology, 46, 4449–4457.CrossRefGoogle Scholar
  37. Shin, S., Umh, H. N., & Kim, Y. (2013). Simple analysis for interaction between nanoparticles and dye-containing vesicles as a biomimetic cell-membrane. Bulletin of the Korean Chemical Society, 34, 231–236.CrossRefGoogle Scholar
  38. Šimůnek, J., He, C., Pang, L., & Bradford, S. (2006). Colloid-facilitated solute transport in variably saturated porous media. Vadose Zone Journal, 5, 1035–1047.CrossRefGoogle Scholar
  39. Sondi, I., & Salopek-Sondi, B. (2004). Silver nanoparticles as antimicrobial agent: a case study on E. coli as a model for Gram-negative bacteria. Journal of Colloid and Interface Science, 275, 177–182.CrossRefGoogle Scholar
  40. Song, J. E., Phenrat, T., Marinakos, S., Xiao, Y., Liu, J., Wiesner, M. R., et al. (2011). Hydrophobic interactions increase attachment of gum arabic-and PVP-coated Ag nanoparticles to hydrophobic surfaces. Environmental Science and Technology, 45, 5988–5995.CrossRefGoogle Scholar
  41. Sun, T. Y., Bornhöft, N. A., Hungerbühler, K., & Nowack, B. (2016). Dynamic probabilistic modeling of environmental emissions of engineered nanomaterials. Environmental Science and Technology, 50, 4701–4711.CrossRefGoogle Scholar
  42. Sun, Y., Gao, B., Bradford, S. A., Wu, L., Chen, H., Shi, X., et al. (2015). Transport, retention, and size perturbation of graphene oxide in saturated porous media: Effects of input concentration and grain size. Water Research, 68, 24–33.CrossRefGoogle Scholar
  43. Taghavy, A., Mittelman, A., Wang, Y., Pennell, K. D., & Abriola, L. M. (2013). Mathematical modeling of the transport and dissolution of citrate-stabilized silver nanoparticles in porous media. Environmental Science and Technology, 47, 8499–8507.Google Scholar
  44. Tian, Y., Gao, B., Silvera-Batista, C., & Ziegler, K. J. (2010). Transport of engineered nanoparticles in saturated porous media. Journal of Nanoparticle Research, 12, 2371–2380.CrossRefGoogle Scholar
  45. Tosco, T., Bosch, J., Meckenstock, R. U., & Sethi, R. (2012). Transport of ferrihydrite nanoparticles in saturated porous media: role of ionic strength and flow rate. Environmental Science and Technology, 46, 4008–4015.CrossRefGoogle Scholar
  46. Tufenkji, N., & Elimelech, M. (2004). Correlation equation for predicting single-collector efficiency in physicochemical filtration in saturated porous media. Environmental Science and Technology, 38, 529–536.CrossRefGoogle Scholar
  47. Tufenkji, N., & Elimelech, M. (2005). Breakdown of colloid filtration theory: Role of the secondary energy minimum and surface charge heterogeneities. Langmuir, 21, 841–852.CrossRefGoogle Scholar
  48. Vaidyanathan, R., & Tien, C. (1989). Hydrosol deposition in granular beds—An experimental study. Chemical Engineering Communications, 81, 123–144.CrossRefGoogle Scholar

Copyright information

© Springer Nature B.V. 2019

Authors and Affiliations

  1. 1.Environmental Fate and Exposure Research GroupKorea Institute of ToxicologyJinjuRepublic of Korea
  2. 2.Department of Mineral Resources and Energy EngineeringChonbuk National UniversityJeonjuRepublic of Korea
  3. 3.Yeosu Joint Inter Agency Chemical Emergency Preparedness CenterJeollanamdoRepublic of Korea

Personalised recommendations