Skip to main content
Log in

Adsorption of Eu(III) from Aqueous Solutions of Zn,Al- and Mg,Al-Layered Double Hydroxides, Intercalated by Citrate Ions, and Their Magnetic Forms

  • PHYSICAL CHEMISTRY OF WATER TREATMENT PROCESSES
  • Published:
Journal of Water Chemistry and Technology Aims and scope Submit manuscript

Abstract

We studied the adsorption extraction of Eu(III) from aqueous media by Zn,Al- and Mg,Al-layered double hydroxides (LDHs), intercalated by citrate ions, and their composites with magnetic properties. Cations typical of natural waters (Na+, K+, Ca2+, Mg2+) do not affect the efficiency of water purification from Eu(III), and humic acids even increase it when using composite materials. The following conditions for the extraction of Eu(III) were determined: pH of the aqueous medium, adsorption kinetics, adsorbent dose, and the effect of organic and inorganic macrocomponents of aqueous media. The adsorption equilibrium is achieved for the studied citrate forms of LDH and their magnetic composites after 1 h of contact of the aqueous solution with the solid phase of the adsorbents. Based on the parameters of kinetic models and linear correlation coefficients, we demonstrated that Eu(III) adsorption with these LDH forms is most reliably described by a pseudosecond order model in the entire range of adsorption durations, in contrast to the pseudofirst-order model. This indicates the prevailing mechanism for the extraction of Eu(III) due to chemisorption, and the equilibrium adsorption values calculated theoretically from the pseudosecond-order model are in good agreement with the experimental ones. The adsorption isotherms of Eu(III) on the citrate forms of Zn,Al- and Mg,Al-LDHs and their magnetic composites were processed using the Freundlich and Langmuir equations; these adsorption models satisfactorily describe the experimental data (correlation coefficients ≥0.99). The forms of the presence of Eu(III) in aqueous solutions are calculated at different pH values in the presence of citrate ions and natural organic ligands (fulvic acids). We propose the mechanism of removal of Eu(III) from aqueous media. The results give grounds to recommend the studied materials as effective adsorbents of radionuclide-complexing agents for the purification of contaminated surface water and liquid radioactive waste using adsorption technology with magnetic separation of sludge.

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

Access this article

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

Instant access to the full article PDF.

Fig. 1.
Fig. 2.
Fig. 3.
Fig. 4.

Similar content being viewed by others

REFERENCES

  1. Tarasevich, Yu.I., Prirodnye sorbenty v protsessakh ochistki vody (Use of Natural Sorbents for Water Purification), Kiev, 1981.

  2. Vasilechko, V., Grishchuk, G., Nizhnik, O., and Kalichak, Ya., Acid-modified Transcarpathian clinoptilolite as a sorbent for the extraction of trace amounts of europium (III), Visn. L’viv. Univ., Ser. Khim., 2015, no. 56-1, pp. 192–202.

  3. Shabalin, B.G., Yaroshenko, K.K., and Kolyabina, I.L., Study of 90Sr and 137Cs sorption kinetics by natural, acid and alkali-modified clinoptilolithams of the Sokirnitskoe deposit, Yad. Energ. Dovkillya, 2020, no. 1 (16), pp. 99–111.

  4. Kozhevnikova, N.M., Sorption of europium (III) ions by natural mordenite-containing tuff, Chem. Sustainable Dev., 2017, vol. 25, no. 3, pp. 285–289.

    CAS  Google Scholar 

  5. Odnovolova, A.M., Sofronov, D.S., Bryleva, E.Yu., Baumer, V.N., Mateichenko, P.V., Desenko, S.M., and Beda, A.A., Extraction of cobalt, europium, cerium, strontium, and copper from aqueous solutions by Fe2O3 and Fe3O4 particles, Sorbtsionnye Khromatogr.Protsessy, 2015, vol. 15, no. 4, pp. 523–531.

    CAS  Google Scholar 

  6. Strelko, V.V., Milyutin, V.V., Psareva, T.S., Kransov, VA., Khan, V.E., Meleshkevich, S.I., Zhuravlev, I.Z., Zakutevskii, O.I., and Yakovlev, V.I., Sorption-coagulation treatment of liquid radioactive waste uranium and transuranium elements, Probl. Bezpeki At. Elektrostn. Chornoilya, 2016, no. 26, pp. 96–102.

  7. Veleshko, I.E., Veleshko, A.N., Rumyantseva, E.V., Rozanov, K.V., Budantseva, N.A., Gal’braikh, L.S., and Dmitrieva, N.A., Sorption of radionuclides by chitin-melanin glucan complex of mycoton, Khim. Rastit. Syr’ya, 2011, no. 4, pp. 39–48.

  8. Zakutevskii, O.I., Psareva, T.S., and Strelko, V.V., Sorption of U(VI) Ions on sol-gel-synthesized amorphous spherically granulated titanium phosphates, Russ. J. Appl. Chem., 2012, vol. 85, no. 9, pp. 1366–1370.

    Article  Google Scholar 

  9. Strelko, V.V., Milyutin, V.V., Gelis, V.M., Psareva, T.S., Zhuravlev, I.Z., Shaposhnikova, T.A., Mil’grandt, V.G., and Bortun, A.I., Sorption of cesium radionuclides onto semicrystalline alkali metal silicotitanates, Radiochemistry, 2015, vol. 57, no. 1, pp. 73–78.

    Article  CAS  Google Scholar 

  10. Kameda, T., Takeuchi, H., and Yoshioka, T., Kinetics of uptake of Cu2+ and Cd2+ by Mg–Al layered double hydroxides intercalated with citrate, malate, and tartrate, Colloids Surf., A, 2010, vol. 355, pp. 172–177.

    Article  CAS  Google Scholar 

  11. Pshinko, G.N., Kosorukov, A.A., Puzyrnaya, L.N., and Goncharuk, V.V., Layered double hydroxides intercalated with EDTA as effective sorbents for U(VI) recovery from wastewater, Radiochemistry, 2011, vol. 53, no. 3, pp. 303–307.

    Article  CAS  Google Scholar 

  12. Kosorukov, A.A., Pshinko, G.N., Puzyrnaya, L.N., and Kobets, S.A., Extraction of U(VI) from aqueous media by layer double hydroxides intercalated by chelating agents, J. Water Chem. Technol., 2013, vol. 35, no. 3, pp. 104–111.

    Article  Google Scholar 

  13. Pavlovic, I., Pérez, M.R., Barriga, C., and Ulibarri, M.A., Adsorption of Cu2+, Cd2+ and Pb2+ ions by layered double hydroxides intercalated with the chelating agents diethylenetriaminepentaacetate and meso-2,3-dimercaptosuccinate, Appl. Clay Sci., 2009, vol. 43, no. 1, pp. 125–129.

    Article  CAS  Google Scholar 

  14. Carlino, S., The intercalation of carboxylic acids into layered double hydroxides: a critical evaluation and review of the different methods, Solid State Ionics, 1997, vol. 98, pp. 73–84.

    Article  CAS  Google Scholar 

  15. Kameda, T., Takeuchi, H., and Yoshioka, T., Uptake of heavy metal ions from aqueous solution using Mg–Al layered double hydroxides intercalated with citrate, malate, and tartrate, Sep. Purif. Technol., 2008, vol. 62, pp. 330–336.

    Article  CAS  Google Scholar 

  16. Kameda, T., Takeuchi, H., and Yoshioka, T., Hybrid inorganic/organic composites of Mg–Al layered double hydroxides intercalated with citrate, malate, and tartrate prepared by co-precipitation, Mater. Res. Bull., 2009, vol. 44, pp. 840–845.

    Article  CAS  Google Scholar 

  17. Meyn, M., Beneke, K., and Lagaly, G., Anion-exchange reactions of layered double hydroxides, Inorg. Chem., 1990, vol. 29, no. 26, pp. 5201–5207.

    Article  CAS  Google Scholar 

  18. Prevot, V., Forano, C., Besse, J. P., and Abraham, F., Syntheses and thermal and chemical behaviors of tartrate and succinate intercalated Zn3Al and Zn2Cr layered double hydroxides, Inorg. Chem., 1998, vol. 37, pp. 4293–4301.

    Article  CAS  Google Scholar 

  19. Zhang, J., Zhang, F., Ren, L., Evans, D.G., and Duan, X., Synthesis of layered double hydroxide anionic clays intercalated by carboxylate anions, Mater. Chem. Phys., 2004, vol. 85, no. 1, pp. 207–214.

    Article  CAS  Google Scholar 

  20. Reichle, W.T., Kang, S.Y., and Everhardt, D.S., The natural of the thermal decomposition of a catalytically active anionic clay mineral, J. Catal., 1986, vol. 101, pp. 352–359.

    Article  CAS  Google Scholar 

  21. Li, R., Wang, J.J., Zhou, B., et al., Enhancing phosphate adsorption by Mg/Al layered double hydroxide functionalized biochar with different Mg/Al ratios, Sci. Total Environ., 2016, vol. 559, pp. 121–129.

    Article  CAS  Google Scholar 

  22. Tronto, J., Reis, M.J.D., Silverio, F., Balbo, V.R., Marchetti, J.M., and Valim, J.B., In vitro release of citrate anions intercalated in magnesium aluminium layered double hydroxides, J. Phys. Chem. Solids, 2004, vol. 65, pp. 475–480.

    Article  CAS  Google Scholar 

  23. Puzyrnaya, L.N., Shunkov, V.S., Pshinko, G.N., and Kosorukov, A.A., Magnetic sorbents for removing U(VI) from aqueous media, Radiochemistry, 2018, vol. 60, no. 3, pp. 281–286.

    Article  CAS  Google Scholar 

  24. Shou, J., Jiang, C., Wanga, F., Qiu, M., and Xu, Q., Fabrication of Fe3O4/MgAl-layered double hydroxide magnetic composites for the effective decontamination of Co(II) from synthetic wastewater, J. Mol. Liq., 2015, vol. 207, pp. 216–223.

    Article  CAS  Google Scholar 

  25. Koilraj, P. and Sasaki, K., Fe3O4/MgAl-NO3 layered double hydroxide as a magnetically separable sorbent for the remediation of aqueous phosphate, J. Environ. Chem. Eng., 2016, vol. 4, no. 1, pp. 984–991.

    Article  CAS  Google Scholar 

  26. Zhang, X., Wang, J., Li, R., Dai, Q., Gao, R., Liu, Q., and Zhang, M., Preparation of Fe3O4C-layered double hydroxide composite for magnetic separation of uranium, Ind. Eng. Chem. Res., 2013, vol. 52, pp. 10152–10159.

    Article  CAS  Google Scholar 

  27. Zhang, X., Ji, L., Wang, J., et al., Removal of uranium(VI) from aqueous solutions by magnetic Mg–Al layered double hydroxide intercalated with citrate: kinetic and thermodynamic investigation, Colloids Surf., A, 2012, vol. 414, pp. 220–227.

    Article  CAS  Google Scholar 

  28. Mahmoud, M.R. and Someda, H.H., Mg–Al layered double hydroxide intercalated with sodium lauryl sulfate as a sorbent for 152+154Eu from aqueous solutions, J. Radioanal. Nucl. Chem., 2012, vol. 292, pp. 1391–1400.

    Article  CAS  Google Scholar 

  29. Puzyrnaya, L.N., Pshinko, G.N., Yatsik, B.P., Zub, V.Ya., and Kosorukov, A.A., Extraction of U(VI) from aqueous media with layered Zn,Al and Mg,Al double hydroxides intercalated with citrate Ions and with their magnetic nanocomposites, Radiochemistry, 2020, vol. 62, no. 1, pp. 50–61.

    Article  CAS  Google Scholar 

  30. Upor, E., Mohai, M., and Novak, G., Photometric Methods in Inorganic Trace Analysis, Amsterdam: Elsevier, 1985.

    Google Scholar 

  31. Ho, Y.S. and McKay, G., The kinetics of sorption of divalent metal ions onto sphagnum moss peat, Water Res., 2000, vol. 34, no. 3, pp. 735–742.

    Article  CAS  Google Scholar 

  32. Kornilovich, B.Yu., Mas’ko, A.N., Pshinko, G.N., and Spasenova, L.N., The effect of fulvic acids on the sorption of Eu(III) by the mineral components of soils, Radiokhimiya, 1997, vol. 39, no. 4, pp. 370–374.

    Google Scholar 

  33. Pshinko, G., Spasenova, L., and Kornilovich, B., Complexation and sorption of europium(III) ions onto clay minerals in the presence of fulvic acids, Adsorpt. Sci. Technol., 2004, vol. 22, no. 8, pp. 629–638.

    Article  Google Scholar 

Download references

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to G. N. Pshinko.

Additional information

Translated by O. Zhukova

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Pshinko, G.N., Puzyrnaya, L.N., Kosorukov, A.A. et al. Adsorption of Eu(III) from Aqueous Solutions of Zn,Al- and Mg,Al-Layered Double Hydroxides, Intercalated by Citrate Ions, and Their Magnetic Forms. J. Water Chem. Technol. 42, 79–87 (2020). https://doi.org/10.3103/S1063455X20020071

Download citation

  • Received:

  • Revised:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.3103/S1063455X20020071

Keywords:

Navigation