Abstract
Montmorillonite clay was organically modified with thoron (TH) and was employed as an adsorbent for removal of cobalt(II) radionuclides from aqueous solutions. Batch adsorption experiments, under several operational parameters such as pH, contact time, initial adsorbate concentration, adsorbent dosage, ionic strength, and temperature, were conducted to determine the optimum conditions for efficient removal of cobalt(II) radionuclides. The obtained data showed that almost complete removals were achieved for cobalt(II) at pH values ≥ 3.5 using TH-modified montmorillonite (TMM), while only 63% were obtained by unmodified clay at pH ≥ 5.4. Adsorption kinetic data of cobalt(II) were better fitted by the pseudo-second order kinetic model and its adsorption rate was controlled by film diffusion. Both Langmuir and Freundlich models had the ability to well describe the equilibrium data of cobalt(II) radionuclides at the studied temperatures. The adsorption capacity of TMM (0.85 mmol/g) was found to be not only nine times that of unmodified montmorillonite (0.097 mmol/g), but also higher than those reported in literature using various unmodified and modified clays. Thermodynamic parameters (ΔH°, ΔS°, and ΔG°) were calculated. Among the examined desorbing agents, both Al3+ and EDTA were succeeded to desorb most of cobalt(II) radionuclides (desorption % ~ 90%) loaded onto TMM. The results of this study clarified that TMM can be considered as an effective adsorbent for removal of cobalt(II) radionuclides from aqueous solutions.
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Abdul Nishad P, Bhaskarapillai A, Velmurugan S, Narasimhan SV (2012) Cobalt (II) imprinted chitosan for selective removal of cobalt during nuclear reactor decontamination. Carbohydr Polym 87:2690–2696. https://doi.org/10.1016/j.carbpol.2011.11.061
Bhattacharyya KG, Gupta SS (2006) Kaolinite, montmorillonite, and their modified derivatives as adsorbents for removal of Cu(II) from aqueous solution. Sep Purif Technol 50:388–397. https://doi.org/10.1016/j.seppur.2005.12.014
Boyd GE, Adamson AW, Myers LS (1947) The exchange adsorption of ions from aqueous solutions by organic zeolites: II. Kinetics. J Am Chem Soc 69:2836–2848 https://pubs.acs.org/doi/10.1021/ja01203a066
Chen CL, Wang XK (2007) Sorption of Th (IV) to silica as a function of pH, humic/fulvic acid, ionic strength, electrolyte type. Appl Radiat Isot 65:155–163. https://doi.org/10.1016/j.apradiso.2006.07.003
Chen L, Yu S, Liu B, Zuo L (2012) Removal of radiocobalt from aqueous solution by different sized carbon nanotubes. J Radioanal Nucl Chem 292:785–791. https://doi.org/10.1007/s10967-011-1514-z
Combernoux N, Schrive L, Labed V, Wyart Y, Carretier E, Moulin P (2017) Treatment of radioactive liquid effluents by reverse osmosis membranes: from lab-scale to pilot-scale. Water Res 123:311–320. https://doi.org/10.1016/j.watres.2017.06.062
Derakhshani E, Naghizadeh A (2018) Optimization of humic acid removal by adsorption onto bentonite and montmorillonite nanoparticles. J Mol Liq 259:76–81. https://doi.org/10.1016/j.molliq.2018.03.014
Długosz O, Banach M (2018) Kinetic, isotherm and thermodynamic investigations of the adsorption of Ag+ and Cu2+ on vermiculite. J Mol Liq 258:295–309. https://doi.org/10.1016/j.molliq.2018.03.041
Essington ME (2004) Soil and water chemistry: an integrative approach. CRC Press LLC, Boca Raton
Ezzat A, Mahmoud MR, Soliman MA, Saad EA, Kandeel A (2017) Evaluation of sorptive flotation technique for enhanced removal of radioactive Eu(III) from aqueous solutions. Radiochim Acta 105:205–213. https://doi.org/10.1515/ract-2016-2618
Ferhat M, Kadouche S, Drouiche N, Messaoudi K, Messaoudi B, Lounici H (2016) Competitive adsorption of toxic metals on bentonite and use of chitosan as flocculent coagulant to speed up the settling of generated clay suspensions. Chemosphere 165:87–93. https://doi.org/10.1016/j.chemosphere.2016.08.125
Gao Y, Shao Z, Xiao Z (2015) U(VI) sorption on illite: effect of pH, ionic strength, humic acid and temperature. J Radioanal Nucl Chem 303:867–876. https://doi.org/10.1007/s10967-014-3385-6
Ghassabzadeh H, Torab-Mostaedi M, Mohaddespour A, Maragheh MG, Ahmadi SJ, Zaheri P (2010) Characterizations of Co(II) and Pb(II) removal process from aqueous solutions using expanded perlite. Desalination 261:73–79. https://doi.org/10.1016/j.desal.2010.05.028
Giles CH, McEvan TH, Nakhwa SN, Smith D (1960) Studies in adsorption: part XI. A system of classification of solution adsorption isotherms, and its use in diagnosis of adsorption mechanisms and in measurement of specific surface areas of solids. J Chem Soc 4:3973–3993. https://doi.org/10.1039/jr9600003973
Gok O, Ozcan A, Erdem B, Ozcan AS (2008) Prediction of the kinetics, equilibrium and thermodynamic parameters of adsorption of copper(II) ions onto 8-hydroxy quinolone immobilized bentonite. Colloids Surf A Physicochem Eng Asp 317:174–185. https://doi.org/10.1016/j.colsurfa.2007.10.009
Gu P, Zhang S, Li X, Wang X, Wen T, Jehan R, Alsaedi A, Hayat T, Wang X (2018) Recent advances in layered double hydroxide-based nanomaterials for the removal of radionuclides from aqueous solution. Environ Pollut 240:493–505. https://doi.org/10.1016/j.envpol.2018.04.136
Guerra DJL, Mello I, Resende R, Silva R (2013) Application as absorbents of natural and functionalized Brazilian bentonite in Pb2+ adsorption: equilibrium, kinetic, pH, and thermodynamic effects. Water Resour Industry 4:32–50. https://doi.org/10.1016/j.wri.2013.11.001
Guo Z, Li Y, Zhang S, Niu H, Chen Z, Xu J (2011) Enhanced sorption of radiocobalt from water by Bi(III) modified montmorillonite: a novel adsorbent. J Hazard Mater 192:168–175. https://doi.org/10.1016/j.jhazmat.2011.05.004
Gupta S, Babu BV (2009) Removal of toxic metal Cr(VI) from aqueous solutions using sawdust as adsorbent: equilibrium, kinetics and regeneration studies. Chem Eng J 150:352–365. https://doi.org/10.1016/j.cej.2009.01.013
Han H, Cheng C, Hu S (2017) Facile synthesis of gelatin modified attapulgite for the uptake of uranium from aqueous solution. J Mol Liq 234:172–178. https://doi.org/10.1016/j.molliq.2017.03.076
He M, Zhu Y, Yang Y, Han B, Zhang Y (2011) Adsorption of cobalt(II) ions from aqueous solutions by palygorskite. Appl Clay Sci 54:292–296. https://doi.org/10.1016/j.clay.2011.09.013
Ho YS, McKay G (1999) Pseudo-second order model for sorption process. Process Biochem 34:451–465. https://doi.org/10.1016/S0032-9592(98)00112-5
IAEA (1981) Decontamination of operational nuclear power plants, Vienna, IAEATECDOC-248. https://inis.iaea.org/collection/NCLCollectionStore/_Public/13/680/13680247.pdf
Jiang M, Jin X, Lu X, Chen Z (2010) Adsorption of Pb(II), cd(II), Ni(II) and cu(II) onto natural kaolinite clay. Desalination 252(2010):33–39. https://doi.org/10.1016/j.desal.2009.11.005
Kebabi B, Terchi S, Bougherara H, Reinert L, Duclaux L (2017) Removal of manganese (II) by edge site adsorption on raw and milled vermiculites. Appl Clay Sci 139:92–98. https://doi.org/10.1016/j.clay.2016.12.041
Lagergren S (1898) About the theory of so-called adsorption of soluble substances. Kungl Svenska vetenskapsakademiens handlingar 241:1–39
Langmuir L (1918) Adsorption of gases on plane surfaces of glass, mica and platinum. J Am Chem Soc 40:1361–1403. https://doi.org/10.1021/ja02242a004
Lazarevic S, Jankovic-Castvan I, Potkonjak B, Janackovic D, Petrovic R (2012) Removal of Co2+ ions from aqueous solutions using iron-functionalized sepiolite. Chem Eng Process 55:40–47. https://doi.org/10.1016/j.cep.2012.01.004
Liu X, Cheng C, Xiao C, Shao D, Xu Z, Wang J, Hu S, Li X, Wang W (2017) Polyaniline (PANI) modified bentonite by plasma technique for U(VI) removal from aqueous solution. Appl Surf Sci 411:331–337. https://doi.org/10.1016/j.apsusc.2017.03.095
Mahmoud MR, Othman SH (2018) Efficient decontamination of naturally occurring radionuclide from aqueous carbonate solutions by ion flotation process. Radiochim Acta 106:465–476
Mahmoud MR, Sharaf El-deen G, Soliman MA (2014) Surfactant-impregnated activated carbon for enhanced adsorptive removal of Ce(IV) radionuclides from aqueous solutions. Ann Nucl Energy 72:134–144. https://doi.org/10.1016/j.anucene.2014.05.006
Mahmoud MR, Soliman MA, Allan KF (2015) Adsorption behavior of samarium(III) from aqueous solutions onto PAN@SDS core-shell polymeric adsorbent. Radiochim Acta 103:443–456. https://doi.org/10.1515/ract-2014-2299
Mahmoud MR, Rashad GM, Metwally E, Saad EA, Elewa AM (2017) Adsorptive removal of 134Cs+, 60Co2+ and 152+154Eu3+ radionuclides from aqueous solutions using sepiolite: single and multi-component systems. Appl Clay Sci 141:72–80. https://doi.org/10.1016/j.clay.2016.12.021
Manohar DM, Noeline BF, Anirudhan TS (2006) Adsorption performance of Al-pillared bentonite clay for the removal of cobalt(II) from aqueous phase. Appl Clay Sci 31:194–206. https://doi.org/10.1016/j.clay.2005.08.008
Marco-Brown JL, Guz L, Olivelli MS, Schampera B, Sánchez RMT, Curutchet G, Candal R (2018) New insights on crystal violet dye adsorption on montmorillonite: kinetics and surface complexes studies. Chem Eng J 333:495–504. https://doi.org/10.1016/j.cej.2017.09.172
Margerum DW, Byrd SH, Reed SA, Banks CV (1953) Preparation and properties of 2-(2-Hydroxy-3,6-disulfo-1-naphthylazo)-benzenearsonic acid (Thorin). Anal Chem 25:1219–1221 https://pubs.acs.org/doi/abs/10.1021/ac60080a022
Metwally SS, Ayoub RR (2016) Modification of natural bentonite using a chelating agent for sorption of 60Co radionuclide from aqueous solution. Appl Clay Sci 126:33–40. https://doi.org/10.1016/j.clay.2016.02.021
Mukhopadhyay R, Manjaiah KM, Datta SC, Yadav RK, Sarkar B (2017) Inorganically modified clay minerals: preparation, characterization, and arsenic adsorption in contaminated water and soil. Appl Clay Sci 147:1–10. https://doi.org/10.1016/j.clay.2017.07.017
Omar H, Arida H, Daifullah A (2009) Adsorption of 60Co radionuclides from aqueous solution by raw and modified bentonite. Appl Clay Sci 44(2009):21–26. https://doi.org/10.1016/j.clay.2008.12.013
Osmanlioglu AE (2018) Decontamination of radioactive wastewater by two-staged chemical precipitation. Nucl Eng Technol 50:886–889. https://doi.org/10.1016/j.net.2018.04.009
Petrucci RH, Harwood WS (1997) General chemistry: principles and modern applications, 7th ed. Prentice Hall, New Jersey
Rashad GM, Mahmoud MR, Elewa AM, Metwally E, Ebtissam AS (2016) Removal of radiocobalt from aqueous solutions by adsorption onto low-cost adsorbents. J Radioanal Nucl Chem 309:1065–1076. https://doi.org/10.1007/s10967-016-4726-4
Rashad GM, Soliman M, Mahmoud MR (2018) Removal of radioselenium oxyanions from aqueous solutions by adsorption onto hydrous zirconium oxide. J Radioanal Nucl Chem 317:593–603. https://doi.org/10.1007/s10967-018-5916-z
Rathnayake SI, Martens WN, Xi Y, Frost RL, Ayoko GA (2017) Remediation of Cr (VI) by inorganic-organic clay. J Colloid Interface Sci 490:163–173. https://doi.org/10.1016/j.jcis.2016.11.070
Ren X, Zhang Z, Luo H, Hu B, Dang Z, Yang C, Li L (2014) Adsorption of arsenic on modified montmorillonite. Appl Clay Sci 97–98:17–23. https://doi.org/10.1016/j.clay.2014.05.028
Shahwan T, Erten HN, Unugur S (2006) A characterization study of some aspects of the adsorption of aqueous Co2+ ions on a natural bentonite clay. J Colloid Interface Sci 300:447–452. https://doi.org/10.1016/j.jcis.2006.04.069
Sparks DL (2003) Environmental soil chemistry, second edition. Academic Press, Elsevier Science, USA
Temkin MJ, Pyzhev V (1940) Kinetics of ammonia synthesis on promoted iron catalysts. Acta Physiochim URSS 12:327–356
Unuabonah EI, Adebowale KO, Olu-Owolabi BI, Yang LZ, Kong LX (2008) Adsorption of Pb(II) and Cd (II) from aqueous solutions onto sodium tetraborate-modified kaolinite clay: equilibrium and thermodynamic studies. Hydrometallurgy 93:1–9. https://doi.org/10.1016/j.hydromet.2008.02.009
Wang G, Hua Y, Su X, Komarneni S, Ma S, Wang Y (2016) Cr(VI) adsorption by montmorillonite nanocomposites. Appl Clay Sci 124–125:111–118. https://doi.org/10.1016/j.clay.2016.02.008
Wang J, Chen Z, Shao D, Li Y, Xu Z, Cheng C, Asiri AM, Marwani HM, Hu S (2017) Adsorption of U(VI) on bentonite in simulation environmental conditions. J Mol Liq 242:678–684. https://doi.org/10.1016/j.molliq.2017.07.048
Weber WJ, Morris JC (1963) Kinetics of adsorption on carbon from solution. J Sanit Eng Div 89:31–60
Xiao Y, Huang L, Long Z, Feng Z, Wang L (2016) Adsorption ability of rare earth elements on clay minerals and its practical performance. J Rare Earths 34:543–548. https://doi.org/10.1016/S1002-0721(16)60060-1
Yao W, Yu S, Wang J, Zou Y, Lu S, Ai Y, Alharbi SN, Alsaedi A, Hayat T, Wang X (2017) Enhanced removal of methyl orange on calcined glycerol-modified nanocrystallined Mg/Al layered double hydroxides. Chem Eng J 307:476–486. https://doi.org/10.1016/j.cej.2016.08.117
Yusan S, Gok C, Erenturk S, Aytas S (2012) Adsorptive removal of thorium (IV) using calcined and flux calcined diatomite from Turkey: evaluation of equilibrium, kinetic and thermodynamic data. Appl Clay Sci 67–68:106–116. https://doi.org/10.1016/j.clay.2012.05.012
Zhu H, Xiao X, Guo Z, Han X, Liang Y, Zhang Y, Zhou C (2018) Adsorption of vanadium (V) on natural kaolinite and montmorillonite: characteristics and mechanism. Appl Clay Sci 161:310–316. https://doi.org/10.1016/j.clay.2018.04.035
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Soliman, M.A., Rashad, G.M. & Mahmoud, M.R. Organo-modification of montmorillonite for enhancing the adsorption efficiency of cobalt radionuclides from aqueous solutions. Environ Sci Pollut Res 26, 10398–10413 (2019). https://doi.org/10.1007/s11356-019-04478-7
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DOI: https://doi.org/10.1007/s11356-019-04478-7