Adsorption Removal of Sr by Barium Impregnated 4A Zeolite (BaA) From High Radioactive Seawater Waste

Barium이 함침된 4A 제올라이트 (BaA)에 의한 고방사성해수폐액에서 Sr의 흡착 제거

  • Received : 2015.11.02
  • Accepted : 2016.01.05
  • Published : 2016.06.30


This study investigated the removal of Sr, which was one of the high radioactive nuclides, by adsorption with Barium (Ba) impregnated 4A zeolite (BaA) from high-radioactive seawater waste (HSW). Adsorption of Sr by BaA (BaA-Sr), in the impregnated Ba concentration of above 20.2wt%, was decreased by increasing the impregnated Ba concentration, and the impregnated Ba concentration was suitable at 20.2wt%. The BaA-Sr adsorption was added to the co-precipitation of Sr with $BaSO_4$ precipitation in the adsorption of Sr by 4A (4A-Sr) within BaA. Thus, it was possible to remove Sr more than 99% at m/V (adsorbent weight/solution volume)=5 g/L for BaA and m/V >20 g/L for 4A, respectively, in the Sr concentration of less than 0.2 mg/L (actual concentration level of Sr in HSW). It shows that BaA-Sr adsorption is better than 4A-Sr adsorption in for the removal capacity of Sr per unit gram of adsorbent, and the reduction of the secondary solid waste generation (spent adsorbent etc.). Also, BaA-Sr adsorption was more excellent removal capacity of Sr in the seawater waste than distilled water. Therefore, it seems to be effective for the direct removal of Sr from HSW. On the other hand, the adsorption of Cs by BaA (BaA-Cs) was mainly performed by 4A within BaA. Accordingly, it seems to be little effect of impregnated Ba into BaA. Meanwhile, BaA-Sr adsorption kinetics could be expressed the pseudo-second order rate equation. By increasing the initial Sr concentrations and the ratios of V/m, the adsorption rate constants ($k_2$) were decreased, but the equilibrium adsorption capacities ($q_e$) were increasing. However, with increasing the temperature of solution, $k_2$ was conversely increased, and $q_e$ was decreased. The activation energy of BaA-Sr adsorption was 38 kJ/mol. Thus, the chemical adsorption seems to be dominant rather than physical adsorption, although it is not a chemisorption with strong bonding form.


Strontium;Adsorption/Removal;4A zeolite;Co-precipitation of Sr with $BaSO_4$;Adsorption kinetics;High-radioactive seawater waste


  1. Report of Japanese government to the IAEA Ministerial Conference on nuclear safety, "The accident at TEPCO's Fukushima nuclear power stations", June (2011).
  2. Side event by government of Japan at 56th IAEA General Conference, "Current status of Fukushima Daiichi nuclear power station", September 17 2012.
  3. S. Koyama, "Generation and treatment of radioactive contained wastewater in the Fukushima nuclear power plant accident", CRIEPI, July 22 (2013).
  4. Tokyo Electric Power Company, "Supplementary materials related equipment for the multi nuclide removal", A specific nuclear facility assessment review meeting (The 2nd meeting), Note 4, January 24 (2013).
  5. Tokyo Electric Power Company, "Nuclide analysis results of water at water treatment facility", March 26 2013. fukushima-np/images/handouts_120326_08-e.pdf.
  6. H. Rindo, "Current status and perspective of Fukushima accident remediation", 10th Anniversary of Korean Radioactive Waste Society, Jeju, Korea, October 17 (2013).
  7. Y. Kani, M. Kamosida, and D. Watanabe, "Removal of radionuclides from wastewater at Fukushima Daiichi nuclear power plant: Desalination and adsorption methods", Hitachi Ltd. (2013).
  8. Wikipedia, "Fukushima disaster cleanup", January 2014.
  9. Tokyo Electric Power Company, "Status of contaminated water treatment and tritium at Fukushima Daiichi nuclear power station", April 22 2014.
  10. IAEA Report, "Handing and Treatment of radioactive aqueous wastes", IAEA-TECDOC-654 (1992).
  11. S. Chitra, S. Viswanathan, S.V.S. Rao, and P.K. Sinha, "Uptake of cesium and strontium by crystalline silicotitanates from radioactive waste", J. Radioanal. Nucl. Chem., 287, 955-960 (2011).
  12. E.D. Collins, D.O. Compbell, L.J. King, J.B. Knauer, and R.M. Wallace, "Evaluation of zeolite mixture for decontaminating high-activity level waste at the Three Mile Island Unit 2 nuclear power station", IAEA TC-518/4 (1984).
  13. Y. Kondo, N. Kubota, T. Abe, and K. Nagato, "Development of partitioning method: Recovery and utilization useful elements in spent fuel (Literature survey)", 8-27, 149-169, JAERI-M 91-147 (1991).
  14. J.A. Dean, "Lange's Handbook of Chemistry", 12th Edition, 4-25-4-114, McGraw-Hill Book Company, New York (1979).
  15. H. Hedstrom, H. Rameback, and C. Ekberg, "A study of the Arrhenius behavior of the co-precipitation of radium, barium, strontium sulfate", J. Radioanal. Nucl. Chem., 298(2), 847-852 (2013).
  16. A.I. Cohen and L. Gordon, "Co-precipitation in some binary sulphate systems", Talanta, 7, 195-211 (1961)
  17. J. Flouret, Y. Barre, H. Muhr, and E. Plasari, "Design of an intensified co-precipitation reactor for the treatment of liquid radioactive wastes", Chem. Eng. Sci., 77, 176-183 (2012)
  18. V. Pacary, Y. Barre, and E. Lasri, "Method for the prediction of nuclear waste solution decontamination by co-precipitation of strontium ions with barium sulphate using the experimental data obtained in nonradioactive environment", Chem. Eng. Research & Design, 88, 1142-1147 (2010).
  19. A.R. Felmy, D. Rai, and D.A. Moore, "The solubility of $(Ba,Sr)SO_4$ precipitates : Thermodynamic equilibrium and reaction path analysis", Geochemca et Cosmochimica Acta, 57(18), 4345-4363 (1993).
  20. H. Mimura and T. Kanno, "Distribution and fixation of cesium and strontium in zeolite A and Chabazite", J. Nucl. Sci. & Tech. 22(4), 284-291 (1985).
  21. J.W. Rolly, "Utilization of zeolites for the removal of radioactivity from liquid waste stream", ORNL TM-7782 (1981).
  22. M.W. Munthli, E. Johan, H. Aono, and N. Matsue, "$Cs^+$ and $Sr^{2+}$ adsorption selectivity of zeolites in relation to radioactive decontamination", J. Asian Ceramic Societies, 2015,
  23. A. Merceille, E. Weinzaepfel, Y. Barre, and A. Grandjean, "The sorption behaviour of synthetic sodium nonatitanate and zeolite A for removing radioactive strontium from aqueous wastes", Sep. and Purification Tech., 96, 81-88 (2012)
  24. D. M. Ruthven, "Principles of adsorption and adsorption process", Wiley- Interscience Press, NewYork (1984).
  25. I. Nouri, I. Ghoudbane, O. Hamadaoui, and M. Chiba, "Batch sorption dynamics and equilibrium for the removal of cadmium ions from aqueous phase using wheat barn", Hazard Mater., 149, 115-125 (2007).
  26. K. Volchek, M.Y. Miah, W. Kuang, Z. Demaleki, and F.H. Tezel, "Adsorption of cesium on cement mortar from aqueous solutions", J. Hazard Mater., 194, 331-337 (2011).
  27. Y.S. Ho and G. McKay, "Sorption of dye from aqueous solution by peat", Chem. Eng. J., 70, 115-124 (1998).
  28. B. Acemioglu, "Batch kinetic study of sorption of methylene blue by perlite" Chem. Eng. J., 106, 73-81 (2005).
  29. T. Shahwan, D. Akar, and A.E. Eroglu, "Physicochemical characterization of the retardation of aqueous $Cs^+$ ions by natural kaolinite and clinoptilolite minerals", J. Colloid and Interface Sci., 285, 9-17 (2005).
  30. N. Bektas, B. Akman, and S. Kara, "Kinetic and equilibrium studies in removing lead ions from aqueous solution by natural sepiolite", J. Hazard Mater., B112, 115-122 (2004).
  31. A. Bouzidi, F. Souahi, and S. Hanini, "Sorption behavior of cesium on Ain Oussera soil under different physicochemical conditions", J. Hazard Mater., 184, 640-646 (2010).
  32. R.C. Martinez, M.T. Olguin, and M.S. Rios, "Cesium sorption by clinoptilolite-rich tuffs in batch and fixbed systems", Desalination, 258, 164-170 (2010).

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