Browse > Article

Precipitation behaviors of Cs and Re(/Tc) by NaTPB and TPPCl from a simulated fission products-$(Na_2CO_3-NaHCO_3)-H_2O_2$ solution  

Lee, Eil-Hee (Korea Atomic Energy Research Institute)
Lim, Jae-Gwan (Korea Atomic Energy Research Institute)
Chung, Dong-Yong (Korea Atomic Energy Research Institute)
Yang, Han-Beum (Korea Atomic Energy Research Institute)
Kim, Kwang-Wook (Korea Atomic Energy Research Institute)
Publication Information
Journal of Nuclear Fuel Cycle and Waste Technology(JNFCWT) / v.8, no.2, 2010 , pp. 115-122 More about this Journal
Abstract
In this study, the removal of Cs and Tc from a simulated fission products (FP) solution which were co-dissolved with U during the oxidative-dissolution of spent fuel in a mixed carbonate solution of $(Na_2CO_3-NaHCO_3)-H_2O_2$ was investigated by using a selective precipitation method. As Cs and Tc might cause an unstable behavior due to the high decay heat emission of Cs as well as the fast migration of Tc when disposed of underground, it is one of the important issues to removal them in views of the increase of disposal safety. The precipitation of Cs and Re (as a surrogate for Tc) was examined by introducing sodium tetraphenylborate (NaTPB) and tetraphenylphosponium chloride (TPPCl), respectively. Precipitation of Cs by NaTPB and that of Re by TPPCl were completed within 5 minutes. Their precipitation rates were not influenced so much by the temperature and stirring speed even if they were increased by up to $50^{\circ}C$ and 1,000 rpm. However, the pH of the solution was found to have a great influence on the precipitation with NaTPB and TPPCl. Since Mo tends to co-precipitate with Re at a lower pH, especially, it was effective that a selective precipitation of Re by TPPCl was carried out at pH of above 9 without co-precipitation of Mo and Re. Over 99% of Cs was precipitated when the ratio of [NaTPB]/[Cs]>1 and more than 99% of Re, likewise, was precipitated when the ratio of [TPPCl]/[Re]>1.
Keywords
Cs; Re; Tc; Selective precipitation; NaTPB; TPPCl; Carbonate; Solubility;
Citations & Related Records
Times Cited By KSCI : 1  (Citation Analysis)
연도 인용수 순위
1 E. H. Lee, J. K. Lim, D. Y. Chung, H. B. Yang, J. H. Yoo and K. W. Kim, "The oxidative-dissolution behaviors of fission products in a $Na_2CO_3-H_2O_2$ solution", J. Radioanal. Nucl. Chem.. 281, pp 339-346 (2009).   DOI   ScienceOn
2 J. H. Park, Y. H. Yoo, W. M. Chung, K. I. Lee, M. S. Woo and D. S. Whang, "A review on the process technology for Mo-99 production", KAERI/AR-401/94 (1994).
3 J. C. Fanning, "The solubilities of the alkali metal salts and the precipitation of Cs+ from aqueous solution", Coord. Chem. Rev., 140, pp. 27-36 (1995).   DOI   ScienceOn
4 S. M. Ponder and T. E. Mallouk, "Recovery of ammonium and cesium ions from aqueous waste streams by sodium tetraphenylborate", Ind. Eng. Chem. Res., 38, pp. 4007-4010 (1999).
5 P. Blazy, E. A. Jdid, A. Floreancig and B. Mottet, "Selective recovery of rhenium from gas-scrubbing solutions of Molybdenite roasting using direct precipitation and separation on resins", Sep. Sci. Technol., 28(11&12), pp. 2073-2096 (1993).   DOI
6 D. D. Walker and M. A. Ebra, "Nuclear waste solution", US Pat. No. 4654173 (1987).
7 E. H. Lee, J. K. Lim, D. Y. Chung, H. B. Yang and K. W. Kim, "The characteristics of an oxidative dissolution of simulated fission product oxides in $(NH_4)_2CO_3$ solution containing $H_2O_2$", J. Korean Radioactive Waste Soc., 7(2), pp. 93-100 (2009).   과학기술학회마을
8 S. Aldridge, P. Warwick, N. Evans and S. Vines, "Degradation of tetraphenylphosphonium bromide at high pH and its effect on radionuclide solubility", Chemosphere, 66, pp. 672- 676 (2007).   DOI   ScienceOn
9 C. F. Baes, Jr. and R. E. Mesmer, "Th hydrolysis of cations", Robert E. Krieger Pub. Company, Malabar, Florida (1986).
10 S. M. Peper, L. F. Brodnax, S. E. Field, R. A. Zehnder, S. N. Valdez and W. H. Runde, "Kinetic study of the oxidative dissolution of $UO_2$ in aqueous carbonate media", Ind. Eng. Chem. Res., 43, pp. 8188-8193 (2004).   DOI   ScienceOn
11 Y. Kondo, M. Kubota, T. Abe and K. Nagato, "Development of partitioning method: Recovery and utilization of useful elements in SF (Literature survey)", JAERI-M 91-147, (1991).
12 Y. Asano, N. Asanuma, T. Ito, M. Kataoka, S. Fujino, T. Yamamura, W. Sugiyama and H. Tomiyasu, "Study on a nuclear fuel reprocessing system based on the precipitation method in mild aqueous solutions", Nucl. Technol., 120, pp. 198-210 (1997).
13 N. Asanuma, M. Harada, Y. Ikeda and H. Tomiyasu, "New approach to nuclear fuel reprocessing in non-acidic aqueous solutions", J. Nucl. Sci. Technol. 38(10), pp. 866-871 (2001).   DOI   ScienceOn
14 J. A. Dean, "Lange's Handbook of Chemistry", 12th Edition, McGraw-Hill Book Company. (1979).
15 Report to Congress, "DOE spent nuclear fuel recycling program plan", US Department of Energy (2006).
16 R. A Peterson, J. O. Burgess, D. D. Walker, D. T. Hobbs, S. M. Serkiz, M. J. Barnes and A. R. Jurgensen, "Decontamination of high-level waste using a continuous precipitation process", Sep. Sci. Tech., 36(5&6), pp. 1307-1321 (2001).   DOI
17 K. W. Kim, D. Y. Chung, H. B. Yang, J. K. Lim, E. H. Lee, K. C. Song and K. S. Song, "A conceptual process study for recovery of uranium alone from spent nuclear fuel by using high alkaline carbonate media", Nucl. Tech., 166, pp. 170-179 (2009).
18 S. Rollin, K. Spahiu and U. B. Eklund, "Determination of dissolution rates of spent fuel in carbonate solutions under different redox conditions with a flow-through experiment", J. Nucl. Mater., 297, pp. 231-243 (2001).   DOI   ScienceOn
19 F. Clarens, J. de Pablo, I. Casa, J. Gimenez, M. Rovira, J. Merino, E. Cera, J. Bruno, J. Quinones and A. M. Esparza, "The oxidative dissolution of unirradiated $UO_2$ by hydrogen peroxide as a function of pH", J. Nucl. Mater., 35, pp. 225-231 (2005).
20 N. Asanuma, M. Harada, M. Nogami, K. Suzuki, T. Kikuchi, H. Tomiyasu and Y. Ikeda, "Anodic dissolution of $UO_2$ Pellet containing simulated fission products in ammonium carbonate solution", J. Nucl. Sci. Technol., 43(3), pp. 255-262 (2006).   DOI   ScienceOn
21 "The challenges and directions for nuclear energy policy in Japan, Japan's nuclear energy national plan", Ministry of Economy, Trade and Industry (METI), Japan (2006).
22 K. W. Kim, J. K. Lim, D. Y. Chung, H. B. Yang, K. C. Song, K. Y. Jee and E. H. Lee, "A process for the recovery of uranium from spent nuclear fuel by using a high alkaline carbonate solution", Korea Patent Application No. 38599 (2008)., "Process for recoverying isolated uranium from spent nuclear fuel using a highly alkaline carbonate solution", US Patent Application No. 12/337,599 (2008).