Influence of alpha and gamma radiolysis on Pu retention in the solvent TBP/kerosene

Gao, Yang; Zheng, Weifang; Cao, Xiaoming; Chen, Shaolei

doi:10.2478/nuka-2014-0024

Abstract

In light of the issue of radiolysis of the solvent system in PUREX process, alpha and gamma radiation stability of tributyl phosphate (TBP)/kerosene (OK) have been studied in this paper, in which 238Pu dissolved in the organic phase and ⁶⁰Co are selected as alpha and gamma irradiation sources, respectively. The amount of the degradation products not easily removed after the washing process has been measured by the plutonium retention. The effects of the absorbed dose, the TBP volume fraction, the cumulative absorbed dose and the presence of UO₂²⁺ and Zr⁴⁺ on the radiolysis of the solvents have been investigated. The results have indicated that the Pu retention increases with the increase of the absorbed dose after alpha or gamma irradiation, and is larger for the solvent containing less TBP. There is competition between UO₂²⁺ and Pu⁴⁺ to complex with the degradation products, and Zr⁴⁺ accelerates the radiolysis of the system.

References

1. Mincher, B. J., Modolo, G., & Mezyk, S. P. (2009). The effects of radiation chemistry on solvent extraction: 1. Conditions in acidic solution and a review of TBP radiolysis. Solvent Extr. Ion Exch., 27(1), 1-25. DOI: 10.1080/07366290802544767.10.1080/07366290802544767
Search in Google Scholar
2. Tahraoui, A., & Morris, J. H. (1995). Decomposition of solvent extraction media during nuclear reprocessing: Literature review. Sep. Sci. Technol., 30(13), 2603-2630. DOI: 10.1080/01496399508013706.10.1080/01496399508013706
Search in Google Scholar
3. Schulz, W. W., & Navratil, J. D. (1987). Science and technology of tributyl phosphate. Boca Raton, FL, USA: CRC Press, Inc.
Search in Google Scholar
4. Burr, J. G. (1958). The radiolysis of tributyl phosphate. Radiat. Res., 8(3), 214-221. DOI: 10.2307/3570477. 10.2307/3570477
Search in Google Scholar
5. Burger, L. L., & McClanahan, E. D. (1958). Gamma radiolysis. Tributyl phosphate and its diluent systems. Ind. Eng. Chem., 50(2), 153-156. DOI: 10.1021/ ie50578a025.
Search in Google Scholar
6. Wagner, R. M., Kinderman, E. M., & Towle, L. H. (1959). Radiation stability of organophosphorus compounds. Ind. Eng. Chem., 51(1), 45-46. DOI: 10.1021/ie50589a033.10.1021/ie50589a033
Search in Google Scholar
7. Wilkinson, R. W., & Williams, T. F. (1961). The radiolysis of tri-n-alkyl phosphates. J. Chem. Soc., 4098-4107. DOI: 10.1039/JR9610004098.10.1039/jr9610004098
Search in Google Scholar
8. Hardy, C. J., & Scargill, D. (1961). Studies on monoand di-n-butylphosphoric acids-III. The extraction of zirconium from nitrate solution by di-n-butylphosphoric acid. J. Inorg. Nucl. Chem., 17(3/4), 337-349. DOI: 10.1016/0022-1902(61)80160-7.10.1016/0022-1902(61)80160-7
Search in Google Scholar
9. Haase, K. D., Schulte-Frohlinde, D., Kouřīm, P., & Vacek, K. (1973). Low-temperature radiolysis of organic phosphates studied by electron spin resonance. Int. J. Radiat. Phys. Chem., 5(4), 351-360. DOI: 10.1016/0020-7055(73)90060-0.10.1016/0020-7055(73)90060-0
Search in Google Scholar
10. Jin, H., Wu, J., Zhang, X., Fang, X., Yao, S., Zuo, Z., & Lin, N. (1999). The examination of TBP excited state by pulse radiolysis. Radiat. Phys. Chem., 54(3), 245-251. DOI: 10.1016/S0969-806X(98)00198-4.10.1016/S0969-806X(98)00198-4
Search in Google Scholar
11. Canva, J. (1965). Effects of protection and of sensibilization in the radiolytic decomposition of phosphate tributyl. Radiochim. Acta, 4(2), 88-91. DOI: 10.1524/ract.1965.4.2.88.10.1524/ract.1965.4.2.88
Search in Google Scholar
12. Barelko, E. P., Solyanina, I. P., & Tsvetkova, Z. I. (1966). Radiation-chemical stability of TBP in solutions of hydrocarbons. Atom. Energy, 21(4), 946-950. DOI: 10.1007/BF01885923.10.1007/BF01885923
Search in Google Scholar
13. Bellido, A. V., & Rubenich, M. N. (1984). Infl uence of the diluents on the radiolytic degradation of TBP in TBP, 30%(v/v)-diluent-HNO3 systems. Radiochim. Acta, 36(1/2), 61-64. DOI: 10.1524/ ract.1984.36.12.61.10.1524/ract.1984.36.12.61
Search in Google Scholar
14. Blanco, R. E., Blake, C. A. Jr., Davis, W. Jr., & Rainey, R. H. (1963). Survey of recent developments in solvent extraction with tributyl phosphate. Oak Ridge: Oak Ridge National Laboratory. (ORNL-TM-527).10.2172/4755206
Search in Google Scholar
15. Egorov, G. F., Tkhorzhnitskii, G. P., Zilberman, B. Ya., Shmidt, O. V., & Goletskii, N. D. (2005). Radiation chemical behavior of tributyl phosphate, dibutylphosphoric acid, and its zirconium salt in organic solutions and two-phase systems. Radiochemistry, 47(4), 392-397. DOI: 10.1007/s11137-005-0108-4.10.1007/s11137-005-0108-4
Search in Google Scholar
16. Stieglitz, L., & Becker, R. (1985). Chemische und radiolytische Solventzersetzung im PUREX-prozeß. Kerntechnik, 46, 76-80.
Search in Google Scholar
17. Brodda, B. G., & Heinen, D. (1977). Solvent performance in THTR nuclear fuel reprocessing. Part II. On the formation of dibutyl phosphoric acid by radiolytic and hydrolytic degradation of the TBP-n-paraffi n extractant. Nucl. Technol., 34(3), 428-437.
Search in Google Scholar
18. Peterman, D. R., Mincher, B. J., Riddle, C. L., & Tillotson, R. D. (2010). Summary report on gamma radiolysis of TBP/n-dodecane in the presence of nitric acid using the radiolysis/hydrolysis test loop. Idaho Falls: Idaho National Laboratory. (INL/EXT-10-19866).10.2172/993164
Search in Google Scholar
19. Aneheim, E., Ekberg, C., Fermvik, A., Foreman, M. R. St. J., Grüner, B., Hájková, Z., & Kvičalová, M. (2011). A TBP/BTBP-based GANEX separation process - Part 2: Ageing, hydrolytic, and radiolytic stability. Solvent Extr. Ion Exch., 29(2), 157-175. DOI: 10.1080/07366299.2011.539462.10.1080/07366299.2011.539462
Search in Google Scholar
20. Becker, R., Stieglitz, L., & Bautz, H. (1983). Untersuchung der strahlenchemischen TBP-Zersetzung unter den Bedingungen des PUREX-Prozesses. Karlsruhe: Kernforschungszentrum. (KfK-3639).
Search in Google Scholar
21. Tallent, O. K., Mailen, J. C., & Pannell, K. D. (1980). Purex diluent degradation. Oak Ridge: Oak Ridge National Laboratory. (ORNL/TM-8814).
Search in Google Scholar
22. Baroncelli, F., & Grossi, G. (1965). The complexing power of hydroxamic acids and its effect on the behaviour of organic extractants in the reprocessing of irradiated fuels. I. The complexes between benzohydroxamic acid and zirconium, iron(III) and uranium(VI). J. Inorg. Nucl. Chem., 27(5), 1085-1092. DOI: 10.1016/0022-1902(65)80420-1.10.1016/0022-1902(65)80420-1
Search in Google Scholar
23. Becker, R., Baumgartner, F., & Stieglitz, L. (1977). Identifi cation of complexing radiolytic products of the purex systems (20% TBP-dodecane-HNO3). Karlsruhe: Kernforschungszentrum. (KfK-2304).
Search in Google Scholar
24. Becker, R., & Stieglitz, L. (1973). Untersuchung der Zersetzungsprodukte im System 20% vol. Tributylphosphat- Dodekan-Salpetersäure. Karlsruhe: Kernforschungszentrum. (KfK-1373).
Search in Google Scholar
25. Barney, S. G., & Bouse, D. G. (1977). Alpha radiolysis of tributyl phosphate-effect of diluents. Richland, WA: Atlantic Richfi eld Hanford Company. (ARH-ST-153).10.2172/7300558
Search in Google Scholar
26. Lloyd, M. H., & Fellows, R. L. (1985). Alpha radiolysis and other factors affecting hydrolysis of tributyl phosphate. Oak Ridge: Oak Ridge National Laboratory. (ORNL/TM-9565).10.2172/5534740
Search in Google Scholar
27. Cong, H. F., Li, H. B., Su, Z., Yuan, J. Q., Liu, Z. Y., Song, F. L., Wang, X. R., & Lin, C. S. (2013). α-Radiolysis behavior of 30% TBP-kerosene-HNO3 extraction system I. Analysis of DBP and MBP in radiolysis products. J. Nucl. Radiochem., 35(4), 222-227. DOI: 10.7538/hhx.2013.35.04.0222.
Search in Google Scholar
28. Su, Z., Li, H. B., Cong, H. F., Song, F. L., Yuan, J. Q., Liu, Z. Y., Wang, X. R., & He, H. (2013). α-Radiolysis behavior of 30% TBP-kerosene-HNO3 extraction system II. Formation of carbonyl compounds of solvent radiolysis. J. Nucl. Radiochem., 35(5), 270-274. DOI: 10.7538/hhx.2013.35.05.0270.
Search in Google Scholar
29. Fermvik, A. (2011). Comparison of the effect of alpha and gamma radiolysis on the extraction of americium by C5-BTBP in cyclohexanone. J. Radioanal. Nucl. Chem., 289(3), 811-817. DOI: 10.1007/s10967-011-1163-2.10.1007/s10967-011-1163-2
Search in Google Scholar
30. Mincher, B. J., Mezyk, S. P., Groenewold, G., & Elias, G. (2011). A comparison of the alpha and gamma radiolysis of CMPO. Idaho Falls: Idaho National Laboratory. (INL/EXT-11-22543).10.2172/1027928
Search in Google Scholar
31. Mezyk, S. P., Mincher, B. J., Ekberg, C., & Skarnemark, G. (2013). Alpha and gamma radiolysis of nuclear solvent extraction ligands used for An(III) and Ln(III) separations. J. Radioanal. Nucl. Chem., 296(2), 711-715. DOI: 10. 1007/s10967-012-2036-z.10.1007/s10967-012-2036-z
Search in Google Scholar
32. Sharpe, P. H. G., Miller, A., & Bjergbakke, E. (1990). Dose rate effects in the dichromate dosimeter. Int. J. Radiat. Appl. Instrum., Part C Radiat. Phys. Chem., 35(4/6), 757-761. DOI: 10.1016/1359-0197(90)90311-5.10.1016/1359-0197(90)90311-5
Search in Google Scholar
33. Gao, Y., Zheng, W. F., Cao, X. M., & Chen, S. L. (2014). Gamma and alpha radiolysis of TBP solvent. Nucl. Sci. Tech., 25, S10310. DOI: 10.13538/j.1001-8042/nst.25.S10310.
Search in Google Scholar

Influence of alpha and gamma radiolysis on Pu retention in the solvent TBP/kerosene

Abstract

Paradigm

My account