Radiolysis products and degradation mechanism studies on tri-isoamyl phosphate (TiAP)
-
Ruifen Li
,
Jinhua Wang
,
Lan Zhang
Abstract
As an alternate extractant for spent fuel reprocessing, the radiolysis properties of TiAP should be systematically studied to evaluate the feasibility of using it in engineering scale. In this paper, the irradiation stability of TiAP was investigated by using the concept of radiolysis ratio and G value. It is found the extent of radiolysis would be increased with the increasing of absorbed doses, but decreased with the increasing of pre-equilibrium aqueous HNO3 concentration. Furthermore, the radiolysis products were analyzed qualitatively and quantitatively with gas, liquid and ion chromatograph, based on which the possible radiolysis mechanism of TiAP was also concluded.
Acknowledgements
The research was funded by the Priority Research Program of the Chinese Academy of Sciences (XDA02030400).
References
1. Srinivasan, N., Balasubramanian, G. R., Chitnis, R. T., Venkateswaran, S., Kulkarni, R. T.: Laboratory studies on acid thorax process, BARC-681. BARC Report: Mumbai, (1973).Search in Google Scholar
2. Schmieder, H., Petrich, G.: Impurex: a concept for an improved purex process. Radiochim. Acta. 48, 181 (1989).10.1524/ract.1989.48.34.181Search in Google Scholar
3. Suresh, S., Subramaniam, T. G., Srinivasan, P. R., Rao, V.: Studies on U-Th separation using tri-sec-butyl phosphate. Solvent Extr. Ion Exch. 13, 415 (1995).10.1080/07366299508918283Search in Google Scholar
4. Schmieder, H., Petrich, G.: Impurex: a concept for an improved purex process. Radiochim. Acta. 48, 181 (1989).10.1524/ract.1989.48.34.181Search in Google Scholar
5. McKibben, J. M.: Chemistry of the purex process. Radiochim. Acta. 36, 3 (1984).10.1524/ract.1984.36.12.3Search in Google Scholar
6. Brahmmananda Rao, C. V. S., Srinivasan, T. G., Vasudeva Rao, P. R.: Studies on the extraction of actinides by substituted butyl phosphonates. Solvent Extr. Ion Exch. 30, 262 (2012).10.1080/07366299.2011.639250Search in Google Scholar
7. Pathak, P., Prabhu, D., Kanekar, A., Manchanda, V.: Distribution studies on Th (IV), U (VI) and Pu (IV) using tri-n-butylphosphate and N, N-dialkyl amides. Radiochim. Acta. 94, 193 (2006).10.1524/ract.2006.94.4.193Search in Google Scholar
8. Borkowski, M., Ferraro, J. R., Chiarizia, R., McAlister, D. R.: First study of third phase formation in the U(VI) or Th(IV)/HNO3TBP/alkane systems. Solvent Extr. Ion Exch. 20, 313 (2002).10.1081/SEI-120004807Search in Google Scholar
9. Chiarizia, R., Jensen, M. P., Borkowski, M., Ferraro, J. R., Thiyagarajan, P., Littrell, K. C.: Third phase formation revisited: the U(VI), HNO3-TBP, n-dodecane system. Solvent Extr. Ion Exch. 21, 1 (2003).10.1081/SEI-120017545Search in Google Scholar
10. Vasudeva Rao, P. R., Kolarik, Z.: A review of third phase formation in extraction of 361 actinides by neutral organophosphorus extractants. Solvent Extr. Ion Exch. 14, 955 (1996).10.1080/07366299608918378Search in Google Scholar
11. Suresh, S. S., Srinivasan, T. G., Vasudeva Rao, P. R.: Studies on U-Th separation using tri-sec-butyl phosphate. Solvent Extr. Ion Exch. 13, 415 (1995).10.1080/07366299508918283Search in Google Scholar
12. Natarajan, R., Raj, B.: Fast reactor fuel reprocessing technology in India. J. Nucl. Sci. Technol. 44, 393 (2007).10.1080/18811248.2007.9711299Search in Google Scholar
13. Pathak, P. N., Veeraraghavan, R., Manchanda, V. K.: Separation of uranium and thorium using tris (2-ethylhexyl) phosphate as extractant. J. Radioanal. Nucl. Chem. 240, 15 (1999).10.1007/BF02349130Search in Google Scholar
14. Suresh, A., Brahmmananda Rao, C. V. S., Srinivasulu, B., Sreenivasan, N. L., Subramaniam, S., Sabharwal, K. N., Sivaraman, N., Srinivasan, T. G., Natarajan, R., Vasudeva Rao, P. R.: Development of alternate extractants for separation of actinides. Energy Procedia 39, 120 (2013).10.1016/j.egypro.2013.07.198Search in Google Scholar
15. Sreenivasulu, B., Suresh, A., Sivaraman, N., Vasudeva Rao, P. R.: Co-extraction and co-stripping of U (VI) and Pu (IV) using tri-isoamylphosphate and tri-n-butyl phosphate in n-dodecane fromnitric acid media under high loading conditions. Radiochim. Acta. 104, 227 (2016).10.1515/ract-2015-2472Search in Google Scholar
16. Mincher, B., Modolo, G., Mezyk, S.: Review article: 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 (2009).10.1080/07366290802544767Search in Google Scholar
17. Kuno, Y., Hina, T.: Degradation of tributylphosphate inhighly radioactive liquid waste of nuclear fuel reprocessing. Radiochim. Acta. 60, 193 (1993).10.1524/ract.1993.60.4.193Search in Google Scholar
18. Neace, J. C.: Diluent degradation products in the purex solvent. Sep. Sci.Technol. 18, 1581 (1983).10.1080/01496398308056116Search in Google Scholar
19. Bellido, A., Rubenich, M.: Influence of the diluent on theradiolytic degradation of TBP in TBP, 30%(v/v)-diluent-HNO3 systems. Radiochim. Acta. 36, 61 (1984).10.1524/ract.1984.36.12.61Search in Google Scholar
20. Smith, D., Edwards, H., Hughes, M., Courtney, B.: Odorless kerosene degradation and the formation of interfacial deposits during the alkaline solvent wash in the purex process. Sep. Sci. Technol. 32, 2821 (1997).10.1080/01496399708002224Search in Google Scholar
21. Danilov, N. A., Korpusor, G. V., Vtkina, O. B.: Regularities of the extraction of rare element with triisoamyl phosphate [C]. In: Proceeding of ISEC 88, Moscow: USSR, (1988).Search in Google Scholar
22. Sreenivasulu, B., Suresh, A., Sivaraman, N., Vasudeva Rao, P.:Co-extraction and co-stripping of U (VI) and Pu (IV) using tri-isoamylphosphate and tri-n-butyl phosphate in n-dodecane fromnitric acid media under high loading conditions. Radiochim. Acta. 104, 227 (2016).10.1515/ract-2015-2472Search in Google Scholar
23. Siddall, T. H., III: Trialkyl phosphates and dialkyl alkylphosphonates in uranium and thorium extraction. J. Ind Eng Chem. 51, 41 (1959).10.1021/ie50589a032Search in Google Scholar
24. Hasan, S. H., Shukla, J. P.: Tri-iso-amyl phosphate (TAP): an alternative extractant to tri-butyl phosphate (TBP) for reactor fuel reprocessing. J. Radioanal. Nucl. Chem. 258, 563 (2003).10.1023/B:JRNC.0000011753.65662.64Search in Google Scholar
25. Liu, C., Li, R., He, S. H., Li, Z., Luo, Y., Li, Q. N., Zhang, L.: Extraction behavior of U(VII) and Th(IV) by tri-iso-amyl phosphate and tri-sec-butyl phosphate. J. Radioanal. Nucl. Chem. 36, 282 (2014) (in Chinese).Search in Google Scholar
26. Stieglitz, L., Becker, R.: Chemical and radiolytic solvent degradation in the purex process. Nukleare Entsorgung. 2, 333–350 (1983).Search in Google Scholar
27. Hardy, C. J., Scargill, D.: Studies on mono- and di-butylphosphoric acids-I. The separation of mono- and di-butylphosphoric acids by solvent extraction and by paper chromatography. J. Inorg. Nucl. Chem. 10, 323–327 (1959).10.1016/0022-1902(59)80125-1Search in Google Scholar
28. Sreenivasulu, B., Suresh, A., Rajeswari, S., Ramanathan, N., Antony, M. P., Sivaraman, N., Joseph, M.: Physicochemical properties and radiolytic degradation studies on tri-iso-amyl phosphate (TiAP). Radiochim. Acta. 105, 249 (2017).10.1515/ract-2016-2674Search in Google Scholar
29. Egorov, G. F., Tkhorzhnitskii, G. P., Zilberman, B. Y., Schmidt, O. V., Goletskii, N. D.: Radiation chemical behavior of tributyl phosphate, dibutylphosphoric acid, and its zirconium salt in organic solutions and two-phase systems. Radiochemistry 47, 359 (2005).10.1007/s11137-005-0108-4Search in Google Scholar
30. Holland J. P., Merklin J. F., Razvi J.: The radiolysis of dodecane-tributyl phosphate solutions. Nucl. Instrum. Methods 153, 589 (1978).10.1016/0029-554X(78)91011-XSearch in Google Scholar
31. Razvi J., Merklin J. F.: The radiolysis of dodecane-tributylphosphate solutions. II. Liquid products. Nucl. Instrum. Methods 169, 223 (1980).10.1016/0029-554X(80)90123-8Search in Google Scholar
32. Burger L. L., McClanahan E. D.: Tributyl phosphate and its diluent systems, Nucl. Technol. 50, 153 (1958).10.1021/ie50578a025Search in Google Scholar
33. Egorov G. F., Tkhorzhnitskii G. P., Zilberman B.Y., Shmidt O. V., Goletskii N. D.: Radiation chemical behavior of tributyl phosphate, dibutyl phosphoric acid, and its zirconium salt in organic solutions and two phase systems. Radiochemistry 47, 392 (2005).10.1007/s11137-005-0108-4Search in Google Scholar
34. Tripathi, S. C., Sumathi, S., Ramanujam, A.: Effects of solvent recycling on radiolytic degradation of 30% tributyl phosphate-ndodecane-HNO3 system. Sep. Sci. Technol. 34, 2887 (1999).10.1081/SS-100100811Search in Google Scholar
35. Barelko, E. P., Solyanina, I. P.,Tsvetkova, Z. I.: Radiation-chemical stability of TBP in solutions of hydrocarbons. Sov. Atom. Energy 21, 946 (1966).10.1007/BF01885923Search in Google Scholar
36. Blanco, R. E., Blake, Jr., C. A., Davis, Jr., W., Rainey, R. H.: Survey of recent developments in solvent extraction with tributyl phosphate. Oak Ridge National Lab, Tennessee (1963).10.2172/4755206Search in Google Scholar
37. Mincher, B. J., Modolo, G., Mezyk, S. P.:The effects of radiation chemistry on solvent extraction: 1. Conditions in acidic solution and a review of TBP. Solvent Extr. Ion Exch. 27, 1 (2009).10.1080/07366290802544767Search in Google Scholar
38. Wang, J. H., Bao, B. R., Wu, M. H.: The qualitative and quantitative analysis of the light hydrocarbons produced by radiation degradation of N, N-Diethylhydroxylamine. J. Radioanal. Nucl. Chem. 262, 451 (2004).10.1023/B:JRNC.0000046776.15434.dfSearch in Google Scholar
39. Wang, J. H., Wang, S. X., Bao, B. R.: Gaseous product generated by radiation degradation of N, N-diethylhydroxylamine aqueous solution. Nucl. Sci. Technol. 9, 79 (2008).10.1016/S1001-8042(08)60027-5Search in Google Scholar
40. Sheng, H., Li, F., Xiang, L.: The radiation stability of the extraction agent research (IV)-the radiolysis products of phosphate of butyl acetate and three sec-butyl phosphate (in Chinese). Atomic Energy Sci. Techno. 8, 692 (1965).Search in Google Scholar
41. Sheng, H., Xiang, C., Xin, M.: The radiation stability of the extraction agent research-the radiolysis of hybrid system of TBP-Water (in Chinese). At. Energy Sci. Technol. 1, 52 (1981).Search in Google Scholar
42. Soria, A. C., García-Sarrió, M. J., Sanz, M. L.: Volatile sampling by headspace techniques. TrAC Trends Anal. Chem. 71, 85 (2015).10.1016/j.trac.2015.04.015Search in Google Scholar
43. Tahraoui, A., Morris, J. H.: Decomposition of solvent extraction media during nuclear reprocessing: literature review. Sep. Sci. Technol. 30, 2603 (1995).10.1080/01496399508013706Search in Google Scholar
44. Zhizhong, W., Wang, S. Y., Sheng, H.: The radiation stability of the extraction agent research-the radiolysis of methyl phosphate bi-isoamyl and methyl phosphate bi-n-butyl (in Chinese). Atomic Energy Sci. Techno. 6, 744 (1981).Search in Google Scholar
45. Sheng, H., Xiang, L., Chen, Y.: The radiation stability of the extraction agent research (I)-Comparison radiolysis products of each isomer of tributyl phosphate (in Chinese). Atomic Energy Sci. Techno. 7, 767 (1964).Search in Google Scholar
©2018 Walter de Gruyter GmbH, Berlin/Boston
Articles in the same Issue
- Frontmatter
- Studies on the uptake of Am(III) and Eu(III) on ionic liquid modified polystyrene-divinyl benzene
- Performance evaluation of hollow fiber renewal liquid membrane for extraction of uranium(VI) from acidic sulfate solution
- Effect of carbonate on U(VI) sorption by nano-crystalline α-MnO2
- Comparison of some organic and inorganic ion exchangers concerning the sorption of Ce(III), Te(IV), Zr(IV), Hf(IV) and Nb(V)
- Evaluation of Mn bioaccumulation and biosorption by bacteria isolated from spent nuclear fuel pools using 54Mn as a radioindicator
- Preparation and biological evaluation of 99mTc N-histamine as a model for brain imaging: in silico study and preclinical evaluation
- Radiolysis products and degradation mechanism studies on tri-isoamyl phosphate (TiAP)
- Effects of γ irradiation on bis(2-ethylhexyl)phosphoric acid supported by macroporous silica-based polymeric resins
Articles in the same Issue
- Frontmatter
- Studies on the uptake of Am(III) and Eu(III) on ionic liquid modified polystyrene-divinyl benzene
- Performance evaluation of hollow fiber renewal liquid membrane for extraction of uranium(VI) from acidic sulfate solution
- Effect of carbonate on U(VI) sorption by nano-crystalline α-MnO2
- Comparison of some organic and inorganic ion exchangers concerning the sorption of Ce(III), Te(IV), Zr(IV), Hf(IV) and Nb(V)
- Evaluation of Mn bioaccumulation and biosorption by bacteria isolated from spent nuclear fuel pools using 54Mn as a radioindicator
- Preparation and biological evaluation of 99mTc N-histamine as a model for brain imaging: in silico study and preclinical evaluation
- Radiolysis products and degradation mechanism studies on tri-isoamyl phosphate (TiAP)
- Effects of γ irradiation on bis(2-ethylhexyl)phosphoric acid supported by macroporous silica-based polymeric resins
