Radiolysis of Tributyl Phosphate by Particles of High Linear Energy Transfer

Pearson, J.; Nilsson, M.

doi:10.1080/07366299.2014.924305

Radiolysis of Tributyl Phosphate by Particles of High Linear Energy Transfer

Journal Article · Thu Jul 03 00:00:00 EDT 2014 · Solvent Extraction and Ion Exchange

DOI:https://doi.org/10.1080/07366299.2014.924305· OSTI ID:1454601

Pearson, J. ^[1]; Nilsson, M. ^[2]

Univ. of California, Irvine, CA (United States). Chemical Engineering and Materials Science; UC Berkeley
Univ. of California, Irvine, CA (United States). Chemical Engineering and Materials Science

Tributyl Phosphate (TBP), used in chemical separation processes for used nuclear fuel, is susceptible to radiolysis causing losses in process performance. Here, we have studied its degradation by exposing dry 1M TBP/n-dodecane solutions to gamma radiation from a cesium-137 source and in a mix of low and high linear energy transfer (LET) radiation by irradiating samples in the UC Irvine TRIGA® reactor and utilizing the ¹⁰B(n,α)⁷Li reaction. In a 1 M solution of TBP in n-dodecane the degradation of TBP (G^-_TBP) was found to be 0.36 and 0.14 μmol/J for low and high LET radiation, respectively. The formation of dibutyl phosphoric acid, DBP, (G⁺_DBP) in this solution was found to be 0.18 and 0.047 μmol/J for low and high LET radiation, respectively. In samples exposed to low LET as well as a mix of low and high LET a variety of TBP degradation products containing phosphorus were observed indicating that other degradation products than DBP and the monobutyl diacid (MBP) were formed. Our results for both low and high LET radiation compare well with previous studies on these systems indicating that high LET degrades TBP to a lesser extent than gamma radiation. Available data for high LET is not as abundant as for low LET making such comparisons challenging. Nevertheless, our method yields a value for G⁺_DBP that agrees well with previous alpha radiolysis studies indicating that our method shows promise for studying high LET radiolysis in liquid-liquid extraction systems.

Research Organization:: Univ. of California, Irvine, CA (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE). Nuclear Energy University Program

DOE Contract Number:: AC07-05ID14517

OSTI ID:: 1454601

Journal Information:: Solvent Extraction and Ion Exchange, Journal Name: Solvent Extraction and Ion Exchange Journal Issue: 6 Vol. 32; ISSN 0736-6299

Publisher:: Taylor and Francis

Country of Publication:: United States

Language:: English

References (22)

Radiation-chemical stability of TBP in solutions of hydrocarbons Barelko, E. P.; Solyanina, I. P.; Tsvetkova, Z. I. Soviet Atomic Energy, Vol. 21, Issue 4 https://doi.org/10.1007/BF01885923	journal	October 1966
Studies of high linear energy transfer dosimetry by 10B(n,α)7Li reactions in aqueous and organic solvents Pearson, J.; Jan, O.; Miller, G. E. Journal of Radioanalytical and Nuclear Chemistry, Vol. 292, Issue 2 https://doi.org/10.1007/s10967-011-1479-y	journal	October 2011
Development of a method for high LET irradiation of liquid systems Pearson, J.; Jan, O.; Wariner, A. Journal of Radioanalytical and Nuclear Chemistry, Vol. 298, Issue 2 https://doi.org/10.1007/s10967-013-2549-0	journal	May 2013
Radiation Chemical Behavior of Tributyl Phosphate, Dibutylphosphoric Acid, and Its Zirconium Salt in Organic Solutions and Two-Phase Systems Egorov, G. F.; Tkhorzhnitskii, G. P.; Zilberman, B. Ya. Radiochemistry, Vol. 47, Issue 4 https://doi.org/10.1007/s11137-005-0108-4	journal	July 2005
The radiolysis of dodecane-tributylphosphate solutions Holland, J. P.; Merklin, J. F.; Razvi, J. Nuclear Instruments and Methods, Vol. 153, Issue 2-3 https://doi.org/10.1016/0029-554X(78)91011-X	journal	July 1978
The radiolysis of dodecane-tributylphosphate solutions II. Liquid products Razvi, Junaid; Merklin, Joseph F. Nuclear Instruments and Methods, Vol. 169, Issue 1 https://doi.org/10.1016/0029-554X(80)90123-8	journal	February 1980
Application of gas chromatography–tandem mass spectrometry to the analysis of inhibition of dimerisation of tributylphosphate under radiolysis Lamouroux, C.; Virelizier, H.; Moulin, C. Journal of Chromatography A, Vol. 917, Issue 1-2 https://doi.org/10.1016/S0021-9673(01)00674-4	journal	May 2001
Heavy ion radiolysis of organic materials LaVerne, Jay A.; Chang, Z.; Araos, M. S. Radiation Physics and Chemistry, Vol. 60, Issue 4-5 https://doi.org/10.1016/S0969-806X(00)00357-1	journal	January 2001
The radiobiological principles of boron neutron capture therapy: A critical review Hopewell, J. W.; Morris, G. M.; Schwint, A. Applied Radiation and Isotopes, Vol. 69, Issue 12 https://doi.org/10.1016/j.apradiso.2011.04.019	journal	December 2011
Radiolysis study of actinide complexing agent by irradiation with helium ion beam Sugo, Yumi; Taguchi, Mitsumasa; Sasaki, Yuji Radiation Physics and Chemistry, Vol. 78, Issue 12 https://doi.org/10.1016/j.radphyschem.2009.06.031	journal	December 2009
Radiation Stability of Organophosphorus Compounds Wagner, R. M.; Kinderman, E. M.; Towle, L. H. Industrial & Engineering Chemistry, Vol. 51, Issue 1 https://doi.org/10.1021/ie50589a033	journal	January 1959
Radiation chemical studies with heavy ions: oxidation of ferrous ion in the Fricke dosimeter LaVerne, Jay A.; Schuler, Robert H. The Journal of Physical Chemistry, Vol. 91, Issue 22 https://doi.org/10.1021/j100306a050	journal	October 1987
Radiation Chemistry Studies with Cyclotron Beams of Variable Energy: Yields in Aerated Ferrous Sulfate Solution ¹ Schuler, Robert H.; Allen, Augustine O. Journal of the American Chemical Society, Vol. 79, Issue 7 https://doi.org/10.1021/ja01564a012	journal	April 1957
Oxidation of Ferrous Sulfate by Ionizing Radiations from (n, α) Reactions of Boron and Lithium ^1a Schuler, Robert H.; Barr, Nathaniel F. Journal of the American Chemical Society, Vol. 78, Issue 22 https://doi.org/10.1021/ja01603a011	journal	November 1956
Radiolysis of Tri-n-butyl Phosphate Williams, T. F.; Wilkinson, R. W.; Rigg, T. Nature, Vol. 179, Issue 4558 https://doi.org/10.1038/179540a0	journal	March 1957
801. The radiolysis of tri-n-alkyl phosphates Wilkinson, R. W.; Williams, T. Ffrancon Journal of the Chemical Society (Resumed) https://doi.org/10.1039/jr9610004098	journal	January 1961
Review Article: The Effects of Radiation Chemistry on Solvent Extraction: 1. Conditions in Acidic Solution and a Review of TBP Radiolysis Mincher, Bruce J.; Modolo, Giuseppe; Mezyk, Stephen P. Solvent Extraction and Ion Exchange, Vol. 27, Issue 1 https://doi.org/10.1080/07366290802544767	journal	January 2009
The Radiation Chemistry of CMPO: Part 2. Alpha Radiolysis Mincher, Bruce J.; Mezyk, Stephen P.; Elias, Gracy Solvent Extraction and Ion Exchange, Vol. 32, Issue 2 https://doi.org/10.1080/07366299.2013.850300	journal	January 2014
Identification of minor products obtained during radiolysis of tributylphosphate (TBP) Lesage, Denis; Virelizier, Henri; Jankowski, Christophe K. Spectroscopy, Vol. 13, Issue 4 https://doi.org/10.1155/1997/565194	journal	January 1997
Alpha radiolysis and other factors affecting hydrolysis of tributyl phosphate Lloyd, M. H.; Fellows, R. L. https://doi.org/10.2172/5534740	report	January 1985
The Radiolysis of Tributyl Phosphate Burr, John G. Radiation Research, Vol. 8, Issue 3 https://doi.org/10.2307/3570477	journal	March 1958
Study of Solvent Degradation in Reprocessing MOX Spent Fuel Solvent Degradation and Its Effect on Pu Purification Cycle [ＭＯＸ燃料再処理における溶媒劣化　　Ｐｕ精製工程における溶媒劣化とその影響] Kawaguchi, Yoshihito; Morimoto, Kazuyuki; Kitao, Takahiko Transactions of the Atomic Energy Society of Japan, Vol. 8, Issue 3 https://doi.org/10.3327/taesj.J08.034	journal	January 2009

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