Radiolysis of Tributyl Phosphate by Particles of High Linear Energy Transfer

Abstract

Tributyl Phosphate (TBP), used in chemical separation processes for used nuclear fuel, is susceptible to radiolysis causing losses in process performance. 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.