High Linear Energy Transfer Degradation Studies Simulating Alpha Radiolysis of TRU Solvent Extraction Processes

Treatment of used nuclear fuel through solvent extraction separation processes is hindered by radiolytic damage from radioactive isotopes present in used fuel. The nature of the damage caused by the radiation may depend on the radiation type, whether it be low linear energy transfer (LET) such as gamma radiation or high LET such as alpha radiation. Used nuclear fuel contains beta/gamma emitting isotopes but also a significant amount of transuranics which are generally alpha emitters. Studying the respective effects on matter of both of these types of radiation will allow for accurate prediction and modeling of process performance losses with respect to dose. Current studies show that alpha radiation has milder effects than that of gamma. This is important to know because it will mean that solvent extraction solutions exposed to alpha radiation may last longer than expected and need less repair and replacement. These models are important for creating robust, predictable, and economical processes that have strong potential for mainstream adoption on the commercial level. The effects of gamma radiation on solvent extraction ligands have been more extensively studied than the effects of alpha radiation. This is due to the inherent difficulty in producing a sufficient and confluent dose of alpha particles within a sample without leaving the sample contaminated with long lived radioactive isotopes. Helium ion beam and radioactive isotope sources have been studied in the literature. We have developed a method for studying the effects of high LET radiation in situ via ¹⁰B activation and the high LET particles that result from the ¹⁰B(n,α)⁷Li reaction which follows. Our model for dose involves solving a partial differential equation representing absorption by ¹⁰B of an isentropic field of neutrons penetrating a sample. This method has been applied to organic solutions of TBP and CMPO, two ligands common in TRU solvent extraction treatment processes. Rates of degradation of TBP and CMPO and their respective degradation products in the presence of high LET radiation are presented and discussed. These results are also compared to gamma studies performed in our lab and other gamma and alpha studies found in the literature. The possible application of this method to a variety of other solvent extraction ligands to study the effects of high LET radiation is also considered.