Low and High LET Degradation Studies of Metal-Loaded Organic Phase Ligands in the ALSEP Process

Bustillos, Christian G.; Ngelale, Randy O.; Nilsson, Mikael

doi:10.1080/07366299.2023.2202224

Low and High LET Degradation Studies of Metal-Loaded Organic Phase Ligands in the ALSEP Process

Journal Article · Wed Apr 26 00:00:00 EDT 2023 · Solvent Extraction and Ion Exchange

DOI:https://doi.org/10.1080/07366299.2023.2202224· OSTI ID:2005129

^[1]; Ngelale, Randy O. ^[2]; Nilsson, Mikael ^[3]

Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
University of California, Irvine, CA (United States)

Organic solutions comprising the Actinide Lanthanide Separation Process (ALSEP) solvent consisting of 0.5 M 2-ethylhexyl phosphonic acid mono-2-ethylhexyl ester (HEH[EHP]) and 0.05 M N,N,N’,N’-tetra(2-ethylhexyl)diglycolamide (T2EHDGA) in n-dodecane were subjected to low LET and high LET irradiation before and after equilibration with an aqueous phase of 3 M HNO₃. Degradation dose constants revealed greater ligand degradation due to gamma irradiation than alpha irradiation for both ligands. Furthermore, equilibration with nitric acid did not have a significant impact on ligand degradation for either irradiation source. Identified degradation products were similar for both gamma and alpha irradiation and occurred mostly through the rupture of the N–C_carbonyl and C–O_ether bonds for T2EHDGA and the C–Oether bond in HEH[EHP]. Acid contact appears to alter the degradation pathway by favoring the formation of higher molecular weight recombination products. Furthermore, mixed T2EHDGA-HEH[EHP]-NO₃ complexes were formed with Nd(III) after extraction from 3 M HNO₃, and low LET gamma irradiation of the Nd(III) loaded organic solution produced similar degradation products as the organic solution absent of Nd(III). Interestingly, and likely due to the greater radiolytic susceptibility of T2EHDGA than HEH[EHP], a HEH[EHP]-Nd(III) complex appears to form as the T2EHDGA degrades with increasing absorbed dose.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 2005129

Report Number(s):: LLNL-JRNL--832885; 1050094

Journal Information:: Solvent Extraction and Ion Exchange, Journal Name: Solvent Extraction and Ion Exchange Journal Issue: 4 Vol. 41; ISSN 0736-6299

Publisher:: Taylor and FrancisCopyright Statement

Country of Publication:: United States

Language:: English

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