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@ARTICLE{Verlinden:1015012,
author = {Verlinden, Bart and Van Hecke, Karen and Wilden, Andreas
and Modolo, Giuseppe and Binnemans, Koen and Cardinaels,
Thomas and Kowalski, Piotr M.},
title = {{F}irst-principles study of the radiolytic degradation of
diglycolamides},
journal = {Radiochimica acta},
volume = {111},
number = {10},
issn = {0033-8230},
address = {Berlin},
publisher = {De Gruyter},
reportid = {FZJ-2023-03542},
pages = {741–750},
year = {2023},
abstract = {Understanding the degradation mechanisms of organic
compounds in an extreme radiolysis induced environment is
important for designing efficient organic extractants for
the separation of radionuclides from used nuclear fuel. In
this paper, we present an in-depth computational
chemistry-based molecular level analysis of the radiolytic
degradation of diglycolamides, with a focus on structural
and thermodynamic aspects of the process. The most
vulnerable parts of the organic ligands prone to attack and
degradation by radicals are identified via electronic
density and bond strength analysis. We identified the C–O
of the ether group as the weakest bond, which is further
weakened by methylation. A plausible degradation path
resulting from breaking the C–O bond by H radical attack
is obtained by computation of free energy of the process. To
investigate realistic reaction conditions, we accounted for
the impact of solvation effects on the thermodynamic
quantities, including solvation entropy effects. The
resulting degradation mechanism is consistent with
experimentally observed degradation products.},
cin = {IEK-6 / IEK-13},
ddc = {610},
cid = {I:(DE-Juel1)IEK-6-20101013 / I:(DE-Juel1)IEK-13-20190226},
pnm = {1412 - Predisposal (POF4-141) / GENIORS - GEN IV Integrated
Oxide fuels recycling strategies (755171) / Atomistic
modeling of radionuclide-bearing materials for safe
management of high level nuclear waste.
$(jara0037_20191101)$ / ENENplus - Attract, Retain and
Develop New Nuclear Talents Beyond Academic Curricula
(755576)},
pid = {G:(DE-HGF)POF4-1412 / G:(EU-Grant)755171 /
$G:(DE-Juel1)jara0037_20191101$ / G:(EU-Grant)755576},
typ = {PUB:(DE-HGF)16},
UT = {WOS:001066010000001},
doi = {10.1515/ract-2023-0176},
url = {https://juser.fz-juelich.de/record/1015012},
}