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@ARTICLE{Horne:866055,
author = {Horne, Gregory P. and Wilden, Andreas and Mezyk, Stephen P.
and Twight, Liam and Hupert, Michelle and Stärk, Andrea and
Verboom, Willem and Mincher, Bruce J. and Modolo, Giuseppe},
title = {{G}amma radiolysis of hydrophilic diglycolamide ligands in
concentrated aqueous nitrate solution},
journal = {Dalton transactions},
volume = {48},
issn = {0300-9246},
address = {London},
publisher = {Soc.},
reportid = {FZJ-2019-05296},
pages = {17005-17013},
year = {2019},
abstract = {The radiation chemistry of a series of hydrophilic
diglycolamides (DGAs: TEDGA, Me-TEDGA, Me2-TEDGA, and TPDGA)
hasbeen investigated under neutral pH, concentrated, aqueous
nitrate solution conditions. A combination of
steady-stategamma and time-resolved pulsed electron
irradiation experiments, supported by advanced analytical
techniques and multiscalemodeling calculations, have
demonstrated that: (i) the investigated hydrophilic DGAs
undergo first-order decay withan average dose constant of
(-3.18 ± 0.23) 10–6 Gy–1; (ii) their degradation
product × distributions are similar to those underpure
water conditions, except for the appearance of NOx adducts;
and (iii) radiolysis is driven by hydroxyl and nitrate
radicaloxidation chemistry moderated by secondary
degradation product scavenging reactions. Overall, the
radiolysis ofhydrophilic DGAs in concentrated, aqueous
nitrate solutions is significantly slower and less
structurally sensitive than underpure water conditions,
similar to their lipophilic analogs. Overall, acid
hydrolysis, not radiolysis, is expected to limit theiruseful
lifetime. These findings are promising for the deployment of
hydrophilic DGAs as actinide aqueous phase strippingand
hold-back agents, due to the presence of high concetrations
of nitrate in envisioned large-scale process conditions.},
cin = {IEK-6},
ddc = {540},
cid = {I:(DE-Juel1)IEK-6-20101013},
pnm = {161 - Nuclear Waste Management (POF3-161) / GENIORS - GEN
IV Integrated Oxide fuels recycling strategies (755171) /
SACSESS - Safety of ACtinide Separation proceSSes (323282)},
pid = {G:(DE-HGF)POF3-161 / G:(EU-Grant)755171 /
G:(EU-Grant)323282},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:31691689},
UT = {WOS:000498690100017},
doi = {10.1039/C9DT03918J},
url = {https://juser.fz-juelich.de/record/866055},
}