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@ARTICLE{Byrnes:453944,
author = {Byrnes, Ian and Lind, Ole Christian and Hansen, Elisabeth
Lindbo and Janssens, Koen and Salbu, Brit},
title = {{C}haracterization of radioactive particles from the
{D}ounreay nuclear reprocessing facility},
journal = {The science of the total environment},
volume = {727},
issn = {0048-9697},
address = {Amsterdam [u.a.]},
publisher = {Elsevier Science},
reportid = {PUBDB-2021-00301},
pages = {138488 (1-12)},
year = {2020},
abstract = {Radioactive particles originating from nuclear fuel
reprocessing at the United Kingdom Atomic Energy Authority's
Dounreay Facility were inadvertently released to the
environment in the late 1950s to 1970s and have subsequently
been found on site grounds and local beaches. Previous
assessments of risk associated with encountering a particle
have been based on conservative assumptions related to
particle composition and speciation. To reduce uncertainties
associated with environmental impact assessments from
Dounreay particles, further characterization is
relevant.Results of particles available for this study
showed variation between Dounreay Fast Reactor (DFR) and
Materials Test Reactor (MTR) particles, reflecting
differences in fuel design, release scenarios, and
subsequent environmental influence. Analyses of DFR
particles showed they are small (100–300 μm) and contain
spatially correlated U and Nb. Molybdenum, part of the DFR
fuel, was identified at atomic concentrations below $1\%.$
Based on SR-based micrometer-scale X-ray Absorption Near
Edge Structure spectroscopy (μ-XANES), U may be present as
U(IV), and, based on a measured Nb/U atom ratio of ~2,
stoichiometric considerations are commensurable with the
presence of UNb$_2$O$_7$. The MTR particles were larger
(740–2000 μm) and contained U and Al inhomogeneously
distributed. Neodymium (Nd) was identified in atomic
concentrations of around 1–2\%, suggesting it was part of
the fuel design. The presence of U(IV) in MTR particles, as
indicated by μ-XANES analysis, may be related to oxidation
of particle surfaces, as could be expected due to corrosion
of UAl$_x$ fuel particles in air. High $^{235}$U/$^{238}$U
atom ratios in individual DFR (3.2 ± 0.8) and MTR (2.6 ±
0.4) particles reflected the presence of highly enriched
uranium. The DFR particles featured lower $^{137}$Cs
activity levels (2.00–9.58 kBq/particle) than the MTR
(43.2–641 kBq $^{137}$Cs/particle) particles. The
activities of the dose contributing radionuclides
$^{90}$Sr/$^{90}$Y were proportional to $^{137}$Cs
($^{90}$Sr/$^{137}$s activity ratio ≈ 0.8) and particle
activities were roughly proportional to the size. Based on
direct beta measurements, gamma spectrometry, and the
VARSKIN6 model, contact dose rates were calculated to be
approximately 74 mGy/h for the highest activity MTR
particle, in agreement with previously published estimates.},
cin = {DOOR ; HAS-User},
ddc = {610},
cid = {I:(DE-H253)HAS-User-20120731},
pnm = {899 - ohne Topic (POF3-899)},
pid = {G:(DE-HGF)POF3-899},
experiment = {EXP:(DE-H253)D-L-20150101},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:32339828},
UT = {WOS:000537414400014},
doi = {10.1016/j.scitotenv.2020.138488},
url = {https://bib-pubdb1.desy.de/record/453944},
}