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@INPROCEEDINGS{Klinkenberg:1016753,
author = {Klinkenberg, Martina and Brandt, Felix and Barthel, Juri
and Bosbach, Dirk},
title = {{S}olid-solution formation of ({B}a,{S}r,{R}a){SO}4:
{M}icroscopic approaches},
reportid = {FZJ-2023-03739},
year = {2023},
abstract = {The minerals of the isostructural barite ((Ba,Sr)SO4) group
are frequently occurring and characterized by their low
solubility. These sulfates are associated with the formation
of technically enhanced naturally occurring radioactive
material (TENORM). The radioactivity of TENORM is often a
result of solid solution formation with 226Ra because of the
higher thermodynamic stability compared to the pure
endmember RaSO4. The (Ra,Ba,Sr)SO4 is also relevant for the
safety assessment of deep geological repositories for spent
nuclear fuel. In this contribution, the application of
microscopic approaches on the solid-solution formation of
(Ba,Sr,Ra)SO4 to understand macroscopic observations will be
discussed.A combination of scanning electron microscopy
(SEM), energy dispersive x-ray spectrometry (EDX), focused
ion beam (FIB), transmission electron microscopy (TEM) as
well as time of flight secondary ion mass spectroscopy
(ToF-SIMS) and atom probe tomography (APT) was applied to
unravel the up-take of 226Ra into (Ba,Sr,Ra)SO4 on a
molecular scale. SEM-EDX was used to follow the
morphological and chemical evolution of the sulfate
particles during the Ra-uptake. The Ra-uptake into the solid
was observed by a 3D analysis of complete grains via
ToF-SIMS. The FIB, producing very small samples and
extremely thin samples for TEM and atom probe tomography
(APT), enables the detailed investigation of even highly
radioactive materials due to the low radioactivity of the
FIB sections. TEM and APT were applied to unravel the
details of this recrystallization process from the solid
materials perspective, indicating an important role of fluid
inclusions and internal porosity typical for these sulfates.
Our studies not only show that 226Ra is taken up
structurally during recrystallisation of (Ba,Sr)SO4, but
also that kinetically controlled initial stages eventually
are followed by thermodynamically controlled Ra-uptake which
can be described via solid-solution aqueous-solution
modeling.},
month = {Oct},
date = {2023-10-04},
organization = {21st Jena Remediation Symposium, Jena
(Germany), 4 Oct 2023 - 6 Oct 2023},
subtyp = {Invited},
cin = {IEK-6 / ER-C-2},
cid = {I:(DE-Juel1)IEK-6-20101013 / I:(DE-Juel1)ER-C-2-20170209},
pnm = {1411 - Nuclear Waste Disposal (POF4-141)},
pid = {G:(DE-HGF)POF4-1411},
typ = {PUB:(DE-HGF)24},
url = {https://juser.fz-juelich.de/record/1016753},
}