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@ARTICLE{MarquesFernandes:1017537,
author = {Marques Fernandes, Maria and Klinkenberg, Martina and
Baeyens, Bart and Bosbach, Dirk and Brandt, Felix},
title = {{A}dsorption of {B}a and 226{R}a on illite: {A} comparative
experimental and modelling study},
journal = {Applied geochemistry},
volume = {159},
issn = {0883-2927},
address = {Amsterdam [u.a.]},
publisher = {Elsevier Science},
reportid = {FZJ-2023-04186},
pages = {105815 -},
year = {2023},
abstract = {Illite, smectite and illite/smectite mixed layers are major
phases in various argillaceous rock formations foreseen as
potential host rocks for the deep geological disposal of
high-level radioactive waste and are important sorbents for
cationic radionuclides potentially released in the
repository. 226Ra is a critical radionuclide in the safety
analysis and an important source of radioactivity in
technically enhanced naturally occurring radioactive
materials. A comprehensive study was carried out on the
adsorption of Ba and Ra on purified homoionic Na-illite
(Illite du Puy) over a wide range of experimental conditions
(pH, concentration, ionic strength) allowing for the
development of a quasi-mechanistic Ba/Ra adsorption model
for illite. Ba adsorption isotherms obtained at fixed ionic
strength and pH exhibit a non-linear behaviour in the Ba
equilibrium concentration range between ∼10−7 and
∼10−2 M. The pH dependent adsorption of trace 226Ra and
Ba was investigated at different ionic strengths and
evidenced a more pronounced adsorption of 226Ra than Ba on
illite. Finally, a competition experiment of trace 226Ra in
the presence of increasing Ba concentrations showed an
unexpected 226Ra adsorption behaviour which was not observed
for montmorillonite in earlier studies. This large set of
experimental data could be successfully modelled by Ba/226Ra
exchange reactions against Na, together with selectivity
coefficients, on two different site types, namely planar
sites and high affinity sites. The modelling of the pH
dependent adsorption of Ba and 226Ra at high ionic strength
and high pH required an additional surface complexation
reaction. Two additional exchange sites had to be introduced
to quantitatively describe the 226Ra uptake on illite in the
226Ra/Ba competition experiment. The nature of these sites,
however, remains unclear. The implementation of the 226Ra
adsorption model into predictive transport modelling codes
is of key importance for the safety analysis of deep
geological disposal of radioactive waste.},
cin = {IEK-6},
ddc = {550},
cid = {I:(DE-Juel1)IEK-6-20101013},
pnm = {1411 - Nuclear Waste Disposal (POF4-141) / EURAD - European
Joint Programme on Radioactive Waste Management (847593)},
pid = {G:(DE-HGF)POF4-1411 / G:(EU-Grant)847593},
typ = {PUB:(DE-HGF)16},
UT = {WOS:001102594700001},
doi = {10.1016/j.apgeochem.2023.105815},
url = {https://juser.fz-juelich.de/record/1017537},
}