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@INPROCEEDINGS{Bosbach:154632,
author = {Bosbach, Dirk and Brandt, Felix and Klinkenberg, Martina
and Vinograd, Victor and Rozov, Konstantin and Weber,
Juliane and Breuer, Uwe},
title = {{R}adionuclide solubility control in solid solution –
aqueous solution systems: {R}adium solubility in the
presence of barite},
reportid = {FZJ-2014-03922},
year = {2014},
abstract = {The migration of radionuclides in the geosphere is to a
large extend controlled by sorption processes onto minerals
and colloids. On a molecular level, sorption phenomena
involve surface complexation, ion exchange as well as
co/precipitation reactions. Coprecipitation leads to the
formation of structurally incorporated radionuclides in a
host structure. Such solid solutions are ubiquitous in
natural systems - most minerals in nature are atomistic
mixtures of elements rather than pure compounds. Deriving a
thermodynamic model requires a molecular level concept
including information such as the actual substitution
mechanism, site occupancies and related ordering phenomena.
However, radionuclide solubility controlled by solid
solutions is currently not considered in long term safety
assessments for a nuclear waste repository system. One
reason is related to the fact that only a limited number of
rather simple solid solution systems have been studied to a
sufficient level.The control of Radium solubility in
(Ra,Ba,Sr)S04 solid solution - aqueous solution systems
under relevant conditions will be discussed. ln general, its
solubility is significantly reduced if it is controlled by a
binary (Ra,Ba)S04 solid solution or an even more complex
ternary (Ra,Ba,Sr)S04 solid solution. New experimental data
as well as computational approaches using first principle
calculations will be discussed. ln particular with respect
to the conditions of interest here, one quest always needs
to be considered: Do measured data of the solid solution and
the aqueous solution represent equilibrium conditions or do
they represent a metastable situation? The challenge to
derive thermodynamic data from experiments in aqueous
solution at rel. low temperatures with potentially
metastable states will be discussed.},
month = {Jul},
date = {2014-07-14},
organization = {Workshop "Radiation damage in
structures - Relevance for nuclear
waste disposal" Körber-Stiftung, Forum
für Impulse, Hamburg (Germany), 14 Jul
2014 - 15 Jul 2014},
subtyp = {Invited},
cin = {IEK-6 / ZCH},
cid = {I:(DE-Juel1)IEK-6-20101013 / I:(DE-Juel1)ZCH-20090406},
pnm = {142 - Safety Research for Nuclear Waste Disposal (POF2-142)
/ HITEC - Helmholtz Interdisciplinary Doctoral Training in
Energy and Climate Research (HITEC) (HITEC-20170406)},
pid = {G:(DE-HGF)POF2-142 / G:(DE-Juel1)HITEC-20170406},
typ = {PUB:(DE-HGF)31},
url = {https://juser.fz-juelich.de/record/154632},
}