% IMPORTANT: The following is UTF-8 encoded. This means that in the presence
% of non-ASCII characters, it will not work with BibTeX 0.99 or older.
% Instead, you should use an up-to-date BibTeX implementation like “bibtex8” or
% “biber”.
@INPROCEEDINGS{Brandt:902899,
author = {Brandt, Felix and Klinkenberg, Martina and Caes, Sébastien
and Poonoosamy, Jenna and Renterghem, Wouter Van and
Barthel, Juri and Lemmens, Karel and Bosbach, Dirk and
Ferrand, ; Karine},
title = {{D}issolution of simplified nuclear waste glass and
formation of secondary phases},
reportid = {FZJ-2021-04654},
year = {2021},
abstract = {Immobilization of high-level and intermediate-level nuclear
wastes by vitrification in borosilicate glass is a
well-established process. There is a consensus between the
waste management agencies of many countries and many experts
that vitrified nuclear waste should be disposed of in a deep
geological waste repository and therefore its long-term
behavior needs to be taken into account in safety
assessments. In contact with water, borosilicate glass is
metastable and dissolves. In static dissolution experiments,
often a surface alteration layer (SAL) forms on the
dissolving glass, and later sometimes secondary phases form.
Based on boron or lithium release rates, commonly three
stages of glass dissolution are defined as a function of the
reaction progress: (I) initial dissolution, described by a
congruent glass dissolution at the highest rate, (II)
residual dissolution, characterized by a glass dissolution
rate several orders of magnitude lower than the initial one,
and (III) resumption of glass alteration with initial rates.
Microscopically, the formation of a complex SAL has been
identified as a prerequisite for the slower dissolution
kinetics of stage II. Stage III is typically observed under
specific conditions, i.e., high temperature and/or high pH
driven by the uptake of Si and Al into secondary phases.
Different glass dissolution models explaining the mechanisms
of the SAL formation and rate-limiting steps have been
proposed and are still under debate.In this article
different aspects of glass dissolution from recent studies
in the literature and our own work are discussed with a
focus on the microscopic aspects of SAL formation, secondary
phase formation and the resumption of glass dissolution.
Most of the experiments in the literature were performed
under near-neutral pH conditions and at 90 ∘C, following
standard procedures, to understand the fundamental
mechanisms of glass dissolution. The example of interaction
of glass and cementitious materials as discussed here is
relevant for safety assessments because most international
concepts include cement e.g., as lining, for plugs, or as
part of the general construction of the repository. The aim
of the investigations presented in this paper was to study
the combined effect of hyperalkaline conditions and very
high surface area/volume ratios (SA/V=264000m−1) on the
dissolution of international simplified glass (ISG) and the
formation of secondary phases at 70 ∘C in a synthetic
young cement water containing Ca (YCWCa). The new results
show that the SA/V ratio is a key parameter for the
dissolution rate and for the formation of the altered glass
surface and secondary phases. A comparison with similar
studies in the literature shows that especially on the
microscopic and nanoscale, different SA/V ratios lead to
different features on the dissolving glass surface, even
though the SA-normalized element release rates appear
similar. Zeolite and Ca-silicate-hydrate phases (CSH) were
identified and play a key role for the evolution of the
solution chemistry. A kinetic dissolution model coupled with
precipitation of secondary phases can be applied to relate
the amount of dissolved glass to the evolution of the
solution's pH.},
month = {Nov},
date = {2021-11-10},
organization = {Interdisciplinary research symposium
On the safety of nuclear disposal
practices 2021, Berlin, online
(Germany), 10 Nov 2021 - 12 Nov 2021},
subtyp = {Other},
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/902899},
}