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2016 - MUlton e Sellier - Multi-Scale Analysis of Alkali-Silica Reaction (ASR)
2016 - MUlton e Sellier - Multi-Scale Analysis of Alkali-Silica Reaction (ASR)
a r t i c l e i n f o a b s t r a c t
Article history: Alkali–silica reaction expansions are disturbed by a variety of mechanisms (alkali leaching, ASR-gel permeation
Received 7 September 2015 through cracks, chemical conditions in pore solution water and its dependence on temperature). An important
Accepted 8 December 2015 consequence is the difficulty of using the expansion test on specimens to analyse the behaviour of ASR-
Available online 8 January 2016
damaged structures. The paper focuses on the influence of leaching: alkali transport and consumption are
modelled using a multi-scale approach (aggregate and concrete scales). The evaluation of the alkali concentration
Keywords:
Alkali–silica reaction (ASR) (C)
below which expansion stops is needed to perform relevant analysis in various alkali conditions and this alkali
Alkali (D) threshold is quantified according to calcium concentration and temperature. The impact of the coupling between
Expansion (C) alkali transport in aggregate and silica reactivity is also studied. Lastly, the consequences of leaching on ASR-
Leaching expansion are analysed in two case studies drawn from the literature.
Modelling (E) © 2015 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.cemconres.2015.12.007
0008-8846/© 2015 Elsevier Ltd. All rights reserved.
S. Multon, A. Sellier / Cement and Concrete Research 81 (2016) 122–133 123
with pagg the aggregate porosity, Sr the degree of water saturation, [Na+]
!
the alkali concentration in solution, φagg
Na the alkali flow in the aggregate
and SNa, the rate of alkali binding in ASR-gels per unit of time and of ag-
gregate volume.
The alkali flow depends on the coefficient of diffusion of alkali in the
aggregate Dagg:
! ! þ
φagg
Na ¼ −Dagg grad½Na : ð2Þ
2.2.2.1. Attack of silica and alkali fixation. The rate of alkali binding in ASR-
gels (the sink term SNa of the mass balance equation applied at the
aggregate scale) is driven by the reactivity of the aggregate. In the
Fig. 1. Alkali mass balance at aggregate scale (with diffusion and fixation in ASR-gels), at absence of precise quantification of the different mechanisms involved
concrete scale and at specimen scale (diffusion in the specimen). in the aggregate attack, it is assumed that linear kinetics is sufficient to
consider the silica attack and the ASR-gel precipitation according to an
alkali threshold [17]. This is a simplified approach compatible with
At the aggregate scale, the alkali mass balance equation has to experimental results on pore solution extraction [19].
consider the diffusion and the fixation of alkali in ASR-gels. In order to The form chosen for the rate of alkali fixation is similar to the one
be as representative as possible of the different types of aggregate used in [17]:
attacks [11–13], analysis of ASR cannot consider the alkali diffusion in D Eþ
reactive aggregate as the only driving mechanism of ASR-kinetics. At ∂Na f ½Naþ −½Naþ thr
ðCa;T Þ
least two main phenomena should be taken into consideration (Fig. SNa ¼− ¼− ð3Þ
∂t τASR
1): ionic transport (to have alkali and silica in the same place) and the
chemical reaction (attack of silica to form gels). The impact of the with τASR the characteristic time of silica attack, which can be consid-
coupling between alkali diffusion and silica reactivity on the distribu- ered to represent silica reactivity (even though, in reality, it combines
tion of ASR-gels in aggregate and concrete is analysed in the following both the kinetics of the reactive silica dissolution and the kinetics of
part. the ASR-gel production) and [Na+]thr (Ca, T) the alkali concentration
At concrete scale, the alkali diffusion equation takes the alkali flow “threshold” below which the reaction products cause negligible expan-
!
φcNa due to external boundary conditions into account (Fig. 1). The alkali sion. In the first version of this model [17], considering a constant
124 S. Multon, A. Sellier / Cement and Concrete Research 81 (2016) 122–133
threshold of alkali in Eq. (3) was necessary and sufficient to model In consequence, [Na+]thr(Ca,T), the alkali limit under which expansion
the ASR-expansion of concrete with different alkali contents in mois- stops, is not constant and has to be quantified according to the calcium
ture conditions [17]. But this same assumption leads to expansion concentration and the temperature. Based on the thermodynamic
rates that are too different for the expansion of specimens kept in equilibrium of portlandite [16], calcium concentration (in mol/l) in
NaOH solution and no threshold was taken into account for such the pore solution can be approximated from alkali concentration (in
calculations [9]. In fact, it is not really a threshold of silica attack, mol/l) and absolute temperature by [26]:
but an apparent threshold due to the difference of composition of
2þ
the reaction products according to the calcium concentration [18]. Ca ¼ 0:357 expð386:8 ½Naþ −0:01 T−1:4 ½Naþ T Þ: ð5Þ
The alkali concentration threshold, for which gel is no longer suffi-
ciently expansive, is not constant as supposed in [17] but depends
The main interest of this simplified relation is that it enables calcium
on the calcium concentration and the temperature, which can be
concentration to be evaluated from alkali and temperature. Thus, it is
approximated through the simplified approach proposed in the
not necessary to model calcium diffusion, which limits the number of
next part.
different variables in the numerical resolution.
For this mechanism of reaction, the Arrhenius energy is taken to be
Kim et al. [19] measured the evolution of alkali concentration in
80 kJ/mol [20] to represent the dependence on thermal conditions.
mortars subjected to ASR (Fig. 2). From this experiment, it was possible
Eq. (3) leads to an evaluation of the alkali bound in ASR-gels. Usually,
to evaluate the alkali threshold at about 0.325 mol/l at 23 °C. For such an
the molar ratio between silica (SiO2) and alkali (Na2O) present in gels in
alkali concentration and temperature, Eq. (5) gives a calcium concentra-
laboratory conditions is about 5 [21,22]. The number of ASR-gel moles
tion of about 0.11 mmol/l (Fig. 3). At 23 °C, if the alkali concentration
produced by the reaction is assumed to be equal to the number of
becomes lower than 0.325 mol/l, Kim et al. show that expansion
moles of silica attacked by alkalis and can thus be deduced from the
stops [19]. For this limit, the [Na+]/[Ca2+] ratio is around 3000. Finally,
following equation:
[Na+](Ca,T)
thr
can be defined as:
∂nmol
gel 5 ∂Na f thr ðT Þ
¼ ð4Þ ½Naþ ðCa;T Þ ¼ ρsol Ca2þ ð6Þ
∂t 2 ∂t
ρ(T) +
sol , the [Na ]/[Ca
2+
] limit ratio, depends on the different solubility
2.2.2.2. Alkali threshold. Based on thermodynamics modelling, Kim and constants of the species acting in these processes (silica gels with more
Olek showed that the formation of ASR-gels stopped when the alkali or less alkali and calcium) and thus on temperature since the variations
concentration became lower than a threshold value [18]. The rate of of the constants with temperature are different [18].
alkali binding (Eq. (3)) can be read as a simplified representation If the [Na+]/[Ca2+] ratio is higher than ρ(T) sol , alkali ions are predomi-
using only the alkali concentration to represent the disequilibrium: nant and gels are very expansive (Fig. 3). If calcium becomes preponder-
- For high alkali concentration (high [Na+]/[Ca2 +] ratio), the silica ant compared to alkali (ratio lower than ρ(T) sol ), expansive gel stops being
attack is rapid and large quantities of alkali are bound by gels. produced [18]. Using Kim et al.'s experimental results ([19], Fig. 2), the
ASR-gel contains mainly alkali and silica [18] and is very expansive ratio ρ(T)sol can be evaluated for three temperatures (23, 38 and 55 °C —
[23,24]. Fig. 2). It is interesting to note the good agreement of the variation of
- For lower alkali concentration, portlandite is dissolved and calcium ρ(T)
sol determined from Kim et al.'s experiments with the Van't Hoff law
concentration increases (decrease of [Na+]/[Ca2+] ratio). The rate for a standard enthalpy change of 205.9 kJ/mol (Fig. 4), with ρ(293) sol
of alkali binding decreases and gel becomes rich in calcium [18]. equal to 1.54e3. This law was used to perform the following case studies.
Such gels with high calcium content have low bound water contents With such equations, it is important to note that the alkali threshold
[25] and could cause less expansion [23,24]. is not constant even during a single expansion test at a uniform temper-
ature. In the case of an expansion test without external supply of alkali:
Fig. 2. Evolution of alkali concentration in mortars subjected to ASR for three temperatures Fig. 3. Calcium concentration (mol/l) according to alkali concentration (mol/l) in solution
(experimental results from Kim et al. [19]). at 23 °C due to portlandite equilibrium and limit of expansion of ASR-gels.
S. Multon, A. Sellier / Cement and Concrete Research 81 (2016) 122–133 125
Fig. 7. Profiles of alkali bound in ASR-gels for an aggregate of mean diameter of 2 mm:
(a) coefficient of diffusion of 1e−13 m2/s and characteristic time of reaction of 1000 days,
(b) coefficient of diffusion of 1e−15 m2/s and characteristic time of reaction of 100 days.
Fig. 6. Profiles of free alkali in an aggregate of mean diameter of 2 mm: (a) coefficient of The Arrhenius energy was taken to be 40 kJ/mol [32,33] to represent
diffusion of 1e−13 m2/s and characteristic time of reaction of 1000 days, (b) coefficient
the influence of thermal conditions on diffusion with interaction with
of diffusion of 1e−15 m2/s and characteristic time of reaction of 100 days.
C–S–H in concrete.
The distribution of aggregate sizes is not homogeneous in
with pc the concrete porosity, Sr the degree of saturation (assumed specimens, and particularly, close to the concrete skin. This concrete
! heterogeneity can be the cause of expansion gradient between core
constant), [Na+]c the alkali concentration in the concrete solution, φcNa and external surface. The impact of the aggregate size distribution on
c
the alkali flow at the specimen scale, and S∑Na f the sink term to ASR-expansion and cracking in specimens should be analysed through
account for alkali bound in ASR-gels at each time step determined at probabilistic approach in future work. By sake of simplicity, the
the aggregate scale. assumption of homogeneous distribution is adopted in this work. The
The alkali flow in concrete depends on its coefficient of diffusion in sink term of bound alkali can be calculated from the alkali flow in
the concrete: aggregate (Fig. 1):
agg
! ! c
S∑ 2
Na f ¼ − ∑ N agg 4πRagg φNa r ¼ Ragg ð9Þ
φcNa ¼ −Dc grad½Naþ c : ð8Þ agg
S. Multon, A. Sellier / Cement and Concrete Research 81 (2016) 122–133 127
Fig. 8. Slices of specimens (100 × 100 mm cross section) subjected to ASR in moderate leaching condition (aggregate coefficient of diffusion of 1e−14 m2/s and characteristic time of
reaction of 500 days). Top: distribution of alkali in specimen, middle: gradient of free and bound alkali in aggregates in the core and at the external surface of the specimen, bottom:
resulting distribution of ASR-gels in specimen.
with Nagg the number of reactive aggregates of each size per concrete the specimen (top of Fig. 8), takes the consumption of alkali ingress in
volume, Ragg the aggregate size and φagg
Na (r =Ragg) the alkali flow in the aggregates into account (middle of Fig. 8) and leads to the determina-
aggregate. tion of the resulting gradient of volume of ASR-gels in the specimen
In the following calculations, the equations of transport in the (bottom of Fig. 8). Due to the alkali gradient, the equations at the aggre-
aggregate and of ASR reaction (Eqs. (1) and (3), aggregate scale) and gate scale have to be solved at different points of the specimen. Accord-
Eq. (7) of global diffusion (concrete scale) are weakly coupled. The ing to the kinetics of gel formation, the impact of alkali leaching can be
chemical approach proposed in the paper considers the diffusion in more or less pronounced. The analysis is more difficult when the
128 S. Multon, A. Sellier / Cement and Concrete Research 81 (2016) 122–133
– the absence of expansion for small reactive particles, large aggregates expand due to the effect of a network of cracks
– the delay of expansion at the beginning of the reaction for large developing in them; this aggregate cracking could make the expansion
reactive particles, followed by a slope break of the expansion rate, slower. These factors, not yet considered in the model, can explain a part
whereas alkali consumption does not show any slope break but of the difference in the start of expansions curves between small and
has an exponential evolution [19] as would be expected for large aggregates. Chemical considerations could also explain the lack
equations of diffusion and reaction. of expansion at the beginning of the reaction by the differences of
expansive behaviour of ASR-products according to their time of forma-
tion. ASR-gels produced during the initial time of reaction could be less
Several assumptions can explain this behaviour. Previous modelling efficient to cause expansion [50–53]. This phenomenon can also be
assumed that it could be explained by the migration of ASR-gels in described as a non-expansive surface absorption of alkali by reactive
connected porosity very close to the reactive aggregate [14–17,39,41, silica at the beginning of the processes [54].
46]. This assumption appeared to be valid since very small distances Consequently, a part of the gels produced by ASR, φ0_exp, has to be
were necessary to obtain good quantification (less than 10 μm) [17]. removed from the total gel volume to represent this effect. Finally the
This assumption may be suitable for very reactive aggregate. In this pressure in ASR-gel can be written as:
case, the gels are first produced close to the cement paste and can partly
migrate in the surrounding porosity [11,47–49]. However, many
agg c
reactive aggregates do not show any gels in cement paste before the pgel ¼ M gel φgel −φ0 exp −φel −φcr ð10Þ
first cracking [11,12,45,49]. Other explanations concerning the aggre-
gates characteristics effects can also be derived from fracture mechan-
ics: cracks development in aggregate and resulting concrete cracking with Mgel the Biot Modulus of gel in aggregate. As not all the porosity of
are dependant of the internal reactive silica distribution in aggregate, aggregate is filled by ASR-gels, the Biot Modulus is assessed according to
of the shape, of the size of aggregates relatively to the specimen ones, the volume of ASR-gels φgel contained by the aggregate as proposed by
and of the distance of the aggregates from the edges. Moreover, very usual poromechanics [55–57].
S. Multon, A. Sellier / Cement and Concrete Research 81 (2016) 122–133 129
The mechanisms resulting in only little expansion at the beginning Finally, the aggregate pressure on the concrete is linked to the gel
of the reaction should be progressive. Therefore, the volume of ASR- pressure through:
gels leading to slight expansion at the beginning of the reaction was
taken to be proportional to ASR-gel pressure as proposed in [58]. pagg ¼ bgel pgel : ð15Þ
4 3
3 pgel
φ0 exp ¼ π Ragg − Ragg −t 0 exp ð11Þ As proposed in [43,56], the poromechanical constitutive law then
3 Rt
becomes:
X
with t0_exp an average thickness to quantify the volume of the gels σ ¼ K cd ðε−εan Þ− bagg pagg ð16Þ
agg
inefficient for expansion. This parameter was calibrated to obtain the
volume of ASR-gels that had to be removed to obtain non-expansion
with Kcd the concrete compressibility taking account of damage in the
of the smallest reactive particles and the delay in expansion for the
mechanical modelling used here, and εan the anelastic strains due to
largest.
creep and cracking.
With Eq. (11), gel pressure acts on the concrete as soon as gel is
Finally, in the poromechanics approach proposed in this paper, the
formed but the majority of the gel does not cause expansion until the
ASR-expansion of concrete results from two causes: the pressure due
gel pressure causes stress equal to the tensile strength of the material.
to the aggregate deformation under ASR-gel formation and the cracking
Once the stress induced by this gel pressure exceeds the tensile
induced by ASR-gels in the aggregate.
strength, the volume of gels inefficient for expansion is assumed to be
reached and all the supplementary gels cause pressure.
3. Case studies
In poromechanics, the elastic volumetric deformation of pore
volume containing gels φagg
el can be assessed by:
The previous equations are now used to analyse two experiments in
leaching conditions drawn from the literature. The first one is the well-
φagg ¼ bgel εagg ð12Þ documented experiment on the impact of leaching on ASR-expansion
el el
performed by Lindgård [5,60]. In this study, the alkali leaching and
expansion were both evaluated on the same specimens. This provided
bgel is the Biot coefficient due to gel formation in the aggregate. As for data that was very interesting for the analysis of the effect according
the Biot modulus, it is assessed according to the gel volume in the to specimen size and environmental storage. The second experiment
aggregate [55–57]. is one used to evaluate the impact of the competition between diffusion
The volume of concrete cracks φccr can be assessed by plastic or into reactive aggregates and leaching out of the specimen. To simplify
damage modelling. The calibration of the parameters acting on the the analysis and the comparison, the values of the parameters depend-
expansion level (V molgel and t0_exp) will be modified according to the
ing on temperature are given for the reference temperature of 20 °C. In
capacity of the concrete to restrain the expansion due to gel formation the calculations, the values at storage temperature during the test are
[59]. Therefore, the parameters V mol gel and t0_exp will depend on the
calculated through the Arrhenius law with the activation energies
assumptions of the mechanical modelling used and particularly on the given in the first part of this paper.
assessment of the loss of rigidity due to cracking (with or without
crack reclosure, consideration of creep, etc.). In the present work, the 3.1. Impact of leaching on expansion
previous anisotropic damage modelling coupled with creep presented
in [44] was used. However, the cracking criterion is on the gel pressure The impact of leaching on ASR-expansion was analysed from exper-
(Eq. (10)) here, which causes aggregate cracking first and then leads to imental results obtained at 38 °C on specimens with cross sections of
concrete cracking. 70 × 70 mm and 100 × 100 mm kept at 95% RH and in water [5,60,
61]. The experiments gave alkali leaching (Fig. 10) and measured
2.4.2. Resulting pressure in concrete expansion (Fig. 11) over two years for the two sizes of specimens and
At the concrete scale (Fig. 9), the volumetric deformation of aggre- for two moisture conditions (95% with limited leaching and in water
gate under ASR-gel pressure, φagg def , leads to the deformation of the
with high leaching) [5]. The total alkali leaching (alkali content at the
concrete, which can be evaluated through the action of an equivalent bottom of the storage containers and alkali content in the lining) was
pressure of aggregate on the concrete: given at two time steps (1 and 2 years). For the other time steps, the
alkali content at the bottom of the storage containers was given (but
not the alkali content in the lining). To obtain data of the total leaching
pagg ¼ M agg φagg
def
−φcel ð13Þ for intermediate time steps between the beginning and the first year
and between the first and the second years, it was supposed that the
ratio between alkali in the containers and total leached alkali was the
with Magg the Biot Modulus of aggregate in concrete determined by same throughout the experiments (Fig. 10).
usual poromechanics [55–57] and φcelthe elastic deformation of the The first difficulty encountered in analysing the results was to repre-
concrete, and: sent the external conditions of leaching. The storage at 95% RH does not
give a boundary condition that is easy to model for alkali external diffu-
φcel ¼ bagg εcel ð14Þ sion since such storage should not lead to leaching. In reality, the
leaching was due to the condensation of water vapour on the surfaces
of specimens following small temperature variations during the tests.
The boundary condition was obtained by inverse analysis of the total
with bagg the Biot coefficient of aggregate pressure on concrete (due to leached alkali given by experiments (Fig. 10). As alkali bound by ASR-
gel pressure in the aggregate). It is assessed according to the aggregate gels influences this total amount of leached alkali, the inverse analysis
content in the concrete through usual poromechanics relationships of boundary conditions and the calibration of expansion parameters
[55–57]. It is thus possible to evaluate the gel pressure according to were performed simultaneously for the most limited leaching
the conditions of compressibility of ASR-gels, aggregate and concrete. (specimens with cross section of 100 × 100 mm kept at 95% RH).
130 S. Multon, A. Sellier / Cement and Concrete Research 81 (2016) 122–133
Table 1
Parameters for the calculations presented in the two case studies for the reference temper-
ature of 20 °C.
Fig. 12. Advancement of ASR in one size of aggregate in the specimens of Lindgard's experiments [5] after 30 and 100 weeks.
4. Conclusion diagnosis. Scale-up methods have been used and combined to quantify
the phenomenon (alkali diffusion and chemical reactions at the aggre-
Alkali–silica reaction expansion tests can be disturbed by several gate scale, alkali transport at the specimen scale taking into account
phenomena in laboratory conditions. One of the main consequences is the alkali consumption from the lower scale). At the aggregate scale, a
the difficulty of using expansion tests on specimens to analyse the mass balance equation with a sink term is necessary to obtain simplified
behaviour of ASR-damaged structures. Modelling has to take these but realistic kinetics of ASR-expansion. The alkali transport in aggregate
effects into account to help in the analysis of laboratory tests and to is necessary to reproduce the dependence of the ASR kinetics on size for
make the link between experimentation on specimens and structural aggregates with high and intermediate reactivity. The sink term
depending on alkali concentration is necessary to represent alkali
fixation and to reproduce ASR kinetics of aggregates with low reactivity
and mixes of reactive aggregate of different sizes (particularly the im-
pact of the finest reactive particles for aggregates with intermediate
reactivity).
Fig. 13. Expansion according to aggregate size [59] (points) and numerical modelling Fig. 14. Pessimum effect in expansion due to aggregate size, experimentation and
(curves). modelling.
132 S. Multon, A. Sellier / Cement and Concrete Research 81 (2016) 122–133
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