Bentonite Behavior in Nuclear Repositories
Bentonite Behavior in Nuclear Repositories
https://doi.org/10.1007/s11440-022-01689-0 (0123456789().,-volV)(0123456789().
,- volV)
RESEARCH PAPER
Received: 16 December 2021 / Accepted: 24 August 2022 / Published online: 5 December 2022
The Author(s) 2022
Abstract
It is assumed that clay materials such as bentonites will be used as the buffer and backfill of high-level radioactive waste
disposal. Due to the very long timescale, the design can be based only on mathematical models that have been thoroughly
validated via the use of high-quality laboratory data. The presentation of an extensive laboratory dataset, accompanied by
the validation of a bentonite constitutive model, comprises the main topic of this paper. The objectives of the laboratory
research were to determine the basic hydromechanical properties of BCV bentonite and to study the stress path behaviour
of this bentonite. The laboratory results revealed that the hydromechanical behaviour is highly dependent on the stress path
assumed, as well as the method of water introduction into the sample. The results further indicate that the micro- and
macrostructures are constantly evolving, which exerts a significant impact on the determination of the material properties
and the development of mathematical models. Moreover, it was demonstrated that swelling pressure tests, although they
are typically considered to be element tests (with constant fields of state variables), when adopted by researchers for the
calibration of constitutive models, do not in fact constitute element tests. A hypoplastic model of the behaviour of bentonite
was implemented and validated using the experimental data obtained. It was demonstrated that the hypoplastic model
accurately predicted the main behavioural features of bentonite that are important in terms of the prediction of the
behaviour of the buffer in nuclear waste repositories.
Keywords BCV Bentonite Element test Hydraulic conductivity Hypoplastic model Mechanical properties
Mathematical model Swelling
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Fig. 1 Scheme of the deep geological repository planned in the Czech Republic SÚRAO
SURAO, was to obtain similarly comprehensive data to a hypoplastic bentonite material model for FEM analysis
that contained in datasets available on other widely used purposes [15, 16]. The model was subsequently employed
bentonites such as MX-80 bentonite (Cui et al. [5] and in the interpretation of the behaviour of the material
FEBEX bentonite [21]). All the tests were performed by observed during the laboratory experimentation phase.
the various laboratories involved on the same batch of
bentonite in order to ensure the consistency of the tested
material, which is rather unusual for other bentonite data- 2 BCV bentonite
sets available in the literature. In order to obtain similar
datasets for the development and calibration of models, The Czech DGR concept is based on the use of bentonites
experimental results are usually obtained from various extracted from Czech bentonite deposits. BCV (Bentonite
sources that consider differing batches of material over Černý Vrch) is a Ca/Mg bentonite extracted from the Černý
several years ([6], Thatcher [20]). Since bentonites are vrch bentonite deposit located in the České Středohořı́ Mts.
natural materials, their composition and properties vary in the NW of the Czech Republic. BCV bentonite was chosen
between both sources and batches (Dixon [6]), which may as a suitable representative of Czech bentonites [9] and was
lead to biased results. A single batch-based complex first subjected to testing in 2017. Following the pilot char-
dataset provides high-quality data for the development and acterisation of BCV (Červinka et al. [3]), this bentonite was
validation of constitutive models. used in a number of laboratory [22] and Baryla et al. [1] and
The investigation of the stress path behaviour is particu- in situ projects [11] and Svoboda et al. [19].
larly important since it is known that bentonite materials BCV is produced industrially by Keramost a.s. at their
evince complex (micro)structures and that the state of the Obrnice plant. The bentonite treatment process commences
material leads to changes in its various properties and beha- with the sieving of the coarse material employing a sieve
viour. This may have important consequences in terms of the with a 20 9 20 cm mesh. The bentonite is then homo-
design of the engineered barrier system (EBS) since, for genised in a roller mill from where it is transferred to a
example, the swelling pressure may differ significantly rotary oven where the material is dried (average tempera-
depending on whether, and to what extent, the deformation of ture of 110 C) for 45 min. The drying process ensures a
the material is allowed. It is important to note that the water content of around 10% and results in the preparation
experimental dataset presented in this paper does not include of the material for final milling and air sieving. The pro-
the consideration of experiments conducted at elevated tem- cessing of the BCV material leads to a mixture where 1%
peratures. The effect of temperature is also being studied of the total weight of the grains can be larger than
extensively and will be described in forthcoming publications. 0.315 mm and at least 70% of the grains are smaller than
The data obtained from the laboratory research was used 0.063 mm. The material is supplied in 48 kg bags, larger
as a tool for the development, calibration and validation of bags or tanks [22].
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BCV bentonite (see Tables 1 and 2) exhibits a high Table 2 Results of the silicate analysis of BCV bentonite [14]
proportion of minerals from the smectite group (Ca/Mg Wt % BCV_2017
montmorillonite of over 60%), while other clay minerals
(kaolinite, illite) are present to a lesser extent. With respect SiO2 51.86
to the accessory phases, the presence of genesis-related Fe- TiO2 2.34
carbonates (siderite, ankerite) and Fe oxides (mainly goe- Al2O3 15.56
thite) is of particular interest [9] and [14]. Fe2O3 11.41
It is the proportion of iron-rich phases and the iron- FeO 0.14
enrichment of the smectite in octahedral positions [7] that MgO 2.82
differentiates Czech bentonites from international stan- MnO 0.20
dards and the Ca-bentonites extracted from the majority of CaO 2.83
European deposits. Na2O 0.37
The cation exchange capacity of BCV bentonite is K2O 1.02
63.7 ± 2.2 meq/100 g and the major exchangeable cations P2O5 0.51
consist of magnesium (42.0 ± 0.6 meq/100 g) and calcium F 0.12
(15.1 ± 1.8 meq/100 g). The density of the solid particles is CO2 1.68
2.76 ± 0.02 g/cm3. The total specific surface area of BCV C 0.17
bentonite (employing EGME) is 438 ± 6 m2/g (Červinka et al. S \ 0.010
[3]). H2O(?) 9.06
The liquid limit according to the ČSN EN ISO Total 100.09
17892–12 standard [4] is 130% (according to Laufek et. al. H2O(-) 9.23
[14]) and 139% (according to Červinka et. al. [3], Haus-
mannová et. al. [9]).
This study involved the investigation of a BCV ben-
tonite powder and a uniaxially compacted powder. The
investigation of the water permeability and the total pres-
batch of the material that was subjected to experimentation
sure. The cells allowed for bottom-up saturation and the
was named BCV_2017; for more detailed information, see
continuous monitoring of total pressure at the top or both at
Laufek et al. [14].
the top and bottom, depending on the type of test. Gener-
ally, only the top total measurement approach is used for
the determination of the swelling pressure. Measurement
3 Laboratory investigation on both sides is applied only in selected tests aimed at
of the hydromechanical properties obtaining more accurate data for model calibration
purposes.
3.1 Swelling pressure (constant volume)
The top and bottom of the samples were fitted with
sintered steel permeable plates so as to prevent the leaching
The swelling pressure was measured using a constant
(‘‘mobilisation’’) of the material. The piston and the force
volume cell apparatus that allowed for the combined
sensor for the measurement of the total (or swelling)
pressure of the bentonite were positioned on the top side
Table 1 Mineralogical composition of BCV bentonite (determined between the flange of the chamber and the surface of the
using X-ray diffraction, calculated via the Rietveld method) [14] sample. A force sensor was connected to a central data
Wt% Original BCV logger.
The bentonite was uniaxially compacted into the hollow
Anatase 2.3
steel cylinder that formed the central part of the cell. Two
Quartz 11.4
laboratories were responsible for the investigation of the
Montmorillonite 69.7
swelling pressure and permeability—the Czech Technical
Mg-calcite 3.7
University (CTU) and Charles University (CU) laborato-
Goethite 3.1
ries. This allowed for the crosschecking of the results and
Hematite –
procedures.
Kaolinite 5.0 The setup used at the Charles University is shown in
Ankerite 0.6 Fig. 2. Bentonite samples of 50 mm in diameter were
Siderite 0.5 compacted directly into the cells using 36 g of bentonite
Illite 3.7 powder (hygroscopic water content of 11%). The height of
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the samples varied in the range 9–13 mm depending on the dismantling, the samples were cut into slices of a thickness
required initial dry density. The samples were saturated of approximately 2 mm and the water content of each slice
with distilled water through the bottom base. The water was determined by means of the gravimetric method. This
was not pressurised during the saturation process (Fig. 2a). allowed for the determination of the water saturation dis-
The increase in the swelling pressure was monitored until a tribution in the samples. Note that the final sample (dis-
constant value was attained. Pressure and volume con- mantled at 333.78 h) was found to be fully saturated—the
trollers were connected to both bases for the measurement change in the water content along the top of the sample was
of the hydraulic conductivity (Fig. 2b), and a constant caused by the change in the dry density which, in turn, was
pressure gradient was applied. The hydraulic conductivity caused by swelling during the saturation process (which led
was measured once a constant flow rate had been attained. to density changes).
The setup used by the Czech Technical University team is
shown in Fig. 3. Bentonite samples of 30 mm in diameter and 3.2 Swelling under a constant load (oedometric
heights of 20 mm were compacted directly into the cell rings. tests)
Distilled water was used as the saturation medium, which was
propelled by compressed argon, typically at a pressure of The hydromechanical behaviour of the BCV 2017 was
1 MPa. The saturation pressure applied does not influence the investigated via the conducting of oedometric tests. A
measured values provided the saturation pressure is lower sample with a diameter of 120 mm and a height of 30 mm
than the swelling pressure of the sample [8]. The water flow was placed in a cylindrical brass cell fitted with porous
was determined manually using a graded capillary tube-based stone at the top and the bottom to allow for the saturation/
flow meter in the inflow part. Testing continued until the flow desaturation of the sample. The sample was allowed to
and the total pressure stabilised (see the example in Fig. 4). deform uniaxially (compaction/swelling) via the movement
The water flow over at least the four latest consecutive of a piston positioned on the top of the sample. The test
intervals was used for the determination of the coefficient of was pressure controlled and with free deformation. The
permeability (average of the four results). The water pressure selected uniaxial load was transferred to the sample via the
source was subsequently disconnected so as to allow for the piston, while the sample deformation was monitored via
determination of the swelling pressure (Laufek et al. [14]). the movement of the piston.
Figure 5 illustrates the dependency of the swelling This setup enabled the investigation of the stress path
pressure on the dry density as recorded by the two labo- dependence and hysteresis, as well as the influence of
ratories; the data is taken from Laufek et al. [14]. Figure 6 saturation via the alteration of the load scenario and the
shows the dependency of the hydraulic conductivity on the water regime.
dry density, again, as determined by the CTU and the CU. Three main scenarios were investigated:
Figure 7 illustrates the temporal saturation evolution for
• Initial saturation without loading (Scenario I)—com-
a dry density of approximately 1600 kg/m3. A series of
pacted samples were saturated at minimum loading (the
samples with a dry density of * 1600 kg/m3 was saturated
weight of the piston of the apparatus) then loaded
followed by dismantling at predetermined intervals. During
incrementally up to 700 kPa with free access to water,
Fig. 2 Configuration of the constant volume cells for the measurement of the swelling pressure (a) and the hydraulic conductivity (b) at the
Charles University
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Fig. 3 Configuration of the constant volume cells for the measurement of the swelling pressure and the hydraulic conductivity at the Czech
Technical University
Fig. 4 Measurement of the permeability and total pressure (BCV qd = 1597 kg/m3)
123
and subsequently incrementally unloaded with free clearly indicate the presence of path dependence especially
access to water. in the initial stage. However, once the samples have
• Saturation without loading after a dry cycle (Scenario become fully saturated and fully loaded, they converge to
II)—samples with natural water contents were loaded form very similar curves.
incrementally up to 700 kPa, unloaded incrementally,
saturated at minimum loading (the weight of the piston 3.3 Swelling pressure at a constant volume
of the apparatus) and loaded incrementally up to versus free swelling at constant loading
700 kPa with free access to water.
• Saturation under loading (Scenario III)—samples with The incrementally loaded oedometric test revealed the
natural water contents were loaded incrementally up to importance of the stress path on the evolution of pressure.
700 kPa, saturated at 700 kPa, unloaded incrementally Further research was subsequently conducted aimed at the
with free access to water, and loaded incrementally up investigation of the influence of the stress path on the
to 700 kPa with free access to water. swelling pressure.
A series of single-stage free swelling under constant
Figure 8 illustrates the results of Scenario I, Fig. 9 those
load tests were also conducted. Compacted samples (three
of Scenario II and Fig. 10 those of Scenario III. The results
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Fig. 7 Saturation development of the BCV 2017 over time (BEACON deliverable D4.1)
initial densities were considered) were positioned in the 4 THM hypoplastic double-structure model
oedometer, loading was applied (up to 7 different loads) for bentonite
and saturation initiated. The final density was determined
once the deformation process had stabilised. The BCV dataset discussed in the previous section was
Figure 11 presents a comparison of the results of the adopted for the evaluation of a THM hypoplastic double-
constant volume cell testing (shown in red in the figure; structure model for bentonite. The model was developed by
data taken from Fig. 5) and the measurements obtained for Mašı́n [16] via the hierarchical enhancement of an earlier
free swelling under loading (shown in green in the figure). model by Mašı́n [15] that did not consider the effects of
The arrows commence at the initial dry density and end at temperature. The earlier model comprised, in turn, the
the final dry density (the blue arrows represent the relevant double-structure enhancement of earlier hypoplastic mod-
saturation phase from the oedometric tests described in the els for unsaturated and saturated soils. Interested readers
previous subchapter). are urged to refer to these references for details of the
The data clearly indicates a significant systematic dif- creation of the models. In contrast to the model version of
ference between the values of the attained swelling pres- Mašı́n [16], an additional enhancement that replaced the
sure. If deformation is allowed during saturation and original bi-linear form of the water retention curve by a
swelling, the swelling pressure is lower than the constant smooth formulation was introduced to the latest model. For
volume for the same final dry density. Mathematical reasons of conciseness, the reader is referred to Mašı́n [16]
material models need to take this factor into account. for the complete model formulation. Here, only the chan-
ges in the formulation of the model from Mašı́n [16] are
123
123
Fig. 10 Scenario III - saturation at full loading (after dry loading cycle)
Fig. 11 Comparison of the swelling pressure - Urestricted swelling under constant load vs Swelling pressure at constant volume
123
123
1 rk
a_scan ¼ s_ ð4Þ
sD ð1 ae Þ
where r k represents the ratio of the scanning curve slope (in
the lns vs. lnSr plane) and the slope of the main drying and
wetting curves. For the original model, this ratio was given
by:
8
>
> 1 for s ¼ sD and s_ [ 0
<
1 for s ¼ ae sD and s\0
_
rk ¼ k ð5Þ
>
> pscan
¼ 0:1 otherwise
:
kp
123
Fig. 14 Evolution of the degree of saturation in the THM hypoplastic model during the cyclic water retention test. Comparison of the original bi-
linear logarithmic formulation (right) with the new smooth formulation (left)
Figure 15 (left) presents predictions of the oedometric for BCV bentonite, the experimental results for B75 ben-
loading–unloading experiments conducted on saturated tonite tested at the CTU were simulated. It was assumed
BCV bentonite performed at the CU; they demonstrate the that the unconfined compression strength of the two types
good level of representation of the loading–unloading of bentonite (extracted from the same deposit) would not
behaviour. The samples were prepared by means of the differ substantially. Cylindrical samples with aspect ratios
compaction of the bentonite powder to a dry density of of 1:1 were tested at various dry densities and an initial
1270 kg/m3, which swelled under oedometric conditions at water content of 6%, corresponding to a suction of
a constant load of 10 kPa and was subsequently subjected 100 MPa for the B75 bentonite. The experiments were
to oedometric loading–unloading. In this case, only the simulated using the BCV parameters and an initial suction
saturated loading–unloading phase was simulated (a com- value of 100 MPa. It should be stressed that while the
parison of the predictions of the swelling-loading–unload- model considers the strength parameter critical state fric-
ing oedometric tests with various path combinations is tion angle uc , the assumed effective stress for the
presented later in Fig. 23; the figure shows the void ratio macrostructure, calculated using the following Eq. (8), is
e with respect to the vertical stress rv). Although initially key to the uniaxial compressive strength calculation:
highly pre-consolidated, the samples almost immediately rM ¼ rnet 1SM ð8Þ
r s
attained normal compression lines, thus demonstrating that
the swelling process led to a decrease in the apparent pre- The unconfined strength evinced a good level of repre-
consolidation. The model provided a good representation sentation for the lower dry density sample, whereas it was
of both the loading and unloading stiffness. slightly underestimated for the higher dry density samples.
Figure 15 (right) shows the predictions of the uniaxial The reasonably good uniaxial compressive strength pre-
compression experiments conducted on unsaturated com- dictions thus indicate the suitability of the adopted effec-
pacted bentonite. In this case, since no data was available tive stress formulation.
Fig. 15 Predictions of the oedometric loading–unloading testing of saturated BCV bentonite (left) and the uniaxial loading experiments on
unsaturated compacted B75 bentonite at a water content of 6% (right)
123
The accurate prediction of the high uniaxial compressive demonstrated in Fig. 19, which shows the value of the state
strength can be explained with the assistance of the pre- variable relative void ratio re, where a value of 1 indicates
dictions of the water retention curves. Compacted bentonite that the normal compression line state has been attained. It
with three differing initial dry densities (1200, 1600 and is important to note that the prediction of irreversible
1900 kg/m3) was tested under constant volume (Fig. 16) microstructural deformation was a consequence of the high
and unconfined (Fig. 17) conditions. Note that the uncon- swelling properties of BCV bentonite, a factor that was not
fined WRC curves were calculated with a higher parameter so pronounced in the calibration of the model for other
N (see Table 3 for the definition thereof) value of 1.67, bentonites. However, it has not been physically substanti-
since the original value of 1.62 led to divergence. While ated and should be corrected in future versions of the
under the unconfined conditions, the model slightly model.
underpredicted the water content and the degree of satu- A further indicator considered in the model concerned
ration, the trends concerning the effect of dry density were the macrostructural effective stress. The Bishop effective
well predicted, including a lower water content at low stress equation was adopted in the model for the
suctions for the high dry density samples than for the other macrostructure with a factor v equal to the macrostructural
two tests. Less satisfactory predictions were, however, degree of saturation SM r . As already mentioned, in order to
produced by the free swelling experiments; although the predict the high uniaxial compressive strength of com-
drying curves were represented reasonably well, the water pacted bentonite, SM r must be assigned a non-negligible
content was significantly underestimated in the wetting (albeit low) value even for high suction values (see
curves. The reason for this discrepancy is as follows. Since Fig. 18). This non-negligible effective stress contributes to
the macrostructural water content was relatively low the irreversibility of the microstructural void ratio (the
(Fig. 18), the behaviour was predominantly affected by enhanced effective stress shifts the state towards the nor-
that of the microstructure and, since the microstructure was mal compression line, which subsequently limits the
considered to be fully saturated, the water retention curves microstructural swelling) and, moreover, limits the swel-
were primarily affected by the microstructural void ratio. ling potential, which is predicted reasonably well by the
Since the microstructural response was considered to be model (Fig. 20). It should be noted at this point that the
reversible in the model, the water retention curves should experimental evidence indicated a dry macrostructure for
have exhibited a low degree of hysteresis, i.e. from the higher suction values, which was clear from both the
macrostructural part only (Fig. 18). However, since BCV is ESEM images [18] and from the fact that the water content
a highly swelling bentonite, the slope of the microstructural of bentonite at higher suctions is known to be independent
swelling line is in fact close to that of the normal com- of the dry density (e.g. [17]. Thus, relating the high
pression line. Moreover, since the macrostructural effective strength of compacted bentonite with the macrostructural
stress is non-negligible so as to ensure the correct predic- degree of saturation SM r (a concept that originated from the
tion of the uniaxial compression strength (Fig. 15), the idea that the matric suction strengthens the inter-aggregate
state approaches the normal compression line during the contacts through water menisci) appears to be a simplifi-
wetting process (which is considered to be the boundary of cation of reality, since other physico-chemical phenomena
the microstructural swelling in the model), thus breaching also play a role at the inter-aggregate contact points. These
the reversibility of the microstructural deformation. This is
Fig. 16 Predictions of the water retention tests for compacted BCV bentonite under constant volume conditions at three differing initial dry
densities of 1200, 1600 and 1900 kg/m3
123
Fig. 17 Predictions of the water retention tests for compacted BCV bentonite under free swelling conditions at three differing initial dry densities
of 1200, 1600 and 1900 kg/m3 (calculated applying N = 1.67)
Fig. 18 Predictions of the macrostructural quantities (macrostructural water content and macrostructural degree of saturation) for the water
retention testing of compacted BCV bentonite under free swelling conditions at three differing initial dry densities of 1200, 1600 and 1900 kg/m3
(calculated applying N = 1.67)
123
Fig. 20 Predictions of the swelling pressure tests (left) and the oedometric swelling under constant load experiments at three differing initial dry
densities (right) of the unsaturated compacted BCV bentonite
Fig. 22 Comparison of the predictions of the selected swelling pressure tests and the oedometric swelling experiments for the constant load test.
The tests selected are indicated by yellow circles in Fig. 21
123
123
123
Fig. 27 Swelling pressure experiment at a dry density of 1597 kg/m3 from Fig. 24 compared with an identical experiment with a bottom
saturation pressure of 1 kPa
Table 4 Values of the parameters of the THM hypoplastic model for 745942) and research Project No. TK01010063 awarded by the
BCV bentonite Technology Agency of the Czech Republic. The second author is also
grateful for the institutional support provided by the Centre for
Parameter Unit Value Geosphere Dynamics (UNCE/SCI/006).
uc 25
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jm – 0.1
sr kPa -1000
em – 1.0
r0 References
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