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Exa 2
Exa 2
Abstract: In a Swedish repository for the disposal of heat-emitting waste, the long-term thermal
stability of the bentonite engineered barrier forms a key component of the safety case. Central to
such consideration is the evolution of hydraulic permeability and a potential degradation of hydrau-
lic properties, in response to prolonged thermal exposure of the clay. To address this issue, a
detailed programme of laboratory-based experiments has been undertaken at both the British Geo-
logical Survey and Studiecentrum voor Kernenergie/Centre d’Etude de L’Energie Nucleaire, in
order to examine the hydraulic behaviour of bentonite that had previously been exposed to elevated
temperatures. Hydraulic properties were calculated from both steady-state pressure gradients and
from analysis of the pressure transients. Inspection of the data found no significant difference
in hydraulic behaviour between the virgin material and clay samples taken from the Canister
Retrieval Test. Based on these observations, the authors find no evidence for an adverse increase
in hydraulic conductivity of bentonite as a result of prolonged thermal exposure to temperatures
of 80 8C.
Gold Open Access: This article is published under the terms of the CC-BY 3.0 license.
The thermal alteration of clay minerals resulting represent a major alteration of the smectite com-
in the transition of smectite to illite is a well- ponent in the bentonite and would compromise
established phenomenon and has been empirically repository safety performance.
observed by numerous researchers in the past (e.g. However, this work is in direct contradiction to
Velde et al. 1986; Bruce et al. 1987; Freed & earlier results presented by Pusch (1985), who,
Peacor 1989; Velde & Vasseur 1992; Lanson et al. after examining bentonite samples from the buffer
2009; Mosser-Ruck et al. 2010). A review of mass test (BMT) performed at Stripa in the early
thermal stability of bentonite is given by Meunier 1980s, reported no significant changes in perme-
et al. (1998). If such a reaction were to occur in a ability and concluded that ‘the influence of heating
repository for heat-emitting waste, this thermally was insignificant and that the important physical
driven alteration and restructuring of the clay lat- properties, swelling and permeability, were not
tice to a lower swelling form of clay mineral altered’. While temperatures in the BMT were
would have a profound impact on the hydrome- higher than those reported in the CRT (i.e. 125 v.
chanical and geochemical properties of the resul- 80 8C, respectively), the test was of much shorter
tant material. There is no single thermal activation duration (i.e. 1 year as opposed to 5 years for the
energy for such reactions to occur, as these pro- CRT). Villar & Gómez-Espina (2009) performed
cesses are highly dependent on the geochemistry a series of hydraulic tests on Febex bentonite com-
of the system (e.g. Mosser-Ruck et al. 2010). How- pacted to a range of dry densities from 1.5 to
ever, recent work by Pusch et al. (2010) suggests 1.7 m3 mg21. While no consistent results were
that early-onset hydraulic degradation (i.e. an obtained, permeability was seen to increase with
increase in hydraulic permeability) can occur in temperature. However, while the increase in perme-
compact bentonite subject to prolonged tempera- ability could not solely be explained by changes in
tures of only 80 8C. While the experimental detail viscosity, the magnitude of permeability increase
underpinning these observations is unclear, the was an order of magnitude less than that report by
authors report a two order of magnitude increase Pusch & Weston (2012), and no consistent behav-
in permeability for two clay samples taken from iour was observed.
the Canister Retrieval Test (CRT) test performed To investigate this issue, an independent pro-
at the Äspö underground research laboratory. If gramme of laboratory-based experiments was
correct, such an increase in permeability would undertaken in parallel at the British Geological
From: Norris, S., Bruno, J., Cathelineau, M., Delage, P., Fairhurst, C., Gaucher, E. C., Höhn, E. H.,
Kalinichev, A., Lalieux, P. & Sellin, P. (eds) 2014. Clays in Natural and Engineered Barriers for Radioactive
Waste Confinement. Geological Society, London, Special Publications, 400, 589– 601.
First published online May 12, 2014, http://dx.doi.org/10.1144/SP400.31
# 2014 The Authors. Publishing disclaimer: www.geolsoc.org.uk/pub_ethics
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Survey (BGS) and Studiecentrum voor Kernenergie where Ss (m21) is the specific storage, K (m s21) is
(SCK-CEN), to examine the hydraulic behaviour the hydraulic conductivity, h (m) is the hydraulic
of bentonite exposed to elevated temperatures. head and x (m) is distance in the flow direction.
To prevent bias and to ensure impartiality, the This equation must be solved subject to the bound-
studies were conducted in isolation. Complemen- ary conditions:
tary approaches were adopted by each institute Q ∂h
(described below) to measure hydraulic permeabil- q = = −K (2)
ity under a range of test conditions. In an attempt As ∂x x=0
to replicate the experiments of Pusch et al. (2010),
and
preserved test material was taken from a number
of locations within the same CRT experiment. In h = 0 at x = Ls (3)
addition, a control sample of ‘virgin’ bentonite, sup-
plied by Clay Technology AB, was examined to where q (m s21) is the Darcy velocity, Q (m3 s21) is
define the hydraulic properties of unaltered mate- the volumetric flow rate, As (m2) and Ls (m) are the
rial without thermal loading. cross-sectional area and length of the specimen,
To minimize perturbation of the clay during respectively. Hydraulic head is related to the pore
testing, the BGS opted to perform a series of long- pressure, P (Pa), by
term controlled flow-rate experiments in which the
P
magnitude of the hydraulic gradient imposed across h= (4)
each sample is a dependent variable, simply related rw g
to the volumetric flow rate. In these tests, head
gradient is allowed to slowly evolve in response to where rw (kg m23) is the density of water and g
the imposed flow rate. As such, if hydraulic per- (¼9.81 m s22) is the acceleration due to gravity.
meability had increased owing to thermal degra- The head at x ¼ 0 and flow at x ¼ Ls as functions
dation of the buffer, then the differential pressure of time were obtained by numerically inverting the
for a given flow rate would scale accordingly, result- Laplace transform solution given in Appendix 1.
ing in proportionately smaller differential pres- Five parameters are required to define the solution.
sures. Ascending and descending flow cycles were Three are experimentally determined: Q, As and
imposed across each sample to examine any under- Ls. The remaining two are the material proper-
lying hysteresis while the specimen was subject to ties that the test is designed to determine (i.e. K
a fixed backpressure. and Ss). In order to estimate the values of these
At the same time, a complimentary programme parameters, a general nonlinear least squares fit-
of constant pressure tests was performed at SCK- ting routine was used to minimize the differences
CEN. In these experiments flux in and out of between the calculated curves and the measured
the sample was carefully controlled by two high- head data.
precision syringe pumps, in order to accurately Hydraulic conductivity was also calculated
measure hydraulic behaviour under steady-state from the head gradient at steady state, enabling the
conditions. As part of the test programme exper- two values to be compared. Permeability, k (m2),
iments were performed for different durations to
examine the impact of calculating permeability
under non-equilibrium conditions during the transi-
ent phase of testing. An attempt was also made to
measure the hydraulic conductivity using a much
smaller gradient, that is, a 1 m water column to
investigate what effect, if any, this may have on
permeability.
Data reduction
Data were transferred to a spread sheet for proces-
sing and plotting. Hydraulic transients were very
well-defined and largely free of experimental noise.
The one-dimensional equation of flow is Fig. 1. Cut-through isometric diagram of the test vessel
showing the location of the injection and backpressure
ports, position of sintered filters and location of cap
screws. One end-closure is shown removed from of the
∂h ∂2 h
Ss =K 2 (1) bore of the vessel to illustrate individual
∂t ∂x system components.
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Fig. 2. Schematic of the high pressure ‘constant head’ experimental set-up with syringe pump.
was calculated from hydraulic conductivity using Constant volume apparatus (BGS)
the relationship
Figure 1 shows a schematic of the constant volume
K hw permeameter designed and commissioned specifi-
k= (5)
rw g cally for this experimental study. In this geom-
etry the specimen is volumetrically constrained,
where hw is the viscosity of water (¼0.001002 preventing dilation of the clay in any direction. The
Pa s). apparatus consists of four main components: (a) a
thick-walled dual-closure stainless steel pressure
Experimental system vessel; (b) a fluid injection system; (c) a backpres-
sure system; and (d) a data acquisition system oper-
Independent laboratory studies were undertaken at ating within a LabViewTM environment. Pressure
the BGS and SCK-CEN on supplied samples of in the injection and backpressure circuits is con-
compact bentonite. Each laboratory performed a tinuously monitored through independent pressure
series of flow measurements using custom-designed transducers providing a check on system pres-
apparatus imposing a constant volume boundary sures. Testing was performed in an air-conditioned
condition. These systems are described in detail laboratory at a nominal air temperature of around
below. 20 + 0.5 8C.
Fig. 3. Schematic of the low pressure ‘constant head’ experimental set-up using water columns to set the gradient.
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Fig. 4. Schematic layout of the Canister Retrieval Test, CRT (Eng 2008). Temperature (T), pressure (P), pore
pressure (U) and relative humidity (W) sensors were located in five of the blocks. Outputs from these devices were used
to track the state of hydration within the clay. Samples for this study came from rings R7 and R8. Copyright SKB.
The pressure vessel is comprised of a dual- digital control unit. The position of each pump
closure tubular vessel manufactured from 316 stain- piston is determined by a digital encoder with
less steel rated to 70 MPa. Each end-closure is each step equivalent to a change in volume of
secured by 12 high-tensile steel cap screws that 4.8 nL, yielding a flow accuracy of 0.5% of the
can also be used to apply a small pre-stress to the set-point. Movement of the pump piston is con-
specimen if required. The 60 mm internal bore of trolled by a micro-processor, which continuously
the pressure vessel is honed to give a polished monitors and adjusts the rate of rotation of the
surface. Each end-closure has a dedicated port encoded disc using a DC-motor connected to the
through which the pressure in each of the filters piston assembly via a geared worm drive. This
can be independently monitored. allows each pump to operate in either constant
Volumetric flow rates are controlled or moni- pressure or constant flow modes. A programme
tored using a pair of high-precision ISCO-100, written in LabVIEWTM elicits data from the pump
Series DM, syringe pumps operated from a single at pre-set time intervals of 2 min.
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Table 1. Shows the basic physical properties of all test samples prior to testing assuming a specific gravity for
the mineral solids of 2.77 mg m23
Inspection of the table indicates all samples started with a slight degree of desaturation ranging from 95 to 98% for ring 8 and from
90 to 93% for ring 7 (the latter measurements are based on off-cut material from the neighbouring core).
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Table 2. Flow in and out, injection and backpressure and head gradient for each test stage of
sample CRT-1 at steady-state
Inspection of the data indicates a good mass balance between flow in and out with difference less than or equal to 0.3 ml h21.
Fig. 6. Flow into specimens CRT-1 to -3 during the initial EQ stages (Table 2). Positive flow represent uptake of
distilled water by the specimens. Inspection of the data indicates the bulk of the inflow occurs within the first 5 days
which then tails off to near zero flow from 12 days onwards.
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Fig. 7. Flow and pressure data for tests CRT-1, -2 and -3 respectively. Inspection of the data shows well-defined
transients leading to steady-state conditions. Discrete spikes in data in [1] relate to small temperature fluctuations within
the laboratory. Problems with the air conditioning system between 100 and 107 days resulted in a considerable noise
within the data. However, projection of the flux and pressure asymptotes prior to this event suggests that it had no long
term deleterious effect on the data.
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Table 3. Hydraulic properties based on steady-state and transient analysis of the data, showing
hydraulic permeability and specific storage values for each test stage
a control. Cylindrical test specimens with an exter- of compact bentonite. Each test comprised a series
nal diameter of 60 mm were manufactured by a of stages (Table 2) designed to initially hydrate,
combination of hand-trimming using a tubular for- equilibrate and then determine baseline hydraulic
mer with a sharpened leading edge (Horseman & behaviour. During the initial EQ stage, the speci-
Harrington 1994) and machine lathing (Harrington men is exposed to distilled water on both faces of
et al. 2012). Sample lengths were 53.9, 60.0 and the core, with the same pressure at either end of
59.7 mm, respectively, for samples CRT-1, CRT-2 the sample. A constant flow rate (CFR) stage is
and CRT-3. used to evaluate permeability and involves pump-
Table 1 shows the basic physical properties ing distilled water through the filter disc at low vol-
of the test specimens. Porosity and degree of satur- umetric flow rates, with the same solution as the
ation are based on an average grain density of backpressuing fluid at the downstream end. Spe-
2.77 mg m23. Post-test measurements of saturation cific storage is defined by numerical modelling of
indicate the samples were fully hydrated. This is the flow transients.
confirmed by measurements of inflow during the During each equilibrium stage the sample
equilibrium (EQ) stages of each test. rapidly hydrates, exhibiting a well-defined transient
leading to a near-zero flow condition after around 13
SCK-CEN days (Fig. 6). By the end of each EQ stage, volume-
tric flow into the clay had reduced to an average flux
SCK-CEN received samples from ring 7 of the of less than 0.1 ml h21. Post-test measurements of
CRT at 2258. Samples were taken at 665, 765 and saturation indicate that all test samples were fully
790 mm radial distance. At each of these distances hydrated.
samples were taken, from which cylindrical cores Table 2 shows steady-state values for flow in
with a diameter of 38 mm were prepared using a and out of the specimens as well as injection and
lathe. Samples with a length of 20 mm were pre- backpressure pressures for each stage of hydraulic
pared to measure bulk density and water content testing (Fig. 7). The small discrepancy between
and the derived properties as given in Table 1. fluxes relates to minor leakage (≤0.3 ml h21) from
Samples 50 mm long were prepared for the hydrau- one of the test systems. To accommodate this,
lic conductivity measurements. hydraulic properties for all specimens have been
calculated for both inflow and outflow data
(Table 3). Transient analysis of the pressure data
Results has been undertaken in a similar manner, yielding a
Controlled flow rate experiments (BGS) second estimate for conductivity/permeability and
an indication for the specific storage of the sam-
A series of well-constrained hydraulic measure- ples (Table 3, Fig. 8; Appendix 1). Examination
ments were undertaken by BGS on three specimens of the conductivity data shows little variation in
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Fig. 8. Typical fits for hydraulic transient data (for CRT-1) based on backpressure flow rates. Plot [1] yields a good
fit between predicted and measured pressures. In plot [2] there is a fairly good correlation between predicted and
measured flux though some of the detail of the transients are less well-represented by the model. To improve model fits,
data from test stages were individually fitted using an automated least-squares procedure optimized against the injection
pressure (presented in Table 3).
values between the data processing methods, indi- provides no evidence for the alteration of bentonite
cative of the quality of the raw data and the good following sustained thermal exposure of up to 5
mass balance obtained during hydraulic testing. years in duration. This observation is supported by
Based on analysis of the complete dataset Dueck et al. (2010) who also noted similar results
(including analysis of the transient data), for fluxes for tests on CRT material.
in the range 1.6–4.6 ml h21, the mean hydraulic In these tests, head gradient was allowed to
permeability is 4.7 × 10221 m2 (standard devia- slowly evolve during each test stage as a dependent
tion ¼ 0.4 × 10221 m2). The mean specific storage variable, simply related to the volumetric flow rate.
(Ss) for the same range of flux is 1.5 × 1025 m21 As such, if hydraulic permeability had increased
(standard deviation ¼ 0.5 × 1025 m21). These owing to thermal degradation of the buffer (Pusch
small standard deviations clearly demonstrate very et al. 2010), then the differential pressure for a
little variation in permeability across the range given flow rate would scale accordingly, resulting
of flow rates imposed. Inspection of the data in proportionately smaller differential pressures.
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Fig. 9. Flow in and out of the specimens plotted against head gradient. A small amount of hysteresis in flow between
advancing and decreasing cycles is observed in the data. Extrapolation of the results towards the y-axis indicates no
significant threshold (i.e. non-Darcian behaviour) to flow.
A cross plot of flow rate against head gradient Constant head: controlled flow rate
(Fig. 9) clearly shows that large head gradients are experiments (SCK-CEN)
a necessary requirement for the movement of very
small volumetric flow rates across the sample. The Flow data for the sample CRT-6 (R7-225-790) at
data exhibits only minor hysteresis between increas- 1 MPa inlet pressure are shown in Figure 10. The
ing and decreasing flow cycles. While controlled cumulative inflow during the first 25 days was
flow rates were varied from 1.6 to 4.6 ml h21, significantly higher than afterwards. It was also sig-
values for head gradient (a dependent variable in nificantly higher than the outflow even when taking
this study) ranged from 3150 m m21 (at the lowest into account the evaporation at the outlet. This
flow) to 9131 m m21 (at the highest). Linear regres- clearly shows that the sample was not fully saturated
sion of the data in Figure 9 yields threshold values at the onset of testing and that, when subject to
close to zero, indicating the bentonite exhibits relatively modest injection pressures of 1.0 MPa,
little if any significant threshold (i.e. non-Darcian can take 90 days or more to reach full saturation.
behaviour) to hydraulic flow. This observation is The initial degree of saturation of the samples was
supported by recent work by Villar & Gómez- found to be between 90 and 93%. This may relate
Espina (2009) who undertook a series of hydraulic to desiccation during sample preparation (drying
and hydromechanical tests for a range of clay den- during adjustment on the lathe) or reflect the state
sities at varying temperature. Their results, for of saturation of the material as shipped. However,
clays with similar dry density, yielded only one what is clear is that, owing to the resaturation of the
test where flow was not detected. This observation, samples in the first month, the derivation of hydrau-
performed at a low hydraulic gradient, may reflect lic conductivity during this time would result in
the resolution of the measurement system rather an overestimation of the fully saturated hydraulic
than a true threshold to flow. conductivity/permeability values (Table 4). As
Table 4. Hydraulic properties derived from constant head experiments on samples CRT-4 to 6
Pusch et al. (2010), as a result of thermal expo- Substituting using equation (A7) and re-arranging,
sure of the clay to temperatures of 80 8C for up we have
to 5 years. q 1 e(−lL)
A=− (A9)
K l p (e( lL) + e(−lL) )
Funding for this study was provided by the Swedish
Nuclear Fuel and Waste Management Co. (SKB). This and
paper is published with the permission of the Director, q 1 e(lL)
British Geological Survey (NERC). B= (A10)
K l p (e(lL) + e(−lL) )
Thus we may write the Laplace transform of the head at
x ¼ 0 as
Appendix 1
q
h(x = 0) = tanh (l Ls ) (A11)
Kpl
Consider a specimen of length Ls and cross-sectional area
As with hydraulic head initially everywhere at zero. A fluid Similarly, we may write the Laplace Transform of the
flow of Q is initiated at t ¼ 0 into the specimen at the end flow at x ¼ Ls as
x ¼ 0 and the response of the hydraulic head at x ¼ 0 is
∂h q
sought as a function of time. q(x = Ls ) = −K
= (A12)
∂x x = Ls p cosh (lLs )
The equation of one-dimensional flow is given by
The head at x ¼ 0 and flow at x ¼ Ls as functions of time
∂h ∂2 h are obtained by numerically inverting the Laplace trans-
Ss = K 2 (A1) form solutions given in equations (A11) and (A12) using
∂t ∂x
the method of Talbot (1979). Five parameters are required
where Ss is the specific storage, K is the hydraulic conduc- to define the solution. Three are experimentally deter-
tivity and h is the hydraulic head. This equation must be mined: Q, As and Ls. The remaining two are the material
solved subject to the boundary conditions properties that the test is designed to determine (i.e. K
and Ss). In order to estimate the values of these parameters,
Q ∂h
= −K
a general nonlinear least squares fitting routine was used to
q= (A2)
As ∂x x = 0 minimize the differences between the calculated curves
and the measured head data.
and
h = 0 at x = Ls (A3)
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