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Transp Porous Med (2010) 81:277293

DOI 10.1007/s11242-009-9398-x

Characterizing the Gas Permeability of Natural


and Synthetic Materials
C. Barral L. Oxarango P. Pierson

Received: 30 July 2007 / Accepted: 13 April 2009 / Published online: 6 May 2009
Springer Science+Business Media B.V. 2009

Abstract The objective of this article is to propose an experimental method to compare


the gas permeability of all the different materials used as gas barrier, such as compacted clay
liners or geomembranes. This method is based on the falling pressure experiment, allowing
the determination of a single coefficient whatever the material tested. This coefficient is the
time constant , which is obtained by analytical solutions of the simplified equations describing the transport of gas through the material. The domain of validity is specified for porous
media, thanks to a numerical solution of the complete equations system. Two applications
are presented, showing the applicability of the method on compacted clay liners and on high
density polyethylene geomembranes.
Keywords Falling pressure experiment Gas permeability Numerical solution
Clay Geomembrane

1 Introduction
Gas movement in soils is of particular interest in many fields, including agriculture, petroleum
engineering, and environmental protection (Springer et al. 1998). For example, in the case
of municipal solid waste facilities, to avoid gas emission from landfill into the atmosphere
and to recover this gas for energy production purposes, waste is covered over by a variety
of materials. Such materials, used as barrier to rainwater seeping and biogas emission, are
as diverse as compacted clay liners (CCL), geosynthetic clay liners (GCL: manufactured

C. Barral L. Oxarango P. Pierson (B)


LTHE (UMR 5564 CNRS/INPG/IRD/UJF), University Joseph Fourier, BP 53, 38041 Grenoble Cedex 9,
France
e-mail: patrick.pierson@ujf-grenoble.fr
C. Barral
e-mail: barral.camille@free.fr
L. Oxarango
e-mail: laurent.oxarango@bvra.ujf-grenoble.fr

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sandwiched clay between two geotextiles), bituminous, or synthetic geomembranes (Didier


et al. 2000).
In such applications, where engineers and designers must select one or several materials,
it is very difficult to compare their permeability characteristics, since they may correspond
to different kinds of flow, mainly convective or diffusive flow, corresponding to different
physical laws. Lots of permeability tests, described in Sect. 2, allow the determination of
different coefficients characterizing the gas permeability, but do not allow the comparison of
all the materials used as gas barriers.
The objective of this study is to propose a method to determine a single quantity to characterize the gas permeability of any liner, whatever its porosity, under specific experimental
conditions, in the laboratory.
A brief review of the phenomenological background concerning gas migration through
different types of materials and of the corresponding tests is first presented (Sect. 2), where
the falling pressure experiment appears to be adapted to all the materials tested. A solution
of the equations describing gas transport during the falling pressure experiment is then
proposed in two cases:
(1) The case of pure convective gas flow described by Darcys law (Sect. 3): A simplified
solution is here proposed, the conditions of acceptance of which are given in Sect. 4,
thanks to a numerical study.
(2) The case of pure diffusive flow described by Ficks law (Sect. 5): The method is then
applied to an experimental study conducted on compacted clay and to an HDPE (high
density polyethylene) geomembrane (Sect. 6).

2 Gas Permeability Measurement Background


2.1 Phenomenological Aspect
The main driving force which is the cause of gas migration can be the total pressure gradient
or the concentration gradient, depending on the porous structure of the material: pore size,
connectivity, and tortuosity, . . . (Rowe et al. 1995; Vangpaisal and Bouazza 2004):
(1) In porous media such as unsaturated soils, in the absence of possible transport by
advection with flowing water, the gradient of the total gas pressure p in the voids of the
material is generally the main driving force (Bouazza and Vangpaisal 2003). The onedimensional flow of gas (convective flow), considered here as ideal gas, in isothermal
conditions and when gravitational effects are neglected, can be described by the extended
Darcys law (1). Therefore, the application of the model is limited to the cases where
inertia is negligible compared to the viscous effects. It corresponds to a Reynolds number of less than 6 (Yu 1985). For instance, it is confirmed for landfill gas migration if
the characteristic grain sizes of the porous medium are smaller than 2 mm (McBean et al.
1995):
q(z, t) =

k dp(z, t)

dz

(1)

where q(z, t) is the gas volumetric flux (Darcy velocity: m/s), is the dynamic viscosity (Pi),
dp(z, t)/dz is the gas pressure gradient (Pa/m) in the material along the one-dimensional gas
flow (z), and k is the effective gas permeability coefficient (m2 ).
Here, k potentially depends on the medium water saturation (through relative permeability effect for instance, Dullien 1979). It may also include slip flow effect, the so-called

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Klinkenberg effect, even if it is generally neglected in landfill application (Brusseau 1991;


Vangpaisal and Bouazza 2004). Thus, k characterizes the gas permeability of a material at a
given water content and in a given gas pressure condition.
(2) In media such as highly saturated fine-grained soils (Aubertin et al. 2000) or synthetic
geomembranes, the main driving force is the concentration gradient of each constituent i
of the gas in the material. It means that each constituent of the gas flows differently in the
material, while the Darcy velocity is negligible (diffusive flow). The one-dimensional mass
flow qmi (z, t) (kg/(m2 s) of the constituent of interest i can here be described by Ficks law
(or the law of diffusion):
dcmi (z, t)
,
dz

qmi (z, t) = Di

(2)

where Di is the diffusion coefficient (m2 /s) and cmi is the concentration of the permeant i
in the material (kg/m3 ).
Since the permeant concentration cmi (z, t) in the material m is much more difficult to
measure than the permeant concentration c f i (t) in adjacent fluids f , Eq. 2 is also often
approached by considering the quantity of permeant qmi (t) which migrates from one side of
the material to the other side, as a function of the difference in the concentration c f i (t) of
the permeant in the adjacent fluids (Sangam and Rowe 2001; Pierson and Barroso 2002):
qmi (t) = Pi

c f i (t)
,
L

(3)

where L is the material thickness (m) and Pi is a permeability coefficient (m2 /s). Pi is a function of the diffusion coefficient Di and takes also into account the absorption and desorption
phenomena of the permeant into and from the material, respectively. In the simplest case
where the material is in contact with adjacent fluids for sufficient time at a constant temperature and where the permeant does not interact with the material (which is the case for HDPE
geomembranes for example), Pi and Di are related by the Eq. 4 (Sangam and Rowe 2001),
corresponding to a linear isopleth (cmi = Sm f i c f i ):
Pi = Sm f i Di ,

(4)

where Sm f i is the partitioning coefficient, which is supposed to be a constant at the upstream


and downstream surfaces of the specimen tested, for the couple (materialpermeant). This is
valid in the case of a similar fluid on both sides and if the concentration difference c f i (t)
remains small (Aminabhavi and Naik 1998).
Equation 3 may also be written according to the difference pi (t) of the permeant partial
pressure in the adjacent fluids (Pa) (Rogers 1985):
qmi (t) = Pi

pi (t)
,
L

(5)

where Pi is the permeability coefficient of permeant i in the material, expressed in s.


Comparing the gas permeability of such different materials is a difficult goal, since the
transport mechanism is different from one material to another one, with generally, a combination of both mechanisms.
(3) Two transfer mechanisms have been pointed out. The convective mechanism, described
by the Darcy law, is associated with the momentum balance (Whitaker 1999). On the other
hand, the diffusive mechanism, described by the Fick law, is associated with the species
mass balance of a given gas component. The transported quantities are obviously not of the
same type even if both regimes lead to a transfer of the gas through the porous medium. In

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order to evaluate the transition between the two regimes (i.e., a regime including both transfer mechanisms), the advective/diffusive transport of the studied chemical species has to be
considered. This means that the transport of the chemical species by the flow average velocity
is not negligible. The relative weight of this advective mechanism is usually compared to the
diffusive mechanism with the macroscopic Peclet number:
Pe = u L/(Di0 ),

(6)

where u is a characteristic velocity at the macroscale, L is a representative length of the specimen (for instance its thickness), is the material porosity, and Di0 is the diffusion coefficient
in air.
This Peclet number evaluates the average advection within the pores using an averaged
pore velocity u/. The velocity u can be estimated from the total gas volume passing through
the specimen during a characteristic time of the experiment. The diffusion intensity is estimated as the diffusion of the considered gas in the air that fills the pores. This assumption
tends to overestimate the diffusion, since it does not take into account the effect of tortuosity
that can be very sensitive in low-porosity materials. The diffusive regime occurs for Pe  1,
while the advective regime corresponds to Pe  1. In the transition region around Pe = 1,
both mechanisms are of the same order of magnitude. In the framework of this article, the
attention is focused on the low Peclet number regime that is described by a purely diffusive
model and the high Peclet number regime. In this last case, the effects of molecular mixing
are not considered anymore and the overall gas flow is only studied with the Darcy law.
For intermediate Peclet number, the effective permeability and the effective diffusion coefficient have to be determined together. Moreover, dispersion effects are likely to introduce
a potentially non-linear dependance between these coefficients. As far as the experimental characterization of transfer in porous media is concerned in this article, changing the
operating conditions appears to be preferable if the experiment appears to be realized in the
transition regime. Indeed, the determination of two coupled parameters generally increases
drastically the experimental errors and requires a heavier experimental process.
2.2 Experimental Aspect and Different Tests
(1) There are many methods and tests used to characterize natural soils, based on the extended
Darcys law (1) and determining the effective gas permeability k:
Tests are generally conducted in a steady state on unsaturated soils (Eischens and Swanson
1996; Samingam et al. 2003), rocks (Cosse 1996), geosynthetic clay liners (Didier et al.
2000; Shan and Yao 2000; Bouazza and Vangpaisal 2003; Vangpaisal and Bouazza 2004),
or cement-based materials (Gall and Daian 2000; Loosveldt et al. 2002). Results show that
when the water content increases, corresponding to a lower volume available in the material for gas migration, measurement becomes more and more difficult, leading to relative
uncertainties of up to 100% when the water content is over 100% in geosynthetic clay liners (Shan and Yao 2000; Bouazza and Vangpaisal 2003). Gall and Daian (2000) obtain an
important dispersion of permeability values (four orders of magnitude) at 90% of saturation
in cement-based materials.
Therefore, low permeabilities in porous media must be determined in an unsteady state
(Selvadurai and Carnaffan 1997). Figg (1973) proposes an unsteady-state method to determine the air permeability of the concrete: the initial pressure in the chamber in contact
with the specimen tested is lowered by a vacuum pump. The time necessary to obtain a
given pressure increase in the chamber characterizes the air permeability of this specimen.
Calogovic (1995), Yssorche et al. (1995), and Claisse et al. (2003) propose to determine an

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281

Fig. 1 Schematics of the falling pressure experiment

air permeability coefficient from Figgs experiment by applying Darcys law: Calogovic and
Yssorche neglect the influence of air compressibility. Claisse proposes to use an analytical
axisymmetric solution of the problem of gas flow around a hole. This method may be applied
to in situ assessment of cover concrete, but not to laboratory tests of thin specimens.
Li et al. (2004) propose a falling pressure experiment to measure the air permeability
of asphalt (Fig. 1): air under pressure pc (0) is introduced into a chamber in contact with the
specimen tested. Once this upstream chamber is isolated, the reduction in the air pressure
p(t), due to air migration through the specimen, is recorded. An analytical solution (7) of the
simplified equation describing the variations over time of the air chamber pressure allows
the determination of the effective permeability coefficient k:

 
+ exp t
  ,
p(t) = patm 
exp t

(7)

where = [ pc (0) + patm ]/[ pc (0) patm ], = vL/Apatm k, patm is the atmospheric
pressure (Pa), v is the air chamber volume (m3 ), and A is the specimen area (m2 ).
(2) Concerning geomembranes, different tests characterizing the mass transfer through
the material, also exist:
(i) The immersion test consists in immersing the specimen tested in the permeant in liquid
phase and in weighing the specimen periodically: the migration of the permeant into the
specimen increases its weight; this variation in weight can be approached by an analytical solution to Ficks equation, leading to the possible determination of the diffusion
coefficient (Crank 1975).
(ii) The pouch test (Matrecon 1988) consists in filling a geomembrane pouch with the
permeant and immersing it in deionised water to create a concentration gradient of
the permeant and its migration across the geomembrane. The corresponding permeant
flow and diffusion coefficient are obtained by weighing the pouch periodically and
analyzing the immersion bath.
(iii) The ASTM D1434 test gives the gas permeability characteristics of plastic films by
the determination of the diffusion coefficient corresponding to a gas which migrates
across a material specimen separating two chambers: one is filled with the gas tested at
a specific high pressure; the other one is either in contact with ambient air (volumetric
procedure in steady state conditions) or initially at a very low pressure obtained by a
vacuum pump (manometric procedure in unsteady-state conditions).

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(iv) The ASTM E96 test is dedicated to water vapor migration: the corresponding water
vapor transmission rate and diffusion coefficient are measured on a specimen, sealed
into the mouth of a test dish with distilled water in it. The relative humidity difference
between both sides of the specimen is controlled and is here the driving force for water
vapor migration across the specimen, resulting in a weight loss of the dish assembly.
(v) The gas permeation pouch test (Pierson and Barroso 2002) consists in recording the
decrease in the gas pressure inside a geomembrane pouch. It is observed that this
decrease in pressure can be approached by a simple exponential law, characterized by
one time constant (Barroso et al. 2006), suggesting that a simplified solution of the
Eq. 3 is possible in the experimental conditions of this test, as Li et al. (2004) obtained
the simplified solution (7) for asphalt porous media.
The goal of the next sections is to present such simplified solutions adapted to all media.

3 Modeling the Falling Pressure Experiment in the Case of Pure Convective Flow
In the case of pure convective gas flow across the material, the differential equation (8) governing the transient variation of the gas pressure p in the material tested can be obtained
from extended Darcys law (1), combined with the equation of continuity and the ideal gas
law (Baehr and Hult 1991; Li et al. 2004):
dp(z, t)
k d 2 p 2 (z, t)
=
,
dt
2
dz 2

(8)

where is the material porosity.


A numerical solution of this non-linear problem is proposed in Sect. 4.
Considering the experimental conditions of the falling pressure method, the gas transported across the specimen tested is the mass flow rate of gas dm(t) / dt (kg/s) freed by the
upstream chamber (Fig. 1):
dm(t)
dc (t)
=v
,
(9)
dt
dt
where v is the upstream chamber volume and c (t) is the gas density in the chamber. Equation
9 is the ideal gas law in isothermal conditions:
pc (t)
pc (0)
=
,
c (t)
c (0)

(10)

where pc (t) is the gas pressure in the upstream chamber.


Combining Eqs. 9 and 10:
dm(t)
c (0) dpc (t)
=v
.
dt
pc (0) dt

(11)

Equation 12 can be obtained from Eq. 1 written at z = 0, combined with Eqs. 10 and 11:
Ak dp 2 (z, t)
dpc (t)
=
|z=0 ,
dt
2v
dz

(12)

where A is the specimen area and where pc (t) = p(0, t).


Equation 12 corresponds to a flux upstream boundary condition for Eq. 8. The downstream boundary condition is a uniform pressure at z = L (generally atmospheric pressure)
as expressed in Eq. 13:

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283

p(L , t) = patm .

(13)

Li et al. (2004) proposes the analytical solution (7) of the approximated Eq. 14 derived
from (12), if the function p 2 (z) is approached by a linear function, which is acceptable for a
small specimen thickness L and a great chamber volume (the numerical study in Sect. 4 will
specify this):

dpc (t)
Ak  2
p pc2 (t) .
=
dt
2vL atm

(14)

If during the test, pc (t) is closed to patm , the approximation (15) can be considered:
2
patm
pc2 (t) 2 p atm ( patm pc (t)).

(15)

It leads to the simple analytical solution (16)(17) of the Eq. 14:




t
pc (t) = patm + ( pc (0) patm ) exp ,

(16)

where is the time constant:


=

vL
.
Akpatm

(17)

4 Numerical Solution of the Non-linear Problem


In this section, a numerical study of the differential problem (8) describing the compressible
Darcy flow within a porous material is presented. The pressure falling experiment (Fig. 1)
is modeled using the boundary conditions (12) and (13). The initial condition is a uniform pressure pc (0) in the medium. The one-dimensional problem is discretized with finite
volumes using a second-order implicit scheme in space and a second order CrankNicholson scheme in time. The non-linearity of the pressure dependency is handled with the
NewtonRaphson iterative method. The numerical study presented in this section is used to
estimate the accuracy of the approximate solution (16)(17). Thus, a fitting method is used
to evaluate the permeability through a linear regression on the logarithm of Eqs. 1617.
The physical dimensions used to simulate the falling pressure experiment are those of the
experimental set up presented in Sect. 6.1. They are summarized in Table 1 and correspond to
an unsaturated clay liner. The dependency of the gas permeability on the water saturation is
not considered in the framework of this study. This means that the permeability k in equation
(8) is the effective gas permeability for a given saturation state. We assume that the water
phase remains steady (no flow or evaporation) during the experiment. This is relevant as far
as the experiment timescale is short. Further studies are currently in progress to evaluate the
dependency of the gas permeability of the clay on its water content.
As depicted in the Sect. 3, two assumptions are required to obtain the exponential model
for the upstream chamber depletion. The evolution of the pressure along the porous domain
Table 1 Characteristics of the clay specimen and of the pressure falling experimental apparatus

Aptian clay specimen

Thickness L (m)

Permeation
surface A (m2 )

Upstream chamber
volume v (m3 )

Water content
W (%)

0.10

418.4 104

3235.6 106

17

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C. Barral et al.

Fig. 2 Spatial pressure distribution within the porous domain for a high initial pressure (4.e5 Pa) [k =
1.e-11 m2 , kfit = 9.66e-12 m2 , e = 0.1]

Fig. 3 Upstream pressure Vs Time for various initial pressures [e = 0.1, k = 1.e-11 m2 ]

at different time steps is presented in Fig. 2. The initial pressure is set to 400 kPa. Even if a
non-linear behavior is in evidence, it appears to occur mainly for an average pressure gradient
significantly higher than that in the experimental conditions (Sect. 6.1). Moreover, the impact
of an increasing initial pressure on the fitted permeability remains small in the experimental
range (Fig. 3). We assume that the mathematical assumptions used to obtain the approximate solution are relevant in a large range of initial pressure gradient. However, a significant
effect of gas expansion can be observed in both Figs. 2 and 4. The gas initially compressed
within the porous domain appears to flow out in a first stage. This short period of depletion
within the material appears to trigger significantly the beginning of the upstream chamber
depletion. This phenomenon puts forward a weakness of the approximate exponential model.
The porosity of the material is not taken into account, since the exponential solution is based

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285

Fig. 4 Effect of the specimen porosity on the upstream chamber depletion [k = 1e-11 m2 ]
Table 2 Influence of the geometric parameters on the fitted permeability coefficient value

L (m)

v (m3 )

K (m2 )

K f it (m2 )

0.1
0.5
0.9
0.1
0.1
0.5
0.5

0.1
0.1
0.1
0.1
0.1
0.01
0.001

3.2356 103
3.2356 103
3.2356 103
3.2356 103
3.2356 103
3.2356 103
3.2356 103

1011
1011
1011
1014
1017
1011
1011

9.59 1012
8.20 1012
7.12 1012
9.59 1012
9.59 1012
9.80 1012
9.99 1012

S D (%)
4.1
18.0
28.8
4.1
4.1
2.0
0.1

RV
0.129
0.739
1.163
0.129
0.129
0.0739
0.00739

on the mass balance within the chamber (Eq. 12). The effect of an increasing porosity for
a given permeability (k = 1011 m2 ) is presented in Fig. 4. As the pore volume increases,
the upstream chamber depletion significantly slows down. The impact on the fitted value of
the permeability k f it is drastic: the standard deviation SD with the imposed value k, defined
with Eq. 18, increases from 4.51% for a porosity of 0.128.8% for a porosity of 0.9:


k k f it 
S D = 100
.
(18)
k
The Table 2 summarizes the dependency of the quality of the approximate exponential
solution on the different parameters of the problem. The intrinsic value of the permeability
k has no effect on the quality of the fitted value. Calculations in a large range from 1011 to
1017 m2 only change the duration of the experiment. The standard deviation remains equal
to 4.1%. As presented above, the porosity appears to have a strong impact. The assumption of
an influence of the pore volume is confirmed by the results obtained with a decreasing thickness of the porous membrane. The standard deviation decreases from 18.0% for a thickness
of 0.1 m to 0.1% for a thickness of 0.001 m.
The Fig. 5 summarizes the standard deviations between the real and the fitted value of the
permeability with respect to the ratio RV between the pore volume and the upstream chamber
volume:

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C. Barral et al.

Fig. 5 Standard Deviation between kfit and k for various RV values

RV =

AL
.
v

(19)

This result was obtained for different values of the upstream chamber volume, specimen
area and porous medium thickness and porosity. One should note that the relation between
R V and S D does not depend on which parameter changes. In order to limit the intrinsic error
associated with the use of the approximate exponential solution lower than 15%, the ratio
R V must be lower than 0.5. This means that the upstream chamber volume must be at least
twice the pore volume of the porous material.
This numerical investigation of the complete mathematical problem describing the falling
pressure permeability measurement has put forward various results:
The approximate exponential solution (16)(17) describes with a good accuracy the complete non-linear problem as far as a limited pressure gradient is imposed at the beginning
of the experiment.
A significant effect of the gas depletion in the pore volume of the material is evidenced. The
parameter RV appears to be a good estimator of the validity of the experiment geometrical
configuration.

5 Modeling the Falling Pressure Experiment in the Case of Pure Diffusive Flow
In the case of pure diffusive gas flow across the material, combining Ficks law (2) and the
equation of continuity in the material, Eq. 20 is obtained:
d 2 cmi (z, t)
dcmi (z, t)
.
=D
dt
dz 2

(20)

Analytical solutions of Eq. 20 exist (Crank 1975), but require the gas concentration inside
the material to be known. For experiments where the gas concentration is measured in the

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287

adjacent fluids, Eq. 5 presented in Sect. 2 may be considered in the case where the gas does
not interact with the material.
In order to obtain a simplified solution similar to Eq. 16 obtained for porous media, Eq. 5
is combined with Eqs. 9 and 10 under the form (21) where pG is the partial pressure of the
gas considered (i.e., nitrogen as considered in the experiment of Sect. 6.2) in the ambient air,
with a negligible variation over time, and pc (t) is the chamber pressure (which is supposed
to be filled with the gas being tested):
dpc (t)
Apc (0)P 
=
( pG pc (t)) .
dt
vc (0)L

(21)

Considering the ideal gas law in isothermal condition (20),


RTc
pc (0)
=
,
c (0)
M

(22)

where R is the universal gas constant, Tc is the constant gas temperature in the upstream
chamber (K), and M is the molar mass of the gas (kg/mol), the analytical solution of Eq. 21
is


t
pc (t) = pG + ( pc (0) pG ) exp
,
(23)

where is the time constant:


=

vL M
.
A P  RTc

(24)

Therefore, as far as the experimental results show a function pc (t) which can be reasonably approached by Eq. 23 (which is the same as Eq. 16 obtained in Sect. 3), it is possible
to compare all the materials used as a gas barrier by the time constant . This result does
not depend on the driving force: total pressure gradient for convective flow, concentration
gradient for diffusive flow, or a combination of both of them. will be even smaller if the
material is a poorer gas barrier. Furthermore, once is determined, Eqs. 17 and 24 give the
quantities k and P  , respectively, the effective permeability coefficient of a medium where
the gas flow occurs by pure convective flow and the permeability coefficient of a medium
where the gas flow occurs by pure diffusive flow.

6 Experimental Study
Two quite different applications of the falling pressure method are presented here:
The first one concerns a porous material consisting of a compacted clay specimen tested
in a similar cell as represented in Fig. 1.
The second one concerns a very low permeability material: a HDPE geomembrane seam,
which is tested with the gas permeability pouch test, better adapted to this kind of material.
The objective of this experimental study here is not to compare different materials (further
tests are being conducted), but to show two possible applications of the method proposed
here.

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6.1 Test on a Clay Sample


The falling pressure method is applied to clay used in landfill.
In order to create parallel epipedicaptian clay samples (0.4 m long, 0.1 m wide, 0.1 m
high), the clay is screened and then hydrated until a chosen moisture content. After the
homogeneization, this clay is statically compacted with an energy of compaction of 100% in
a special mold which allows compacting twice the sample on top and on bottom. The final
clay samples have an uniform porosity equal to 30% and are carefully packed and stored to
preserve their moisture content until the gas experiment.
A specific apparatus (Fig. 6) is then used to study the clay samples (Table 1) (Barral et al.
2007). One sample is placed on props in a plexiglas box to create an upstream chamber. A
lateral sealing is carried out with bentonite around the specimen. The upstream chamber is
filled with nitrogen at a relative pressure of 4 kPa. One should note that the geometrical characteristics of the apparatus have been designed so that the limit value of 0.5 for the ratio R V
corresponds to a porosity of 0.4 (assumed to be the upper bound for the aptian clay porosity).
The gas pressure relaxation to the atmospheric pressure is presented in Fig. 7. Three independent tests have been conducted on the same specimen. Even if the measurement noise
appears to be sensitive, the accordance between the different tests is satisfactory. We can
observe in the Fig. 7 that the permeability measurement takes only 1.3 s, which proves that
the drying effects are negligible during the experiment. Then, a fitting procedure is used to
calculate the time constant from Eq. 16 using the first 1.3 s of the experiment (corresponding to 70 measurement points). Finally, the gas permeability coefficient k of the specimen is
calculated from Eq. 17 using the geometrical characteristics of the apparatus (Table 3).
The dispersion of the results is less than 20% which is acceptable for permeability measurements. As far as very small timescales are considered in this experiment, the gas permeability
of the tested material has to be lower than a specific bound: in order to achieve a good fit of
the depletion curve, at least six experimental points are necessary. Considering the sampling
rate of the pressure sensor (20 ms), the time constant must be higher than 0.12 s, which
corresponds to a permeability coefficient lower than 1011 m2 (relative uncertainty: 20%).
The calculation of the Peclet number (Eq. 6) with the characteristics of the clay specimen

Fig. 6 Experimental apparatus for clay specimen gas permeability measurements

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289

Fig. 7 Gas pressure in the upstream chamber during falling pressure experiments
Table 3 Time constant and corresponding permeability obtained with the falling pressure experiment

(s)
k (m2 )

Test 1: p(0) patm = 4.3 kPa

Test 2: p(0) patm = 4.2 kPa

Test 3: p(0) patm = 3.9 kPa

0.47
3.0 1012

0.52
2.7 1012

0.56
2.5 1012

and of the pressure falling experimental apparatus gives Pe = 50 which corresponds to the
advective regime.
6.2 Test on an HDPE Geomembrane
The gas permeation pouch test presented in Sect. 2 allows the characterization of non-flexible
geomembranes (Pierson and Barroso 2002) and geomembrane seams (Barroso et al. 2006).
Here are presented the results obtained on a circular pouch made of two seamed pieces of
HDPE geomembranes (0.6 m diameter, 1.5 mm thickness), filled with nitrogen (Fig. 8). The
Table 4 presents the characteristics of the material tested and the pouch geometry. A perfect
circular shape cannot be obtained by the seam: the important issue is the determination of
the pouch area in contact with the ambient air, which must be as precise as possible. One
must also pay attention to the connection of the pouch inside to the gas supply, where the
geomembrane is sandwiched and compressed between two washers through which the gas
tube goes (Pierson and Barroso 2002).
Figure 9 shows the linear variation over time (during the first 40 days of the test) of the
quantity:

Ln


pc (t) p N2
,
pc (0) p N2

where p N2 is the mean partial pressure of nitrogen in the ambient air during the test.

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Table 4 Characteristics of the geomembrane specimen and of the pouch geometry


Type of geomembrane

Density

Thickness L

Total
permeation
surface A

Inner volume
of the pouch v

Geonap
(distributed by
Siplast-France)

0.943 kg/m3

1.5 103 m

0.635 m2

0.04296 m3

0.63 m

Seam made by
thermal hot dual
wedge method
Fig. 8 Circular pouch for measuring the nitrogen permeability of HDPE geomembrane

The application of the method developed in Sect. 5 should require the measurement of
the nitrogen partial pressure in the pouch. This cannot be obtained in this experiment where
the total pressure in the pouch is measured. It progressively differs from the nitrogen partial
pressure, mainly because of the diffusion of oxygen into the pouch. However, the resulting
error is here acceptable (illustrated with the linear variation of Fig. 9), since nitrogen is the
main component of air and since the first month of a 6-months duration test is here considered.
Such results confirm the approximated solution (23) and lead to the time constant:
= 3.03 107 s (relative uncertainty: 6%). The corresponding permeability coefficient
obtained from Eq. 24 is: PN 2 = 3.7 1017 s (relative uncertainty: 15%), which may be
compared to the results obtained by different authors for nitrogen transport through HDPE
geomembranes (Table 5).
It may be observed that the orders of magnitude are the same. Differences necessarily
exist, since different qualities of HDPE are considered (comparable densities, but different
additives used), except for Pierson test. Furthermore, the nitrogen flow through the geomembrane is here due to a concentration gradient and to a total pressure gradient, making open
to criticism the calculation of PN 2 . The calculation of the Peclet number (Eq. 6) with the

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291

Fig. 9 Result of the falling pressure experiment on HDPE geomembrane pouch


Table 5 Comparison of nitrogen permeability coefficients of HDPE geomembranes
Authors

Encyclopedia of polymers

Lamberta

Piersonb

This study

p N  (1017 s)

1.1

2.0

3.1

3.7

a Test similar to the ASTM 1434 test (Lambert 1994)


b Result obtained from the gas permeability pouch test, considering a pseudo steady state (Pierson and Barroso

2002)

characteristics of the geomembrane specimen, the pouch geometry, and considering a maximum porosity of the geomembrane equal to 0.01, gives Pe = 5 105 which represents
the diffusive regime.
Once again, this analysis highlights the advantage of using the time constant to compare
the gas permeability of different materials instead of using permeability coefficients.
In the case of very low permeability materials, the test limit is in relation with the acceptable duration of the test: several months may be necessary (Barroso et al. 2006) and even
very small leaks through the seams or seals may appear as no longer negligible.

7 Conclusion
This study shows it is possible to compare the gas permeability through very different materials (porous media or very low permeability media) where the gas flow occurs by convective
flow, diffusive flow, or combined flow. Such a comparison is possible by the determination
of a unique quantity, the time constant . This quantity is obtained after the approximation
of the response of a material specimen to the falling pressure test by an exponential law.
A permeability coefficient may be derived from by the use of Eq. 17 (pure convective
flow) or Eq. 24 (pure diffusive flow). Obviously, in the whole range of the medium porosity
and gas permeability, a transition between the two regimes must occur. The advantage of
the method is that the same quantity will still be representative of the gas permeability of
the material as far as the geometrical characteristics of the apparatus are the same. A unique

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apparatus which may be used to test clay liners as well as synthetic liners has just been
designed: results will be soon available.
It should be observed that the method is still valid at high water content, contrary to
many steady-state methods generally used to measure the gas permeability of porous media,
because of the very small gas pressure gradient applied: Steady-state methods require high
pressure gradients to make the gas flow measurement possible, which generate uncontrolled
water movements inside the material, with a possible drying effect.
The limit of the method proposed here when applied to porous materials may be defined
by the quantity Rv (Eq. 19), in relation to the geometry of the measurement cell: studying
material with high porosity should require a higher volume of the upstream chamber (leading
to a huge apparatus) or a small specimen area (increasing the relative influence of edge effect
and of the corresponding leaks). A limit of the pressure gradient should also be respected
to avoid problems of leakage as well as uncontrolled water movement inside the specimen.
Finally, the sampling rate of the pressure sensor has to be carefully taken into account to get
an accurate measurement of the upstream chamber depletion.
Concerning very low permeability materials, the acceptable test duration is the limit: the
measurement of the gas permeability of HDPE geomembranes is possible, but may require
a timescale of several months.
The method is now applied to compare the biogas permeability of the different materials used in landfill cover applications, considering their possible deformation due to waste
settlement.

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