GAS PERMEABILITY

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DOI 10.1007/s11242-009-9398-x

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

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

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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C. Barral et al.

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).

2.1 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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279

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)

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)

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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C. Barral et al.

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

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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C. Barral et al.

(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)

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)

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)

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)

t

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

(16)

=

vL

.

Akpatm

(17)

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

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.

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)

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)

=

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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C. Barral et al.

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

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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 )

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.

123

290

C. Barral et al.

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

123

291

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

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

123

292

C. Barral et al.

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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