Академический Документы
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Культура Документы
DOI 10.1007/s11242-009-9398-x
Received: 30 July 2007 / Accepted: 13 April 2009 / Published online: 6 May 2009
Springer Science+Business Media B.V. 2009
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
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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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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)
pi (t)
,
L
(5)
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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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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)
(10)
(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)
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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)
(16)
vL
.
Akpatm
(17)
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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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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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)
(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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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.
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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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Encyclopedia of polymers
Lamberta
Piersonb
This study
p N (1017 s)
1.1
2.0
3.1
3.7
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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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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