Geotextiles and Geomembranes 44 (2016) 656e672

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Geotextiles and Geomembranes

journal homepage: www.elsevier.com/locate/geotexmem

Review

A review of the performance of geosynthetics for environmental

protection*
N. Touze-Foltz a, *, H. Bannour c, 1, C. Barral b, 2, G. Stoltz d, 3
a
Irstea, Antony Regional Center, Hydrosystems and Bioprocesses Research Unit, 92761 Antony, France
b
Conservatoire National des Arts et Metiers, 2, rue Cont
e, 75141 Paris cedex 03, France
c
ISSAT, Sousse, Tunisia
d
RECOVER Research Unit, Irstea, 3275 Route C ezanne, CS 40061, 13182 Aix-en-Provence cedex 5, France

a r t i c l e i n f o a b s t r a c t

Article history: This paper, which is based on an Invited Lecture for the 7th International Conference on Environmental
Received 15 April 2015 Geotechnics, gives an updated overview of the properties of transfer of geosynthetic liner materials
Received in revised form used in environmental applications. To begin, the water-retention curves of geosynthetic clay liners
26 March 2016
(GCLs) are discussed, with the focus being on the high temperatures that can be encountered and the
Accepted 15 May 2016
Available online 7 June 2016
concomitant risk of desiccation. Next, an overview is given of quantifying advective transfer through
intact geomembranes (virgin or after exposure on site) and through multicomponent GCLs. Experi-
mental quantification of advective transfer through composite liners is also addressed, whereby
Keywords:
Geosynthetic
geomembranes or the film or coating of a multicomponent GCL is damaged. Finally, based on a
Geomembrane literature review including the most recent data, the discussion turns to the diffusion of organic and
Geosynthetic clay liner inorganic species through virgin and aged geomembranes and GCLs. The synopsis of the most recent
Advection data presented here in terms of elementary transfer mechanisms, either advective or diffusive, should
Diffusion contribute to improving the quantification of transfer through barrier systems. These four topics were
Measurement selected as they correspond to the fields of expertise of the co-authors in which they have been
publishing in the past 20 years.
© 2016 Elsevier Ltd. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 657
2. Experimental determination of hydraulic behavior under unsaturated conditions of geosynthetic clay liners . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 658
3. Quantification of advective transfer through geomembranes and multicomponent geosynthetic clay liners . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 659
3.1. Quantification of advective transfer through geomembranes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 659
3.1.1. Background . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 659
3.1.2. Flow rates for virgin geomembranes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 660
3.1.3. Flow rates for geomembranes after on-site exposure . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 660
3.2. Quantification of advective transfer through intact multicomponent geosynthetic clay liners . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 660
4. Quantification of flow rates in composite liners with a GCL and multicomponent GCLS with damaged film or coating . . . . . . . . . . . . . . . . . . . . . . . . 661
4.1. Flow rates and interface transmissivity in composite liners with a geosynthetic clay liner . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 661
4.1.1. Case of virgin geosynthetic clay liners containing sodium bentonite . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 661
4.1.2. Influence of geomembrane on flow rate . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 662
4.1.3. Influence on flow rate of concrete in contact with geosynthetic clay liner . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 663

*
Review of this paper was handled by A. Bouazza.
* Corresponding author. Tel.: +33 1 40 96 60 39.
E-mail addresses: nathalie.touze@irstea.fr (N. Touze-Foltz), hajerbannour@gmail.com (H. Bannour), camille.barral@lecnam.net (C. Barral), guillaume.stoltz@irstea.fr
(G. Stoltz).
1
Tel.: +216 58779292.
2
Tel.: +33 1 40 27 22 91; fax: +33 1 58 80 86 01.
3
Tel.: +33 442666964; fax: +33 442668865.

http://dx.doi.org/10.1016/j.geotexmem.2016.05.008
0266-1144/© 2016 Elsevier Ltd. All rights reserved.
 N. Touze-Foltz et al. / Geotextiles and Geomembranes 44 (2016) 656e672 657

4.1.4. Influence on flow rate of composition of bentonite in geosynthetic clay liner . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 663
4.1.5. Influence of bentonite ageing on flow rate . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 663
4.1.6. Summary of results . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 663
4.2. Flow rates in multicomponent geosynthetic clay liners when coating or film is damaged . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 664
5. Diffusion in lining materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 665
5.1. Composition of leachate from landfills . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 665
5.2. Quantifying properties of transfer of chemicals through liner materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 665
5.2.1. Theory of diffusive transfer through geosynthetic clay liners . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 665
5.2.2. Theory of diffusive transfer through geomembranes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 665
5.3. Absorption onto components of geosynthetic clay liners . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 666
5.3.1. Case of organic pollutants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 666
5.3.2. Case of inorganic pollutants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 666
5.4. Diffusive transfer through geosynthetic clay liners . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 666
5.4.1. Diffusion of inorganic species through geosynthetic clay liners . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 666
5.4.2. Diffusion of organic species through geosynthetic clay liners . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 667
5.4.3. Aged GCLs after cation exchange . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 667
5.5. Diffusive transfer through geomembranes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 667
5.5.1. Diffusion of inorganic species . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 667
5.5.2. Diffusion of organic species . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 667
5.5.3. Effect of geomembrane ageing on diffusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 669
6. Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 670
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 671

1. Introduction the clay, which contradicts the definitions of clay geosynthetic

barriers. In the following the words GM or GCL will thus be used
Recent years have seen many advances in the understanding of instead of barriers. To clearly distinguish between the various
issues related to the use of geosynthetics such as geomembranes materials, the term “multicomponent GCL” is used systematically in
(GMs) and geosynthetic clay liners (GCLs) as contaminant barriers the following for a GCL that contains a coating or an attached film.
also respectively known as polymeric or bituminous barriers for the The function of a barrier material is to control contaminant
first ones and clay geosynthetic barriers for the latter transport and thereby isolate the contaminants from the environ-
This paper presents an updated version of an Invited Lecture for ment over the long term. To ensure this, methods to quantify
the 7th International Conference on Environmental Geotechnics contaminant transfer through liner materials were developed (some
(Touze-Foltz et al., 2014) and focuses on the performance of geo- very recently). This paper discusses quantification in the laboratory
synthetics for environmental protection (e.g., landfills or mining of the properties of transfer in geomembranes and GCLs. The
applications). The geosynthetics under study are those whose elementary transfer modes focused on herein are advection, which
function is to ensure the lining, in other words, GMs and GCLs. In is the transport of liquid due to a difference in hydraulic head be-
the Recommended Descriptions of Geosynthetics Functions, Geo- tween the two sides of a liner material, and diffusion, which is
synthetics Terminology, Mathematical and Graphical Symbols of transfer of liquid due to different concentrations of a given
the International Geosynthetics Society, GMs are defined as planar, contaminant on the two sides of a liner material. No attempt is made
relatively impermeable, polymeric (synthetic or natural) sheets for here to quantify the performance of barrier systems on the field scale
use in civil-engineering applications. GCLs are defined as an by accounting for the combined effect of advection and diffusion.
assembled structure of geosynthetic materials and low-hydraulic- This aspect was previously discussed extensively by, for example,
conductivity earth material (clay) in the form of a manufactured Rowe (2005, 2007; 2012). Instead, the objective here is to discuss the
sheet to be used in civil-engineering applications. The EN ISO 10318 material properties of geomembranes and GCLs and how they can be
standard (AFNOR, 2006a) defines geosynthetic barriers, which may quantified, with the emphasis on recent innovative developments.
be polymeric, bituminous, or clay geosynthetic barriers (GBR-Cs), The quantified elementary transfer properties can subsequently be
according to which component fulfills the barrier function. A GBR-C used for modeling at the barrier scale to predict contaminant
is defined as factory assembled structure of geosynthetic materials transfer, although this falls outside the scope of this paper.
in the form of a sheet which acts as a barrier. The barrier function is Temperature is a factor that may influence the long-term per-
essentially fulfilled by clay. As explained below, this definition does formance of barrier systems (Rowe, 2005). In waste-containment
not allow the interchangeable use of geosynthetic barriers and facilities, heat may be generated in various ways (Ali et al., 2014).
GCLs. In fact, multicomponent GCLs are now available on the For the biodegradation of waste, the temperature may rise to 60
C
market. The following proposed definitions are currently being under normal operation in municipal solid-waste landfills. Singh
discussed by the ASTM D35 terminology task group and may be and Bouazza (2014) mention that, due to the combined effect of
added in the future to the ASTM terminology standard D4439 (von solar radiation and brine processing, liners containing brines pro-
Maubeuge et al., 2011). Currently, a multicomponent GCL is defined duced from coal seam-gas wells can be exposed continuously to
as a GCL with an attached film, coating, or membrane that de- temperatures close to 70e80
C. One potential consequence of
creases the hydraulic conductivity, protects the clay core, or both. elevated temperatures is the development of thermal gradients
An adhered GCL is a GCL product in which the clay component is across the liner toward the cooler subgrade soil. Such thermal
bonded by adhesion to a film or membrane. A coated GCL is a GCL gradients can create a risk of outward moisture movement and
product with at least one layer that consists of a solidified synthetic possible desiccation of the mineral liner, which may be a GCL (Singh
substance that was applied to the GCL as a fluid (von Maubeuge and Bouazza, 2014).
et al., 2011). In this case, as illustrated in Section 3.2, the coating Thus, to adequately predict transfer through barrier systems,
or attached film may ensure the liner function much more so than understanding the hydraulic behavior under unsaturated
658 N. Touze-Foltz et al. / Geotextiles and Geomembranes 44 (2016) 656e672

conditions of GCLs is of vital importance, because their capability to
serve as a barrier to fluids is intimately linked to the uptake of
moisture by the bentonite and can be affected by temperature.
Section 2 of this paper is thus dedicated to providing a synopsis of
existing data that elucidates the retention curves of GCLs.
Quantifying advective transfer in geomembranes and multi-
component GCLs is addressed in Section 3, where an insight is
given into advective transfer through geomembranes after expo-
sure on site. There, data are presented that were collected from
hydraulic applications that can be of interest for using geo-
membranes as, for example, landfill covers.
The quantification of advective transfer through a damaged GM,
or through a hole in the attached film or coating of a multicom-
ponent GCL appears in Section 4. This section also discusses the role
played by the composition of the GM [high-density polyethylene
(HDPE) or bituminous], and of the bentonite (sodium or calcium),
by the ageing of the bentonite through cation exchange and
hydrationedesiccation cycles, and by the use of a multicomponent
GCL rather than a more classical GM-GCL composite liner.
Finally, section 5 summarizes the parameters that, based on
existing data from the literature, govern diffusion through GCLs and
GMs for virgin and aged materials.
2. Experimental determination of hydraulic behavior under
unsaturated conditions of geosynthetic clay liners
When installed in composite liners at the bottom of landfills,
GCLs present an as-manufactured water content close to 10%. The
suction of the bentonite contained in GCLs depends on the ambient
relative humidity and can be as high as 1000 MPa (Beddoe et al.,
2010). After installation, GCLs typically hydrate from both the
liquid flux through defects in the geomembrane and from the
transfer of vapor and liquid water from the underlying soil through
the GCL (Azad, 2011; Beddoe et al., 2010). Accurately predicting the
hydraulic characteristics of composite liners requires knowledge of
both the water-retention curve (WRC) of the GCL and the volu-
metric changes of such liners during hydration.
GCLs hydrate under a compressive stress corresponding to the
overburden load generated by waste. Assuming a typical depth of
waste deposits of between 20 and 30 m and using a density of
800e1000 kg/m3 for the waste leads to vertical stresses of up to
300 kPa applied to GCLs at the bottom of landfills.
As summarized in Table 1, many experimental studies have
investigated the water-retention properties of GCLs (Daniel et al.,
1993; Barroso et al., 2006a; Southen and Rowe, 2007; Abuel-
Naga and Bouazza, 2010; Beddoe et al., 2010, 2011; Hanson
et al., 2013). Motivated by the contrasting water-retention
characteristics of geotextile and bentonite, these studies
focused on determining the WRCs of GCLs under confining stress.
The difficulty of determining the WRCs of GCLs could arise from a
capillary barrier to water continuity developing between the
bentonite and the water-retention equipment, which could affect
resulting WRC.
The effect on the transport characteristics of confining stress
applied along a wetting path was investigated by Abuel-Naga and
Bouazza (2010), who applied a stress of 50 kPa by using a modi-
fied triaxial apparatus that combines a thermocouple psychrometer
and a relative humidity sensor, and by Beddoe et al. (2011), who
applied a small stress of 2 kPa by using a high-capacity tensiometer
and a capacitive relative-humidity sensor. Siemens et al. (2013)
used a numerical simulation done with the SEEP/W finite-
element software (GeoStudio, 2007) to study how confining
stresses of 2 and 100 kPa affect water retention in GCLs.
More recently, Bannour et al. (2014) developed a new laboratory
methodology to determine the WRCs of GCLs under various
stresses. Constant vertical stresses of 10, 50, 100, and 200 kPa,
corresponding to different waste-layer thicknesses, were applied to
GCL specimens placed in controlled-suction oedometers. The suc-
tion was set to mimic a wetting path from the initial dry state to
zero suction and the capillary barrier effect of the carrier geotextile
was circumvented by using the vapor-control technique. To obtain
the two largest values of suction (4.2 and 8.5 MPa), they applied the
standard technique of controlling relative humidity by using a
saturated saline solution. For lower suction (0.1, 0.5, 1, and 2.8 MPa),
they adapted the osmotic technique to control vapor by using
calibrated concentrations of polyethylene-glycol solutions,
ensuring a continuous series of applied suction along the wetting
path, down to zero suction. Measurements were complemented by
standard saturated oedometer swelling tests with water infiltration
at zero suction. The measurements were made on a needle-
punched GCL containing sodium bentonite. The experimental
water-retention curves obtained under various confining stresses
allowed the following conclusions to be drawn, which are consis-
tent with conclusions from previous studies:
 Increasing vertical stress results in a decrease in water uptake
along the wetting path accompanied by a reduction in the
swelling capacity and in the saturated hydraulic conductivity of
the GCL (Fig. 1).
 In the low-suction range, a GCL hydrating at a high confining
stress hydrates faster than one at a lower confining stress. At a
higher confining stress, GCLs have the benefit of a higher suction
where the saturated hydraulic conductivity is achieved and, for
a given suction, their saturated degree is higher than that of an
unconfined GCL.
 Water retention in bentonites depends only slightly on
bentonite density, which is attributed to the predominance of
physicochemical clayewater interactions.

Table 1
Published investigations of GCL water-retention curves.

Authors Technique used Confining stress (kPa) Water cycle

Daniel et al. (1993)
Southen and Rowe (2005)
Barroso et al. (2006a)
Southen and Rowe (2007)
Abuel-Naga and Bouazza (2010)
Beddoe et al. (2010)
Beddoe et al. (2011)
Hanson et al. (2013)
Bannour et al. (2014)
a
“SCM” stands for “suction-control method” and “MCM” stands for “moisture-control method.”
Thermocouple Psychrometer (SCM)a and vapor equilibrium (MCM) 0 Wetting path
Pressure-plate technique (SCM) 0 Drying
Filter Paper (MCM) 0 Wetting path
Pressure plate (SCM) and pressure membrane extractors (SCM) 0-0.5-3-100 Drying path
Thermocouple psychrometer (MCM) and a capacitive relative humidity sensor (MCM)r 50 Wetting path
High-capacity tensiometers (MCM) and capacitive relative humidity sensors (MCM) 2 Drying path
High-capacity tensiometers (MCM) and capacitive relative humidity sensors (MCM) 2 Wetting/Drying path
Pressure plate-Filter paper and relative humidity methods 0 Wetting/Drying path
Oversaturated salt solution with forced vapor circulation and polyethylene glycol 0-10-50-100-200 Wetting
solution with forced vapor circulation
 N. Touze-Foltz et al. / Geotextiles and Geomembranes 44 (2016) 656e672 659

Fig. 1. Fits made by using van Genuchten's expression in a two-dimensional representation to experimentally determined water-retention curves for various vertical stresses.

 Two well-known equations for WRCs (van Genuchten, 1980;
Fredlund and Xing, 1994) correctly fit the data.
Additionally, Bannour et al. (2014) proposed two new expres-
sions that include stress effects for WRCs. The corresponding sur-
faces were represented in three-dimensional graphs that show how
water content depends on stress and suction along a wetting path.
They also discussed the possible validity of the state-surface
concept applied to GCLs under stress and concluded that the val-
idity of this concept would likely be confirmed by constant-suction
compression measurements on hydrated bentonites.
These results indicate the importance of rapidly confining GCLs
once they are installed so as to make them more rapidly operational
and hydrated in barrier systems. In addition, a resistant bonding
structure is also recommended to naturally confine the GCL, even
under low stress.
3. Quantification of advective transfer through
geomembranes and multicomponent geosynthetic clay liners
This development gave rise to a French standard and, following
this, to a European standard (EN 14150; AFNOR, 2006b) for
measuring steady-state liquid flow through a geomembrane under
a hydraulic pressure difference of 100 kPa between opposite sides
of the geomembrane. The test method and apparatus described in
EN 14150 allow flows to be accurately measured down to
106 m3 m2 d1. The two-part cell described in this standard (see
Fig. 2) is made of stainless steel because the cell must resist
oxidation during long-term immersion. In each part of the cell, a
cavity allows hydraulic pressure to be applied. A porous disc placed
in the downstream cavity prevents deformation of the geo-
membrane. The cell is designed to clamp the specimen with no
leaks. No tightening system is required because clamping between
flat surfaces is usually sufficient. For bituminous geomembranes, a
bitumen rubber sealant can be used.
The minimum diameter of the measuring chambers is 0.2 m. The
cell is equipped with a liquid inlet on the upstream part, a liquid
outlet on the downstream part, and flushing valves on each part.

3.1. Quantification of advective transfer through geomembranes

3.1.1. Background
A GM is a nonporous medium, which means that the material
contains no voids, but only free spaces of size similar to that of a
solvent molecule. Transport in GMs thus occurs at the molecular
level (Lambert and Touze-Foltz, 2000). However, gases and liquids
can migrate through the intact GMs by an activated diffusion pro-
cess that differs from the liquid convection process that occurs in
the pores of porous soils (Barroso, 2005). Different driving forces
may cause diffusion; for example, concentration, hydraulic, or
temperature gradients. Diffusion has also been shown to occur even
if there is no gradient: this phenomenon is called self-diffusion
(Eloy-Giorni, 1993).
An instrument was first developed in France (Eloy-Giorni, 1993;
Pelte, 1993; Durin et al., 1998; Lambert and Touze-Foltz, 2000) to
quantify flow rates through GMs under the influence of a hydraulic Fig. 2. Photograph of stainless-steel cell and pressure volume controllers of type-B
gradient. device for measuring flow rate in geomembranes.
660 N. Touze-Foltz et al. / Geotextiles and Geomembranes 44 (2016) 656e672

10-5 measured in the range 2.9  105 to 1.5  103 m3 m2 d1 for a
hydraulic head of 0.5 m. One oxidized bituminous GM that was
inflow covered during the 30 years since its installation had a flow rate
outflow identical to that of virgin bituminous GMs, which means that no

Bitumen 3.5 mm
hydraulic evolution was detected. A recent study (Touze-Foltz et al.,
Flow rate (m3/m2/d)

10-6 2015) presents the results obtained from an elastomeric bitumi-

Bitumen 5.5 mm
nous GM and an oxidized bituminous GM after 15 years of exposure
FPP 1 mm

HDPE 1.5 mm
HDPE 1,5 mm
HDPE 1.5 mm
in a pond, during which time neither GM was covered. The flow

HDPE 2.5mm
EPDM 1.5 mm
FPO 2 mm

HDPE 0.75 mm rate through the elastomeric bituminous GM was one order of
Structured HDPE 0.75 mm
FPP 1 mm

magnitude lower than that through the oxidized bituminous GM.

PVC-P 1 mm
FPO 3 mm

PVC-P 1 mm
FPP 1 mm

10-7 The flow rate through the elastomeric bituminous GM, whose
HDPE0.5 mm
FPP 1 mm

bitumen had not been altered, was close to 1.9  106 m3 m2 d1.
Both of these studies concluded by recommending that oxidized
bituminous GMs not be left exposed after installation.
Noval et al. (2015) also recently studied the evolution over 21
10-8 years of an ethylene propylene diene terpolymer (EPDM) GM
installed in a pond in the Canary Islands. After 21 years, the flow
0 2 4 6 8 10 12 14 16 18
rate remained below 106 m3 m2 d1. Further joint studies based
Test number
on samplings from ponds are ongoing between CEDEX (Spain),
Fig. 3. Synopsis of measurements of flow rate through geomembranes made as per EN IFSTTAR (France), and Irstea (France) to better understand the
14150 with Type-B device (from Touze-Foltz and Zanzinger, 2009) (FPP: flexible temporal evolution of the properties, including the hydraulic
polypropylene, EPDM: ethylene-propylene-diene terpolymer, HDPE: high-density properties, of HDPE and plasticized polyvinyl chloride (PVC-P) GMs.
polyethylene, PVC-P: plasticized polyvinyl chloride, FPO: flexible polyolefine).

3.2. Quantification of advective transfer through intact

Volume measurements can be done by using capillary tubes
multicomponent geosynthetic clay liners
(Type-A devices) or pressure-volume controllers (type-B devices).
Fig. 3 summarizes the measurements done with a type-B device.
Multicomponent GCLs have recently been introduced to the
This device allows the application of a constant pressure when
market to seal landfills, dams, dikes, ponds etc. Because these GCLs
measuring the volume and consists of a cylinder in which a piston
combine a GCL and a coating or film, their hydraulic properties fall
slides. An automatically controlled motor applies the required
between GMs and GCLs. Very recently, instruments have been
pressure by moving the piston. Finally, a pressure sensor included in
developed to characterize transfer through these materials. Lucas
the system measures the pressure. Displacement of the piston cor-
(2002) studied hydraulic flows through a multicomponent GCL
responds to a variation of the volume of the liquid. A type-B device
composed of a uniform layer of granular sodium bentonite encap-
uses at least three temperature transducers, with one placed on each
sulated between a slit-film woven geotextile and a virgin staple
pressure-volume controller and one on the cell. Temperature mea-
fiber nonwoven geotextile. Tests in accordance with ASTM D5084
surements are then used to correct variations in volume.
(ASTM, 2010) conducted on this multicomponent GCL estimated a
The validity of a measurement is determined by comparing
hydraulic conductivity of about 5.0  1012 m/s. However, Lucas
upstream and downstream flow rates. Although these values
also suggested the possibility that sidewall leakage occurred during
should be equal in theory, in practice this is rarely the case for GMs.
the tests. Cleary and Lake (2011) estimated the hydraulic conduc-
For flow rates greater than or equal to 106 m3 m2 d1, upstream
tivity of the same multicomponent GCL by using three different
and downstream flow rates are considered to be equal if they differ
types of permeameters. All results, except for the specimens tested
by less than 10% of the flow rate measured on the upstream side. In
in the constant-head, fixed-wall, double-ring permeameter, gave
particular circumstances where testing according to the described
hydraulic conductivities below 1.0  1011 m/s.
test method gives values for a GM that lie below the threshold of
In these studies, the mass per unit area of the coating in the
sensitivity of the test method, then the liquid flow is assumed to be
multicomponent GCL was less than 100 g/m2, which resulted in a
less than 106 m3 m2 d1.
nonuniform coating, so the watertightness was ensured by the clay
core. Touze-Foltz et al. (2012a,b) and Barral and Touze-Foltz (2012)
3.1.2. Flow rates for virgin geomembranes developed a procedure whereby devices from NF EN 14150 (AFNOR,
Most flow rates obtained for virgin GMs are below the threshold, 2006b) designed to measure flow rate through GMs are combined
as can be seen from Fig. 3. In France, the definition of a GM as per the with a rigid-wall permeameter from NF P84-705 (AFNOR, 2008),
standard NF P84-500 (AFNOR, 2013) states that the flow rate which is designed to measure flow rate through GCLs, to measure
measured according to EN 14150 must be less than 105 m3 m2 d1. flow rates through multicomponent GCLs (see Fig. 4). Indeed, the
regular measurement device used in NF P84-705 to measure flow
3.1.3. Flow rates for geomembranes after on-site exposure rate through GCLs is not able to measure small flow rates in
The testing device described by EN 14150 has also been used to multicomponent GCLs. It was thus required to use a measuring
quantify the evolution of the hydraulic properties of GMs used in device for precise measurements of flow rates in GMs combined
hydraulic applications. To the best of our knowledge, no such data with the rigid-wall permeameter.
exist for environmental applications. Data obtained in hydraulic Barral et al. (2014) extended their study to include three GCLs and
applications are thus briefly reported here because they could be five different multicomponent GCLs from several manufacturers.
useful; for example, for landfill covers. Two multicomponent GCLs were coated with a coating with areal
Touze-Foltz et al. (2010a,b) reported the case of six oxidized density below 100 g/m2 and above than 200 g/m2, respectively. Three
bituminous geomembranes. They showed that, when an oxidized multicomponent GCLs were laminated with a film having various
bituminous GM remains exposed for ten to fifteen years, the hy- different thicknesses and bonding modes. The features of the GCLs
draulic performance decreases to the level of protection similar to are presented in Table 2 and the features of the multicomponent
what would be provided by a 1-m-thick clay layer, with flow rates GCLs appear in Table 3. Fig. 5 shows the results obtained for the three
 N. Touze-Foltz et al. / Geotextiles and Geomembranes 44 (2016) 656e672 661

flow rate and hydraulic conductivity in regular GCLs. The flow rates
obtained (without any modification of the GCL standard) are pre-
sented in Fig. 6 and range from 1.4  1011 to 2.2  1011 m/s for a
hydraulic head of 0.1e0.6 m. These flow rates are closer to GCL flow
rates than to flow rates in GMs, which are known for virgin GMs to
be around 106 m3 m2 d1. The flow rate through multicomponent
GCLs with an adhesive bounded film thicker than 0.2 mm or with a
coating with a density exceeding 200 g/m2 is closer to the flow rate
in GMs than to the flow rate in GCLs, which implies that, in such
products, flow rate is controlled by the coating or attached film
rather than by the bentonite. Thus these GCLs cannot be considered
as clay geosynthetic barriers. They cannot be presented as GMs
because the flow rate through them exceeds the allowable flow rate
through GMs established in NF P84-500 (i.e., 105 m3 m2 d1).
Thus, the terminology standard for geosynthetics, EN ISO 10318,
lacks the appropriate vocabulary to label some multicomponent
GCLs.

4. Quantification of flow rates in composite liners with a GCL

and multicomponent GCLS with damaged film or coating

4.1. Flow rates and interface transmissivity in composite liners with

a geosynthetic clay liner

4.1.1. Case of virgin geosynthetic clay liners containing sodium

Fig. 4. Experimental device for measuring flow rates through multicomponent GCLs.
multicomponent GCLs for which the thickness of the film coating
exceeded 0.2 mm (M1 to M3, see Table 3). The results show that flow
rates in multicomponent GCLs are one order of magnitude greater
than those usually found for virgin GMs (i.e. 106 m3 m2 d1).
For the two multicomponent GCLs with the light coating (M4)
and with perforations by needling (M5), flow rates were measured
according to NF P84-705, which is the standard used to quantify
bentonite
The work done over the past years regarding the characteristics
of GCLs that are part of a composite liner mainly focused on the
situation where the GCL (which contains sodium bentonite) is
located under a hole in a HDPE GM. As indicated by Brown et al.
(1987), the flow through a defect in the GM depends on the con-
tact between the GM and the underlying soil liner. According to
these authors, if the contact is not perfect, fluid that has migrated
through the defect spreads laterally within the gap (i.e., the inter-
face) between the GM and the underlying soil. The area covered by
this interface flow is called the “wetted area.” Finally, the liquid
migrates into and through the soil liner.
Contact between the GM and the GCL was quantified in terms of
the flow rate through the composite liner and in terms of interface
transmissivity. Various situations were tested to evaluate the flow

Table 2
Characteristics of GCLs.

GCL Type of bentonite Cover GTXa Carrier GTX Thickness under 10 kPa (mm) Measured total dry mass per unit
area in specimen (kg/m2)

G1 Sodium/Powder Woven Non-woven 5.7 4.8

G2 Sodium/Granular Non-woven Woven 7.4 6
G3 Sodium/Powder Woven with surface coating and fleece Woven with surface coating 9.2 5.9
a
“GTX” stands for “geotextile.”

Table 3
Characteristics of multicomponent GCLs.

Multi Type of bentonite Cover GTX Carrier GTX Thickness Measured total Bonding type Film or coating Film or coating
component under 10 kPa (mm) dry mass per thickness (mm) measured
GCL unit area of total dry mass per
bentonite in unit area (kg/m2)
specimen
(kg/m2)

M1 Sodium Powder Woven Non-woven 5.2 4.58 Coated 0.4 < ef < 0.7 0.25 < mf < 0.4
M2 Sodium Granular Non-woven Woven 6.6 5.28 Adhered ~0.25 ~0.2
M3 Sodium Granular Slit film woven Non-woven 5.8 4.41 Adhered ~0.25 ~0.2
M4 Sodium Powder Slit film woven Non-woven 5.1 4.13 Coated _a <0.1
M5 Sodium Powder Woven/Surface Woven/Surface coating 9.6 5.7 Stitch-bonded 0.2 < ef < 0.3 ~0.1
coating and fleece
a
Not measurable.
662 N. Touze-Foltz et al. / Geotextiles and Geomembranes 44 (2016) 656e672

10-3
1,E-03

M1; differential pressure 50 kPa M1; average from latest 7 days

upstream flow rate (m3/m2/d)

M2; differential pressure 50 kPa M2; average from latest 7 days

M3; differential pressure 50 kPa M3; average latest 7 days

1,E-04
10-4

1,E-05
10-5

-6
10
1,E-06
0 1 2 3 4 5 6 7 8

Time (Days)

Fig. 5. Synopsis of upstream flow rates obtained for multicomponent GCLs for the latest seven days of measurements with a differential pressure of 50 kPa [adapted from Touze-
Foltz et al. (2012a,b)].

through a smooth GM in contact with a GCL (Harpur et al., 1993;
Barroso et al., 2006b, 2010). Harpur et al. (1993) verified that, un-
der steady-state conditions, the most significant fraction of the flow
occurs along the interface between the GM and the cover geotextile
of the GCL, through the cover geotextile, and along gaps between
the cover geotextile of the GCL and the bentonite. A less significant
amount of fluid percolates through the bentonite and below the
GCL. Barroso et al. (2006b; 2010) examined how hydraulic head,
pre-hydration of the GCL, and confining stress affects the GM-GCL
interface transmissivity. The results show that it is difficult to
identify general trends for the influence of hydraulic head, pre-
hydration, and confining stress on the interface transmissivity.
Nevertheless, for flow rate, accounting for both the initial water
content of the specimen and the confining stress appears to be
important (Barroso et al., 2006b). The effect of confining stress on
flow rate depends on the initial water content of the specimen. In
fact, the flow rate in pre-hydrated GCLs is about one order of
magnitude larger for a confining stress of 50 kPa than for a
confining stress of 200 kPa. For non-pre-hydrated specimens, the
flow rates for both confining stresses are similar under steady-
state-flow conditions (Barroso et al., 2006b).
4.1.2. Influence of geomembrane on flow rate
Barroso et al. (2008) investigated the case of a textured HDPE
geomembrane in contact with the GCL. Three different textured
geomembranes were used in these experiments. The results show
that the measurements are reproducible: the initial measurements
give a larger flow rate for smooth geomembranes than for textured
geomembranes; however, further measurements show that texture
has only a small impact on steady-state flow rates. This suggests
that, in the early phases of such measurements, water flows more
easily at the interface of smooth GMs. A texture seems to reduce the
space available at the interface for water flow. However, with time,
the sodium bentonite in the GCL swells, resulting in a better contact
between the GM and the GCL.
Bannour et al. (2013a) studied the effect of bituminous GMs in
contact with a GCL instead of a HDPE GM. This practice is not
recommended for environmental applications because doubts exist

1,E-03
10-3
upstream flow rate (m3/m2/d)

1,E-04
10-4

1,E-05 M4; 60 cm; 10 kPa M4; average from latest 7 days

10-5
M5; 60 cm; 10 kPa M5; average from latest 7 days
G1; 60 cm; 10 kPa G1; average from latest 7 days
G2; 60 cm; 10 kPa G2; average from latest 7 days
G3; 10 cm; 10 kPa G3; average latest 7 days
-6
10
1,E-06
0 1 2 3 4 5 6 7 8

Time (Days)

Fig. 6. Synopsis of upstream flow rates obtained for GCLs and multicomponent GCLs for the latest seven days of measurements.
 N. Touze-Foltz et al. / Geotextiles and Geomembranes 44 (2016) 656e672
about the chemical compatibility of the bituminous GM with
leachate for example; however, it works fine for hydraulic appli-
cations or landfill covers where no environmental stakes are
involved. Bannour et al. reported no significant difference in terms
of flow rates compared to the combination of a bituminous GM or a
HDPE GM, independently of which bituminous geomembrane face
(rough or smooth) is in contact with the GCL.
4.1.3. Influence on flow rate of concrete in contact with
geosynthetic clay liner
Rowe and Hosney (2014) examined the performance of four
GCLs for use as a hydraulic barrier below concrete-lined sewage-
treatment lagoons. Their research was based on a series of
laboratory-scale measurements designed to detect the change over
a 14 month period in the interface transmissivity, q, between the
GCLs and a 0.1-m-thick cast-in-place concrete above the GCL. The
four GCLs contained either untreated bentonite, polymer-enhanced
bentonite, granular bentonite, or powder bentonite. An increase in
the wastewater head from 1 to 2.5 m results in a decrease in the
interface transmissivity. For the GCL with untreated granular
bentonite, q ¼ 1.5  1011 m2/s (under 1 m) and decreases by about
one order of magnitude under 2.5 m. The change in interface
transmissivity of the GCL with polymer-enhanced granular
bentonite is greater than or similar to that for the GCL with un-
treated granular bentonite. For the GCL with untreated powder
bentonite and with 1280 g/m2 of bentonite in the cover geotextile,
q ¼ 1.8  1012 and 3.5  1013 m2/s at 1 and 2.5 m head,
respectively.
4.1.4. Influence on flow rate of composition of bentonite in
geosynthetic clay liner
The relationship between the composition of the bentonite in
the GCL (i.e., sodium or calcium bentonite) and flow rates in the GCL
was determined by Mendes et al. (2010), who concluded that the
composition of the bentonite and the manufacturing process of the
GCLs studied do not affect the transmissivity across the GM-GCL
interface under steady-state flow. They also noticed that, for holes
in the GM with diameters ranging from 4 to 10 mm, the diameter
has no significant influence on the flow rate through the GM-GCL
composite liner. The expansion of the sodium bentonite is effec-
tive in blocking the puncture in the geomembrane, leading to a
significant reduction in flow rate. These results suggest that GCLs
initially containing sodium bentonite, whose hydraulic conductiv-
ity increases due to cation exchange, can maintain low trans-
missivity at the GM-GCL interface and low flow rate through the
composite liner when used in a composite liner. This question will
be addressed in the next section.
4.1.5. Influence of bentonite ageing on flow rate
During its service life in a landfill barrier system, the bentonite
in the GCL is continuously subjected to cation exchange, whereby
sodium cations, which initially are between the bentonite platelets,
are replaced by multivalent cations that originate either in the
cover or in the bottom liner and that transfer upon contact with the
leachate or soil liner. Cation exchange leads to a decrease in GCL
swelling capacity (Lin and Benson, 2000; Barral et al., 2012) and
water absorption (Melchior, 2002) and to an order-of-magnitude
increase in hydraulic conductivity compared with virgin GCLs
(Egloffstein, 2001; Benson, 2013). Finally, as pointed out by
Egloffstein (2001), complete cation exchange occurs after one to
two years when the GCL is used in unsaturated conditions. To
simulate this situation, Rowe and Abdellaty (2012, 2013) made
measurements that show that the steady-state flow rate in GM-GCL
composite liners remains similar to that of virgin GCLs containing
sodium bentonite despite an increase in the hydraulic conductivity
663
of the GCL of the composite liner due to permeation by a highly
concentrated NaCl solution that results in cation exchange.
However, the GCL can also be subjected to wetedry cycles due to
moisture or temperature gradients generated across the whole
barrier by climatic conditions, especially in landfill covers and
dams. Wet-dry cycles damage GCLs; for example, desiccation with
shrinkage cracks leads to preferential flow paths when the GCL
hydrates (Melchior, 2002). The effect of cation exchange and
wetedry cycles on the hydraulic performance of GCLs has been
studied previously and is highly documented, especially as regards
landfill covers (Lin and Benson, 2000; Egloffstein, 2001, 2002;
Melchior, 2002; Southen and Rowe, 2005; Benson et al., 2007;
Bouazza et al., 2007; Meer and Benson, 2007; Zanzinger and
Touze-Foltz, 2009; Touze-Foltz et al., 2010b; Barral et al., 2012;
Benson, 2013). This effect represents the primary mode of degra-
dation for bentonite in GCLs. In fact, the combination of cation
exchange and wetedry cycles more strongly affects the swelling
capacity of the bentonite and causes a greater increase in the hy-
draulic conductivity of the GCL than does cation exchange alone, to
the point that the GCL no longer acts as a hydraulic barrier
(Egloffstein, 2001; Melchior, 2002; Meer and Benson, 2007; Benson
et al., 2007). In fact, after a number of wetedry cycles, shrinkage
cracks, which occur after desiccation, may not fully heal when the
bentonite hydrates. Cation exchange combined with wetedry cy-
cles occurring over the service life of GCLs lead to a significant in-
crease (four to five orders of magnitude) in the hydraulic
conductivity of the GCL. This raises the question of how the increase
in hydraulic conductivity affects the hydraulic characteristics of a
GM-GCL composite liner when the GM covering the GCL has a hole.
Bannour et al. (2014) used laboratory measurements to address
the question of how cation exchange combined with wetedry cy-
cles affects the flow rate and interface transmissivity of a GM-GCL
composite liner. Three of the GCLs measured were exhumed from
a dam and a fourth GCL was exhumed from a landfill. These
exhumed GCLs had endured cation exchange combined with
wetedry cycles, which had led to an increase in their hydraulic
conductivity and a decrease in their swell index. The flow rates of
these exhumed GCLs were compared with that of a composite liner
containing virgin GCLs: although the increase in hydraulic con-
ductivity of the GCL renders it permeable as a single liner, steady-
state flow rates and interface transmissivities for composite liners
containing GCLs that were pre-exposed to cation exchange and
wetedry cycles are of the same order of magnitude as for com-
posite liners containing virgin GCLs. Thus, the flow rate through
composite liners containing GCLs that were subjected to cation
exchange and wetedry cycles is not linked to hydraulic conduc-
tivity, even if the hydraulic conductivity of GCLs exhumed from
field sites has increased by four to five orders of magnitude with
respect to virgin GCLs. Thus, ageing of GCLs is not a concern when
they are used in a composite liner.
4.1.6. Summary of results
Fig. 7 gives an overview of the various interface transmissivity
data obtained from the studies discussed above. All data were ob-
tained under the conditions of geomembrane-GCL contact defined
by Barroso (2005), which means that the interface transmissivity
may be related to the hydraulic conductivity kGCL of the GCL as
follows:
log q ¼ 2:2322 þ 0:7155 log kGCL : (1)
In Equation (1), q is the interface transmissivity and kGCL is the
hydraulic conductivity of the GCL.
Recently, Bannour et al. (2015) defined the additional contact
condition given by Equation (2) (see Fig. 7) for composite liners
664 N. Touze-Foltz et al. / Geotextiles and Geomembranes 44 (2016) 656e672

Mendes et al. (2010)

-6
10
1E-06 Barroso et al (2006)

-7
Barroso et al (2008)
10
1E-07
Barroso et al. (2010)
Interface transmissivity, θ(m2/s) 10-8 Rowe and Abdellaty (2012)
1E-08
Bannour et al. (2013a)
10
-9 Excellent Bannour et al. (2014b)
1E-09

-10
10
1E-10
-11
10
1E-11
GM- GCL (after
10-12 cation exchange and
1E-12 GM- GCL (virgin) wetting drying cycles)
-13
10
1E-13
10-12
1E-12
-11
1E-11
10 -10
1E-10
10 -9
1E-09
10 -8
1E-08
10 -7
101E-07 10-61E-06 10-51E-05

Hydraulic conductivity (m/s)

Fig. 7. Synopsis of transmissivity taken from the literature for GCLs in contact with geomembranes and for GCLs after cation exchange and wet-dry cycles.

containing GCLs whose hydraulic exceeds 1010 m/s. This contact
condition is valid for GCLs pre-exposed to cation exchange and
wetedry cycles and can also be extended to GCLs containing cal-
cium bentonite. Therefore, the GM-GCL contact condition initially
given by Barroso (2005) for effective GCLs (i.e., kGCL less than
1010 m/s) is enhanced and readjusted for all GCLs, whatever their
composition or field history:
log q ¼ 8:5965 þ 0:1476 log kGCL :
4.2. Flow rates in multicomponent geosynthetic clay liners when
coating or film is damaged
A study was recently undertaken to determine whether the flow
rates through a multicomponent GCL with damaged coating or
attached film fall in the range obtained for more classical composite
liners with a GCL (Bannour et al., 2013b). Indeed, the results ob-
tained in the steady state do fall within the range of values obtained
for geomembrane-GCL interfaces.
To address a limitation in the measurements performed by
Bannour et al. (2013b) Bannour and Touze-Foltz (2015) extended
their work by making measurements on the meter scale, so that edge
effects become negligible (see Fig. 8). For all multicomponent GCLs
characterized, the coating or attached film was less than 0.7 mm
(2) thick. Steady-state results indicate that the flow rates range from
4.61  1012 to 3.01  1011 m3/s with interface transmissivities
ranging from 1.20  1011 to 7.59  1011 m2/s, which are broadly in
line with flow rates obtained from conventional GM-GCL composite
liners. Consequently, when the coating or attached film is damaged,
the thickness and rigidity of the coating or attached film appears not
to affect the steady-state flow rate and interface transmissivity,
which leads to good contact at the interface. The swell index and
mass per unit area of bentonite in multicomponent GCLs influence
the flow rate when a film is attached (i.e., glued) to the cover

Bannour and Touze-Foltz (2014) GCL 1 (m)

Bannour and Touze-Foltz (2014) GCL 2 (m)
Bannour and Touze-Foltz (2014) GCL 3 (m)
Bannour et al. (2013b) GCL 1 (dm)
Flow rate, Q (m3/s)

Bannour et al. (2013b) GCL 2 (dm)

Bannour et al. (2013b) GCL 3 (dm)

0 200 400 600 800 1000 1200

Time (h)

Fig. 8. Comparison of decimeter- and meter-scale flow-rate dynamics along multicomponent-GCL interfaces.
 N. Touze-Foltz et al. / Geotextiles and Geomembranes 44 (2016) 656e672
geotextile of the GCL. It is thus important that the mass of bentonite
in the GCL be sufficient so that the swelling capacity of samples leads
to better contact at the interface and thus to better performance of
the multicomponent GCL.
5. Diffusion in lining materials
5.1. Composition of leachate from landfills
Besides gaseous emissions, and in particular that of methane
and trace gases caused by the degradation of organic wastes,
leachate emissions from landfills pose the main potential long-term
environmental threat (Kjeldsen et al., 2002). Traditionally, leachate
analyses as a part of regular landfill monitoring have focused on
nitrogen content, oxygen consumption measured in the form of
biological oxygen demand or chemical oxygen demand, heavy
metals, and “classic” persistent organic pollutants such as dioxins
or polychlorinated biphenyls (Van Praagh et al., 2011).
Metals and metalloids are still recognized as priority pollutants.
In contrast with most organic pollutants, metals and metalloids do
not degrade in landfills. They are thus maintained in landfills and
are mobilized in the liquid or gaseous phases. The literature reports
considerable concentrations of metals and metalloids in leachate;
for example, Cd appears at a concentration of 0.2e20 mg/L, Cr at
5e600 mg/L, Mn at 0.01e70 mg/L, and Fe at 0.3e220 mg/L (Pinel-
Raffaitin et al., 2006).
Landfills also contain micropollutants with toxic effects (acute
toxicity, genotoxicity, reproductive toxicity, etc.) (Sisinno et al., 2000;
Takigami et al., 2002). The presence of organic contaminants in
leachate from municipal solid-waste landfills has been clearly
demonstrated in several countries (Oman and Hynning, 1993; Ahel
and Tepic, 2000; Robinson et al., 2001; Hiroshi et al., 2002).
Van Praagh et al. (2011) reviewed the Swedish and international
literature on analytical techniques and on the results of analysis
and quantification of several compounds or groups of emerging
organic pollutants in leachate. In eleven studies of organic sub-
stances in landfill leachate in various countries, a total of 592
different compounds were identified. The major fraction of the
substances identified may be categorized into the following groups
(in descending order of number of detections): phenolic com-
pounds, aromatic hydrocarbons, heterocyclic substances, carbox-
ylic acids, phthalates, anilines, aliphatic acids, phenoxy acids,
organo phosphorous substances, terpenoids, and triazines, some of
which are used as pesticides.
Quantifying the transfer to the surrounding environment of
organic pollutants from compounds emerging from leachate is thus
of primary importance.
5.2. Quantifying properties of transfer of chemicals through liner
materials
5.2.1. Theory of diffusive transfer through geosynthetic clay liners
Rowe and Booker (1987) developed a model for predicting the
one-dimensional transport of contaminants through soils of finite
thickness. The model accounts for realistic landfill parameters such
as dynamic surface-boundary concentrations, as is the case for
municipal solid-waste landfills. Lake and Rowe (2004), Rowe et al.
(2005), Rosin-Paumier et al. (2011), and Mendes et al. (2013; 2014a)
used this model to predict the one-dimensional transport of con-
taminants through a saturated GCL for a single reactive solute
without degradation. The model is based on Equation (3):
vC v2 C vC
n ¼ nDe 2  rd Kd (3)
vt vz vt
665
Where C is the concentration in the GCL at depth z and time t, n
is the total porosity of the GCL, De is the effective diffusion coeffi-
cient, rd is the dry density, and Kd is the sorption coefficient.
Diffusion coefficients can be estimated by solving Equation (3)
in combination with finite-mass boundary conditions (see Rowe
et al., 2004) for the measurement setup. Note that “finite mass”
refers to the fact that the concentration changes in time at both
boundaries because of mass transfer through the GCL and sampling
for the measurements. The sorption coefficient Kd is first deter-
mined from batch adsorption measurements (Lake and Rowe,
2004; Rowe et al., 2005; Ganne et al., 2008; Ahari et al., 2011).
Based on knowledge of the sorption coefficients of the various
components of a GCL (geotextiles, geotextile fibers in the bentonite,
bentonite), an equivalent sorption coefficient Kdeq for the entire
GCL may be calculated by using the method suggested by Rowe
et al. (2005), which accounts for sorption in the geotextile, the
bentonite, and geotextiles fibers in the bentonite. An overall
diffusion coefficient for the entire GCL can then be calculated for
each experiment and each contaminant, treating the entire GCL as a
homogeneous material.
5.2.2. Theory of diffusive transfer through geomembranes
The diffusion of vapor or aqueous permeants through geo-
membranes occurs in three steps: adsorption, diffusion, and
desorption. First, the contaminant is partitioned between the
source medium and the adjacent geomembrane surface. Second,
driven by chemical potential, the compound diffuses through the
geomembrane. Finally, the compound partitions between the outer
geomembrane surface and the receiving medium (Sangam and
Rowe, 2001). When a GM is immersed for sufficient time in a
fluid containing a contaminant of interest, equilibrium is reached
between the concentration cg in the GM and the concentration cf in
the fluid. These concentrations are related by Henry's law:
cg ¼ Sgf cf (4)
Where Sgf is the partition coefficient, which can be calculated
from batch sorption measurements (Sangam and Rowe, 2001). The
diffusion of organic compounds through a GM can be modeled by
using Fick's first law:


f ¼ Dg dcg =dz ; (5)
Where f is the mass flux or permeation rate per unit area, Dg is
the diffusion coefficient of organic compounds through the geo-
membrane, cg is the concentration of compound in the geo-
membrane, and z is the distance parallel to the direction of
diffusion. According to Fick's second law, the change in contami-
nant concentration with respect to time t at any point in the GM is
governed by the following differential equation:
vcg v2 cg
¼ Dg 2 (6)
vt vz
Desorption is also described by Henry's law. The partition co-
efficient into the GM is usually equal to the partition coefficient out
of the GM when the source and receptor fluid are the same
(Sangam, 2001). Because measuring the concentration of contam-
inant inside the GM is difficult, the concentration in the fluids on
either side of the geomembrane is used to infer the permeation
characteristics of the GM. The flux associated with the diffusion
process can also be expressed as:
dcf
f ¼ Pg (7)
dz
666 N. Touze-Foltz et al. / Geotextiles and Geomembranes 44 (2016) 656e672
Where Pg is the permeation coefficient or mass-transfer coefficient
(m2/s).
The diffusion coefficient can be obtained from double-
compartment tests (Islam and Rowe, 2009; McWatters and Rowe,
2008, 2010; Sangam and Rowe, 2001, 2005; Touze-Foltz et al.,
2012b) or immersion tests (Park et al., 2012).
5.3. Absorption onto components of geosynthetic clay liners
5.3.1. Case of organic pollutants
5.3.1.1. Adsorption onto geotextiles. To investigate the possible use
of geotextiles to retain pesticides in agricultural watersheds,
Boutron et al. (2009) measured batch adsorption and desorption of
diuron, isoproturon, and azoxystrobin onto and from commercially
available geotextiles. Similar studies were made of the adsorption
and desorption of polyamide, polyester, and polypropylene onto
and from polymeric fibers. Polyamide exhibited a high ability to
sorb diuron, with little desorption. The adsorption onto poly-
propylene and polyester was less significant but still non-negligible
(15% of the initial mass of pesticide in water for isoproturon and
30% for azoxystrobin).
Lake and Rowe (2004), Rowe et al. (2005), and Ganne et al.
(2008) addressed the potential for geotextiles to retain volatile
organic compounds (VOCs) from GCLs. The sorption isotherms are
linear for VOCs and the sorption coefficients range from 7 to 20 mL/
g for 1,2-dichloroethane, 79e102 mL/g for trichloroethylene,
20e41 mL/g for benzene, 87e135 mL/g for toluene, 229e248 mL/g
for ethylbenzene, 263e298 mL/g for m&p-xylene, and
163e192 mL/g for o-xylene. These values were obtained at 22
C.
Rowe et al. (2005) showed that diffusion and sorption depend on
temperature and that both parameters are lower at 7
C than at
22
C for benzene, toluene, ethylbenzene, m&p-xylene, and o-
xylene.
Ahari et al. (2011) studied the sorption of 13 phenolic com-
pounds: phenol, o-cresol, p-cresol, 2-chlorophenol (2-CP), 4-
chlorophenol (4-CP), 2,4-dimethylphenol (2,4-DMP), 3,4-
dimethylphenol (3,4-DMP), 2,4-dichlorophenol (2,4-DCP), 2,4,6-
trichlorophenol (2,4,6-TCP), 2,3,5,6-tetrachlorophenol (2,3,5,6-
TeCP), 2,3,4,6-tetrachlorophenol (2,3,4,6-TeCP), pentachloro-
phenol (PCP), and bisphenol A (BPA). They noticed that the
adsorption isotherms are nonlinear, contrary to what is observed
for VOCs (Rowe et al., 2005; Ganne et al., 2008). Therefore, Ahari
et al. (2011) used the Freundlich model to study adsorption. How-
ever, for the sake of comparing with previous results obtained from
VOCs, they also calculated Kd under the hypothesis of linear sorp-
tion (Ahari et al., 2011). For the compounds studied, all results for
Kd range from 2.7 to 8.9 mL/g. These values for the sorption coef-
ficient remain small compared with those obtained for VOCs. An
important observation is that the amount of chlorophenols sorbed
by geotextiles increases as the number of chlorine atoms in the
molecule increases.
5.3.1.2. Adsorption onto bentonite. Lake and Rowe (2004) also
studied the potential of bentonites to retain VOCs from GCLs. Very
small partition coefficients are reported in the literature (less than
1 mL/g).
Recently, several studies addressed the potential for sorption of
phenolic compounds onto bentonites or organobentonites (Banat
et al., 2000; Yoo et al., 2004; Hameed, 2007; Richards and
Bouazza, 2007; Malusis et al., 2010; Ahari et al., 2011). As stated
above, Ahari et al. (2011) obtained nonlinear adsorption curves for
bentonite, so they used the Freundlich model to model bentonite.
The results obtained are consistent with previous results from Banat
et al. (2000) for phenol. To compare with other published data on
linear adsorption isotherms, they also determined the adsorption
coefficient Kd. To study the adsorption of phenol onto bentonite,
they assumed a linear isotherm. The results obtained under this
assumption range from 2.5 to 2.6 mL/g, which are well within the
range given by Richards and Bouazza (2007) (Kd ¼ 1e5 mL/g) and by
Haijian et al. (2009) for phenol (Kd ¼ 1.2e3.3 mL/g). According to the
results for geotextiles, the adsorption of chlorophenols increases as
the number of chlorine atoms in the molecule increases. This study
also shows that the difference between the amount of phenolic
compounds adsorbed by the geotextile and that absorbed by the
bentonite is smaller than for VOCs.
5.3.2. Case of inorganic pollutants
Lange et al. (2004) examined the migration of various metals (Al,
Fe, Mn, Ni, Pb, Cd, Cu, Zn) through GCLs exposed to a synthetic
municipal solid-waste leachate. The GCLs are found to retard the
migration of the metals, although only under specific pH conditions.
The migration of Mn is the least attenuated. The migration of Al, Fe,
and Cu are strongly retarded, so these metals are retained within the
clay. The migration of Ni, Zn, and Cd is moderately attenuated. In
addition, Ca may have been responsible for the lack of metal reten-
tion of the leachate species. Due to the higher retention at higher pH
and the release of metals at lower pH, adsorption of hydrolyzed
species in addition to cation exchange are hypothesized to be the
mechanisms that contribute the most to metal retention.
5.4. Diffusive transfer through geosynthetic clay liners
5.4.1. Diffusion of inorganic species through geosynthetic clay liners
Lake and Rowe (2000) showed that, for void ratios ranging from
1.5 to 3, the diffusion coefficient of sodium and chloride increases
linearly with the bulk-GCL void ratio. The bulk-GCL void ratio was
defined by Petrov et al. (1997) as:
HGCL  Hs
eb ¼ (8)
Hs
Where HGCL is the GCL height; and Hs is the height of solids in the
GCL. The height Hs is defined by
Mbent Mgeo
Hs ¼ þ (9)
rs ð1 þ w0 Þ rsg
where Mbent is the mass of bentonite per unit area in the GCL, Mgeo
is the mass of geosynthetics per unit area in the GCL, rs is the
density of bentonite solids, rsg is the density of polypropylene
geotextile solids; and w0 is the initial water content of the
bentonite.
The diffusion coefficients of sodium and chloride inferred from
GCL diffusion measurements done with 3e5 g/L solutions decrease
linearly with decreasing final bulk-GCL void ratio. The diffusion
coefficient was shown to depend on the source solution and, upon
significantly increasing the NaCl concentration, the diffusion coef-
ficient inferred also increased. The diffusion coefficients were
estimated to range from 1  1010 to 2  1010 m2/s.
Lange et al. (2009) studied the diffusion of various metals for the
following four cases where a GCL might serve as an effective barrier
against metals and metalloids: acidic rock drainage, gold-mine
tailings, lime-treated mine effluent, and municipal solid waste.
The averaged diffusion coefficients for Cu, Cd, Zn, Fe, and Ni covered
a narrow range from 6.7  1011 to 8.9  1011 m2/s. The diffusion
coefficients for As, Al, Mg, Mn, and Sr range from 8.0  1011 to
1.6  1010 m2/s. The diffusion coefficients of the individual metals
did not change significantly upon changing the composition of the
solution, which suggests that, although the composition of the
solution has some effect on the diffusion coefficient of the metal,
 N. Touze-Foltz et al. / Geotextiles and Geomembranes 44 (2016) 656e672
sorption onto the GCL is the dominant factor controlling the metal
mobility.
5.4.2. Diffusion of organic species through geosynthetic clay liners
The diffusion mechanisms of VOCs were also quantified for
virgin GCLs (Lake and Rowe, 2004; Rowe et al., 2005; Ganne et al.,
2008) containing sodium bentonite. Lake and Rowe (2004)
observed no significant increase in the diffusion coefficient for
bulk-GCL void ratios ranging from 4.1 to 4.8. Their results indicate
that bulk-GCL void ratios ranging from 4.1 to 4.8 correspond to low
normal stress and that the corresponding diffusion coefficients
represent an upper bound for diffusion coefficients. In further
studies, Rosin-Paumier et al. (2011) reported that the composition
of the bentonite (natural sodium versus calcium-activated) has no
significant impact on the diffusion of VOCs. At 23
C, the diffusion
coefficients for VOCs in bentonite range from 1 to 3  1010 m2/s for
bulk-GCL void ratios ranging from 3.7 to 4.8.
Mendes et al. (2013) quantified the diffusion of seven phenolic
compounds through GCLs and reported diffusion coefficients for
virgin GCLs that range from 5  1011 to 1.3  1010 m2/s for meth-
ylphenols and from 5  1011 to 6.3  1011 m2/s for chlorophenols.
These values fall in the lower range of diffusion coefficients reported
in the literature for the diffusion through virgin GCLs.
5.4.3. Aged GCLs after cation exchange
Rosin-Paumier et al. (2011) subjected a GCL containing natural
sodium bentonite to cation exchange by permeating the GCL with a
synthetic leachate containing a mixture of monovalent and divalent
cations in proportions representative of what is found in actual
landfill leachate. They reported that cation exchange leads to an
increase in the hydraulic conductivity of the GCL by a factor 8.5.
They then studied diffusion in three specimens cut from the sample
and subjected to cation exchange and reported an increase in the
diffusion coefficient of VOCs compared with that of virgin GCL
specimens for a bulk-GCL void ratio of 3.9. Trichloroethylene ex-
hibits the largest increase in diffusion coefficient of the VOCs
studied: from 1.0  1010 to 2.6  1010. The diffusion coefficients
for dichloromethane (DCM) and dichloroethane (DCA) increase by a
factor about 1.4 (from 2.3  1010 to 3.1  1010 m2/s and from
1.9  1010 to 2.6  1010 m2/s, respectively). This ratio is not as
large as the analogous ratio for the increase in the hydraulic con-
ductivity of the GCL. In addition, a decrease in the bulk-GCL void
ratio from 3.9 to 3 would negate the effect of cation exchange so
that the diffusion coefficient would not increase for DCM and DCA.
Such a decrease in the bulk-GCL void ratio could occur over the
lifetime of the landfill as the height of the waste increases. Thus, a
detrimental effect of cation exchange on the hydraulic conductivity
of a GCL is not necessarily indicative of a detrimental effect on the
diffusion coefficient of VOCs through GCLs. This result remains to be
confirmed for other GCLs and other pollutants.
For phenolic compounds in aged GCL specimens, diffusion co-
efficients range from 2  1010 to 6.4  1010 m2/s for methyl-
phenols and from 8.1  1011 to 2.5  1010 m2/s for chlorophenols.
Due to the high sorption of methylphenols observed in the control
cell, only the order of magnitude of these diffusion coefficients is
considered significant (Mendes et al., 2013). Mendes et al. (2014a)
also quantified the diffusion of bisphenol A after cation exchange
for the same GCL specimen. They obtained a diffusion coefficient of
2.2  1010 m2/s.
5.5. Diffusive transfer through geomembranes
5.5.1. Diffusion of inorganic species
Rowe (2005) presented the results of a measurement of the
diffusion of chloride through a geomembrane that, at the time of
667
publication, had run for 12 years. The receptor concentration in this
measurement remained below about 0.02% of the source concen-
tration, lying within the range of analytical uncertainty for the
chemical analysis. Rowe (2005) also cites a study by August and
Tatsky (1984) that concludes that negligible diffusion of heavy-
metal salts from a 0.5 M acid solution occurs through a HDPE GM
over a four year measurement period. Based on these results, Rowe
(2012) concluded that an intact GM is an excellent barrier against
advective and diffusive migration of inorganic contaminants from a
leachate.
5.5.2. Diffusion of organic species
August and Tatsky (1984) found that the permeation rates in a
HDPE GM of strongly polar penetrant molecules range from
7  107 m3 m2 d1 for methanol to 9.4  106 m3 m2 d1 for
trichloroethylene.
A number of studies on the use of GMs have focused on the
diffusion of VOCs through virgin HDPE GMs (Park and Nibras, 1993;
Prasad et al., 1994; Müller et al., 1998; Sangam and Rowe, 2001;
Touze-Foltz et al., 2011; Park et al., 2012) virgin PVC, linear low-
density polyethylene (LLDPE) GMs with and without a co-extruded
ethylene vinyl-alcohol (EVOH) inner core (McWatters and Rowe,
2008, 2010; Eun et al., 2014), fluorinated HDPE GMs (Sangam and
Rowe, 2005), and aged HDPE GMs (Rowe et al., 2003; Islam and
Rowe, 2009). The diffusion coefficients of VOCs in virgin HDPE GMs
are 0.37  1013 and 22.8  1013 m2/s for benzene and DCM,
respectively, with partition coefficients ranging from 1.8 to 189. The
resulting permeation coefficient lies between 1 and 70  1012 m2/s.
Sangam and Rowe (2005) examined how surface fluorination of
a HDPE GM affects the diffusion of VOCs. In this study, surface
fluorination consisted of applying elemental fluorine, which ex-
changes with hydrogen along polymer chains at the surface of a
polyolefin substrate. The partition coefficient remains essentially
the same after surface fluorination; however, surface fluorination
reduces both the diffusion and the permeation coefficients by
factors between 1.5 and 4.5, depending on the hydrocarbon
examined.
McWaters and Rowe (2010) studied diffusive migration of the
aqueous and vapor phases of benzene, toluene, ethylbenzene, and
xylenes through a 0.76-mm-thick PVC-P GM and a 0.76-mm-thick
LLDPE GM. For the PVC GM, diffusion coefficients ranged from 5 to
10  1013 m2/s for diffusion from both the aqueous and vapor
states. For the LLDPE GM, diffusion coefficients ranged from 2.5 to
5  1013 m2/s. The partition coefficients for PVC ranged from 100
to 1075 with respect to aqueous-phase concentrations. The parti-
tion coefficients for vapor-phase concentrations ranged from 22 to
290. For the LLDPE GM, partition coefficients ranged from 200 to
475 for aqueous-phase concentrations and from 44 to 123 for
vapor-phase concentrations. The resulting permeation coefficients
thus range from 130 to 750  1012 m2/s for PVC GMs and from 60
to 110  1012 m2/s for LLDPE GMs.
McWaters and Rowe (2010) also studied the diffusive proper-
ties of two coextruded GMs, one with a polyamide inner core and
the other with an EVOH inner core, and a standard 0.53-mm-thick
LLDPE GM. The results indicate a significant reduction in mass flux
through the coextruded GMs compared with the conventional
LLDPE GM. The EVOH coextruded GM has the lowest permeation
coefficients of about 8  1015 m2/s for diffusion from the aqueous
phase. These permeation coefficients for the EVOH coextruded GM
are upper bounds; actual values may be even lower. The polyamide
coextruded GM has higher permeation coefficients than the EVOH
coextruded GM, ranging from 5 to 8  1014 m2/s from the aqueous
phase. The standard LLDPE GM has the highest diffusion co-
efficients, which range from 2 to 4  1013 m2/s. The partition
coefficients for the EVOH coextruded GM range from 160 to 700 for
668 N. Touze-Foltz et al. / Geotextiles and Geomembranes 44 (2016) 656e672

aqueous-phase concentrations. For the polyamide coextruded GM,
the partition coefficients range from 120 to 430 and, for the LLDPE
GM, the partition coefficients range from 180 to 450 for aqueous-
phase concentrations. In summary, the permeation coefficients
range from 2 to 6  1012 m2/s for the EVOH coextruded GM, from
7 to 22  1012 m2/s for the polyamide coextruded GM, and from
60 to 200  1012 m2/s for the LLDPE GM.
The EVOH coextruded GM thus offers a five-to twelve-fold
decrease in the permeation coefficient compared with a 2.0-mm-
thick HDPE GM.
The question is of the prediction of the evolution of the diffusion
coefficient, the partition coefficient, and the permeation coefficient
as it may not be possible in the future to keep on performing
measurements for the variety of contaminants that can be
encountered in environmental applications.
Theory to predict the evolution of the diffusion coefficient, the
partition coefficient, and the permeation coefficient as functions of
solubility, octanolewater partition coefficient, and molecular
diameter of various VOCs is given in the literature for the diffusion
of VOCs through virgin HDPE GMs (Sangam and Rowe, 2001; Joo
et al., 2004; Park et al., 2012).
The diffusion of polybriominated diphenyl ethers (PBDE) (Saheli
et al., 2011) is currently under study.
Touze-Foltz et al. (2012b) studied the diffusion of phenol, o-
cresol, p-cresol, 2,4-xylenol, 3,4-xylenol, 2-chlorophenol, 4-
chlorophenol, 2,4-dichlorophenol, 2,4,6-trichlorophenol, 2,3,4,6-
tetrachlorophenol, 2,3,5,6-tetrachlorophenol, pentachlorophenol,
and BPA through a virgin HDPE GM. The results show that the
partition coefficient is linked to the aqueous solubility and the n-
octanol-water partition coefficient of the contaminant. This latest
result is logical because less polar contaminants are less soluble in
water. No clear link is found with the molecular diameter when all
phenolic compounds are taken into account (especially BPA).
However, for chlorophenols a strong correlation appears between
molecular weight and partition coefficient, which may be related to
polarity. An analysis of the sole chlorophenols (2-CP, 4-CP, 2,4-DCP,
2,3,6-TCP, 2,3,4,6-TeCP, 2,3,5,6-TeCP, and PCP) suggests that the
partition coefficient is closely linked with the degree of substitution

6
1000000
106 1000000
10
Joo et al. (2004) Joo et al. (2004)
Park et al. (2012)
Park et al.(2012)
100000 5 Sangam and Rowe (2001)
105
100000 Phenols (GMB) 10
Phenols (GMB)
VOCs (GMB) VOCs (GMB)
Chlorophenols (v PE Film) 4
10000
10 Chlorophenols (v PE Film)
104
10000 Chlorophenols (a PE Film) Chlorophenols (a PE Film)

1000
10
3

103
1000
2
100
10
Sgf

Sgf

102
100
10

10
1

1 0.1

0.1 0.01
0 0.010.1
0.0010.01 0.1 11 10
10 100
102 1000
10310000
10100000
4 105 106 107
1000000
1000000 -1 0 1 2 3 4 5 6
S (mg/L)
S (mg/l) log Kow

(a) (b)
6
1000000
10 1000000
10
6

Park et al. (2012) Phenols (GMB)

5
Phenols (GMB) VOCs (GMB)
100000
10 1000005 10
VOCs (GMB) Chlorophenols (v PE Film)
Chlorophenols (a PE Film)
Chlorophenols (v PE Film)
4 4
10
10000 Chlorophenols (a PE Film) 10000
10

3
10
1000 103
1000
Sgf

Sgf

2 2
10
100 10
100

10 10

1 1

0.1 0.1
0.45 0.6 0.75 0.9 0 100 200 300
dm (nm) Molecular weight (g/mol)
(c) (d)

Fig. 9. Partition coefficient Sgf as a function of (a) aqueous solubility S, (b) n-octanol-water partition coefficient Kow, (c) molecular diameter dm, and (d) molecular weight for
phenolic compounds and VOCs in diffusion experiments with geomembranes, and for chlorophenols in diffusion experiments with virgin and aged PE films (“v PE Film” and “a PE
Film,” respectively).
 N. Touze-Foltz et al. / Geotextiles and Geomembranes 44 (2016) 656e672 669

10 10

1 1

Dg (x 10-12m²/s)

Dg (x 10-12m²/s)
0.1 0.1

0.01 0.01

Park et al. (2012)

Park et al. (2012)
Sangam and Rowe (2001)
Phenols (GMB) Phenols (GMB)
0.001 0.001
VOCs (GMB) VOCs (GMB)
Chlorophenols (v PE Film) Chlorophenols (v PE Film)
Chlorophenols (a PE Film) Chlorophenols (a PE Film)
0.0001 0.0001
0.0010.01
0 0.010.10.1 1 1 1010100
101000
2 1010000
100000
3 10 1000000
4 10 10000000
5 10 6 107 -1 0 1 2 3 4 5 6
SS(mg/l)
(mg/L) log Kow

(a) (b)

10 10

1 1
Dg (x 10-12m²/s)

0.1
Dg (x 10-12m²/s)

0.1

0.01 0.01
Phenols (GMB)

Joo et al. (2004) VOCs (GMB)

Park et al. (2012) Helmroth et al. (2002)
0.001 Phenols (GMB) 0.001
Brandsch et al. (1999)
VOCs (GMB)
Chlorophenols (v PE Film) Chlorophenols (v PE Film)
Chlorophenols (a PE Film) Chlorophenols (a PE Film)
0.0001 0.0001
0.45 0.6 0.75 0.9 0 100 200 300
dm (nm) Molecular weight (g/mol)

(c) (d)

Fig. 10. Diffusion coefficient Dg as function of (a) aqueous solubility, (b) n-octanol-water partition coefficient Kow, (c) molecular diameter dm, and (d) molecular weight for phenolic
compounds and VOCs in diffusion experiments with geomembranes, and for chlorophenols in diffusion experiments with virgin and aged PE films (“v PE Film” and “a PE Film,” respectively).

of chlorine atoms on the phenolic nucleus, a phenomenon that may
also be attributed to a difference in polarity of the various chlor-
ophenols studied.
The partition coefficients of phenolic compounds are small
compared with those of VOCs with similar chemical structure (e.g.,
benzene compared with phenol and toluene compared with o-
cresol and p-cresol), which suggests that the partition coefficient
decreases as the hydroxyl group solubilizes the molecule.
The diffusion coefficient is well correlated with the aqueous
solubility and the n-octanol-water partition coefficient of the
phenolic compounds (see Fig. 9). A good correlation with the mo-
lecular diameter is also obtained when one disregards the results
obtained for BPA.
These trends are consistent with those previously obtained for
VOCs. However, the range of obtained for the parameters differs
significantly from that obtained for the VOCs, which means that
the empirical equations available in the literature that were
derived for VOCs are not valid for predicting the evolution of the
permeation coefficient (see Fig. 10) of phenolic compounds, except
for predicting its evolution with molecular diameter (excluding
the parameters obtained for BPA). These trends require further
confirmation for other chemical families before attempting to
predict the diffusion coefficient based only on the molecular
diameter (for molecular diameters close to 0.5 nm).
5.5.3. Effect of geomembrane ageing on diffusion
Islam and Rowe (2009) examined the effects of aging of HDPE GMs
on the diffusion and the partition of benzene, toluene, ethylbenzene,
and xylenes. For this study, two different 1.5-mm-thick HDPE GMs
were aged in the laboratory at 85
C by immersion in a synthetic
leachate for up to 32 months. Partition and diffusion measurements
were made at room temperature on both unaged and aged GMs by
using a dilute aqueous solution. The diffusion and partition co-
efficients decrease as aging progresses. After aging the GM for 10e32
months, the inferred permeation coefficients decreased by 36%e62%.
This decrease in the diffusion, partition, and permeation coefficients
is related to the increase during aging in GM crystallinity.
These results for aging are consistent with previous results from
Rowe et al. (2003), who showed that the permeation coefficient for a
14-year-old HDPE GM sampled from a leachate lagoon is between
670 N. Touze-Foltz et al. / Geotextiles and Geomembranes 44 (2016) 656e672
four and five times less than that obtained for unaged HDPE GMs
typical of what is produced today (i.e., no virgin specimen was
available). Measurements were recently performed to elucidate the
effect of GM aging on the diffusion of phenolic compounds through
GMs. The diffusion of 2,4,6-trichlorophenol, 2,3,5,6-
tetrachlorophenol, and pentachlorophenol through two 17-year-old
high-density polyethylene geomembranes (HDPE GMs) was studied
(Touze-Foltz et al., 2016). The first was stored indoors away from
direct sunlight whereas the second was exposed for the entire time in
a south-facing corner of a pond. Both unexposed and exposed spec-
imens, although under different exposure conditions, experienced
ageing. Partition coefficients ranged from 30 to 190, increasing with
the number of chlorine atoms in the contaminant. Diffusion co-
efficients for the unexposed geomembrane ranged from 9  1014 to
2.4  1013 m2/s and from 9  1014 to 2.8  1013 m2/s for the
exposed geomembrane. These values were compared with those
reported in the literature for diffusion of the same phenolic com-
pounds through a virgin HDPE geomembrane from a different
manufacturer: the exposure did not noticeably affect the partition
coefficients or diffusion coefficients. This result was linked to the
temporal evolution of the unexposed geomembrane. Furthermore, in
spite of their 17-year ageing, both geomembrane specimens still had
diffusive characteristics that were consistent with a virgin geo-
membrane obtained from a different manufacturer.
Mendes et al. (2014b) made preliminary measurements of the
diffusion of chlorophenols (4-chlorophenol, 2,4-dichlorophenol,
2,4,6-tricholophenol, 2,3,5,6-tetrachlorophenol, and pentachloro-
phenol) through PE films produced from the same base resin as a
HDPE GM that is commercially available in Europe. The molar mass in
number (Mn) and the molecular weight (Mw) of the resin, as deter-
mined by “ultrahigh-temperature” gas-phase chromatography, are
Mn ¼ 44.1 kg/mol and Mw ¼ 136.7 kg/mol. The PE density is 0.911 kg/
m3 and the crystallinity fraction is 51%. The films were fabricated
from pellets. Some of the virgin PE film specimens were aged by
thermo-oxidation at 105
C, which leads to the formation of carbonyl
compounds (alcohols, carboxylic acids, etc.) and to an expected in-
crease in crystallinity. The final carbonyl concentrations in the
oxidized samples were between 0.1 and 0.4 mol/kg, which was ob-
tained after 300 h of thermo-oxidation (Pons, 2012). For such
carbonyl concentrations, the crystallinity fraction ranged from 54% to
66% according to the calibration curve proposed by Pons (2012) for
the same polymer as used in this study. These results for crystallinity
fraction should be compared with 51% crystallinity fraction for virgin
PE. For PE films, the partition coefficients increase with increasing
number of chlorine atoms for chlorophenols, whereas the diffusion
coefficients generally decrease with increasing number of chlorine
atoms. In addition, the diffusion coefficients decrease with the in-
crease in crystallinity that occurs upon aging. The permeation co-
efficients, however, increase; contrary to what was reported by Rowe
et al. (2003) when they compared the diffusion of chlorinated and
aromatic hydrocarbons through a new modern HDPE GM with that
through a 14-year-old HDPE GM. These results show that the parti-
tion coefficient is linked to the aqueous solubility and the n-octanol-
water partition coefficient of the contaminant. In view of the results
reported by Touze-Foltz et al. (2012a,b), this latest result seems
logical because less polar contaminants are less soluble in water.
Although no clear evidence supports a link with the molecular
diameter, for chlorophenols the molecular weight correlates well
with the partition coefficient; a result that may be related to polarity.
An analysis of the chlorophenols under study (4-CP, 2,4-DCP,
2,4,6-TCP, 2,3,5,6-TeCP, and PCP) implies that the partition coefficient
is closely linked with the degree of substitution of chlorine atoms on
the phenolic nucleusda phenomenon that may also be attributed to
a difference in polarity between the various chlorophenols studied,
as noticed by Touze-Foltz et al. (2012b). The diffusion coefficient and
permeation coefficient correlate well with the aqueous solubility and
the n-octanol-water partition coefficient of the chlorophenols, and
they also correlate well with the molecular diameter.
These trends are consistent with previous trends obtained for
the diffusion of VOCs and phenolic compounds through GMs.
However, the ranges obtained for the parameters differ signifi-
cantly, so the empirical equations published for VOCs cannot be
used to predict the evolution of the partition coefficient of the
chlorophenols studied herein or of the phenolic compounds stud-
ied by Touze-Foltz et al. (2012b). However, equations previously
used in the field of PE films for food packaging and that link the
diffusion coefficient to the molecular mass (Brandsch et al., 1999;
Helmroth et al., 2002) prove to apply to the data discussed herein
for GMs (see Fig. 10).
6. Conclusion
The first objective of this review paper is to present the state-of-
the-art measurement techniques for evaluating properties of
transfer of chemicals in lining materials for landfills. The second
objective is to summarize the current knowledge regarding
advective and diffusive transfer parameters for GMs and GCLs,
included multicomponent GCLs.
The retention curves of GCLs are discussed first because they are
crucial for predicting transfer through barriers, including GCLs that
contain bentonite with a low water content and that may be
installed in environmental applications and therefore subject to
desiccation. Thus, knowledge of the hydration path is important to
adequately predict advective transfer in GCLs or composite liners
containing GCLs. Recently obtained results provide evidence that
load has a significant effect on the retention curves of GCLs.
Section 3 discusses the quantification of advective flow rates in
GMs and multicomponent GCLs. Although no dedicated standard
exists for GCLs, a procedure was recently developed to quantify
advective flow in these materials. The existing methodologies allow
us to study the potential evolution of the flow rate in GMs during
their lifetime at a site and to detect a decrease in performance,
which occurs, for example, to oxidized bituminous GMs when left
uncovered. For multicomponent GCLs, the procedure developed,
which will become a French standard, allows us to differentiate
between the hydraulic performance of the various multicomponent
GCLs currently on the market. The evidence shows that, when the
film or coating is sufficiently thick, it is this component rather than
the bentonite in the GCL that maintains the lining. This brings into
question the definition of multicomponent GCLs that cannot be
categorized as caly geosynthetic barriers.
Section 4 discusses the advective flow rate due to holes either in
GMs used in association with GCLs or in the film or coating of
multicomponent GCLs. The thickness of the film or coating was
found to have no detectable influence on the meter scale. In addi-
tion, results obtained in the steady state are not significantly
impacted by the composition of the GM, its texture, the composi-
tion of the bentonite, or bentonite ageing as regards cation ex-
change and cation exchange combined with hydrationedesiccation
cycles. Based on the data presented herein, the question of GCL
ageing does not appear relevant if the GCL is used in association
with a GM in a composite liner.
Finally, the diffusion of organic and inorganic species through
GCLs and GM is discussed. Until recently very few species had been
investigated. Data now exist on various types of geomembranes,
especially as regards the diffusion of VOCs. A recent study has
shown that the empirical laws used for predicting the diffusion of
VOCs in GMs cannot be extended to other chemical families, such
phenolic compounds. This situation emphasizes the need for
further research in this field.
 N. Touze-Foltz et al. / Geotextiles and Geomembranes 44 (2016) 656e672 671

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