ARTICLE IN PRESS

Geotextiles and Geomembranes 25 (2007) 360–365

www.elsevier.com/locate/geotexmem

Comparison of the equilibrium sorption of five organic compounds to

HDPE, PP, and PVC geomembranes
Edidia K. Nefsoa, Susan E. Burnsb,
a
Malcolm Pirnie, Inc., 701 Town Center Drive, Suite 600, Newport News, VA 23606, USA
b
School of Civil and Environmental Engineering, 790 Atlantic Drive, N.W., Georgia Institute of Technology, Atlanta, GA 30332-0355, USA
Received 4 March 2006; received in revised form 9 November 2006; accepted 3 December 2006
Available online 5 February 2007

Abstract

This experimental investigation quantified the sorption uptake of five commonly encountered organic groundwater contaminants,
methyl tertiary-butyl-ether (MTBE), benzene, trichloroethylene (TCE), 1,2-dichorobenzene (1,2-DCB), and trinitrotoluene (TNT), to
geomembranes made from high density polyethylene (HDPE), polypropylene (PP), and polyvinylchloride (PVC). The organic
compounds were chosen to span a range of aqueous solubilities and chemical properties. The geomembranes tested in this study
exhibited sorption capacities that were of similar magnitude for each of the contaminants tested, with the exception of 1,2-DCB to
HDPE, which exhibited strong uptake in comparison to the other solute/sorbent combinations. In general, the PVC geomembrane
demonstrated the highest sorption capacities, while the HDPE geomembrane demonstrated the lowest sorption capacities. Measured
partitioning coefficients for the contaminant/geomembrane combinations ranged from Sgfo1 to 160, but most commonly had values
between 10 and 75.
r 2007 Elsevier Ltd. All rights reserved.

Keywords: Geomembrane; Sorption; Volatile organic compound

1. Introduction range of chemical properties. Sorption isotherms were

Geomembranes are integral components of composite
liner systems, and are designed to reduce the advective flow
of contaminated leachate from a landfill (Cartaud et al.,
2005; Barroso et al., 2006; Koerner and Koerner, 2006;
Touze-Foltz et al., 2006). They also serve as a protective
barrier against the diffusive movement of inorganic
compounds; however, they are less effective at limiting
the diffusive movement of organic contaminants from
contaminated leachate because the contaminants partition
into and diffuse through the geomembrane material
(Rowe, 2005).
This paper measures the partition coefficients of seven
geomembranes, composed of high density polyethylene
(HDPE), polypropylene (PP), or polyvinyl chloride (PVC),
for five organic contaminants which were chosen to span a
Corresponding author. Tel.: +1 404 894 2285; fax: +1 404 894 2281.
E-mail addresses: enefso@hotmail.com (E.K. Nefso), sburns@gatech.
edu (S.E. Burns).
developed to relate the ratio of the mass of contaminant
sorbed to each geomembrane to the equilibrium aqueous
concentration of the contaminant in solution.
2. Background
Extensive work has been performed to quantify the
partitioning of a variety of organic compounds to HDPE
geomembranes. A comprehensive review of the theoretical
considerations in the partitioning and diffusion of con-
taminants through geomembranes is given in Sangam and
Rowe (2001); however, a summary of the issues critical to
understanding partitioning of contaminants in geomem-
branes is given here for clarity. Movement of organic
contaminants from an aqueous medium through geomem-
branes consists of three steps: (1) partition of the
contaminant between the geomembrane surface and the
aqueous solution, (2) diffusion of the contaminant through
the geomembrane, and (3) partition from the outer edge of
the geomembrane into the receiving medium (Haxo and

0266-1144/$ - see front matter r 2007 Elsevier Ltd. All rights reserved.
doi:10.1016/j.geotexmem.2006.12.002
 ARTICLE IN PRESS
E.K. Nefso, S.E. Burns / Geotextiles and Geomembranes 25 (2007) 360–365 361

Lahey, 1988; Park and Nibras, 1993; Prasad et al., 1994; This study quantifies the sorption of five organic
Park et al., 1996; Sangam and Rowe, 2001; Joo et al., compounds, chosen to span a range of aqueous solubilities,
2004). The partition coefficient represents the concentra- polarities, molecular weights, and molar volumes, to three
tion of the organic compound in the geomembrane to the polymeric geomembranes: HDPE, PP, and PVC. The
concentration in the aqueous medium after equilibrium has sorption results are reported in terms of the partition
been established. The partition coefficient can be presented coefficient.
in dimensionless form through the following relationship
(Sangam and Rowe, 2001):
3. Experimental investigation
cg ¼ Sgf C f ,
Batch sorption experiments were conducted to quantify
the sorptive capacity of geomembranes of three different
where Sgf ¼ partitioning coefficient [dimensionless],
polymeric units: HDPE (four types), PP (2 types), and
cg ¼ equilibrium contaminant concentration in geomem-
PVC. The seven geomembranes were reacted with five
brane [M/L3], and cf ¼ equilibrium contaminant concen-
commonly encountered groundwater contaminants and
tration in solution [M/L3].
leachate constituents: 2-methoxy-2-methylpropane (or,
The quantity of a contaminant sorbed to a geomem-
methyl tertiary-butyl ether, MTBE), benzene, TCE,
brane at equilibrium will be a function of contaminant,
o-dichlorobenzene (1,2-DCB), and trinitrotoluene (TNT).
geomembrane type, and temperature (Sangam and Rowe,
In addition to frequency of detection, the contaminants
2001). When the sorption of contaminants to a sorbent
were chosen to span a range of aqueous solubilities,
follows a linear relationship, as is typically the case for the
sorption affinities, and chemical characteristics (Table 1).
sorption of organic compounds to geomembranes, the
partition coefficient can be measured using a one point test
conducted at a single aqueous concentration. Alternately, 3.1. Materials
the full sorption isotherm can be described by performing a
series of sorption tests over a range of initial aqueous Seven geomembranes were obtained for sorption testing.
concentrations. These included four HDPE geomembranes with different
Aminabhavi and Naik (1998) measured the partition textures and thicknesses (1.016 and 1.524 mm, smooth and
coefficients of 14 organic compounds in one polypropylene rough) obtained from GSE Lining Technology, Inc.
and three polyethylene geomembranes by monitoring the (Houston, TX); a GSE Proflex polypropylene geomem-
increase in the mass of the geomembrane immersed in the brane (1.016 mm) obtained from GSE lining Technology,
fluid of interest, and the data were used to calculate Inc. (Houston, TX), and a scrim reinforced polypropylene
diffusion coefficients based on Fick’s Law. Sangam and geomembrane (1.143 mm) obtained from Stevens Roofing
Rowe (2001) used gas chromatography to determine the Systems (Holyoke, MA); and a PVC geomembrane
partition coefficients of three chlorinated and four aro- (0.752 mm) obtained from the PVC Geomembrane Insti-
matic hydrocarbons to a 2.0 mm thick HDPE geomem- tute (University of Illinois, Urbana Champaign, IL). All
brane, and developed predictive relationships for sorption geomembranes were used as received.
to HDPE as a function of octanol water partition The chemicals used in the investigation included: MTBE
coefficients and chemical molecular weight. The results (Aldrich Chemical Company); benzene (Fisher Scientific);
were also used to develop a mass transport model. Park TCE (Fisher Scientific); 1,2-DCB (Sigma-Aldrich); and
and Nibras (1993) measured the sorption of eleven organic powdered 2,4,6-TNT (C6H2CH3(NO2)3) (Chem Service)
compounds to HDPE geomembranes, and examined the submerged in water; and the radiolabeled chemicals:
14
effects of competitive sorption. Their results were used to C-MTBE (Aldrich Chemical Company); 14C-benzene
predict mass flux relationships of gasoline component (Aldrich Chemical Company); 14C-TCE (Aldrich Chemical
organics through geomembranes. Joo et al. (2004) mea- Company); 14C-1,2-DCB (Aldrich Chemical Company);
sured uptake capacity of HDPE for benzene and trichlor-
oethylene (TCE), in the context of developing a mass Table 1
transport model. Literature reported values for the Properties of organic compounds used in sorption testing
partition coefficient of benzene in HDPE are approxi- Organic Chemical Molecular Density Molar Aqueous
mately 30 (Sangam and Rowe, 2001; Joo et al., 2004), and compound formula weight (g/mL) volume solubility
for TCE in HDPE range from 45 to 85 (Park and Nibras, (g/mol) (mL/mol) 25 1C
1993; Sangam and Rowe, 2001; Joo et al., 2004). (mg/L)
Investigations of the effect of surface fluorination on the MTBE C5H12O 88.15 0.741 119.0 51,000
uptake of HDPE for nine organic compounds demon- Benzene C6H6 78.11 0.8786 88.9 1780
strated that the partitioning coefficient was essentially TCE C2HCl3 131.4 1.4642 89.7 1100
unchanged by the addition of elemental fluorine; however, 1,2-DCB C6H4Cl2 147.0 1.304 112.7 147
the diffusion and permeation coefficients were reduced TNT C7H5N3O6 227.1 1.654 137.3 100
(20 1C)
(Sangam and Rowe, 2005).
 ARTICLE IN PRESS
362 E.K. Nefso, S.E. Burns / Geotextiles and Geomembranes 25 (2007) 360–365
powdered 14C-2,4,6-TNT submerged in water (Eagle Picher
Pharmaceutical Services); and scintillation cocktail (UVA
Chemstores). All radiolabeled chemicals had a radio-
chemical purity of 98% or higher. All chemicals were used
as received. The water used in all experimentation was de-
ionized (Barnstead Nanopure) prior to use.
3.2. Methods
High activity 14C-radiolabled MTBE, benzene, TCE,
and 1,2-DCB were received in liquid forms. Low activity
radiolabeled compounds were prepared by mixing the high
activity radio-labeled compound with the unlabeled com-
pound. Stock solutions of labeled MTBE, benzene, TCE,
and 1,2-DCB were prepared by dissolving the low activity
analytes in de-ionized water. Additional solutions of
analytes were then prepared by diluting the stock solutions
with de-ionized water to produce concentrations of
14
C-MTBE ranging from 0 to 30,000 mg/L, 14C-benzene
ranging from 0 to 1900 mg/L, 14C-TCE ranging from 0 to
1100 mg/L, and 14C-1,2-DCB ranging from 0 to 85 mg/L.
TNT stock solutions were prepared by first drying the wet,
powdered TNT in a glove box filled with nitrogen gas, then
dissolving the dried TNT in de-aired, de-ionized water.
A stock solution of high activity 14C-radiolabled TNT was
prepared by dissolving the powdered TNT in de-ionized
water. A stock solution of low activity radio-labeled TNT
was prepared by mixing the high activity TNT with the
unlabeled TNT stock solution. This low activity radio-
labeled TNT stock solution was then used to prepare
additional radio-labeled TNT solutions by diluting with
de-ionized water to make up concentrations ranging from 0
to 8.5 mg/L.
Concentrations of organic chemicals in the aqueous
samples were estimated through their measured 14C-radio-
activity in solution using a liquid scintillation counter
(Packard, Tri-Carb 1700 TR). Standard curves relating
mass of radioactive material to count measures of
40%
Benzene Remaining in Solution.
35%
30%
25%
20%
15%
10%
5%
0%
0 50 100 150 200 250 300 350 400 450 500 550 600 650 700 750
Time (hours)
Fig. 1. Time to equilibrium for sorption of benzene to PVC geomembrane.
radioactivity were developed for each chemical, and these
standard curves were then used to relate the radioactivity
of a sample to organic mass present. Concentrations were
then determined based on the calibration curves, which
were performed each day.
Sorption of MTBE, benzene, TCE, 1,2-DCB, and TNT
to the seven different geomembranes was quantified by a
conventional batch equilibration technique. Sorbent and
varying concentrations of radiolabeled aqueous organic
solutions were placed in 15 mL glass centrifuge tubes with
Teflon-lined caps, taking care to minimize the headspace in
order to limit volatilization. The mass of sorbent was 2 g
for HDPE geomembranes, 1.5 g for polypropylene geo-
membranes, and 1 g for PVC geomembranes. Between six
and nine batch reactors were prepared for a given organic
solute–sorbent combination. After preparing the batch
reactors, they were placed horizontally on an enclosed
shaker, and rotated at a rate of six rotations per minute at
approximately 20 1C until sorption equilibrium was
achieved. In preparing the geomembranes for batch
sorption experiments, the geomembranes were cut into
small pieces (7  7 mm). Because organic/polymer equili-
brium sorption is a dissolution controlled process, and not
a surface controlled process, sectioning the geomembrane
into smaller pieces does not affect the ultimate sorption
capacity, as was demonstrated by preliminary experimen-
tation (data not shown). Preliminary experimentation was
carried out in order to determine the time at which sorption
equilibrium was achieved for all solute–sorbent combina-
tions. Sorption reactions of MTBE, benzene, TCE, and
1,2-DCB with all geomembranes reached sorption equili-
brium at 24 h, while TNT sorption reactions required 48 h
to reach equilibrium. Sample results for a time-to-
equilibrium test for benzene sorbing to PVC are shown
in Fig. 1. It is important to note that on longer time
scales, plasticizers can leach from flexible geomembranes,
which will shift the chemical balance and create a new
equilibrium.
 ARTICLE IN PRESS
E.K. Nefso, S.E. Burns / Geotextiles and Geomembranes 25 (2007) 360–365 363

Two control tests were performed for each set of batch 50

MTBE
reactors. One tube contained only sorbent (geomembrane) 45 PP

Sorbed Concentration (mg/g)

PP Scrim
and de-ionized water, and was processed in the same 40 PVC
manner as the batch reactors in order to quantify 35
HDPE Smooth

background radiation or contamination. The background

30
radiation was always less than 5 counts/min, indicating that
25
sorbents and glassware were not contaminated with radio-
activity. A second tube was a spike that contained only 20
organic solute with de-ionized water, and was used to 15
account for solute loses due to any additional mechanism 10
besides sorption to the appropriate sorbent. Solute loses 5
were then taken into account while determining the total 0
sorbed concentrations. 0 5000 10000 15000 20000 25000 30000
Once equilibrium was achieved in the batch reactors, Equilibrium Aqueous Concentration (mg/L)
they were removed from the shaker and 500 mL of
supernatant was withdrawn from each tube and added to a Fig. 2. Sorption of MTBE to HDPE, polypropylene, and PVC
geomembranes.
scintillation vial that contained 5 mL of scintillation
cocktail. The scintillation vials were then placed into a
liquid scintillation counter (Packard, Tri-Carb 1700 TR)
where their radioactivity was measured. Sorbed concentra-
tions were calculated as the difference between the initial 50
Benzene PP
and equilibrium aqueous concentrations. All sorption tests 45
Sorbed Concentration (mg/g)
PP Scrim
were performed in duplicate. 40
PVC
HDPE Smooth
35
4. Results and discussion 30
25
The partition coefficient for each compound/geomem-
20
brane combination was calculated according to (Sangam
and Rowe, 2005): 15
10
bcf0 V f0  cfF V fF crg
S gf ¼ , 5
M g cfF
0
where cf0 ¼ initial solution concentration [M/L3], 0 200 400 600 800 1000 1200 1400 1600 1800
cfF ¼ final equilibrium solution concentration [M/L3], Equilibrium Aqueous Concentration (mg/L)
Vf0 ¼ initial solution volume [L3], VfF ¼ final solution
Fig. 3. Sorption of benzene to HDPE, polypropylene, and PVC
volume [L3], Mg ¼ initial mass of geomembrane [M], and
geomembranes.
rg ¼ geomembrane density [M/L3].
Examination of the data for each geomembrane/organic
compound demonstrates that in all cases, the sorption was
best described by a linear isotherm (Figs. 2–6), which is
consistent with previous work with HDPE geomembranes
50
(Aminabhavi and Naik, 1998; Sangam and Rowe, 2001; TCE PP
45
Sorbed Concentration (mg/g)

Joo et al., 2004). With a few exceptions, good linear fits to PP Scrim
40 PVC
all the sorption data were obtained, as measured by their HDPE Smooth
regression coefficient, r2. 35
As was anticipated, the thickness and texture of the four 30
HDPE geomembranes tested did not produce a significant 25
difference in their uptake capacity (Fig. 7), with all four 20
geomembranes (1.016 mm textured, 1.016 mm smooth, 15
1.524 mm textured, and 1.524 mm smooth) showing similar
10
uptake for each of the five compounds, which is consistent
5
with the trends noted in Park and Nibras (1993).
Consistent with the trend of aqueous solubility, con- 0
0 200 400 600 800 1000 1200
taminant uptake increased in the following order for the
Equilibrium Aqueous Concentration (mg/L)
HDPE and PP geomembranes: MTBE, benzene and TCE,
and 1,2-DCB, with MTBE being the most water soluble Fig. 4. Sorption of TCE to HDPE, polypropylene, and PVC geomem-
and the least likely to sorb, and 1,2-DCB being the least branes.
 ARTICLE IN PRESS
364 E.K. Nefso, S.E. Burns / Geotextiles and Geomembranes 25 (2007) 360–365

water soluble and the most likely to sorb (Fig. 7). However, PP geomembranes, with Sgf values similar to those
TNT, which has a low water solubility on the order of that measured for MTBE. In contrast, TNT sorbed significantly
of 1,2-DCB, showed little interaction with the HDPE and to the PVC geomembrane. The PVC interaction with TNT,
can be attributed to the chemical composition of the
geomembrane. While the exact chemical formulation of the
50 PVC geomembrane used in this study was not known, it is
PP
45 1,2-DCB not uncommon for PVC to contain amine functional
Sorbed Concentration (mg/g)

PP Scrim

40
PVC groups in which nitrogen is a primary component. These
HDPE Smooth
35 nitrogen containing functional groups are reactive with
30
nitroaromatic compounds such as TNT, and have been
used as the basis for sensor detection technology used to
25
identify the TNT in landmines (Zhang et al., 1990;
20
Gheorghiu et al., 1999). It is believed that the strong
15 uptake of TNT on the PVC geomembrane can be
10 attributed to the interaction of nitrogen containing groups
5 in the PVC with the nitroaromatic TNT.
0 Partition coefficients measured for the sorption of
0 10 20 30 40 50 60 70 80 90 MTBE to all three geomembranes were 3.7 or lower
Equilibrium Aqueous Concentration (mg/L) (Table 2). For the sorption of benzene to HDPE, the
measured partition coefficients ranged from 19 to 27, which
Fig. 5. Sorption of 1,2-DCB to HDPE, polypropylene, and PVC
geomembranes. is consistent with the findings of previous researchers
(Sangam and Rowe, 2001; Joo et al., 2004). Benzene
exhibited a higher affinity for polypropylene than it did for
0.1
TNT PP HDPE, with partition coefficients of 31–36; however, the
Sorbed Concentration (mg/g)

PP Scrim PVC geomembrane was most sorptive of benzene with a

PVC
HDPE Smooth partition coefficient of 106. The values of the partition
coefficients measured for TCE were similar, although
slightly lower, than those measured for benzene, which is
a slight deviation from the trend predicted by the aqueous
solubilities. This is consistent with the molecular properties
of benzene and TCE, as TCE has a larger molar volume
than benzene, which would limit its penetration into the
polymer matrices when compared to benzene. In general,
1,2-DCB showed the strongest uptake on the geomem-
0.0 branes, with partition coefficient values ranging from
0 1 2 3 4 5 6 7 8
42 for polypropylene to 130–160 for HDPE. While
Equilibrium Aqueous Concentration (mg/L)
these values are quite high, it is important to note
Fig. 6. Sorption of TNT to HDPE, polypropylene, and PVC geomem- that they were gathered at very low concentrations due
branes. (Note the change in scale.) to the low solubility of 1,2-DCB (aqueous solubility at
25  C ¼ 147 mg=L).

180 MTBE Benzene TCE 1,2-DCB TNT

Partition Coefficient (-)

160
140
120
100
80
60
40
20
0
m

ne

op

C
PV
m

le

pr
py
6

ly
01

52

01

52

Po
ro
1.

1.

1.

1.

yp

rim
x

Sm

Sm

l
Te

Te

Po

Sc
PE

PE
PE

PE

D
D

H
H

Fig. 7. Comparison of distribution coefficients for sorption of MTBE, benzene, TCE, 1,2-DCB, and TNT to HDPE, PP, and PVC geomembranes.
 ARTICLE IN PRESS
E.K. Nefso, S.E. Burns / Geotextiles and Geomembranes 25 (2007) 360–365 365

Table 2 textures. Within the polypropylene geomembranes, the

Distribution coefficients for geomembrane sorption of MTBE, Benzene, scrim reinforced membrane exhibited a slightly increased
TCE, and 1,2-DCB
sorption capacity when compared to the non-reinforced
Sorbent Solute Sgf r2 version, especially in the presence of 1,2-DCB. The PVC
geomembrane demonstrated high affinity for benzene and
HDPE textured 1.016 mm MTBE 1.1 0.79 TNT when compared to the other materials.
HDPE textured 1.524 mm MTBE 0.56 0.49
HDPE smooth 1.016 mm MTBE 0.85 0.68
HDPE smooth 1.524 mm MTBE 0.56 0.87
Polypropylene MTBE 1.2 0.95 Acknowledgements
PP scrim reinforced MTBE 2.1 0.99
PVC MTBE 3.7 0.97 The authors wish to thank Dr. James A. Smith for his
HDPE textured 1.016 mm Benzene 27 0.97 assistance in the experimental investigation.
HDPE textured 1.524 mm Benzene 23 0.89
HDPE smooth 1.016 mm Benzene 21 0.98
HDPE smooth 1.524 mm Benzene 19 0.95
Polypropylene Benzene 31 0.97 References
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HDPE textured 1.016 mm 1,2-DCB 160 0.88 composite liner on the leakage through a hole in the geomembrane.
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