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Hydrogeology Journal (2019) 27:581–593

https://doi.org/10.1007/s10040-018-1904-1

PAPER

Assessing the influence of infiltration on the migration of light


non-aqueous phase liquid in double-porosity soil media using a light
transmission visualization method
Motasem Y. D. Alazaiza 1 & Su Kong Ngien 2,3 & Nadim Copty 4 & Mustafa M. Bob 5 & Samira A. Kamaruddin 6

Received: 18 April 2018 / Accepted: 18 November 2018 / Published online: 28 November 2018
# Springer-Verlag GmbH Germany, part of Springer Nature 2018

Abstract
The influence of infiltration on the migration of a light non-aqueous phase liquid (LNAPL) in double-porosity soil using the light
transmission visualization (LTV) technique is investigated. Two LNAPL volumes (low and high volumes) were exposed to two
rainfall intensities (light and heavy infiltration). For comparison purposes, the experiments were also repeated by compacting the
flow chamber with silica sand only to represent the single-porosity medium and to investigate the influence of double-porosity on
LNAPL migration. High-resolution LTV images of the flow chamber during LNAPL injection and subsequent water infiltration
events were collected. Results show that the LNAPL migration depth during injection and its migration velocity were both
correlated to the LNAPL volume. Subsequent water infiltration events caused the LNAPL that was entrapped in the porous media
to be pushed further downward in all the experiments. The LNAPL migration velocity was 1.1 and 1.6 cm/h for the low and high
LNAPL spillage volumes for double-porosity experiments, respectively, a reduction rate of 64.7 and 70% compared to the
LNAPL migration velocity during LNAPL injection, respectively. However, for single-porosity experiments, the LNAPL mi-
gration velocity was 0.7 and 1.2 cm/h for the low and high LNAPL volumes, respectively. Furthermore, it was observed that the
capillary fringe level was depressed in the saturated zone due to the influence of both infiltration and LNAPL volume. This study
demonstrates that the LTV technique is an accurate and cost-effective laboratory tool for the visualization of the time-dependent
influence of infiltration on LNAPL migration in porous media.

Keywords Laboratory experiments/measurements . Light transmission visualization . Double-porosity . Non-aqueous phase


liquid . Porous media

Introduction

The contamination of soil and groundwater by organic com-


* Motasem Y. D. Alazaiza
pounds in the form of non-aqueous phase liquids (NAPLs) is a
my.azaiza@gmail.com
widespread and challenging problem (Luciano et al. 2010).
1
Many of these contaminants are immiscible with water as a
School of Civil Engineering, Universiti Sains Malaysia, result of their low aqueous solubility (Yang et al. 2013). As a
14300 Nibong Tebal, Pulau Pinang, Malaysia
2
result, the contamination of the subsurface by NAPLs can
Faculty of Civil Engineering and Earth Resources, Universiti persist for many years leading to the contamination of large
Malaysia Pahang, Lebuhraya Tun Razak, 26300 Gambang, Pahang,
Malaysia portions of the groundwater (Alazaiza et al. 2018). The migra-
3 tion of NAPL in the subsurface especially in the unsaturated
Centre for Earth Resources Research and Management, Universiti
Malaysia Pahang, Gambang, Malaysia zone is very difficult to predict due to the complex nature of
4 the multiphase system. NAPLs can be categorized into light
Institute of Environmental Sciences, Bogazici University, Bebek,
Istanbul, Turkey non-aqueous phase liquids (LNAPLs) and dense non-aqueous
5 phase liquids (DNAPLs) depending on their density relative to
Department of Civil Engineering, Taibah University, Kingdom of
Saudi ArabiaMadinah City that of water. Chlorinated solvents such as trichloroethylene
6 and tetrachloroethylene are the most common examples of
UTM Razak School of Engineering and Advanced Technology,
Universiti Teknologi Malaysia, Kuala Lumpur, Malaysia DNAPL, whereas petroleum compounds such as benzene,
582 Hydrogeol J (2019) 27:581–593

toluene and xylene (BTEX) are examples of LNAPL (Sweijen due to the closer matching between the refraction index of the
et al. 2014; Karadag et al. 2016). porous media and water relative to the porous media and air
When a NAPL is released into the subsurface, it first mi- (Glass et al. 1989). In LTV systems, the change in fluid con-
grates within the vadose zone under the influence of the grav- tent and fluid saturation can readily be measured instanta-
itational hydrodynamic and capillary forces which depend on neously due to the utilization of digital cameras, which pro-
the distribution of the three-phases: air, water, and NAPL vide a very high density array of spatial measurements over a
within the porous medium. This is true for the case of both very large dynamic range (Niemet and Selker 2001).
LNAPL and DNAPL in the vadose zone. However, in the case When water infiltrates into the subsurface, the water phase
of DNAPL, due to its density which is higher than that of portion will increase, which, in turn affects the migration of
water, it will enter the saturated zone and continue its down- entrapped NAPL. Kamaruddin (2012) carried out an experi-
ward migration in the saturated zone until some hydraulic or mental study to investigate the influence of rainfall on the
capillary barrier is encountered. Understanding the migration migration of LNAPL in silica sand. The author reported that
of NAPLs in subsurface systems is essential for evaluating the LNAPL was easily moved downward by the rainfall re-
contamination source zones as well as to design remediation charge. In addition, the results also showed that the rainfall
schemes (Zheng et al. 2015). recharge could significantly reduce the residual LNAPL satu-
NAPL migration is influenced by three major factors ration at the upper part of the capillary interface.
(Huling and Weaver 1991): (1) fluid properties such as viscos- Subsequently, in another study, Flores et al. (2013) investigat-
ity, density, wettability, residual saturation in porous media, ed LNAPL behavior due to precipitation using a simplified
interfacial tension, solubility and volatility; (2) characteristics image analysis method (SIAM). The study focused on the
of the porous media, which mainly consist of hydrological visualization of LNAPL migration under the influence of rain-
parameters such as soil structure, pore size, capillary pressure, fall intensity in one-dimensional (1D) columns filled with
and hydraulic conductivity; and (3) subsurface conditions sand. The authors noted that the precipitation intensity forced
such as groundwater flow velocity and soil water content. In the LNAPL to migrate downward to different depths depend-
its natural state, many types of soil have two distinct scales of ing on the precipitation intensities despite the fact that the
porosity, which give rise to the term double-porosity soil LNAPL has a density lower than that of water.
structure (Carminati et al. 2008). Double-porosity is a natural The main goal of this study is to investigate the impact of
phenomenon that occurs when two separate pore systems infiltration on the transient LNAPL migration in double-
emerge simultaneously in the structure of a soil (El-Zein porosity soil media using the LTV technique which has not
et al. 2006). Rock aquifers (Pao and Lewis 2002), compacted been studied before. The paper examines the impact of NAPL
soils (Romero et al. 1999), and agricultural top soil (El-Zein saturation by considering two LNAPL injection conditions:
et al. 2006) are examples of geomaterials that potentially har- low LNAPL volume and high LNAPL volume.
bor double-porosity characteristics. Furthermore, the LNAPL was subjected to two different infil-
Numerous researchers have conducted experimental stud- tration intensities: light rainfall intensity and heavy rainfall
ies to investigate the behavior of immiscible fluids in soils intensity. For comparison purposes, the experiments were also
(Bob et al. 2008; Darnault et al. 1998; Kechavarzi et al. repeated by compacting the flow chamber with silica sand
2005; Ngien et al. 2012; Pan et al. 2016; Sa’ari et al. 2015; only to represent single-porosity medium and to investigate
Zheng et al. 2015; Van Geel and Sykes 1997; Sharma and the influence of double-porosity on LNAPL migration. In to-
Mohamed 2003). Several researchers have used a few tech- tal, eight experiments with different LNAPL volumes and
niques to measure fluid saturation including gamma ray (Tuck infiltration intensity combinations were conducted. The next
et al. 1998), X-ray attenuation (Tidwell and Glass 1994), and section presents the preparation of the materials, physical
electrical conductivity probes (Kamon et al. 2003). However, model, experimental setup, and experimental procedures.
the former techniques do not allow the monitoring of fluid The distribution of LNAPL through the soil was acquired
behavior under dynamic conditions. In addition, these tech- using a digital camera as will be discussed later. Finally, the
niques do not allow for the simultaneous observation of the results of this LTV application to LNAPL migration behavior
entire domain of the samples (Flores et al. 2011). In light of are presented and discussed.
these limitations, the light transmission visualization (LTV)
technique has increasingly attracted the attention of several
researchers (Bob et al. 2008; Niemet and Selker 2001; Materials and methods
Zheng et al. 2015). A study by Alazaiza et al. (2015) presented
the usage of three types of photographic methods in NAPL Material characteristics
experiments and showed that LTV is a viable method for
NAPL saturation measurements. It was found that there is a The porous materials used in this study are local silica sand
linear relationship between fluid saturation and light intensity and S300 kaolin, which were used to create the double-
Hydrogeol J (2019) 27:581–593 583

porosity soil structure. Prior to starting the experiments, a around 5 μm. The retained sand on sieve 212 μm was used as
detailed characterization including physical, chemical, and the filler. Scanning electron microscopy (SEM) was carried
mineralogical tests, was carried out for both materials. The out to investigate the micro-structure of the kaolin spheres
physical, chemical, and mineralogical properties can be found with different magnifications as shown in Fig. 1. The SEM
in (Alazaiza et al. 2017). Toluene was used to represent the showed that the kaolin spheres were almost homogeneous
LNAPL. Toluene density is 0.867 kg/m3 and its solubility in without skin effect due to reduced porosity. The sand was
water is 520 mg/L at 25 °C. Additional Toluene properties can washed with distilled water to remove any fine residuals pres-
be found in (Ruffino and Zanetti 2009). ent and then oven dried for 48 h at 45 °C. In order to build the
double-porosity structure, the clay spheres were put layer by
Double-porosity physical model layer in such a manner that they were touching each other.
Between each clay sphere layer, a layer of sand was carefully
The double-porosity structure was created following the meth- poured and then compaction was done by tapping a plastic
od of Lewandowska et al. (2005) using sintered clay spheres hammer on the outer frame of the acrylic model. The volu-
and fine sand. The sintered clay spheres were made of com- metric fraction of 50% macro-pores (silica sand) and 50%
mercially available S300 kaolin (Lotte Chemical Titan, micro-pores (clay spheres) were used. This volumetric frac-
Malaysia), while the sand was commercial local silica sand tion resulted in different weight of sand and clay fractions,
(Lotte Chemical Titan, Malaysia). To make the sintered clay which in turn differ the sand layer thickness. The thickness
spheres, kaolin powder was mixed with a sufficient amount of of each sand layer was 1.15 cm. The total porosity of the
water, so that the spheres could be formed by hand. The clay double-porosity structure was 0.42. Figure 2 shows the distri-
spheres were then put inside a furnace and the temperature bution of clay and sand to create the double-porosity structure.
was increased gradually until it reached 1,000 °C. This pro-
cess was undertaken to harden the kaolin spheres so that fur- Experimental setup
ther disintegration can be avoided during saturation of the
double-porosity soil sample in the study. The clay sphere di- All experiments were conducted inside a two-dimensional
ameter was 6 mm and the average pore size in clay sphere was (2D) flow chamber made of 10-mm acrylic material. The

Fig. 1 SEM images of the


sintered clay material a × 500 b ×
1,000 c × 2,500 d × 5,000
584 Hydrogeol J (2019) 27:581–593

Fig. 2 a Schematic diagram of


the double-porosity porous
medium. b Photograph of the
compacted double-porosity soil
inside the flow chamber after
water saturation

dimensions of the flow chamber were 45 cm height × 30 cm intensity homogenization. Images were acquired using a
width × 1 cm depth. The flow chamber was placed inside a Nikon D 7100 digital camera, which was kept at a fixed dis-
frame fixed to a stainless-steel light box, in front of the light tance of 1.5 m from the light box for all experiments. The
source. At the bottom of the flow chamber, two steel ports camera was controlled using the Nikon Camera Control Pro
were installed and connected to a water tank using plastic Software to avoid displacement and vibrations. All experi-
tubing. A valve was placed between the flow chamber and ments were conducted inside a dark room and the temperature
water tank to control the flow of water into the flow chamber. of the room was maintained at 23 ± 1 °C.
The LTV system used in the present study was based on
that described in Alazaiza et al. (2017). The system comprises Rainfall simulation
of a stainless-steel box with a light source consisting of five
18-W fluorescent tubes at the back of the box as shown in Rainwater is required to observe the influence of infiltration
Fig. 3. In front of the light source, a holographic light-shaping on LNAPL migration. For a typical infiltration simulation, the
diffuser (LSD; Luminit, USA) was placed to achieve light characteristics that should be considered are drop size,

Fig. 3 Schematic diagram of the


light box
Hydrogeol J (2019) 27:581–593 585

intensity, and kinetic energy (Dunkerley 2008). In this study, a Experimental procedures
dripping method was used to simulate a rainfall event due to
its ease of installation and economic advantage. Simulation of The flow chamber was first dry packed with the porous media.
infiltration via the dripping method purposely allows the water After packing, the model was fully saturated with distilled
infiltration to occur as a recharge; therefore, the influence of water from the bottom ports. Thereafter, each experiment
kinetic energy on the model surface can be neglected. Water was divided into three stages as laid out in the next
was released from an adjacent tank using a peristaltic pump subsections.
into a horizontal pipe above the top of the flow chamber. The
pump controls the rate of infiltration in order to produce a Water drainage
constant flow rate. A control head device was used to control
the water head in the water tank. All fittings and pipe connec- After fully saturating the flow chamber with water, the drain-
tions together with a manual valve were glued together to age valve connecting to the bottom ports was opened to allow
achieve a high-water pressure. For all the experiments, small for water drainage. The top of the flow chamber was opened to
holes were drilled along the horizontal pipe at 4-cm intervals prevent a vacuum state from occurring. This stage was pre-
to produce artificial rain. The system was pre-tested by releas- tested to determine the standard duration before the LNAPL
ing water drips into a pan to estimate the water flow rate. As experiments were conducted.
mentioned earlier, two rainfall intensities were simulated in
this study—the light rainfall intensity was selected as LNAPL injection
10 mm/h, while the heavy rainfall intensity was 60 mm/h.
The higher value corresponds to rainfall intensities encoun- In this stage, known volumes of toluene were injected from
tered during heavy storms—for example, in tropical countries the top of the flow chamber through the porous media using a
such as Malaysia, the light rainfall intensity range is from 1 to syringe. At the middle top of the acrylic model, a small open-
10 mm/h. while the heavy rainfall intensity range is from 30 to ing was created in order to insert the needle of the syringe to
60 mm/h (Malaysia Drainage and Irrigation Department inject the toluene into the porous media. The low volume of
Standard 2017). The layout of the experimental setup is shown toluene was 50 ml (1.67 ml/cm2), whereas the high volume
in Fig. 4. was 100 ml (3.33 ml/cm2). After the LNAPL release, the
camera automatically starts to capture images for the charac-
terization of the transient LNAPL distribution.

Rainfall event

Using the upper pump connected to the water tank, the flow
rate was controlled to simulate the light and heavy rainfall
events. The low and heavy rainfall events were 10 and
60 mm/h, respectively each applied for a period of 2 h. After
application of the rainfall event, the model was left to stabilize
for 12 h and the observation of the LNAPL behavior was
continued until it reached a stable state. All images were proc-
essed using Image Pro Premier software (Media Cybernetics,
USA) to extract the light intensity values. The light intensity
was then visualized using Surfer 8.1 software.

Pre-tests for identifying water and LNAPL migration times

Before starting the experiments, a trial experiment was con-


ducted to determine the time needed for water drainage and
LNAPL infiltration in the double-porosity soil. Specifically,
prior to the LNAPL migration stage, the system was water
drained until the sample reached stable water content in the
vadose zone and capillary zone. The stable water content level
was determined based on the changes in the light intensity for
Fig. 4 Schematic diagram showing the flow chamber and rainfall the captured images during the pre-test. More than 80 images
generation system were captured and analyzed in order to measure the variations
586 Hydrogeol J (2019) 27:581–593

in light intensity in the vadose zone and capillary zone. The time needed for the LNAPL distribution to stabilize in the
duration taken for this stage was later used as a standard du- pre-test was later used for all experiments as a standard dura-
ration for the drainage stage for all subsequent experiments. tion for the LNAPL injection stage. Figure 5 shows the light
The sample preparation and the experimental procedure are intensity variations during the LNAPL infiltration over an 18-
also similar to all the experiments as described in the preced- h period. It was observed that the light intensity of the LNAPL
ing. The sole difference in the trial experiment is the time varied in the vadose zone as well as in the capillary zone with
duration was much longer in time compared to the real exper- an increase in time due to the LNAPL movement from the
iments. The trial test was carried out over 1 day with the first point of release at the upper end of the flow chamber to the
6 h dedicated to water drainage, while the rest of the time was capillary zone. Based on these results, the required time for
allotted for LNAPL migration. The test was conducted using LNAPL to reach a stable state was estimated to be approxi-
the high LNAPL volume, which is expected to require a lon- mately 6 h.
ger time to stabilize. The interpretation of the pre-test was
based on the changes in the average light intensity for the
captured images during the water drainage phase as well as
Results and discussion
LNAPL infiltration phase. The water was observed to drain
very fast from the flow chamber because of the high perme-
LNAPL migration before infiltration
ability of the double-porosity due to the presence of macro-
pores in the double-porosity soil (Alazaiza et al. 2017). The
In all the experiments, when the bottom valve was opened, the
drainage process reached a stable level in less than 3 h (i.e. 2 h
water drained from the fully saturated soil samples due to
47 min) after which no changes in light intensity were ob-
gravitational force. The occurrence of two types of porosity
served. Figure 5 shows the change in light intensity as a func-
(i.e. macro-pores and micro-pores) caused the water drainage
tion of time and the time needed for the water drainage to
process to be relatively fast as compared to single-porosity
reach stable conditions. Based on these results, the duration
experiments and the capillary zone was observed after less
of the water drainage stage for all experiments was set at 3 h.
than 3 h. The occurrence of the capillary zone was observed
Based on the water drainage results, LNAPL injection
using the Image Pro Primier software depending on the dif-
commenced after 6 h from the start of the water drainage (or
ference in the light intensity in the vadose zone and the satu-
about 3 h after the drainage seized and the soil moisture con-
rated zone. The average light intensity of the saturated zone
tent reached a steady state. The movement of the injected
was very high as compared to the average light intensity in the
LNAPL was monitored until it reached a stable depth. The
vadose zone. The light intensity of the capillary zone on the

Fig. 5 Pre-test for water drainage and LNAPL infiltration to determine the duration needed to reach stable conditions
Hydrogeol J (2019) 27:581–593 587

other hand was between that of the vadose zone and the satu- changes due to increasing the LNAPL volume resulted in
rated zone. This observation is due to the fact that the light brighter pixels containing higher intensity value.
transmission of the porous media increases with increasing Figure 7 shows the LNAPL migration in the flow chamber
water content (Hoa 1981). When LNAPL was released into as a function of time for two LNAPL volumes considered for
the flow chamber, it migrated deeper into the double-porosity all experiments. The LTV images clearly show that the
soil due to the gravitational force until it reached the capillary LNAPL migration pattern depended on volume of released
zone. From the variations of the light intensity, it was observed LNAPL. The LNAPL was observed to migrate rapidly in the
that the thickness of the saturated zone, capillary zone, and first hour after LNAPL injection with average downward ve-
vadose zone were 21, 11 and 13 cm, respectively. locities of 1.7 and 2.3 cm/h for the cases of 50 and 100 ml of
Based on the captured images, an obvious change in the released LNAPL for double-porosity experiments, respective-
shape and intensity of the red color of the toluene plume was ly. This occurrence is most likely due to the higher pressure
observed during the experiment as shown in Fig. 6. It can be exerted in the case of the larger LNAPL volume. Thereafter,
seen that the LNAPL shape and saturation were changed by the LNAPL velocity started to slow down. The migration
time during the downward migration of the high LNAPL vol- depth of the LNAPL was also observed to be directly depen-
ume in double-porosity soil. All images were calibrated by dent on the LNAPL volume released. From analysis of the
converting the images from a red-green-blue (RGB) system image light intensity variations, the LNAPL migrated 21 and
to a grey level system ranging from 0 to 4096 bits for black to 27 cm downwards for the cases of 50 and 100 ml of spilt
white pixels, respectively, using Image Pro. Premier Software. LNAPL, respectively. The same trend was observed in the
This step is to ensure that the image will produce the full 4,096 duplicate experiments (data are not shown). The higher vol-
grey levels present in the image. The normalized image has a ume of LNAPL provided a higher pressure to overcome the
brighter plume and a darker background which contrasts with capillary forces and force the LNAPL into the finer pores. The
the original grey image that has a darker plume of LNAPL and LNAPL continued its downward migration until equilibrium
a brighter background. The background of the normalized between the capillary (interfacial tension) and gravitational
image is darker because the background of the plume image forces is reached.; moreover, it was observed that the smaller
was subtracted from the background of the initial image. Any LNAPL volume took 2 h to reach a stable depth, whereas the

Fig. 6 Dynamic change of


LNAPL shape and saturation
before rainfall for the case of high
LNAPL volume after a 30 min, b
60 min, c 120 min, d 240 min
588 Hydrogeol J (2019) 27:581–593

Fig. 7 LNAPL migration depth


for low and high cases before
rainfall recharge for single and
double-porosity experiments

high LNAPL volume reached a stable depth after approxi- case, until the LNAPL reached a stable depth. Figure 7 shows
mately 6 h. For single-porosity experiments, the LNAPL the LNAPL depth as a function of time before and after the
was observed to migrate slower than that in double-porosity rainfall event. Once rainfall is applied, water starts to infiltrate
experiments with average downward velocities of 1 cm/h and downwards due to gravity. As a result of hydrodynamic forces
1.8 for the cases of 50 ml and 100 ml of released LNAPL, exerted on the entrapped LNAPL, the LNAPL in turn starts to
respectively, which is most likely due to the occurrence of migrate downwards in all the experiments regardless of the
macro-pores in double-porosity which have a significant ef- LNAPL volume or rainfall intensity, as shown in Fig. 7. The
fect on fluid migration. This observation is in agreement with observations showed that the LNAPL migration velocity was
the findings of Alazaiza et al. (2017). In their study, they relatively slow as compared to LNAPL velocity before water
investigated the PCE behavior in double-porosity medium infiltration in all the experiments. The LNAPL velocity was
and compared it with single-porosity medium. They noted that 1.1 and 1.6 cm/h for the low and high LNAPL spillage vol-
the macro-pores in double-porosity soil which constitute the umes, respectively with a reduction rate of 64.7 and 70% in
main difference in the composition of single and double-po- the LNAPL migration velocity, respectively for the double-
rosity, have a substantial effect on the migration of PCE. porosity experiments. The LNAPL migrated downward until
Alazaiza et al. (2017) compared their results with Ngien it became entrapped in the capillary zone. The LNAPL
et al. (2012) which reported the same results. Ngien et al. reached a depth of 25 and 36 cm for low and high LNAPL
(2012) conducted an experimental study for LNAPL migra- spillage volumes, respectively. For the case of single-porosity
tion in a 1-D column filled with double-porosity aggregated experiments, the LNAPL migration velocity was 0.7 and
kaolin and compared their results with single-porosity. They 1.2 cm/h for the low and high LNAPL spillage volumes, re-
reported that the LNAPL migrated much faster in the double- spectively with a reduction rate of 70 and 66% in the LNAPL
porosity media as compared to those with single-porosity and migration velocity, respectively. This observation emphasizes
this is due to the presence of macro-pores. The LNAPL the influence of double-porosity medium on LNAPL migra-
reached a depth of 16 and 20 cm for the low and high tion under the effect of rainfall which contributes in higher
LNAPL spillage volumes, respectively. LNAPL velocity as compared to single-porosity medium.
The LNAPL reached a depth of 18 and 23 cm for the low
LNAPL migration after infiltration and high LNAPL spillage volumes, respectively.
Figure 8 shows images of the LNAPL migration in all of
At the end of the LNAPL injection stage, the LNAPL reaches the experiments as a result of the imposed infiltration. These
a state of equilibrium whereby the capillary and gravitational images clearly show the resolution of the LTV technique and
forces balance outs each other. This equilibrium status chang- its ability to accurately simulate the downward migration of
es once rainfall infiltrates the contaminated double-porosity the LNAPL. It was also observed that the capillary fringe
medium. The contaminated flow chamber was exposed to a level was lowered in the saturated zone due to the influence
rainfall event for 2 h and subsequently imaged until the of rainfall recharge on the LNAPL plume. This observation
LNAPL reached a stable depth, for a period of 2 h for the high is consistent with a study conducted by Henry and Smith
LNAPL volume case and 6 h for the low LNAPL volume (2002) who reported that upon the surfactant solution
Hydrogeol J (2019) 27:581–593 589

Fig. 8 Influence of rainfall on


LNAPL migration for low and
high-volume cases for single and
double-porosity experiments

reaching the capillary fringe, a depression of the capillary solution has a relatively similar effect compared to the
fringe was observed. Therefore, the observed new reduced mobilized LNAPL since both materials have density less
capillary fringe height means that the contaminant can mi- than that of water. The density of solution surfactant in
grate deeper through the saturated capillary zone and Henry and Smith (2002) study is 0.99. Figures 9, 10 and
approach the water table. It is believed that the surfactant 11 show the general behavior of LNAPL before and after

Fig. 9 LNAPL saturation


showing the influence of rainfall
on LNAPL migration for the case
of high LNAPL volume in
double-porosity experiments a
before rainfall, b after 30 min of
rainfall, c after 60 min of rainfall,
d after 120 min of rainfall (The
dashed line shows the capillary
fringe level before and after
rainfall)
590 Hydrogeol J (2019) 27:581–593

Fig. 10 LNAPL saturation under


a low LNAPL volume before
rainfall, b low LNAPL volume
after rainfall, c high LNAPL
volume before rainfall, d high
LNAPL volume after rainfall for
double-porosity experiment. (The
dashed line shows the capillary
fringe level before and after
rainfall)

infiltration for the double-porosity and single-porosity exper- influences the effect of rainfall recharge on LNAPL move-
iments, respectively. ment. The connectivity of the non-wetting (LNAPL) liquid
Overall, it can be concluded that the two rainfall intensities is most likely to develop when the released liquid volume is
(light and heavy) caused the LNAPL that was entrapped in the sufficient. This behavior means that the greater volume of
porous media to be pushed further downward in all the exper- LNAPL, the more occupation of voids within the soil pores.
iments. In addition, the LNAPL downward migration velocity In turn, a bridge inside the soil pores within the water surface
was decreased in all the experiments with different reduction is created because the LNAPL and water are immiscible
rates. liquids.
For the second factor influencing the LNAPL migration,
Influence of LNAPL spillage volume the initial distribution of LNAPL saturation influences the
way the rainfall recharge affects contaminant movement.
Comparison of the results of two LNAPL spillage volumes When the spillage volume of LNAPL is high, it will more
(low and high) shows that in the case of low LNAPL spillage rapidly migrate deeper due to the high weight of the LNAPL
volume, more LNAPL was spread through the LNAPL zone spillage, which forces the LNAPL further downward with the
when the LNAPL was exposed to a rainfall event. However, in LNAPL occupying the larger soil pores due to capillarity dur-
the case of high LNAPL spillage volume, the LNAPL contin- ing its downward migration. However, for the case of low
ued to migrate vertically downward, as shown in Fig. 9. Two LNAPL spillage volume, the LNAPL migration was found
factors influence the LNAPL migration in high and low to be relatively shallow; thus, the LNAPL saturation was
LNAPL volumes, as reported by Wipfler and Van Der Zee spread within a smaller LNAPL zone. These two conditions
(2001). The first factor is related to the LNAPL occupancy caused different LNAPL saturation distributions and influ-
state in the soil pores while the second factor is related to the enced the available LNAPL-free pores in the vadose zone near
distribution of LNAPL saturation within the LNAPL zone the top surface. In the case of the high LNAPL spillage vol-
during its infiltration. In regard to the first factor, the presence ume, more available pores near the top surface existed where
of the NAPL in the form of continuous blobs within soil pores the LNAPL saturation in this area was low as opposed to the
Hydrogeol J (2019) 27:581–593 591

Fig. 11 LNAPL saturation in


single-porosity experiments for a
low LNAPL volume before
rainfall, b low LNAPL volume
after rainfall, c high LNAPL
volume before rainfall, d high
LNAPL volume after rainfall.
(The dashed line shows the
capillary fringe level before and
after rainfall)

case of the low LNAPL volume. Thus, when the porous media saturated porous media followed by the application of rainfall
was subjected to rainfall event, the water more rapidly infil- events. The results show that upon the injection of LNAPL
trated through the porous media when the volume of the avail- into the flow chamber, the LNAPL migrated downward in the
able pores are high. This infiltration of rainfall recharge result- double-porosity medium under the influence of gravity until
ed in the LNAPL being forced further downward. the LNAPL reached the capillary zone. Interpretation of the
Overall, this study demonstrates the successful application LTV images showed that the LNAPL migration rate was faster
of the LTV technique for monitoring the influence of infiltra- for the case of high volume LNAPL compared to the case of
tion on LNAPL migration in double-porosity soil. LTV pro- low volume LNAPL due to gravity which forced the LNAPL
vides a rapid non-invasive tool with minimal instrumentation into the porous medium at a faster rate. The average migration
to visualize NAPL migration. The LTV technique requires velocity was 1.7 and 2.3 cm/h for the cases of 50 and 100 ml
significantly lower laboratory efforts compared to other visu- of spilt LNAPL, respectively, for double-porosity experi-
alizing techniques such as X-ray and gamma-ray. ments. Thereafter, the LNAPL velocity started to slow down.
The migration depth of the LNAPL depends on the volume
released where the LNAPL migrated deeper in the case of the
Conclusion high LNAPL volume. It was also observed that the LNAPL
migrated downwards 21 and 27 cm for the cases of 50 and
In this paper, laboratory experiments were conducted to inves- 100 ml LNAPL, respectively. For single-porosity experi-
tigate the influence of infiltration on LNAPL migration in ments, the average migration velocity for LNAPL was 1 and
double-porosity soil media using the LTV technique under 1.8 cm/h for the low and high LNAPL spillage volumes,
different conditions. Four experiments were conducted for respectively.
two rainfall intensities (10 and 60 mm/h.) for two volumes Interpretation of the LTV images also showed that the in-
of LNAPL spillage (50 and 100 ml). The same experiments filtration caused the downward movement of the LNAPL
were repeated by filling the flow chamber with silica sand as a entrapped in porous media in all the experiments regardless
single-porosity for comparison purposes. Each experiment of the LNAPL volume and rainfall intensity that was tested.
consisted first of the LNAPL injection in the partially However, the LNAPL downward velocity was 1.1 and 1.6 cm/
592 Hydrogeol J (2019) 27:581–593

h for the low and high LNAPL spillage volumes, respectively, measurements in 2-D models. Adv Water Resour 31:727–742.
https://doi.org/10.1016/j.advwatres.2008.01.016
a reduction rate of 64.7 and 70% relative to the LNAPL mi-
Carminati A, Kaestner A, Lehmann P, Flühler H (2008) Unsaturated
gration velocity during LNAPL injection for double-porosity water flow across soil aggregate contacts. Adv Water Resour 31:
experiments. Furthermore, the LNAPL reached a depth of 25 1221–1232. https://doi.org/10.1016/j.advwatres.2008.01.008
and 36 cm for low and high LNAPL spillage volumes, respec- Darnault CJ, Throop JA, DiCarlo DA, Rimmer A, Steenhuis TS, Parlange
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for increasingly systematic study and reporting. Hydrol Process 22:
downward until it was entrapped in the capillary zone. In
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