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United States Office of Office of Solid Waste EPA/540/4-91-002

Environmental Protection Research and and Emergency March 1991


Agency Development Response

Ground Water Issue


DENSE NONAQUEOUS PHASE LIQUIDS
Scott G. Huling* and James W. Weaver**

Background nonaqueous phase liquids have a specific gravity greater


than water, and the light nonaqueous phase liquids (LNAPL)
The Regional Superfund Ground Water Forum is a group of have a specific gravity less than water.
EPA professionals representing EPAs Regional Superfund
Offices, committed to the identification and the resolution of Several of the most common compounds associated with
ground water issues impacting the remediation of Superfund DNAPLs found at Superfund sites are included in Table 1.
sites. The Forum is supported by and advises the Superfund These compounds are a partial list of a larger list identified
Technical Support Project. Dense nonaqueous phase liquids by a national screening of the most prevalent compounds
is an issue identified by the Forum as a concern of found at Superfund sites (65). The general chemical
Superfund decision-makers. For further information contact categories are halogenated/non-halogenated semi-volatiles
Scott G. Huling (FTS:743-2313), Jim Weaver (FTS:743- and halogenated volatiles. These compounds are typically
2420), or Randall R. Ross (FTS: 743-2355). found in the following wastes and waste-producing
processes: solvents, wood preserving wastes (creosote,
Introduction pentachlorophenol), coal tars, and pesticides. The most
frequently cited group of these contaminants to date are the
Dense nonaqueous phase liquids (DNAPLs) are present at chlorinated solvents.
numerous hazardous waste sites and are suspected to exist
at many more. Due to the numerous variables influencing DNAPL Transport and Fate - Conceptual Approach
DNAPL transport and fate in the subsurface, and
consequently, the ensuing complexity, DNAPLs are largely Fate and transport of DNAPLs in the subsurface will be
undetected and yet are likely to be a significant limiting factor presented from a conceptual point of view. Figures have
in site remediation. This issue paper is a literature evaluation been selected for various spill scenarios which illustrate the
focusing on DNAPLs and provides an overview from a general behavior of DNAPL in the subsurface. Following the
conceptual fate and transport point of view of DNAPL phase conceptual approach, detailed information will be presented
distribution, monitoring, site characterization, remediation, explaining the specific mechanisms, processes, and
and modeling. variables which influence DNAPL fate and transport. This
includes DNAPL characteristics, subsurface media
A nonaqueous phase liquid (NAPL) is a term used to characteristics, and saturation dependent parameters.
describe the physical and chemical differences between a
hydrocarbon liquid and water which result in a physical Unsaturated Zone
interface between a mixture of the two liquids. The interface
is a physical dividing surface between the bulk phases of the Figure 1 indicates the general scenario of a release of
two liquids, but compounds found in the NAPL are not DNAPL into the soil which subsequently migrates vertically
prevented from solubilizing into the ground water. under both the forces of gravity and soil capillarity. Soil
Immiscibility is typically determined based on the visual capillarity is also responsible for the lateral migration of
observation of a physical interface in a water- hydrocarbon DNAPL. A point is reached at which the DNAPL no longer
mixture. There are numerous methods, however, which are holds together as a continuous phase, but rather is present
used to quantify the physical and chemical properties of as isolated residual globules. The fraction of the hydrocarbon
hydrocarbon liquids (31). that is retained by capillary forces in the porous media is

Nonaqueous phase liquids have typically been divided into


two general categories, dense and light. These terms * Environmental Engineer,** Research Hydrologist, U.S.
describe the specific gravity, or the weight of the nonaqueous Environmental Protection Agency, Robert S. Kerr Environmental
phase liquid relative to water. Correspondingly, the dense Research Laboratory, Ada, Oklahoma.

Superfund Technology Support Center for Technology Innovation Office


Ground Water Office of Solid Waste and Emergency
Response, US EPA, Washington, D.C.
Robert S. Kerr Environmental
Research Laboratory Walter W. Kovalick, Jr., Ph.D.
Director
Ada, Oklahoma

1
Table 1. Most prevalent chemical compounds at U.S. Superfund Sites (65) with a specific gravity
greater than one.

Density Dynamic[2] Kinematic Water[4] Henrys Law


Vapor[6]
Compound [1] Viscosity Viscosity[3] Solub. Constant[5] Pressure

Halogenated Semi-volatiles

1,4-Dichlorobenzene 1.2475 1.2580 1.008 8. 0 E+01 1.58 E-03 6 E-01


1,2-Dichlorobenzene 1.3060 1.3020 0.997 1. 0 E+02 1.88 E-03 9.6 E-01
Aroclor 1242 1.3850 4.5 E-01 3.4 E-04 4.06 E-04
Aroclor 1260 1.4400 2.7 E-03 3.4 E-04 4.05 E-05
Aroclor 1254 1.5380 1.2 E-02 2.8 E-04 7.71 E-05
Chlordane 1.6 1.1040 0.69 5.6 E-02 2.2 E-04 1 E-05
Dieldrin 1.7500 1.86 E-01 9.7 E-06 1.78 E-07
2,3,4,6-Tetrachlorophenol 1.8390 1. 0 E+03
Pentachlorophenol 1.9780 1.4 E+01 2.8 E-06 1.1 E-04

Halogenated Volatiles

Chlorobenzene 1.1060 0.7560 0.683 4.9 E+02 3.46 E-03 8.8 E+00
1,2-Dichloropropane 1.1580 0.8400 0.72 2.7 E+03 3.6 E-03 3.95 E+01
1,1-Dichloroethane 1.1750 0.3770 0.321 5.5 E+03 5.45 E-04 1.82 E+02
1,1-Dichloroethylene 1.2140 0.3300 0.27 4. 0 E+02 1.49 E-03 5 E+02
1,2-Dichloroethane 1.2530 0.8400 0.67 8.69 E+03 1.1 E-03 6.37 E+01
Trans-1,2-Dichloroethylene 1.2570 0.4040 0.321 6.3 E+03 5.32 E-03 2.65 E+02
Cis-1,2-Dichloroethylene 1.2480 0.4670 0.364 3.5 E+03 7.5 E-03 2 E+02
1,1,1-Trichloroethane 1.3250 0.8580 0.647 9.5 E+02 4.08 E-03 1 E+02
Methylene Chloride 1.3250 0.4300 0.324 1.32 E+04 2.57 E-03 3.5 E+02
1,1,2-Trichloroethane 1.4436 0.1190 0.824 4.5 E+03 1.17 E-03 1.88 E+01
Trichloroethylene 1.4620 0.5700 0.390 1. 0 E+03 8.92 E-03 5.87 E+01
Chloroform 1.4850 0.5630 0.379 8.22 E+03 3.75 E-03 1.6 E+02
Carbon Tetrachloride 1.5947 0.9650 0.605 8.0 E+02 2. 0 E-02 9.13 E+01
1,1,2,2-Tetrachloroethane 1.6 1.7700 1.10 2.9 E+03 5. 0 E-04 4.9 E+00
Tetrachloroethylene 1.6250 0.8900 0.54 1.5 E+02 2.27 E-02 1.4 E+01
Ethylene Dibromide 2.1720 1.6760 0.79 3.4 E+03 3.18 E-04 1.1 E+01

Non-halogenated Semi-volatiles

2-Methyl Napthalene 1.0058 2.54 E+01 5.06 E-02 6.80 E-02


o-Cresol 1.0273 3.1 E+04 4.7 E-05 2.45 E-01
p-Cresol 1.0347 2.4 E+04 3.5 E-04 1.08 E-01
2,4-Dimethylphenol 1.0360 6.2 E+03 2.5 E-06 9.8 E-02
m-Cresol 1.0380 21. 0 20 2.35 E+04 3.8 E-05 1.53 E-01
Phenol 1.0576 3.87 8.4 E+04 7.8 E-07 5.293E-01
Naphthalene 1.1620 3.1 E+01 1.27 E-03 2.336E-01
Benzo(a)Anthracene 1.1740 1.4 E-02 4.5 E-06 1.16 E-09
Flourene 1.2030 1.9 E+00 7.65 E-05 6.67 E-04
Acenaphthene 1.2250 3.88 E+00 1.2 E-03 2.31 E-02
Anthracene 1.2500 7.5 E-02 3.38 E-05 1.08 E-05
Dibenz(a,h)Anthracene 1.2520 2.5 E-03 7.33 E-08 1 E-10
Fluoranthene 1.2520 2.65 E-01 6.5 E-06 E-02 E-06
Pyrene 1.2710 1.48 E-01 1.2 E-05 6.67 E-06
Chrysene 1.2740 6. 0 E-03 1.05 E-06 6.3 E-09
2,4-Dinitrophenol 1.6800 6. 0 E+03 6.45 E-10 1.49 E-05

Miscellaneous

Coal Tar 1.028(7) 18.98(7)


Creosote 1.05 1.08(8)
[1] g/cc [4] mg/l
[2] centipoise (cp), water has a dynamic viscosity of 1 cp at [5] atm-m3/mol
20oC. [6] mm Hg
[3] centistokes (cs) [7] 45o F (70)
[8] 15.50C, varies with creosote mix (62)
2
Residual
Saturation of
Residual Saturation of DNAPL Gaseous DNAPL in
DNAPL in Soil From Spill Vapors Vadose Zone
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Plume From DNAPL
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After, Waterloo Centre for Groundwater Research, 1989
After, Waterloo Centre for Groundwater Research,

Figure 1. The entire volume of DNAPL is exhausted by residual Figure 2. Migration of DNAPL vapors from the spill area and
saturation in the vadose zone prior to DNAPL reaching subsequent contamination of the soils and ground
the water table. Soluble phase compounds may be water.
leached from the DNAPL residual saturation and
contaminate the ground water.

referred to as residual saturation. In this spill scenario, the 4. Immiscible phase - contaminants may be present as
residual saturation in the unsaturated zone exhausted the dense nonaqueous phase liquids.
volume of DNAPL, preventing it from reaching the water
table. This figure also shows the subsequent leaching The four phase system is the most complex scenario
(solubilization) of the DNAPL residual saturation by water because there are four phases and the contaminant can
percolating through the unsaturated zone (vadose zone). The partition between any one or all four of these phases, as
leachate reaching the saturated zone results in ground-water illustrated in Figure 4. For example, TCE introduced into the
contamination by the soluble phase components of the subsurface as a DNAPL may partition onto the soil phase,
hydrocarbon. Additionally, the residual saturation at or near volatilize into the soil gas, and solubilize into the water phase
the water table is also subjected to leaching from the rise and resulting in contamination in all four phases. TCE can also
fall of the water table (seasonal, sea level, etc.). partition between the water and soil, water and air, and
between the soil and air. There are six pathways of phase
Increasing information is drawing attention to the importance distribution in the unsaturated zone. The distribution of a
of the possibility that gaseous-phase vapors from NAPL in contaminant between these phases can be represented by
the unsaturated zone are responsible for contaminating the empirical relationships referred to as partition coefficients.
ground water and soil (18,47). It is reported that the greater The partition coefficients, or the distribution of the DNAPL
relative vapor density of gaseous vapors to air will be between the four phases, is highly site-specific and highly
affected by gravity and will tend to sink. In subsurface dependent on the characteristics of both the soil/aquifer
systems where lateral spreading is not restricted, spreading matrix and the DNAPL. Therefore, the distribution between
of the vapors may occur as indicated in Figure 2. The result phases may change with time and/or location at the same
is that a greater amount of soils and ground water will be site and during different stages of site remediation.
exposed to the DNAPL vapors and may result in further
contamination. The extent of contamination will depend
largely on the partitioning of the DNAPL vapor phase Solid
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AA AAAA
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therefore, occur in four phases described as follows: AAAA
AAAA
AAAA
AAAA
AAAA
AAAA
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AAAA
AAAA
AAAA
AAAA
AAAA
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AAAA
AAAA
AAAA
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AAAA
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AAAA
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AA AAAAAAAA
AAAAAAAA
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AA
AAAAAAAA AAAA
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AA AAAAAAAAAAAA
AAAA AAAAAAAA AAAA
AAAAAAAAAAAAAAAA
AAAA
AAAAAAAA
AAAAAAAA
AAAAAAAA
AAAA

1. Air phase - contaminants may be present as vapors;


2. Solid phase - contaminants may adsorb or partition onto
the soil or aquifer material; Figure 3. A DNAPL contaminated unsaturated zone has four
3. Water phase - contaminants may dissolve into the water physical states or phases (air, solid, water,
according to their solubility; and immiscible). The contaminant may be present in any
one, or all four phases.

3
Four Phase System AAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAA
AAAAAAAA
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AAAAAA
Partition Coefficients AAAAAAAA
AAAAAAAA
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AAAAAAAA
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AAAAAAAA
AAAA
AAAAAAAA
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AAAAAAAA
AAAA
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Residual
AA
AA
AAAAAA
AA Sand
Vadose AAAA AAAA
AAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAA
K = Soil-water partition coefficient AAAAAAAA
AAAAAAAAAAAA
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Zone AAAA
AAAAAAAA
AAAAAAAA
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DNAPL
AAAAAAAA
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AA
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AA
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AAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAAA
K H = Henry's Constant AAAA
AAAAAAAA
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AAAAAA
AA

Air K'
K"
= DNAPL-water partition coefficient
= DNAPL-air partition coefficient
AAAA
AAAA
AAAA
AAAAAAAA
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AA
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AA

K"
KH Fractured
Rock

K'
DNAPL
Water K
Soil AAAAAAAA
AAAAAAAAAAAA
AAAAAAAA
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AAAAAAAAAAAA
AAAAAAAAAAAA
AAAAAAAAAAAA
AAAAAAAAAAAA
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AAAA
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AAAAAAAAAAAA
AAAAAAAAAAAA
AAAAAAAAAAAA
AAAAAAAAAAAA
AAAAAAAAAAAA
AAAAAAAAAAAA
AAAAAAAAAAAA
AAAAAAAAAAAA
AAAAAAAAAAAA
AAAAAAAAAAAA
AAAAAAAA
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after DiGiulio, 1990 (9)

Figure 4. Distribution of DNAPL between the four phases found Figure 5. DNAPL spilled into fractured rock systems may
in the vadose zone. follow a complex distribution of the preferential pathways.

The concept of phase distribution is critical in decision- small volumes of NAPL may move deep, quickly into the rock
making. Understanding the phase distribution of a DNAPL because the retention capacity offered by the dead-end
introduced into the subsurface provides significant insight in fractures and the immobile fragments and globules in the
determining which tools are viable options with respect to larger fractures is so small (32). Currently, the capability to
site characterization and remediation. collect the detailed information for a complete description of
a contaminated fractured rock system is regarded as neither
DNAPL represented by residual saturation in the four phase technically possible nor economically feasible (61).
diagram is largely immobile under the usual subsurface
pressure conditions and can migrate further only: 1) in water Low permeability stratigraphic units such as high clay content
according to its solubility; or 2) in the gas phase of the formations may also contain a heterogeneous distribution of
unsaturated zone (47). DNAPL components adsorbed onto preferential pathways. As illustrated in Figure 6, DNAPL
the soil are also considered immobile. The mobile phases transport in these preferential pathways is correspondingly
are, therefore, the soluble and volatile components of the complex. Typically, it is assumed that high clay content
DNAPL in the water and air, respectively. formations are impervious to DNAPL. However, as DNAPL
spreads out on low permeable formations it tends to seek out
The pore space in the unsaturated zone may be filled with zones of higher permeability. As a result, preferential
one or all three fluid phases (gaseous, aqueous, immiscible). pathways allow the DNAPL to migrate further into the low
The presence of DNAPL as a continuous immiscible phase permeable formation, or through it to underlying stratigraphic
has the potential to be mobile. The mobility of DNAPL in the units. It is apparent from Figures 5 and 6 that the complexity
subsurface must be evaluated on a case by case basis. The of DNAPL transport may be significant prior to reaching the
maximum number of potentially mobile fluid phases is three. water table.
Simultaneous flow of the three phases (air, water, and
immiscible) is considerably more complicated than two-
phase flow (46). The mobility of three phase flow in a four-
Saturated Zone
phase system is complex, poorly understood, and is beyond
the scope of this DNAPL overview. The relative mobility of The second general scenario is one in which the volume of
the two phases, water and DNAPL, in a three-phase system DNAPL is sufficient to overcome the fraction depleted by the
is presented below in the section entitled Relative residual saturation in the vadose zone, as illustrated in
Permeability. Figure 7. Consequently, the DNAPL reaches the water table
and contaminates the ground water directly. The specific
Generally, rock aquifers contain a myriad of cracks gravity of DNAPL is greater than water, therefore, the DNAPL
(fractures) of various lengths, widths, and apertures (32). migrates into the saturated zone. In this scenario, DNAPL
Fractured rock systems have been described as rock blocks continues the vertical migration through the saturated zone
bounded by discrete discontinuities comprised of fractures, until the volume is eventually exhausted by the residual
joints, and shear zones which may be open, mineral-filled, saturation process or until it is intercepted by a low
deformed, or any combination thereof (61). The unsaturated permeable formation where it begins to migrate laterally.
zone overlying these fractured rock systems also contain the
myriad of preferential pathways. DNAPL introduced into such DNAPL Phase Distribution - Three Phase System
formations (Figure 5) follow complex pathways due to the
heterogeneous distribution of the cracks, conduits, and Due to the lack of the gaseous phase, the saturated zone
fractures, i.e., preferential pathways. Transport of DNAPL containing DNAPL is considered a three-phase system
may follow non-Darcian flow in the open fractures and/or consisting of the solid, water, and immiscible hydrocarbon
Darcian flow in the porous media filled fractures. Relatively (Figure 8). Contaminant distribution in the three-phase

4
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After, Waterloo Centre for Groundwater Research,

Figure 6. DNAPL spilled into a low permeable formation may Figure 8. A DNAPL contaminated saturated zone has three
follow a complex distribution of preferential pathways. phases (solid, water, immiscible). The contaminant
The volume of DNAPL is exhausted in the vadose may be present in any one, or all three phases.
zone prior to reaching the water table.

system is less complex than the four-phase system. Again, system, gaseous vapors from DNAPL in the unsaturated
this is highly dependent on the characteristics of both the zone does have the potential to affect ground-water quality,
aquifer matrix and the DNAPL. Figure 9 indicates the three as was indicated earlier in Figure 2.
phases and the transfer of the mass of contaminant between
the phases. In this scenario, there are only three pathways of Assuming the residual saturation in the saturated zone does
phase distribution in the saturated zone. not deplete the entire volume of the DNAPL, the DNAPL will
continue migrating vertically until it encounters a zone or
Note that when the DNAPL is represented by residual stratigraphic unit of lower permeability. Upon reaching the
saturation in the three-phase system, the mobile phase of the zone of lower permeability, the DNAPL will begin to migrate
contaminant is the water soluble components of the DNAPL laterally. The hydraulic conductivity in the vertical direction is
and the immobile phases are the residual saturation and the typically less than in the horizontal direction. It is not
adsorbed components of the DNAPL associated with the uncommon to find vertical conductivity that is one-fifth or one-
aquifer material. The main mobilization mechanism of the tenth the horizontal value (4). It is expected that DNAPL
residual saturation is removal of soluble phase components spilled into the subsurface will have a significant potential to
into the ground water. When the DNAPL is present as a migrate laterally. If the lower permeable boundary is bowl
continuous immiscible phase, it too is considered one of the shaped, the DNAPL will pond as a reservoir (refer to Figure
mobile phases of the contaminant. While the continuous 10). As illustrated in Figure 11, it is not uncommon to observe
phase DNAPL has the potential to be mobile, immobile a perched DNAPL reservoir where a discontinuous
continuous phase DNAPL may also exist in the subsurface. impermeable layer; i.e., silt or clay lens, intercepts the
Although the saturated zone is considered a three-phase vertical migration of DNAPL. When a sufficient volume of

Residual
Three Phase System
Saturation of
DNAPL in Soil
From Spill DNAPL
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After, Waterloo Centre for Groundwater Research, 1
K = Soil-water partition coefficient
Figure 7. The volume of DNAPL is sufficient to overcome the
residual saturation in the vadose zone and Figure 9. Distribution of DNAPL between the three phases
consequently penetrates the water table. found in the saturated zone.

5
SZ Z
DNAPL
Release
FF
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Figure 10. Migration of DNAPL through the vadose zone to an Figure 12. Perched and deep DNAPL reservoirs.
impermeable boundary.

DNAPL has been released and multiple discontinuous than ground-water flow, and at different rates (refer to Figure
impermeable layers exist, the DNAPL may be present in 13b). Determination of the direction of impermeable
several perched reservoirs as well as a deep reservoir (refer stratigraphic units will therefore provide useful information
to Figure 12). Lateral migration continues until either the concerning the direction of DNAPL transport.
residual saturation depletes the DNAPL or an impermeable
depression immobilizes the DNAPL in a reservoir type Similar to the unsaturated zone, the saturated zone also
scenario. Soluble-phase components of the DNAPL will contains a complex distribution of preferential pathways from
partition into the ground water from both the residual cracks, fractures, joints, etc. DNAPL introduced into such
saturation or DNAPL pools. The migration of DNAPL formations correspondingly follow the complex network of
vertically through the aquifer results in the release of soluble- pathways through an otherwise relatively impermeable rock
phase components of the DNAPL across the entire thickness material. Other pathways which may behave as vertical
of the aquifer. Note, that ground water becomes conduits for DNAPL include root holes, stratigraphic
contaminated as it flows through, and around, the DNAPL windows, disposal wells, unsealed geotechnical boreholes,
contaminated zone. improperly sealed hydrogeological investigation sampling
holes and monitoring wells, and old uncased/unsealed water
As indicated earlier, DNAPL will migrate laterally upon supply wells (72). Transport of the DNAPL may migrate very
reaching a stratigraphic unit of lower permeability. Transport rapidly in these open conduits or follow Darcian flow in the
of DNAPL will therefore be largely dependent on the gradient surrounding porous media or porous media filled fractures. A
of the stratigraphy. Occasionally, the directional gradient of relatively small volume of DNAPL can move deep into a
an impermeable stratigraphic unit may be different than the fractured system due to the low retentive capacity of the
direction of ground-water flow as illustrated in Figure 13a. fractured system. Consequently, fractured clay or rock
This may result in the migration of the continuous phase stratigraphic units, which are often considered lower DNAPL
DNAPL in a direction different from the ground-water flow.
Nonhorizontal stratigraphic units with varying hydraulic
conductivity may also convey DNAPL in a different direction
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