Transp Porous Med (2009) 79:393405

DOI 10.1007/s11242-008-9329-2
Role of NAPL Thermal Properties in the Effectiveness
of Hot Water Flooding
Denis M. OCarroll Brent E. Sleep
Received: 16 October 2007 / Accepted: 21 December 2008 / Published online: 16 January 2009
Springer Science+Business Media B.V. 2009
Abstract Hot water ooding is a thermal nonaqueous phase liquid (NAPL) recovery
technology originally developed in the petroleumindustry that has recently been proposed for
enhanced recovery of NAPLs in the contaminated subsurface. This technology, however, has
received relatively little laboratory or numerical modeling investigation in the contaminant
hydrology community. In this study the utility of ooding NAPL contaminated source zones
at elevated water temperatures was investigated. Simulations were conducted using 16 dif-
ferent geostatistical representations of an actual eld site. Two NAPLs were selected for this
studya light NAPLwith hydraulic properties that have moderate temperature dependencies
and a dense NAPL with significant viscosity temperature dependency. For these two NAPLs,
ooding the source zone with water at elevated temperatures resulted in enhanced NAPL
recovery. However, injection of hot water also resulted in accelerated downward movement
of coal tar DNAPL due to the reduced viscosity at elevated temperatures. NAPL recovery
was also dependent on the source zone architecture with greater NAPL mass recovery when
the NAPL was localized in a small volume at high saturations. These results suggest that hot
water ooding can significantly speed up the recovery of viscous NAPLs and, as such, is a
powerful technique for the remediation of viscous NAPLs.
Keywords NAPL Hot water Thermal Remediation Groundwater
1 Introduction
Thermal remediation techniques, such as hot water ooding, are emerging technologies that
have been proposed to remove significant amounts of nonaqueous phase liquid (NAPL) from
D. M. OCarroll (B)
Department Civil & Environmental Engineering, The University of Western Ontario, London, ON,
Canada N6A 5B9
e-mail: docarroll@eng.uwo.ca
B. E. Sleep
Department of Civil Engineering, University of Toronto, Toronto, ON, Canada M5S 1A4
e-mail: sleep@ecf.utoronto.ca
1 3
394 D. M. OCarroll, B. E. Sleep
the subsurface. These techniques were originally developed in the petroleum industry for
enhanced petroleum recovery and later proposed for the remediation of NAPL contaminated
sites (e.g., Edmondson 1965; Fournier 1965). Hot water ooding exploits the temperature
dependence of uid properties, such as viscosity and interfacial tension, to improve removal
efciencies of viscous NAPLs. Improved NAPLremoval efciencies result in less subsurface
NAPL mass available to act as a long-term source of groundwater contamination. A number
of hot water ooding studies have been completed in the petroleum literature, but they are
not directly applicable to the contaminated subsurface due to differing conditions in petro-
leumreservoirs and subsurface aquifers (e.g., Dokla 1981; Edmondson 1965; Fournier 1965;
Goodyear et al. 1996; Okasha et al. 1998; Willman et al. 1961). To date, limited work has
been conducted to investigate hot water ooding in the contaminated subsurface. In a recent
two-dimensional hot water ooding experiment and numerical modeling study, OCarroll
and Sleep (2007) found that elevated uid temperatures reduced remediation clean up times
for mobile NAPL, but did not reduce residual NAPL saturations. Hot water ooding has also
been applied at a limited number of NAPL remediation eld sites with varying degrees of
success (EPA 2000; Fulton et al. 1991). Although hot water ooding may be an appropriate
remediation alternative at a number of sites, there is an incomplete understanding of the
operating conditions required to maximize NAPL removal. Furthermore, as with any reme-
diation technology, there is always the potential for negative unanticipated consequences of
the remedial technology. The goal of this study is to investigate the impact of temperature
dependencies of NAPL properties and eld scale heterogeneities on the effectiveness of hot
water ushing and to determine if there may be any potential negative impacts associated
with the application of this technology at the eld scale. This study also has important impli-
cations to steam ushing remediation during the initial heating phase before a steam zone
forms, and at the leading edge of the steamzone where a condensation bank forms. As a result
near the leading edge of the steam front both the NAPL and aqueous phases will be present
at elevated temperatures, potentially increasing their subsurface mobility and complicating
steam ooding remedial activities.
2 Methods
2.1 NAPL Hydraulic Properties
In this study, two representative NAPLs with hydraulic property temperature dependencies
were selected to investigate the utility of ooding NAPL contaminated porous media with
water at elevated temperatures. Voltesso 35, a LNAPL, is a commercially available insulat-
ing oil with moderate temperature dependencies (Sleep and Ma 1997). Experimental data
and mathematical relationships for the temperature dependencies of Voltesso 35 hydraulic
properties are available in the literature (OCarroll and Sleep 2007; Sleep and Ma 1997). A
coal tar with significant viscosity temperature dependency was selected as the representative
DNAPL. The coal tar, from a manufactured gas plant site in Charleston, SC, has recently
been the subject of extensive characterization (Kong 2004). The viscosity temperature depen-
dency parameters

and
o
for coal tar were t to experimental data (2897.0

Kand 402.6

K,
respectively) (Kong 2004). It was assumed that the density of the coal tar did not vary with
temperature, consistent with published data (Kong 2004). It was also assumed that the thermal
conductivity and heat capacity of the coal tar is the same as Voltesso 35. The contact angle is
assumed to be zero for all uid pair/soil systems. Capillary pressure/saturation temperature
dependencies are assumed to be solely based on interfacial tension temperature dependencies
1 3
Role of NAPL Thermal Properties in the Effectiveness of Hot Water Flooding 395
(i.e., contact angle is zero at all temperatures). The parameter

is commonly used to describe

capillary pressure/saturation temperature dependencies (Grant and Salehzadeh 1996). Given
that coal tar/water interfacial tension exhibits little temperature dependency it was assumed
that the capillary pressure/saturation relationship was not a function of temperature (Kong
2004).
2.2 Soil Properties
Soil properties for the simulations are based on published studies (Christ et al. 2005; Lemke
et al. 2004a,b). In these studies the authors developed geostatistical representations of soil
properties from a surfactant enhanced aquifer remediation demonstration site in Oscoda, MI
(Abriola et al. 2005; Ramsburg et al. 2005). Geostatistical representations of the subsurface
were employed in this study in order to, as closely as possible, capture heterogeneities present
in the eld. This site was subject to extensive site characterization with 14 vertical and angled
cores. Grain size distributions of 167 subsamples, subdivided fromthe 14 core samples, were
quantied and used to estimate soil sample permeability using the CarmanKozeny equation
(Abriola et al. 2005; Bear 1972; Lemke et al. 2004a):
K =
_

w
g

_
n
3
(1 n)
2
_
d
2
m
180
_
(1)
where K is the hydraulic conductivity (L/T),
w
is water mass phase density (M/L
3
), g
is gravitational acceleration constant (L/T
2
), is the water phase viscosity (M/LT), n is
porosity, and d
m
is the representative soil diameter (L). In the model domain, soil prop-
erties are consistent with those at the sampling locations and statistically homogeneous,
nonuniform permeability sequential Gaussian simulation is used to interpolate the soil prop-
erties between these sampling locations (Lemke et al. 2004a). Representative capillary
pressure/saturation retention properties were estimated using the Haverkamp and Parlange
method (Haverkamp and Parlange 1986) and BrooksCorey retention curve entry pressures
(Brooks and Corey 1964) were estimated using Leverett scaling (Leverett 1941) where
porosity was assumed to be uniform throughout the ow domain (0.36) (Christ et al. 2005;
Lemke et al. 2004a). The Burdine relative permeability model has been used in all sim-
ulations (Burdine 1953). Soil thermal conductivity and heat capacity were assumed to be
8.8 W/m K (Domenico and Schwartz 1998) and 1.93 10
6
J/m
3
K (Jury et al. 1991),
respectively.
2.3 Numerical Model
A variety of numerical models have been developed for simulation of nonisothermal multi-
phase ow and transport with interphase partitioning for environmental applications (Class
et al. 2002; Falta et al. 1992; Pruess 1991) and for petroleumreservoir simulation (Coats et al.
1974; Rubin and Buchanan 1985; Tamim et al. 2000). In the current study, the compositional
simulator, CompSim (McClure and Sleep 1996; OCarroll and Sleep 2007; Sehayek et al.
1999; Sleep 1998; Sleep and Sykes 1993a,b; Sleep et al. 2000a,b) was used to simulate
hot water ooding of viscous NAPLs. CompSim is a three-dimensional, three-phase, nite
difference model for the prediction of NAPL migration and remediation in permeable media
systems. It solves the following species molar balance equation for the movement of species
in uid phase as:
1 3
396 D. M. OCarroll, B. E. Sleep
3

=1
_

t
_

_
S

+ K
,d

b
__
+
_

_
+
_
S

J
D

_
r

_
= 0
(2)
where

is molar phase density (n/L

3
), x

is species mole fraction in phase , is

porosity, S

is phase saturation, K
,d
is the linear sorption coefcient for species in phase
and
b
is the bulk mass density of the soil phase (M/L
3
). q

is the molar-averaged Darcy

velocity vector for phase (L/T), J
D

is the dispersive molar ux vector for species relative

to the other molar-averaged velocity (n/L
2
T), r

represents interphase transfer of species

to or from phase (n/L
3
T), and

represents sources and sinks of species to or from

phase (n/L
3
T).
The molar-averaged Darcy velocity is given by
q

=
kk
r

_
p

gz
_
(3)
where k is the intrinsic permeability tensor (L
2
), k
r
is the relative permeability,

is the
phase viscosity (M/LT), p

is the phase pressure (M/LT

2
),

is the mass density of phase

(M/L
3
), and z is the elevation (L).
The dispersive molar ux is
J
D

(4)
where D

is the dispersion tensor (L

2
/T), dened by Bear (1972). For the low pressure low
temperature conditions used in the present study, complex equations of state, such as those
used in petroleum reservoir models, are not necessary and interphase partitioning of species
can be adequately described by Henrys law and Daltons law if equilibrium conditions exist.
The relationship between mole fractions of a species in water (x
w
), gas (x
g
), and organic
(x
o
) phases is given by
x
w
H = x
g
p
g
= x
o
P

(5)
where H is the Henrys Law constant and P

is the vapor pressure of species .

The multiphase energy transport equation is used to solve for temperature:
3

=1
__

t
_
S

_
+
_

_
+
n
c

=1

_
S

J
D

_
_
+

t
[(1 )U
s

s
] + (T) +
en
= 0 (6)
where U

is the internal energy of phase, U

s
is the internal energy of the soil, h

is the
enthalpy of the phase, h

is the enthalpy of the component in the phase, T is the temper-

ature (K), is the thermal conductivity of the combined soil and uids, and
en
represents
sinks or sources of energy.
The relationship between uid viscosity and temperature is represented as:
log =

_
1
T

1

o
_
(7)
where

and
o
are parameters t to measured data.
CompSim has been used extensively for contaminant hydrology applications (Sehayek
et al. 1999; Sleep 1998; Sleep et al. 2000a,b) and has recently been validated for hot water
1 3
Role of NAPL Thermal Properties in the Effectiveness of Hot Water Flooding 397
ooding of viscous NAPLs in a two-dimensional hot water experiment (OCarroll and Sleep
2007). This code was modied to include energy transport and temperature-dependent uid
properties. Anonhysteretic BrooksCorey capillary pressure/saturation relationship (Brooks
and Corey 1964) was used in all simulations with zero irreducible water saturations and zero
NAPL residual saturations:
P
c
= P
d
(S
w
)
1/
(8)
where P
c
is the capillary pressure (M/LT
2
), P
d
is the entry pressure (L), S
w
is water saturation
and is the pore size index.
The simulation domain was divided into 26 horizontal and 128 vertical blocks (0.3048m
0.0762 respectively) for a total domain size of 7.925m long by 9.754m deep (Christ et al.
2005). It was assumed the width of the simulation domain was 7.925m, consistent with the
simulation domain of Christ et al. (2005). The top and bottom boundaries were assumed
to be no ow boundaries. The side boundaries were assumed to be constant water pressure
(hydrostatic) during NAPL inltration. During the ooding phase of the simulations the
inuent boundary was assumed to be a constant water ow, no ow NAPL boundary and the
efuent boundary was assumed to be a constant total uid pressure boundary, consistent with
conditions expected at a eld site. In all simulations the domain was initially water saturated.
Three different sets of simulations were conducted to investigate the impact of the temper-
ature dependence of NAPL hydraulic properties and water ooding rate on NAPL recovery:
Case 1: Voltesso 35, the representative LNAPL, was injected at a total rate of 3.11
10
2
m
3
/d into a completely water saturated domain for a period of 400days, sim-
ulating leakage of LNAPL from a leaking storage tank or pipeline located below
the water table. The Voltesso 35 injection was distributed over four nodes 0.45m
above the base of the domain at the horizontal midpoint. The LNAPL then redis-
tributed for 300days followed by 710days of water ooding at an average Darcy
velocity of 1.15m/d. The domain is initially at 10

C during Voltesso 35 injection

and redistribution. During the ooding phase water was pumped into the system at
either 10

C, 50

C, or 90

C.
Case 2: Coal tar, a representative DNAPL with significant temperature dependent hydrau-
lic properties (Kong 2004), was injected at a total rate of 3.11 10
2
m
3
/d into a
completely water saturated domain for a period of 400days. The coal tar injection
was distributed over four nodes 0.11m from the top of the domain at the horizon-
tal midpoint. The DNAPL then redistributed for 300days followed by 710days of
water ooding at an average Darcy velocity of 1.15m/d. Similar to the Case 1,
water ooding was conducted at three temperatures, 10

C, 50

C, and 90

C.
Case 3: A series of simulations were carried out to determine the effect of water ood rate
on coal tar recovery. In these simulations the conditions were identical to Case 2
with the exception of the water ooding rate. Here, the average Darcy velocity was
0.58m/d as opposed to 1.15m/d in Case 2.
3 Results and Discussion
Case 1: Results for one of the simulations of Voltesso 35 inltration, redistribution and
water ooding at 10

C using one of the 16 permeability realizations are presented

in Fig. 1. At the termination of Voltesso 35 inltration the NAPL was only present
in the bottom half of the simulated domain at saturations ranging up to 77%. Due to
1 3
398 D. M. OCarroll, B. E. Sleep
permeability contrasts and capillarity the NAPL distribution was highly heteroge-
neous with zones of no NAPL saturation surrounded by zones with relatively high
NAPL saturations. Similar behavior was observed for all 16 permeability realiza-
tions. Following 300days of redistribution the Voltesso 35 migrated both laterally
and vertically, contaminating much of the simulated domain. Figure2 presents a
histogram of the NAPL distribution in the domain averaged over the 16 permeabil-
ity realizations. After NAPL redistribution Voltesso 35 was present in the domain
at much lower saturations (Fig. 2) and maximum saturations decreased slightly to
73%. After water ooding for 710days, at 10

C and an average Darcy velocity of

1.15m/d, an average of 39% of the Voltesso 35 was removed (Fig. 3). However,
the NAPL occupied a larger fraction of the domain but at lower saturations (Fig. 2)
due to the displacement of NAPL through previously uninvaded areas between the
injection and extraction points. These results suggest that, on average, water ood-
ing at ambient temperatures achieves significant NAPL reductions in mobile NAPL
volume under the conditions simulated here, and reduces the mobility of the NAPL
pool through reductions in high NAPL saturations.
In addition to simulation of water ooding at ambient temperature, additional water
ooding simulations for injection temperatures of 50

C or 90

C were conducted
to investigate the impact of elevated system temperatures on Voltesso 35 recovery.
When water at elevated temperatures was pumped into the system, heat was trans-
ferred to the NAPL and porous media phases until the system achieved thermal
equilibrium. The hydraulic properties of Voltesso 35 have moderate temperature
dependencies. For example, the viscosity decreases from 35cP at 10

C to 5.6cP at
50

C and nally to 1.3cP at 90

C. Voltesso 35/water interfacial tension is a weaker

function of temperature, decreasing from 45dynes/cm at 10

C to 25dynes/cm at
90

C. Voltesso 35 recovery increased from 39% at 10

C water ooding to 51% at

50

C and nally to 57% at 90

C. The 95% errors bars on the Voltesso 35 recovery

indicate that recoveries at each of the three temperatures were statistically different
from each other. At 90

C Voltesso 35 recovery was initially rapid and decreased

with time, whereas recovery at the lower temperatures was more gradual. Increasing
temperature with hot water ushing resulted in accelerated upward movement of
Voltesso 35 due to the decreased viscosity of Voltesso 35 at elevated temperatures
(results not shown).
Case 2: As the coal tar inltrated into the porous media NAPL saturations were much higher
than with Voltesso 35 (Figs. 2, 4) due to the much higher NAPL viscosity (1004cP
in comparison to 35cP at 10

C). As a result, the coal tar distribution was less

heterogeneous than Voltesso 35, with the coal tar present in a relatively localized
portion of the system. As the coal tar redistributed in the system it spread hori-
zontally and vertically and coal tar NAPL saturations decreased (Fig. 4). Average
maximum NAPL saturations decreased from 97% following inltration to NAPL
saturations of 93% following redistribution. Following water ooding at 10

C at
an average Darcy velocity of 1.15m/d no coal tar was recovered within 710days
(Fig. 5) due to the low mobility of the coal tar at this temperature. The coal tar
did, however, migrate toward the recovery well and a significant amount of NAPL
invaded previously NAPL free zones at relatively low saturations (Fig. 4). Signifi-
cant improvement in NAPL recovery was achieved with increases in water ooding
temperatures (Fig. 5). At 50

C 37% of the coal tar was recovered at the completion

of the water ooding and 67% of the coal tar was recovered at 90

C. The coal tar

viscosity has a strong temperature dependency with a viscosity of 1004cP at 10

C,
1 3
Role of NAPL Thermal Properties in the Effectiveness of Hot Water Flooding 399
Fig. 1 Example simulation showing (a) inltration (390days), (b) redistribution (690days), and (c) water
ooding at 10

C at a Darcy velocity of 1.15m/d (1,410days) for Voltesso 35

1 3
400 D. M. OCarroll, B. E. Sleep
0.00
0.02
0.04
0.06
0.08
0.10
0.12
0.14
0.16
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7
NAPL Saturation
F
r
a
c
t
i
o
n

D
o
m
a
i
n
Following NAPL Infiltration
Following NAPL Redistribution
Following Water Flooding at 10 deg C
Fig. 2 Average NAPL saturation distribution following Voltesso 35 inltration, redistribution, and water
ooding at 10

C at a Darcy velocity of 1.15m/d

0
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0 100 200 300 400 500 600 700 800
Time Since Water Flooding Initiation (days)
V
o
l
t
e
s
s
o

3
5

F
r
a
c
t
i
o
n

R
e
c
o
v
e
r
e
d
Water Flooding at 10 deg C
Water Flooding at 90 deg C
WaterFlooding at 50 deg C
Fig. 3 Average Voltesso 35 recovery following water ooding at a Darcy velocity of 1.15m/d for the 16
permeability realizations (error bars indicate 95% condence intervals about means)
1 3
Role of NAPL Thermal Properties in the Effectiveness of Hot Water Flooding 401
0.000
0.002
0.004
0.006
0.008
0.010
0.012
0.014
0.016
0.018
0.020
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1
NAPL Saturation
F
r
a
c
t
i
o
n

D
o
m
a
i
n
Following NAPL Infiltration
Following NAPL Redistribution
Following Water Flooding at 10 deg C
Fig. 4 Average NAPL saturation distribution following coal tar inltration, redistribution, and water ooding
at 10

C at a Darcy velocity of 1.15m/d

-0.01
0.09
0.19
0.29
0.39
0.49
0.59
0.69
0 100 200 300 400 500 600 700 800
Time Since Water Flooding Initiation (days)
C
o
a
l

T
a
r

F
r
a
c
t
i
o
n

R
e
c
o
v
e
r
e
d
Water Flooding at 10 deg C
Water Flooding at 50 deg C
Water Flooding at 90 deg C
Fig. 5 Average coal tar recovery following water ooding at a Darcy velocity of 1.15m/d for the 16 perme-
ability realizations (error bars indicate 95% condence intervals about means)
1 3
402 D. M. OCarroll, B. E. Sleep
56cP at 50

C and 1.7cP at 90

C. Similar to the Voltesso 35 recovery at 90

C, coal
tar recovery was initially rapid and gradually decreased, whereas coal tar recovery at
50

C was much more gradual. Greater amounts of coal tar were recovered at 90

C
in comparison to Voltesso 35. Both NAPLs have similar viscosities at 90

C; how-
ever, coal tar saturations were much higher and localized at the initiation of water
ooding (Figs. 2, 4). Due to the higher coal tar saturations, the relative permeability
to NAPL and mobility were higher for the coal tar in comparison with the Voltesso
35 facilitating enhanced NAPL recovery. These results suggest that NAPL source
zone morphology will significantly affect NAPL recovery.
As with Voltesso 35 increased temperatures not only enhanced coal tar recovery,
due to greater NAPL mobility, but also increased the vertical movement of the coal
tar (Fig. 6). The effect was more significant with coal tar than with Voltesso 35, due
Fig. 6 Example simulations showing coal tar NAPL saturations following water ooding at a Darcy velocity
of 1.15m/d (1,410days) at (a) 10

C and (b) 90

C
1 3
Role of NAPL Thermal Properties in the Effectiveness of Hot Water Flooding 403
-0.01
0.09
0.19
0.29
0.39
0.49
0.59
0 100 200 300 400 500 600 700 800
Time Since Water Flooding Initiation (days)
C
o
a
l

T
a
r

F
r
a
c
t
i
o
n

R
e
c
o
v
e
r
e
d
Water Flooding at 10 deg C
Water Flooding at 50 deg C
Water Flooding at 90 deg C
Fig. 7 Average coal tar recovery following water ooding at a Darcy velocity of 0.58m/d for the 16 perme-
ability realizations (error bars indicate 95% condence intervals about means)
to the much larger difference between viscosities at 10

C and 90

C. Also, as the
coal tar is a DNAPL, the enhanced downward movement is of greater concern than
the upward movement of the Voltesso 35 LNAPL. In the case of viscous DNAPLs
that had been in the subsurface for longer periods of time, and were more com-
pletely redistributed, this effect of temperature would not be as significant. Design
of hot water ushing schemes for remediation of viscous DNAPL must consider the
DNAPL zone architecture with respect to this mechanism of potentially enhanced
vertical mobility to avoid increasing the extent of DNAPL contamination.
Case 3: At half the average Darcy velocity coal recovery was still significant at 50

C and
90

C water ooding temperatures but less than the simulations presented in Case 2
(Fig. 7). When normalized to pore volumes ushed, coal tar recovery was less at the
reduced water ooding rate due to reduced imposed water pressure. For example
at 143 pore volumes ushed at 90

C (equivalent to 710days of water ooding at

an average Darcy velocity of 0.58m/d) 57% of the coal tar was recovered when
the average Darcy velocity is 1.15m/d as opposed to 50% recovery when the aver-
age Darcy velocity is 0.58m/d. These results suggest that, when feasible, a higher
ooding rate should be imposed to achieve greater NAPL recovery.
4 Conclusions
A numerical study was conducted to assess the utility of ooding NAPL source zones with
water at elevated temperatures. Simulations were conducted using 16 realizations of soil char-
acteristics (i.e., permeability and entry pressure) from an actual NAPL contaminated eld
site. Two different NAPLs were selected for this study, a LNAPL with moderate hydraulic
1 3
404 D. M. OCarroll, B. E. Sleep
property temperature dependencies and a DNAPL with a strong viscosity temperature depen-
dency. Averages of the simulations using the 16 soil characteristic realizations suggest that
water ooding at elevated temperatures significantly improved NAPL recovery for the two
NAPLs selected. Results also suggest that injection of hot water can result in accelerated
downward movement of viscous DNAPL due to the reduced viscosity at elevated tempera-
tures. Source zone morphology was also an important factor in NAPL recovery. When NAPL
source zone saturations were higher greater NAPL was recovered when the hydraulic prop-
erties were approximately equivalent. Finally larger water ooding rates resulted in higher
governing capillary pressures and NAPL recovery.
The use of hot water ooding should be assessed on a case by case basis as the recovery
will be strongly dependent on the temperature dependence of NAPL hydraulic properties.
Acknowledgments This research was supported by Natural Sciences and Engineering Research Council
(NSERC) of Canada Discovery Grants. The authors would also like to thank John Christ and Lawrence Lemke
for supplying the permeability realizations.
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