role of napl in hot waterflooding

8/10/2019 Role of NAPL in Hot Waterflooding

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Transp Porous Med (2009) 79:393405DOI 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 flooding is a thermal nonaqueous phase liquid (NAPL) recovery

technology originally developed in the petroleum industry 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 flooding NAPL contaminated source zones

at elevated water temperatures was investigated. Simulations were conducted using 16 dif-

ferent geostatistical representations of an actual field site. Two NAPLs were selected for thisstudya light NAPL with hydraulic properties that have moderate temperature dependencies

and a dense NAPL with significant viscosity temperature dependency. For these two NAPLs,

flooding 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 flooding 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 flooding, 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: [email protected]

B. E. Sleep

Department of Civil Engineering, University of Toronto, Toronto, ON, Canada M5S 1A4

e-mail: [email protected]

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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 flooding exploits the temperature

dependence of fluid properties, such as viscosity and interfacial tension, to improve removal

efficiencies of viscous NAPLs. Improved NAPL removal efficiencies result in less subsurfaceNAPL mass available to act as a long-term source of groundwater contamination. A number

of hot water flooding studies have been completed in the petroleum literature, but they are

not directly applicable to the contaminated subsurface due to differing conditions in petro-

leum reservoirs 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 flooding in the contaminated subsurface. In a recent

two-dimensional hot water flooding experiment and numerical modeling study, OCarroll

and Sleep(2007) found that elevated fluid temperatures reduced remediation clean up times

for mobile NAPL, but did not reduce residual NAPL saturations. Hot water flooding has also

been applied at a limited number of NAPL remediation field sites with varying degrees of

success (EPA 2000;Fulton et al. 1991). Although hot water flooding 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 field scale heterogeneities on the effectiveness of hot

water flushing and to determine if there may be any potential negative impacts associated

with the application of this technology at the field scale. This study also has important impli-

cations to steam flushing remediation during the initial heating phase before a steam zoneforms, and at the leading edge of the steam zone 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 flooding 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 flooding 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 ofor coal tar were fit to experimental data (2897.0K and 402.6K,

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 fluid pair/soil systems. Capillary pressure/saturation temperature

dependencies are assumed to be solely based on interfacial tension temperature dependencies

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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 field. This site was subject to extensive site characterization with 14 vertical and angledcores. Grain size distributions of 167 subsamples, subdivided from the 14 core samples, were

quantified and used to estimate soil sample permeability using the CarmanKozeny equation

(Abriola et al. 2005;Bear 1972;Lemke et al. 2004a):

K=

wg

n3

(1 n)2

d2m

180

(1)

where K is the hydraulic conductivity (L/T), w is water mass phase density (M/L3), g

is gravitational acceleration constant (L/T2), is the water phase viscosity (M/LT), n is

porosity, and dm 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 flow 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 be8.8W/m K(Domenico and Schwartz 1998) and 1.93 106 J/m3 K(Jury et al. 1991),

respectively.

2.3 Numerical Model

A variety of numerical models have been developed for simulation of nonisothermal multi-

phase flow and transport with interphase partitioning for environmental applications (Class

et al. 2002; Falta et al. 1992; Pruess 1991) and for petroleum reservoir simulation (Coats et al.

1974;Rubin and Buchanan 1985;Tamim et al. 2000). In the current study, the compositionalsimulator, 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 flooding of viscous NAPLs. CompSim is a three-dimensional, three-phase, finite

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 fluid phase as:

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flooding of viscous NAPLs in a two-dimensional hot water experiment (OCarroll and Sleep

2007). This code was modified to include energy transport and temperature-dependent fluid

properties. A nonhysteretic BrooksCorey capillary pressure/saturation relationship (Brooks

and Corey1964) was used in all simulations with zero irreducible water saturations and zero

NAPL residual saturations:

Pc = Pd(Sw)1/ (8)

wherePcis the capillary pressure (M/LT2),Pdis the entry pressure (L),Swis water saturation

and is the pore size index.

The simulation domain was divided into 26 horizontal and 128 vertical blocks (0.3048 m

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 7.925 m, consistent with the

simulation domain ofChrist et al. (2005). The top and bottom boundaries were assumed

to be no flow boundaries. The side boundaries were assumed to be constant water pressure(hydrostatic) during NAPL infiltration. During the flooding phase of the simulations the

influent boundary was assumed to be a constant water flow, no flow NAPL boundary and the

effluent boundary was assumed to be a constant total fluid pressure boundary, consistent with

conditions expected at a field 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 flooding rate on NAPL recovery:

Case 1: Voltesso 35, the representative LNAPL, was injected at a total rate of 3.11

102 m3/d into a completely water saturated domain for a period of 400 days, sim-

ulating leakage of LNAPL from a leaking storage tank or pipeline located belowthe water table. The Voltesso 35 injection was distributed over four nodes 0.45 m

above the base of the domain at the horizontal midpoint. The LNAPL then redis-

tributed for 300days followed by 710days of water flooding at an average Darcy

velocity of 1.15m/d. The domain is initially at 10C during Voltesso 35 injection

and redistribution. During the flooding phase water was pumped into the system at

either 10C, 50C, or 90C.

Case 2: Coal tar, a representative DNAPL with significant temperature dependent hydrau-

lic properties(Kong 2004), was injected at a total rate of 3.11 102 m3/d into a

completely water saturated domain for a period of 400 days. The coal tar injection

was distributed over four nodes 0.11 m from the top of the domain at the horizon-tal midpoint. The DNAPL then redistributed for 300 days followed by 710 days of

water flooding at an average Darcy velocity of 1.15m/d. Similar to the Case 1,

water flooding was conducted at three temperatures, 10C, 50C, and 90C.

Case 3: A series of simulations were carried out to determine the effect of water flood rate

on coal tar recovery. In these simulations the conditions were identical to Case 2

with the exception of the water flooding 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 infiltration, redistribution and

water flooding at 10C using one of the 16 permeability realizations are presented

in Fig. 1.At the termination of Voltesso 35 infiltration the NAPL was only present

in the bottom half of the simulated domain at saturations ranging up to 77%. Due to

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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 300 days of redistribution the Voltesso 35 migrated both laterally

and vertically, contaminating much of the simulated domain. Figure 2presents ahistogram 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 flooding for 710days, at 10C 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 flood-

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 flooding at ambient temperature, additional water

flooding simulations for injection temperatures of 50C or 90C 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 35 cP at 10C to 5.6cP at

50

C and finally to 1.3 cP at 90

C. Voltesso 35/water interfacial tension is a weakerfunction of temperature, decreasing from 45 dynes/cm at 10C to 25dynes/cm at

90C. Voltesso 35 recovery increased from 39% at 10C water flooding to 51% at

50C and finally to 57% at 90C. 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 90C Voltesso 35 recovery was initially rapid and decreased

with time, whereas recovery at the lower temperatures was more gradual. Increasing

temperature with hot water flushing 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 infiltrated into the porous media NAPL saturations were much higherthan with Voltesso 35 (Figs. 2,4)due to the much higher NAPL viscosity (1004 cP

in comparison to 35cP at 10C). 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 infiltration to NAPL

saturations of 93% following redistribution. Following water flooding at 10C at

an average Darcy velocity of 1.15 m/d no coal tar was recovered within 710 days

(Fig. 5) due to the low mobility of the coal tar at this temperature. The coal tardid, 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 flooding

temperatures (Fig. 5). At 50C 37% of the coal tar was recovered at the completion

of the water flooding and 67% of the coal tar was recovered at 90C. The coal tar

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

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Fig. 1 Example simulation showing (a) infiltration (390 days), (b) redistribution (690 days), and (c) water

flooding at 10C at a Darcy velocity of 1.15m/d (1,410days) for Voltesso 35

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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

FractionDomain

Following NAPL Infiltration

Following NAPL Redistribution

Following Water Flooding at 10 deg C

Fig. 2 Average NAPL saturation distribution following Voltesso 35 infiltration, redistribution, and water

flooding at 10C at a Darcy velocity of 1.15 m/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)

Voltesso

35Fract

ion

Recovered

Water Flooding at 10 deg C


WaterFlooding at 50 deg C

Fig. 3 Average Voltesso 35 recovery following water flooding at a Darcy velocity of 1.15m/d for the 16

permeability realizations (error barsindicate 95% confidence intervals about means)

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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

FractionDomain

Following NAPL Infiltration

Following NAPL Redistribution

Following Water Flooding at 10 deg C

Fig. 4 Average NAPL saturation distribution following coal tar infiltration, redistribution, and water flooding

at 10C 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


CoalTarFraction

Recovered




Fig. 5 Average coal tar recovery following water flooding at a Darcy velocity of 1.15 m/d for the 16 perme-

ability realizations (error barsindicate 95% confidence intervals about means)

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56cP at 50C and 1.7cP at 90C. Similar to the Voltesso 35 recovery at 90C, coal

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

50C 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 90C; how-

ever, coal tar saturations were much higher and localized at the initiation of waterflooding (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 flooding at a Darcy velocity

of 1.15m/d (1,410 days) at (a) 10C and (b) 90C

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-0.01

0.09

0.19

0.29

0.39

0.49

0.59

0 100 200 300 400 500 600 700 800


CoalTarFractionRecovered




Fig. 7 Average coal tar recovery following water flooding at a Darcy velocity of 0.58 m/d for the 16 perme-

ability realizations (error barsindicate 95% confidence intervals about means)

to the much larger difference between viscosities at 10C and 90C. 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 flushing 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 50C and

90C water flooding temperatures but less than the simulations presented in Case 2(Fig. 7). When normalized to pore volumes flushed, coal tar recovery was less at the

reduced water flooding rate due to reduced imposed water pressure. For example

at 143 pore volumes flushed at 90C (equivalent to 710days of water flooding at

an average Darcy velocity of 0.58m/d) 57% of the coal tar was recovered when

the average Darcy velocity is 1.15 m/d as opposed to 50% recovery when the aver-

age Darcy velocity is 0.58 m/d. These results suggest that, when feasible, a higher

flooding rate should be imposed to achieve greater NAPL recovery.

4 Conclusions

A numerical study was conducted to assess the utility of flooding 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 field

site. Two different NAPLs were selected for this study, a LNAPL with moderate hydraulic

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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 flooding 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 flooding rates resulted in higher

governing capillary pressures and NAPL recovery.

The use of hot water flooding 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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role of napl in hot waterflooding

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