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Solvent Systems in Porous Media

H. Luo and A. Kantzas, SPE, University of Calgary and TIPM Laboratory

This paper was prepared for presentation at the 2008 SPE Improved Oil Recovery Symposium held in Tulsa, Oklahoma, U.S.A., 1923 April 2008.

This paper was selected for presentation by an SPE program committee following review of information contained in an abstract submitted by the author(s). Contents of the paper have not been

reviewed by the Society of Petroleum Engineers and are subject to correction by the author(s). The material does not necessarily reflect any position of the Society of Petroleum Engineers, its

officers, or members. Electronic reproduction, distribution, or storage of any part of this paper without the written consent of the Society of Petroleum Engineers is prohibited. Permission to

reproduce in print is restricted to an abstract of not more than 300 words; illustrations may not be copied. The abstract must contain conspicuous acknowledgment of SPE copyright.

Abstract

Solvents can be injected to dilute viscous heavy oil or bitumen and improve the recovery of the vast reserves of heavy oil and

bitumen in Canada. In an evolution of the SAGD and VAPEX processes, some new schemes that use solvent and steam

appeared to offer a more economical and environmentally sound alternative to extract heavy oil and bitumen compared to

SAGD alone. Mass transfer rates determine whether these solvent-assisted processes are feasible for heavy oil and bitumen

recovery. The solvent-bitumen diffusion coefficient is a basic parameter needed. According to previous literature, the

effective diffusion coefficient in porous media is much smaller than the true diffusion coefficient in bulk fluids. However,

good-quality data from diffusion experiments of heavy oil and hydrocarbon solvent systems for effective diffusion

coefficients determination in porous media is still scarce. This paper presents diffusion experiments of liquid solvent in heavy

oil saturated sand using X-ray Computer Assisted Tomography (CAT), and determines the effective diffusion coefficients

based on an updated approach, which considers porosity variation of porous media and volume changes on mixing. In

addition, the relationship between the effective diffusion coefficient of solvent in oil saturated sand pack and the true

diffusion coefficient in bulk fluids is investigated.

Introduction

For the recovery of the vast reserves of heavy oil and bitumen in Canada, some new hybrid steam-solvent processes 1 were

proposed recently and were developed to offer the possibility of higher oil production rates and recoveries, but less energy

and water consumption than SAGD. These methods come by the names of Expanding Solvent SAGD (ES-SAGD), Solvent

Aided Process (SAP), Liquid Addition to Steam for Enhancing Recovery (LASER), Steam Alternating Solvent process

(SAS) and Thermal Solvent Hybrid Process. Hopefully these solvent-assisted processes will become more mature and will be

gradually applied in the field, thus improving the recovery of heavy oil and bitumen. In order to study these mass transfer

processes in porous media quantitatively, the diffusivity of solvent in heavy oil should be investigated further.

According to Butlers work, the molecular diffusion coefficient Do is a strong function of concentration of the

mixture 2, and can be calculated from concentration profiles. In addition, the effect of volume changes due to mixing on

diffusivity determination has been analyzed 3.

In a porous rock, molecular diffusion takes place along tortuous paths. The actual distance traveled by a diffusing

solute is therefore longer than the length of the porous medium. Therefore, the effective diffusivity De in the porous medium

is smaller than the molecular diffusivity Do in the bulk fluids. For the estimation of effective diffusivity in porous solids, two

common empirical relationships can be used. Equation 1 4 gives a rough approximation to the diffusion coefficient in

unconsolidated porous media.

De = Do 2 (1)

A more sophisticated method involves an analogy between electrical conductivity and diffusion in porous media. De

is related to the molecular diffusivity Do by equation 2:

De = Do F (2)

5

where F is the formation electrical resistivity factor . This expression can be used for cemented rocks as well as

2 SPE 113995

unconsolidated packs. The formation resistivity factor is a function of the porosity and can be estimated from Archies

relation:

F = m (3)

The exponent m is called the cementation factor and assumes different values in different packing. For unconsolidated sand

packs 6; the value of the cementation factor is 1.3 6. Although these relationships of effective diffusivity De and molecular

diffusivity Do give us an idea of how to evaluate diffusivity in porous media, more accurate methods need to be applied to

investigate the diffusivity of heavy oil and solvent system in porous media. In this work, an updated approach, which

considers porosity variation of porous media and volume changes on mixing, is used to determine the effective diffusion

coefficients. The relationship between the effective diffusivity of solvent in oil saturated sand pack and the molecular

diffusivity is investigated. With regard to the fluctuating (unsmooth) concentration profiles problem 7 in diffusion

experiments, which is caused by porosity variation of porous media, an updated data processing method will be mentioned

briefly, which can improve the quality of concentration profiles dramatically.

The inter-diffusion of two components in porous media is being studied considering porosity variation of porous media and

volume changes due to mixing. The rates at which the concentrations of the two components CA and CB change at a point are

given by

C A C A

= D A (v C A ) (4)

t x x x

C B C B

= D B (v C B ) (5)

t x x x

DA and DB are the intrinsic diffusion coefficients for component A and B; is porosity of porous media which varies

with location but not with time; and is the velocity of the mass-flow assumed to be in the x direction and dependent only on

the x coordinate and the time t.

Equations (4) and (5) are applicable in the absence of thermal motion or forced diffusion, but they can be applied in

the presence of porosity variation of porous media and volume changes on mixing. The diffusion process discussed is based

on the following assumptions:

z The system is contained in a static cell.

z The porosity variation of porous media in the major diffusion direction is considered.

z There are volume changes due to mixing.

z One-dimensional diffusion in x direction.

z Constant temperature and pressure.

There is a relationship between CA and CB at constant temperature and pressure which is:

VB CB + VA CA = 1 (6)

where the VA and VB are the partial specific volumes of the two components A and B 8. Both VA and VB can vary with the

concentration at certain temperature and pressure conditions. We also assume

(C B / C A ) P .T = V A / VB (7)

(v ) C V C A

= V A D A A VB DB A (8)

x x x x V B x

SPE 113995 3

2

C A x

C V C V C (9)

v = V A ( D A D B ) + B

D A + D B A A B A dx

x

CA V C

B B C A x

where v and CA/ x have been assumed zero at x = -. Substituting equation (9) into equations (4) and (5), we have:

C A C A x D VB C A

2

(10)

x x VB C A C A x

= D C

A dx

t x

CB CB x D VB C A

2

= D CB dx (11)

t x x x VB C A C A x

Equations (10) and (11) are the heterogeneous diffusion model used to describe the diffusion of solvent in heavy oil

saturated porous media, which considers porosity heterogeneity of porous media in the major diffusion direction and volume

changes on mixing. The second terms on the right-hand sides of equations (10) and (11) arise because of the volume changes

on mixing, and they vanish when such changes do not occur.

The initial and boundary conditions are

CA = 0, x = -, t>0 (15)

CA = C, x = , t>0 (16)

For bulk fluid (porosity is 1), D represents molecular diffusivity Do; for porous media (porosity is not 1), D

represents effective diffusivity De.

Because diffusivity is a function of concentration and porosity, equations (10) and (11) are nonlinear partial

differential equations, which can be solved numerically using MATLAB, MAPLE, et cetera, if porosity distribution, volume

change rule and diffusivity are known.

For homogeneous porous media, equation (10) and (11) can be simplified to:

CA CA x D VB CA

2

= D CA dx (17)

t x x x VBCA CA x

CB CB D VB CA

x 2

(18)

t x x x VBCA CA x

= D C

B dx

CA

CA

CA xdCA

1 dx VB (19)

D= xdCA + C AVB

0

2 dCA

2t dCA 0 0 C AVB

CA P,T

4 SPE 113995

To satisfy the boundary conditions, the following integral must be made equal to zero by adjusting the global

coordinate system for the bulk fluid motion.

CA

C C xdC A

V B

xdC + C V B dC A = 0 (20)

0

A

C A

2

0 0 C AV B P ,T

Equation (19) is applied when porosity variation of porous media can be neglected. The first term on the right-hand

side of equation (19) is the usual expression for calculating D from the concentration profiles when there is no volume

change on mixing; the second term is a correction term because of volume changes on mixing.

Small-scale experiments were designed to study the diffusion of solvents in heavy oil saturated sand packs. These

experiments were conducted in aluminum cylinders of 250 cm in volume (diameter: 4.5cm and height: 16cm), which can

bear high pressure. The diffusion process was monitored using a GE9800 CT scanner. X-ray tomography techniques were

employed to generate 2D images of the solvent-oil mixture. These scans were then averaged and converted to solvent and

bitumen concentration profiles, allowing for the calculation of the diffusion coefficients of hydrocarbon solvent in oil sands.

The procedure for the diffusion experiments was as follows; see Figure 1:

1. Mix dry sand and appropriate amount of heavy oil (dead oil) and then pack lower half of the aluminum cylinder with

the mixture.

2. Pack the upper half of the cylinder with dry sand.

3. Seal the cylinder with aluminum cap and evacuate it for 15 minutes.

4. The cylinder, filled with dry sand and oil saturated sand, was scanned.

5. Solvent was injected into the upper half of the cylinder containing dry sand.

6. The cylinder was scanned every 60 minutes for the first twelve hours and then every three hours for the duration of

the experiment.

For illustration purposes, Figure 2 shows CT images of a sand pack sample filled with solvent and heavy oil. It can be seen

that the higher density materials have higher CT number, which are presented in dark grey (heavy oil or lower porosity), and

those of lower density have lower CT number, which are shown in the figure in light grey (solvent or higher porosity).

The oil used in these experiments has a density of 0.978g/cm3 and viscosity of 12000cp at 25oC and the hydrocarbon

solvent considered here is heptane. The experiments were performed at atmosphere pressure and room temperature.

Aluminum shell

Sand + Solvent

As shown in Figure 1, multiple Regions of Interest (ROI) of the samples were selected in which porosity variation of the sand

pack is different. The following procedure was applied to analyze the scanned images for the solvent diffusion in heavy oil

saturated sand packs:

1. A Region of Interest (ROI) was cut and the porosity variation of the region was analyzed.

2. The CT number 9 of the ROI in the horizontal direction was averaged, therefore obtaining CT number profiles of the

mixture with height.

SPE 113995 5

3. Using the density CT number correlations for this specific scanner, the CT number profiles were converted to the

density profiles. The latter were then translated to concentration profiles using an updated approach, which considers

the porosity variation of sand pack at each location.

Using the above method, the quality of the concentration profiles in the sand pack was improved dramatically, as Figures 3-4

show, so the concentration data can be used to calculate the effective diffusion coefficient. This data processing method will

be discussed in a subsequent paper in details.

1

1

Oil concentration, volume fraction

oil concentration, volume fraction

0.8

0.8

0.6

0.6

0.4

0.4

0.2 0.2

0 0

-20.0 -15.0 -10.0 -5.0 0.0 5.0 10.0 15.0 20.0

-20.0 -15.0 -10.0 -5.0 0.0 5.0 10.0 15.0 20.0

location x, mm

Locationx, mm

Figure 3: Concentration profile at time 667 min Figure 4: Concentration profile at time 1502 min

In order to compare the results of effective diffusivity of solvent in heavy oil saturated sand and molecular diffusivity of bulk

fluids, same solvent and oil were used to conduct bulk diffusion experiments. In addition, equation (19), which considers

volume changes on mixing 3, was applied to determine the molecular diffusivity. In Figure 5, the concentration is expressed a

function of x / t1/2. The measured concentration values at various time lie on a single curve, which indicates that the mutual

diffusion coefficient depends on concentration only. As Figure 6 shows, the calculated molecular diffusivity is decreasing

monotonously with the increase of oil concentration, which is reasonable.

6 SPE 113995

0.8

0.6

216 min

341 min

0.4

96 min

0.2

0

-1 -0.5 0 0.5 1

x/SQRT(t), mm.min-0.5

1/2

Figure 5: Concentration dependence on x / t for bulk fluid diffusion

20.00

15.00

D, 10 cm /s

2

-6

10.00

5.00

0.00

0.1 0.3 0.5 0.7 0.9

Heavy oil concentration, volume fraction

By selecting a sample of sand pack with quite homogeneous porosity, the simplified diffusion equation (19) can be

used to evaluate the effective diffusivity of solvent in heavy oil saturated sand. Figure 7 shows the porosity distribution inside

the selected ROI. We can see a very small porosity variation: 0.483-0.502. At the same time, for this homogeneous sample,

porosity variation should still be considered to process experimental data and obtain reasonable concentration profiles,

because that sand density is much higher than liquid density. Figure 8 is the concentration dependence on x / t1/2 for this

homogeneous sample. In Figure 9, the effective diffusivity and molecular diffusivity are compared. It is true that the

tortuosity of porous media influences greatly the diffusivity of fluids inside the pores. Applying the empirical correlations (1)

and (2), the relationship between De and Do is evaluated, as Figure 10 shows. Equation (1) is not applicable for

unconsolidated oil sand; Equation (2) is more suitable and the cementation factor m 1.0 instead of 1.3 for sand packs.

SPE 113995 7

0. 51

Porosity, fraction

0. 5

0. 49

0. 48

0 5 10 15 20 25 30 35

location x, mm

For heterogeneous samples, the more sophisticated diffusion equation (10) should be used to determine the effective

diffusivity of solvent in heavy oil saturated sand, which considers the porosity heterogeneity in the main diffusion direction x

and volume changes on mixing. In order to evaluate the diffusivity of solvent in oil sands using diffusion equation (10), the

following procedure can be used:

1. Find the porosity distribution in the main diffusion direction.

2. Suppose a function of diffusivity D = f (C,) which contains unknown coefficients, for example: D = Do *m. For the

same solvent and heavy oil, Do is a known function of concentration (Figure 9); m is an unknown index.

3. Solve the nonlinear partial differential equation (5) numerically using MATLAB to obtain concentration profiles at

different times.

4. Compare the calculated concentration and experimental data and optimize index m to minimize the mean square

deviation of calculated concentration with respect to experimental data.

Figure 11 shows the porosity distribution of the sand pack in this sample along the main diffusion direction, which

cannot be neglected (porosity is 0.45-0.55). Through minimizing the mean square deviation of calculated concentration with

respect to experimental data, the optimized value of index m 1, which conforms the above result. Figure 12 shows an

example of the comparison between experimental data and calculated concentration using numerical solution of

heterogeneous diffusion model (10).

8 SPE 113995

0.8 667 min

1502 min

0.6 1010 min

0.4

0.2

0

-0.6 -0.4 -0.2 0.0 0.2 0.4

x/SQRT(t), mm.min-0.5

1/2

Figure 8: Concentration dependence on x / t for diffusion in homogeneous sand pack 2

20.00

D, 10 cm /s

2

Molecular diffusivity

-6

10.00

5.00

0.00

0.1 0.3 0.5 0.7 0.9

Heavy oil concentration, volume fraction

Figure 9: Comparison of effective diffusivity and molecular diffusivity for homogeneous sand pack 2

10.00

homogeneous model

8.00

effective diffusivity using correlation 1

D, 10 cm /s

2

-6

4.00

2.00

0.00

0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9

Heavy oil concentration, volume fraction

Figure 10: Comparison of effective diffusivity using different models for homogeneous sand pack 2

SPE 113995 9

0.56

0.54

Porosity, fraction

0.52

0.5

0.48

0.46

0.44

0.42

0 5 10 15 20 25 30

location x, mm

Oil concentration, volme fraction

1

numerical method (m=1)

0.8 Experimental data

numerical method using correlation (1)

0.6

0.4

0.2

0

-16 -12 -8 -4 0 4 8 12

Location x,mm

Figure 12: Comparison of concentration profiles using different methods for heterogeneous

sample (t = 667 min)

Conclusions

1. The molecular diffusivity in bulk fluids is decreasing monotonously with the increase of oil concentration.

2. Concerning the relationship between the effective diffusion coefficient of solvent in oil saturated sand pack and the true

diffusion coefficient in bulk fluids, correlation (1) is not applicable for unconsolidated sand packs; correlation (2) is

suitable and the cementation factor m is around 1.0 instead of 1.3 for sand packs.

3. The impact of porosity heterogeneity of porous media on the diffusion of fluids inside equations is significant when the

porosity heterogeneity is not negligible.

10 SPE 113995

Acknowledgements

The authors wish to acknowledge the contributions of the staff at the Tomographic Imaging and Porous Media Laboratory.

The authors are also grateful to ISEEE and the sponsoring companies of the Canada Research Chair in Energy and Imaging

(Shell, Nexen, Canadian Natural, Devon Canada, Petro-Canada, E-T Energy, Suncor, Schlumberger, Laricina, Paramount,

CMG foundation and Conoco Phillips) for financial support.

Nomenclature

CA = Concentrations of the component A (g/cm3)

CB = Concentrations of the component B (g/cm3)

CTn = CT number

D= Mutual diffusion coefficient (cm2/s)

DA = Intrinsic diffusion coefficients for component A (cm/s)

DB = Intrinsic diffusion coefficients for component B (cm/s)

De Effective diffusivity in the porous medium (cm2/s)

Do Molecular diffusivity in bulk fluids (cm2/s)

F Formation electrical resistivity factor

ROI = Region of interest

t= Time (s)

VA = Partial specific volumes of component A (cm3/g)

VB = Partial specific volumes of component B (cm3/g)

x= Space coordinate measured (cm)

= x / (2t1/2)

= Velocity of the mass-flow (cm/s)

Porosity of porous media

Cementation factor

References

1. Nasr T.N. and Ayodele O.R.: New Hybrid Steam-Solvent Processes for the Recovery of Heavy Oil and Bitumen, SPE 101717, 2006

International Petroleum Exhibition and Conference, Abu Dhabi, U.A.E., Nov 5-8.

2. Oballa, V. and Butler, R.M.: An experimental Study of Diffusion in the Bitumen-Toluene System, J. Can. Pet. Tech. (Mar 1989),

28(2), pg. 63.

3. Luo, H., Salama, D., Kryuchkov, S. and Kantzas, A.: The Effect of Volume Changes Due to Mixing on Diffusion Coefficient

Determination in Heavy Oil and Hydrocarbon Solvent System, SPE 110522, 2007 SPE Annual Technical Conference and Exhibition,

Anaheim, California U.S.A., Nov 1114.

4. Collins, R.E.: Flow of Fluids through Porous Materials, PennWell Publishing Co., Tulsa, Oklahoma USA, (1976), pg. 209.

5. Perkins, T.K. and Johnson, O. C.: A Review of Diffusion and Dispersion in Porous Media, SPE Journal, (1963), pg.70.

6. Pirson, S.J.: Oil Reservoir Engineering, 2nd edition, McGraw Hill Book Company, New York, (1958), pg. 106.

7. Salama, D., Kantzas, A.: Monitoring of Diffusion of Heavy Oils with Hydrocarbon Solvents in the Presence of Sand, SPE/PS-

CM/CHOA 97855, 2005 SPE International Thermal Operations and Heavy Oil Symposium, Calgary, AB Canada, Nov 1-3.

8. Crank, J.: The Mathematics of Diffusion, 2nd edition, Clarendon Press, Oxford, (1975), pg. 234.

9. Kantzas, A.: Investigation of Physical Properties of Porous Rocks and Fluid Flow Phenomena in Porous Media Using Computer

Assisted Tomography, In Situ, (1990), 14(1), pg. 77.

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