Determination of Gas-Diffusion and
Interface-Mass-Transfer Coefficients for
Quiescent Reservoir Liquids
Faruk Civan, SPE, and Maurice L. Rasmussen, U. of Oklahoma
Summary
A physically and mathematically rigorous transient-state equilib-
rium diffusion model is applied for simultaneous determination of
the gas-diffusion and interface-mass-transfer coefficients from
pressure decline by dissolution of gas in quiescent liquids involv-
ing petroleum reservoirs. The short- and long-time analytical so-
lutions of this model are reformulated to enable direct determina-
tion of the best-estimate values of these parameters by regression
of experimental data. Typical experimental data are then analyzed
by means of the present improved methods, and the values ob-
tained are compared with the reported values. The present meth-
odology is proven practical and yields unique and accurate param-
eter values.
Introduction
Gas-diffusivity and interface-mass-transfer coefficients are impor-
tant parameters determining the rate of dissolution of the injection
gases in oil during secondary recovery, and the rate of dissolution
and separation of light gases in reservoir oil and brine, water ta-
bles associated with depleted-reservoir gas storage, drilling mud,
and completion fluids (Hill and Lacey 1934, O’Bryan et al. 1988,
O’Bryan and Bourgoyne 1990, Bodwadkar and Chenevert 1997,
Bradley et al. 2002, Liu and Civan 2005). In order to develop
proper gas-injection strategies, accurate values of these parameters
are required for reservoir simulation and prediction of oil re-
covery by miscible flooding and the optimization of miscibility for
best recovery.
Laboratory measurement of gas diffusivity in quiescent liquids
is usually accomplished through the measurement of the pressure
of gas in contact with certain liquids, such as oil, brine, drilling
mud, and completion fluids in a closed PVT cell (see Fig. 1)
during gas dissolution in the liquid phase. The accuracies of the
available models, including those by Riazi (1996), Sachs (1997,
1998), and Zhang et al. (2000), are limited by the inherent sim-
plifying assumptions involved in the analytic treatment and the
subsequent interpretation of such experimental data. As judged by
the reported studies, there appears to be no consensus among the
available analytical approaches used for diffusivity measurement.
In addition, the previous studies focused mostly on the determi-
nation of gas diffusivity and did not account for interface-mass-
transfer effects. The methodology offered by Civan and Rasmus-
sen (2001, 2002, 2003), and further elaborated in the present paper,
allows for both interface mass-transfer effects and for bulk diffu-
sivity. It is a novel and practical approach that determines param-
eters describing both effects from a given set of pressure-decline
data.
The best estimate of the coefficient of diffusion of gas species
(solute) in a given liquid medium (solvent) is usually inferred
indirectly by matching the prediction of a suitable mathematical
model involving the species transfer by diffusion to experimental
data under prescribed conditions. For this purpose, Sachs (1998)
resorts to the numerical solution of the nonlinear model equations
Copyright © 2006 Society of Petroleum Engineers
This paper (SPE 84072) was first presented at the 2003 SPE Annual Technical Conference
and Exhibition, Denver, 5–8 October, and revised for publication. Original manuscript re-
ceived for review 11 February 2004. Revised manuscript received 24 August 2005. Paper
peer approved 11 September 2005.
March 2006 SPE Journal
incorporating the dependency of the diffusion coefficient on con-
centration without clearly describing the boundary conditions used
in the solution. However, simplified analytical solutions obtained
under special conditions can provide convenience and are there-
fore advantageous. For example, Zhang et al. (2000) have deter-
mined the diffusion coefficient for gas diffusing into heavy oil
using a transient-state diffusion model. Their interpretation tech-
nique is based on the measurement of the gas-pressure decline
during the dissolution of gas in a certain amount of oil. This allows
for determination of the amount of gas dissolved in the liquid
phase, which is then used as the gas/liquid-interface boundary
condition in the liquid phase dissolving-gas species transfer model
to determine the diffusion coefficient.
The reported diffusion coefficients are significantly different
from each other. This signals some inadequacies involved in the
interpretation methods used to analyze experimental data. For ex-
ample, Zhang et al. (2000) use an improper gas/liquid interface-
boundary condition assuming a fixed saturation gas concentration
value for the liquid phase near the interface to be attained only
when the final equilibrium pressure is reached. They also consid-
ered a constant value for the real-gas deviation factor, although it
might deviate significantly from the unity at elevated pressures.
When additional errors are introduced for convenience in the pa-
rameter estimation by invoking lower-order functional approxima-
tions, the reliability and accuracy of the value of the gas-diffusion
coefficient become ambivalent. Upreti and Mehrotra (2002) cor-
rectly considered that the instantaneous saturation gas concentra-
tion of the liquid near the interface varies as the applied gas pres-
sure varies by gas dissolution in the liquid phase.
Civan and Rasmussen (2001, 2002, 2003) applied the general
interface flux continuity condition (Robin boundary condition).
Tharanivasan et al. (2004) determined that this condition yields the
best result in determination of the diffusion coefficient for the
CO2/oil system, but the value of the diffusion coefficient for the
CH4/oil system was insensitive to the choice of the interface
boundary condition. It should be emphasized that the flux conti-
nuity is a general interface condition that simplifies to the point
value condition (Dirichlet boundary condition) considered in their
study as the interface-mass-transfer coefficient assumes a suffi-
ciently large value.
This paper presents some extensions over the previous Civan
and Rasmussen (2001, 2002, 2003) studies. Physically and math-
ematically rigorous improved models, considering equilibrium
diffusion-gas transport in a nonvolatile liquid phase and resistance
of the gas/liquid interface to gas dissolution, are presented and
solved analytically under various conditions. A practical regres-
sional procedure is developed for accurate estimation of the gas-
diffusivity coefficient and the interface-mass-transfer coefficient
by fitting the combined short- and long-time analytical solutions to
experimental data by the method of least-squared error. Various
experimental data are analyzed by means of the present method,
and the diffusion coefficients obtained are compared with those of
previous studies.
General Formulation
Following Zhang et al. (2000), consider the schematic experimen-
tal setup, shown in Fig. 1, operating at isothermal conditions. We
consider a nonvolatile quiescent liquid brought into contact with a
high-pressure pure gas instantly at isothermal conditions. The gas
71
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 Thus, substituting Eqs. 1 through 3 into Eq. 6 leads to the follow-
ing operating equation for the gas phase:
MgH po p
−
RT Zo Z 冋 册
= Q, t ⬎ 0. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (7)

Note that Eq. 7 is different from that of Zhang et al. (2000) be-
cause they assumed a constant real-gas deviation factor value
Z⳱Zo at an initial po gas pressure.
An alternative expression to Eq. 6 for Q can be derived. Let
c(x,t) be the concentration (mass per unit volume) of the gas that
is dissolved in the liquid phase, and let co be its initial value. Then
Q can be expressed as

兰 兰 冋c冉 L , t 冊 − c 册d冉 L 冊, . . . (8)

L 1 x x
Q共t兲 = 关c共x,t兲 − co兴dx = L o
0 0

where L is the height of the liquid column which varies with time
when the gas/liquid solution swells by gas dissolution [i.e.,
L⳱L(t)]. The function Q(t) can be interpreted as the average gas
accumulation in the liquid-phase region, measured per unit area
of cross section.

Gas/Liquid Solution Equations. The mass concentration c and

Fig. 1—Schematic PVT cell used for measurement of gas diffu-
sivity in liquids.
and liquid are referred to as components, and the mixture of the gas
and liquid obtained by dissolution of gas in the liquid is referred to
as a gas/liquid solution. The formulation is presented for gas solu-
bility in a nonvolatile quiescent liquid.
Gas-Phase Equations. The gas properties are considered uniform
and in thermodynamic equilibrium throughout the gas phase. Be-
cause the gas phase is a single-component system, the mass density
␳g of the gas is determined by the real-gas thermal equation of state:
mass fraction w of the gas component in the gas/liquid solution are
related by
c = ␳w, . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (9)
where ␳ denotes the density of the gas/liquid solution. The dis-
solved gas concentration can be also expressed in terms of the
molar concentration X denoting the mole fraction of the dissolved
gas in the gas/liquid solution as
c Ⲑ Mg
X= , . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (10)
␳ⲐM
where M denotes the molecular weight of the gas/liquid solution.
Gas dissolution causes the swelling of the liquid phase (Hill
and Lacey 1934, O’Bryan and Bourgoyne 1990). The variation of
the liquid-phase density by gas dissolution can be expressed by
means of the following isothermal coefficient of expansion at a
prescribed temperature T:

冉 冊
Mgp
␳g = , . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (1) 1 ⭸␳
ZRT ␤=− . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (11)
␳ ⭸w T
where Mg denotes the molecular weight; p and T are the pressure
and temperature of the gas, respectively; R is the universal gas Hill and Lacey (1934) corrected the diffusion-coefficient value
constant; and Z⳱Z(p,T) represents the real-gas deviation factor, for the effect of liquid expansion by swelling caused by gas dis-
correlated empirically as a function of pressure and temperature. solution using the empirical relation
The volume V and mass m of the gas phase are given by
D = Do共1 − X兲2, . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (12)
V = AH . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (2)
where Do is the uncorrected apparent diffusivity, and D is the
m = ␳gV, . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (3) diffusivity value corrected for expansion of volume during gas/
liquid solution swelling.
where A and H denote the cross-sectional area of the test tank and Riazi (1996) and Sachs (1997, 1998) expressed the diffusion
the length of the gas column, respectively. The thickness of the gas coefficient for nonideal mixtures as a function of the species con-
phase varies with time when the gas/liquid solution swells by gas tent in the liquid solution according to
dissolution [i.e., H⳱H(t) ]. If J denotes the mass flux of the gas
diffusing from the gas phase into the liquid phase at the gas/liquid
interface, the gas-phase mass balance is given by D = Do 1 + 冉 ⭸ ln ␾
⭸ ln X 冊
, . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (13)

dm
= −A J|x=0 , t ⬎ 0, . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (4) where ␾ denotes the fugacity coefficient of the dissolving gas in
dt
the solution.
where t is time. The initial gas mass is given by The equation of continuity for the liquid/gas solution undergo-
m = mo, t = 0 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (5) ing swelling caused by gas dissolution is given by

Hence, integrating Eq. 4 with Eq. 5 yields ⭸␳ ⭸共u␳兲

+ = 0, 0 ⱕ x ⱕ L共t兲, t ⬎ 0 . . . . . . . . . . . . . . . . . (14)
⭸t ⭸x
t
mo − m
A
= 兰 J|
0
x=0 dt = Q, t ⬎ 0, . . . . . . . . . . . . . . . . . . . . . . . . . (6) The conservation of the dissolved gas mass in the liquid/gas so-
lution is given by

where Q denotes the cumulative mass of gas dissolved in the liquid ⭸c ⭸共uc兲 ⭸J
+ + = 0, 0 ⱕ x ⱕ L共t兲, t ⬎ 0 . . . . . . . . . . . . . (15)
phase per unit cross-sectional area of the gas/liquid interface. ⭸t ⭸x ⭸x

72 March 2006 SPE Journal

 The constitutive equation for mass flux of the dissolved gas J The sealed tank bottom condition is (Neumann condition)
is given by Fick’s law as
⭸c
⭸w ⭸共c Ⲑ ␳兲 = 0, x = L, t ⬎ 0. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (26)
⭸x
J = −␳D = −␳D , 0 ⱕ x ⱕ L共t兲, t ⬎ 0, . . . . . (16)
⭸x ⭸x Note that as k→⬁, the Robin-type Eq. 24 simplifies to the case for
where D is the coefficient of diffusion. the surface Dirichlet-type boundary condition, given by
c = c*, x = 0, t ⬎ 0. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (27)
Conditions of Solution. The initial conditions are given by
For convenience in the analysis, we define the dimensionless con-
c = co, J = 0, 0 ⱕ x ⱕ L, t = 0. . . . . . . . . . . . . . . . . . . . (17) centration, distance, and time, respectively, as follows:
The velocity of the interface of the gas/liquid solution, moving c − co
cD = . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (28)
because of solution swelling by gas dissolution, is given by, con- c* − co
sidering that the height of the PVT-cell is a constant,
x
dL共t兲 dH共t兲 xD = . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (29)
L
uL共t兲 = =− . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (18)
dt dt Dt
tD = . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (30)
The total and gas component jump mass balances across the gas L2
and gas/liquid solution interface are given by
Consequently, Eqs. 22 through 26 can be transformed into the
␳g共ug − uL共t兲兲 = ␳共u − uL共t兲兲 = c共u − uL共t兲兲 + J, . . . . . . . . . . . . . (19) following dimensionless forms, respectively:
where u is the mass-weighted average velocity and J represents the ⭸cD ⭸2cD
= , 0 ⱕ xD ⱕ 1, tD ⬎ 0 . . . . . . . . . . . . . . . . . . . . . (31)
mass flux of the gas component. ⭸tD ⭸xD2
The value of the diffusing-gas mass flux J|x⳱0 at the gas/liquid
interface, as well as the concentration c of the gas that has been cD = 0, 0 ⱕ xD ⱕ 1, tD = 0 . . . . . . . . . . . . . . . . . . . . . . . . . (32)
absorbed by the liquid, can be determined by solving the transient- ⭸cD
state gas-diffusion model for the gas/liquid solution. − = k 共1 − cD兲, xD = 0, tD ⬎ 0 . . . . . . . . . . . . . . . . . . . (33)
The gas/liquid-interface resistive or hindered gas mass-transfer ⭸xD D
boundary condition is given by cD = 0, xD → ⬁, tD ⬎ 0, . . . . . . . . . . . . . . . . . . . . . . . . . . . (34)
J|x=0 = k共c* − c兲, x = 0, t ⬎ 0, . . . . . . . . . . . . . . . . . . . . . . (20) or
where k is the film mass-transfer coefficient at the gas/liquid in- ⭸cD
= 0, xD = 1, tD ⬎ 0. . . . . . . . . . . . . . . . . . . . . . . . . . . . (35)
terface. The symbol c* denotes the saturation or equilibrium gas ⭸xD
concentration of the liquid phase. The sealed boundary condition
The parameter kD appearing in Eq. 33 can be referred to as a
prevailing at the bottom of the test tank is given by
mass-transfer Biot number because of its analogy with heat-
J = 0, x = L, t ⬎ 0. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (21) transfer problems. It is given by
kD ≡ kL ⲐD. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (36)
Equilibrium Transport Model
The mass-accumulation function Q(t) can be expressed in terms
For all practical purposes, the equilibrium model presented here is
of the nondimensional variables as
applicable to the laboratory tests conducted using the conventional
PVT cells. The solutions for the nonequilibrium gas transport in Q共t兲 = L共c* − co兲QD共tD兲, . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (37)
the gas/liquid solution are presented elsewhere by Civan and Ras-
where QD(tD) is the average of the gas concentration in the gas/
mussen (2001, 2002, 2003). The latter may be important for tests
liquid solution:
involving the sudden contact of significantly high-pressure gases
兰 c 共x ,t 兲dx . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (38)
with liquids, which do not allow sufficient time to attain the equi- 1
QD共tD兲 = D D D D
librium diffusion conditions. 0

Eq. 7 can now be written in nondimensional terms as

冋 册
Mathematical Model. The gas/liquid mixture is very dilute in
typical laboratory tests. Therefore, we assume an ideal solution MH po p
− = QD共tD兲. . . . . . . . . . . . . . . . . . . . . . . (39)
and omit the nonideal solution correction term appearing in Eq. 13. RTL共c* − co兲 Zo Z
Consequently, we neglect the swelling effect, assume an incom-
pressible gas/liquid solution, and take a constant diffusion coeffi- Next, Eq. 39 is applied at any conveniently selected reference
cient (i.e., D≅constant). Then, Eqs. 11 through 14 are no longer pressure value pr measured at a dimensionless time tDr to obtain
needed, and Eqs. 15 and 16 can be manipulated to eliminate J to
obtain
MH po pr
−
RTL共c* − co兲 Zo Zr 冋 册
= QD共tDr兲. . . . . . . . . . . . . . . . . . . . . . (40)

⭸c ⭸2c Then, Eqs. 39 and 40 can be combined as

= D 2, 0 ⱕ x ⱕ L, t ⬎ 0. . . . . . . . . . . . . . . . . . . . . . . (22)
⭸t ⭸x po p共tD兲
−
The initial condition is QD共tD兲 Zo Z共tD兲
= . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (41)
QD共tDr兲 po pr
c = co, 0 ⱕ x ⱕ L, t ⬎ 0. . . . . . . . . . . . . . . . . . . . . . . . . . . (23) −
Zo Zr
The gas/solution interface condition is (Robin condition) This is the key equation for determining the diffusion coefficient D
⭸c and the film mass-transfer coefficient k at the gas/liquid interface
−D = k共c* − c兲, x = 0, t ⬎ 0. . . . . . . . . . . . . . . . . . . . . (24) experimentally. The terms on the right are to be determined by
⭸x measurement of pressure at a given temperature as a function of
The infinite-distance condition is (Dirichlet condition) time, and correlated with the function on the left that is to be
established theoretically using the analytical solutions described in
c = co, x → ⬁, t ⬎ 0. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (25) the next section.

March 2006 SPE Journal 73

 Alternatively, let us suppose that equilibrium obtains after an
effectively long time and that p equals p*, the equilibrium pres-
sure, then QD(t*D)⳱1.0. Thus, if we choose the previously men-
tioned reference pressure value as pr⳱p*, then Eq. 41 can be
written as
po p共tD兲
−
Zo Z共tD兲
QD共tD兲 = . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (42)
po p*
− When the expression in Eq. 47 for cD is substituted into Eq. 38 for
Zo Z*
The expression given by Eq. 42 is convenient over Eq. 41 when the
diffusion test can be carried out until the equilibrium condition is
attained. In the following sections, we apply Eq. 42. However,
Eq. 41 should be used when the tests require a very long time to
reach equilibrium.
Analytical Solutions. In the following treatise, the binary-mixture
gas-diffusivity coefficient D in the gas/liquid solution and the in-
terface-mass-transfer coefficient are determined by solving Eqs. 31
together with the initial and boundary conditions in Eqs. 32
through 34 for short-time (semi-infinite) or Eq. 35 for long-time
(finite-length) for the equilibrium gas transport in the gas/liquid
solution with the results tested against typical experimental data.
Short-Time (Semi-Infinite) Solution (L→ⴥ). Civan (1997,
1999, 2000a, 2000b) applied the analytical solutions for semi-
infinite regions given by Crank (1956) successfully for determi-
nation of the best estimates of the diffusion coefficients in a variety
of problems. These analytical solutions can be applied for the
present case as follows:
冋 冑册
1 tD
QDST共tD兲 = exp共kD2 tD兲erfc共kD公tD兲 − 1 + 2kD
kD
As the mass-transfer Biot number kD→⬁, Eq. 43 simplifies to
QDST共tD兲 = 2 冑 tD
␲
. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (44)
This is the result that would have been obtained if the Dirichlet-
type boundary condition (Eq. 27) had been imposed at the interface.
Strictly speaking, the length L cancels out of the problem for
semi-infinite regions. Thus, these results are more appropriately
regarded as small-time approximations. These special solutions
can be used when the diffusion coefficient is sufficiently low and/
or the test time is sufficiently short that the diffusing gas cannot
effectively reach the bottom of the test tank. The result by Eq. 43
can be obtained formally from the small-time inversion of the
Laplace-transform analysis for the finite-length gas/liquid column
(Civan and Rasmussen 2001, 2002, 2003).
The short-time solution (Eq. 43) itself has two time ranges
embedded within it that are of interest. For very small times,
Eq. 43 can be expanded for small z ⳱ kD√tD to obtain
冋 册
1 2 4 z4 8 z6
QDST共tD兲 ≅ z − z3 + − z5 + + . . . , z → 0
kD 3公␲ 2 15公␲ 6
. . . . . . . . . . . . . . . . . . . . . . . . . . (45)
Thus, for finite kD, when QD is plotted against √tD, the initial slope
is always zero.
On the other hand, when tD is very large, the short-time ap-
proximation by Eq. 43 approaches the asymptote
冑
tD 1
QDST共tD兲 ≅ 2 − , kD公tD → ⬁. . . . . . . . . . . . . . . . . . (46)
␲ kD
In practice, the large-time behavior of the short-time approxima-
tion applies to some midrange of the overall time variation. Thus,
when QD is plotted against √tD,we might expect some midrange
portion of the curve to be nearly parallel to, or coincident with, the
straight-line asymptote by Eq. 46.
Long-Time (Finite-Length) Solution. When the length L is
finite, a Fourier series analytical solution can be obtained (Walas
74
1991) that is essentially valid for large times and impractical for
small times, given by
⬁
sin ␭m
cD = 1 − 4 兺 2␭
m=1 m + sin共2␭m兲
exp共−␭m2 tD兲 cos关␭m共1 − xD兲兴 , . . (47)
where ␭m denotes the roots of
␭m tan ␭m = kD. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (48)
QD and the integration carried out, the result is
⬁
sin2 ␭m
兺␭
2
QD共tD兲 = 1 − 4 e−␭mtD. . . . . . . . . . . . (49)
m=1 m 关 2␭m + sin共 2␭m 兲兴
The complete infinite series satisfies the relation QD (0)⳱0. The
same result is found when the time integral of the mass-flux term
is used in accordance with Eq. 6.
When the time tD is large, only the leading term in the infinite-
series solution is significant, and we have
2
QDLT共tD兲 = 1 − Q1共␭1兲e−␭1tD, . . . . . . . . . . . . . . . . . . . . . . . . . . . . (50)
where
4 sin2 ␭1
Q1共␭1兲 ≡ . . . . . . . . . . . . . . . . . . . . . . . . . . . (51)
␭1关2␭1 + sin共2␭1兲兴
This is known as the long-time approximation. The parameter ␭1
is the smallest positive root of the transcendental equation ␭1 tan
␭1⳱kD. The upper bound ␭1⳱␲/2 corresponds to kD→⬁, which in
turn corresponds to the case for the surface Dirichlet-type bound-
ary condition of Eq. 27.
. . . (43) It is interesting and useful to note that taking the natural loga-
␲
rithm of Eq. 50 leads to the result
ln关1 − QDLT共tD兲兴 = ln关Q1共␭1兲兴 − ␭21tD. . . . . . . . . . . . . . . . . . . . . (52)
Thus, plotting the natural logarithm of [1-QD LT
(tD)] against tD
produces a straight-line curve. This suggests a method for extract-
ing the two unknown coefficients D and k associated with a given
set of pressure-decline data.
Test-Data Analysis and
Interpretation Methodology
The objective is to interpret experimental data and infer from it the
values of the diffusion coefficient D and the interface-mass-
transfer coefficient k. When a given set of data is plotted on one
coordinate vs. another, the nature of the coordinates can make a
difference in the insight that the plot provides.
We wish to use the short-time approximation by Eq. 43 to-
gether with the long-time approximations, either in the form of Eq.
50 or in its counterpart logarithmic form of Eq. 52, to analyze data
generated over the whole time range in the form of QD vs. time t
stemming from the pressure-decline relation (Eq. 42). The reason
this is possible is that, whereas the short-time approximation is
basically valid for short times but fails for very large times, and
because the long-time approximation is basically valid for long
times but fails for very small times, they share a common inter-
mediate-time overlap region in which they are both valid (Civan
and Rasmussen 2001, 2002, 2003). (See Figs. 2 through 5.) In QD
vs. √tD, this overlap region is asymptotic to, and nearly coincides
with, the straight line given by Eq. 46. Plots of QD vs. √tD em-
phasize the short time. On the other hand, plots of ln(1-QD) vs. tD
[or log(1-QD) vs. tD] emphasize the long time. The long-time
approximation (Eq. 52) is characterized by a straight line on the
semilog plots.
An important factor to consider is that the experimental data
are plotted as a function of the real time t and not the non-
dimensional time tD. Thus, in the theoretical formulas we must
make the substitution
t
tD = , . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (53)
C
March 2006 SPE Journal
 Fig. 3—ln(1–QD)–t plot of the CH4-n-pentane data of Riazi (1996)
Fig. 2—QD–t1/2 regression of the CH4-n-pentane data of Riazi
emphasizing the long-time behavior.
(1996) showing short- and long-time approximations used in
parameter determination.

where the coefficient C has the dimensions of time and is given by D = QD

QLT LT
冉 冊
t
;␭
C 1
. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (56)

C = L2 Ⲑ D. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (54)
Thus the theoretical formulas cannot be plotted against the experi-
mental data unless C is specified arbitrarily or developed by some
systematic means. Therefore, the short-time and long-time ap-
proximations Eqs. 43, 50, and 52 are more appropriately expressed
functionally as
␭21
D 兲 = ln关Q1共␭1 兲兴 −
ln共1 − QLT t. . . . . . . . . . . . . . . . . . . . . . . . . (57)
C
As a result, these functions depend on two parameters, C and ␭1.
Now, suppose that the data are given at n discrete points des-
ignated by i going from 1 to n: QDi vs. ti. After plotting the data
vs. √t and on the semilog plots, pick a point im that separates the

D = QD
QST ST
冉 冊t
; ␭ . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (55)
C 1
short-time data from the long-time data (e.g., a point near the
crossover or the intersection of the short- and long-time curves),
and form the following squared-error functions:

Fig. 4—QD-t1/2 regression of the CO2/oil data of Zhang et al.

(2000) showing short- and long-time approximations used in Fig. 5—ln(1–QD)–t plot of the CO2/oil data of Zhang et al. (2000)
parameter determination. emphasizing the long-time behavior.

March 2006 SPE Journal 75

 兺冋 冉 冊册
im
ti 2 bLTL2
E ST共C, ␭1兲 = QDi − QDST ,␭ . . . . . . . . . . . . . . . . . (58) D= . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (70)
i=1 C 1 0.4343␭21

兺冋 冉 冊册
n
ti 2 The value of kD is calculated by Eq. 48:
E LT共C, ␭1兲 = QDi − QDLT ,␭ . . . . . . . . . . . . . . . . . (59) kD = ␭1 tan ␭1. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (71)
i=im C 1
Finally, with kD and D now known, the interface-mass-transfer
E 共C, ␭1兲 = E ST共C, ␭1兲 + E LT共C, ␭1兲. . . . . . . . . . . . . . . . . . . . . (60) film coefficient k can be determined:
Minimizing the function E determines the best estimate values of D
the two parameters C and ␭1 for the least-squared error over the k= k . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (72)
combined short- and long-time behaviors. L D

Identification of the Short- and Long-Time Regions. Often it is

Analysis of the Asymptotic Long-Time Behavior for the Short
difficult to draw accurate tangents to the curve of data when the
Time. The straight-line character of the curves for asymptotic
measured data involve large experimental errors. We select the
long-time behavior for the short-time solution on QD(tD) vs. √t
region of measured data points to construct the straight-line plots
plots (see Fig. 2) suggests a systematic method for extracting the
of the asymptotic long-time behavior for the short-time solution
values of the diffusion coefficient D and the interface-film coef-
Eq. 61 and the long-time solution Eq. 65 in a manner to yield the
ficient k from the data associated with a given physical experiment.
same values for the diffusion coefficient and the Biot number. This
By means of Eq. 46, this relation can be expressed as
is accomplished by equating Eqs. 70 and 63 to yield the same value
QD共tD兲 = −aST + bST公t, . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (61) for the diffusivity coefficient. Hence, the slopes of the straight
lines for the short- and long-time data are related by
in which the intercept and slope of the straight line are given by
0.4343␲␭21 2

aST =
1
,b =
kD ST L
2
冑 D
␲
. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (62)
bLT =
4
bST. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (73)

Eq. 73 is used as guidance for identification of the range of the

Therefore, the diffusion coefficient D and interface-mass-
transfer coefficient k can be calculated from Eqs. 62 and 63, re-
spectively, as follows:
␲L2bST
2
D= . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (63)
4
D D
k= kD = . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (64)
L LaST
Analysis for Large Times. The straight-line character of the
curves for large times on semilog plots (see Fig. 3) suggests a
systematic method for extracting the values of the diffusion coef-
ficient D and the interface-film coefficient k from the data asso-
ciated with a given physical experiment. When the large-time ap-
proximation Eq. 50 using Eq. 51 is expressed in terms of the actual
time t, the data can be correlated with a straight line by means of
a regression analysis in the form of
log10共1 − QD兲 = −aLT − bLTt, . . . . . . . . . . . . . . . . . . . . . . . . . . . (65)
where the y-axis intercept and the slope of the line, measured per
unit time, are given, respectively, by
short- and long-time experimental data.
Sources of Errors in Parameter Values
The construction of straight-line correlation of the short- and long-
time data and calculation of the diffusion coefficient D and mass-
transfer coefficient k from experimental data using the present
method may be subject to various errors.
Simplifying Assumptions. The value of the mass-transfer Biot
number was assumed to remain constant throughout the diffusion
process and the effect of swelling caused by gas dissolution was
neglected in order to be able to derive the analytic solutions used
in the calculations. In reality, the values of the phenomenological
parameters might vary and cause errors. Further, we considered
gas diffusion in quiescent liquids. However, change of density in
the gas/liquid solution may cause a convective mixing phenom-
enon, which may affect the gas-diffusion rate.
Equilibrium Pressure. The value of the gas pressure at equilib-
rium p* should be measured directly by conducting tests over a
sufficiently long time until the equilibrium pressure is attained.
Eq. 42 suggests that this value can be estimated by extrapolating
the plot of the measured gas pressure against time for long

o 共␭1 兲兴 = −log
aLT = −log关QLT 再 4 sin2共␭1兲
␭1 关2␭1 + sin共2␭1兲兴
冎 . . . . . . . . (66)
time. However, extrapolation of experimental data beyond the
measured range may introduce significant error. Nevertheless, this
problem can be alleviated readily either by applying Eq. 41 to use
D only the values measured during a diffusion experiment terminated
bLT = 0.4343␭21 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (67) without waiting until equilibrium or Eq. 42 to use a directly mea-
L2 sured equilibrium pressure value when a diffusion test is continued
Eq. 66 allows ␭1, and thus kD by virtue of the relation ␭1 tan until equilibrium.
␭1⳱kD given by Eq. 48, to be determined. Consequently, the
mass-transfer Biot number kD is determined entirely by the y-axis Digitizing Reported Data. The numerical values of the experi-
intercept. The maximum value of a occurs for the limiting case mental data analyzed in this study were obtained by digitizing the
kD→⬁ and ␭1⳱␲/2. Thus, we have measurements reported by various studies in the form of plots.
Therefore, the data analyzed here might inherently involve some
amax = −log 冋册 8
␲2
= 0.0912 . . . . . . . . . . . . . . . . . . . . . . . . . . . . (68)
digitizing errors.

Straight-Line Intercept Condition. The value of the intercept has

or a limit according to Eq. 68 or Eq. 69. When the experimental data

冋册
are noisy, the straight-line intercept for long time might not be
8 correctly located to meet this limit condition.
amax = −ln = 0.2099. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (69)
␲2
Long-Time Data Measurements. Errors made in obtaining cu-
With ␭1 now determined, the diffusion coefficient D can be solved mulative gas dissolution data are more significant at long times
for from Eq. 67: than for short times. Suppose that the error made in obtaining the

76 March 2006 SPE Journal

experimental value of the dimensionless cumulative gas dissolu-
tion is a certain percent of the true value, that is,
QD⬘exp = 共1 + ␧兲QD⬘true, . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (74)
where ␧ is the percent error measured as a decimal fraction. If the
true value of the dimensionless cumulative gas dissolution is rep-
resented, using Eqs. 74 and 50:
2
QD⬘true = 1 − Qoe−␻ tD. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (75)
Then, for the experimental value of the dimensionless cumulative
gas dissolution, we have
2 2
QD⬘exp = 1 − Qoe−␻ tD + ␧共1 − Qoe−␻ tD兲

2
= 1 − Qoe−␻ tD 1 − ␧ 冋 冉 Qo
2
e␻ tD
−1 冊册 . . . . . . . . . . . . . . . (76)

On a semilog plot, the data would then be represented by the function

ln共1 − QD⬘exp兲 = ln Qo − ␻2tD + ln 1 − ␧ 冋 冉 Qo

2
e␻ tD
−1 冊册 . . . . (77)

This function shows the effect of error. For example, for the rep-
resentative values of Qo⳱0.7 and ␻2⳱2.5, zero error corresponds
to ␧⳱0, and ␧⳱±0.05 corresponds to ±5% error. Data points
measured to within ±5% error would lie between the upper and the
lower curves (Civan and Rasmussen 2002, 2003). Under these
circumstances, the scatter in the data increases as time increases.
Thus, every effort should be taken to obtain data with special
accuracy at long times.

Applications to Gas-Diffusion Tests

Typical reported experimental data are analyzed here for purposes
of illustrating the previously described data analysis and interpre-
tation methodology.
The experimental data of Riazi (1996) and Zhang et al. (2000)
are analyzed. The true value of the gas pressure at equilibrium p*
has not been measured in these studies. However, the final pres-
sure readings are very close to the equilibrium values because the
pressure-decline curves were almost stabilized. Therefore, this
value has been estimated by a short-range extrapolation. Conse-
quently, an uncertain amount of small error may have been intro-
duced into the calculation of the diffusion coefficient and the in-
terface-mass-transfer coefficient. The real gas-deviation factor Z
required for construction of plots of experimental data was deter-
mined according to Peress (2003).
Analysis of the Data of Riazi. Fig. 2 shows the QD–t1/2 regression
of the CH4-n-pentane data of Riazi (1996) using short- and long-
time approximations. Fig. 2 has been used to determine the pa-
rameter values by minimizing Eq. 60. The best-estimate parameter
values yielding the best fit of the experimental data are reported in
Table 1. Fig. 3 shows the ln(1–QD)–t plot of the same CH4-n-
pentane data of Riazi (1996) using short- and long-time approxi-
mations. Alternatively, the long-time portion of the Fig. 3 data
could have been used for determination of the same parameter values.
Analysis of the Data of Zhang et al. Fig. 4 shows the QD–t1/2
regression of the CO2/oil data of Zhang et al. (2000) using short-
and long-time approximations. Fig. 5 shows the ln(1–QD)–t plot of
the same CO2/oil data of Zhang et al. (2000) using short- and
long-time approximations. The best-estimate parameter values
yielding the best fit of their experimental data reported in Table 1
have been determined in the same fashion using Eq. 60.
Quality of Fit and Parameter Values. The quality of fits of ex-
perimental data presented in Figs. 2 through 5 is very good, con-
firming the theory and methodology presented in this paper. Table
1 shows the calculated values of the diffusion and mass-transfer
coefficients, the mass-transfer Biot number, and the ␭1 parameter
determined using the equations of the regressions of the various
experimental data analyzed according to the present interpretation
method. As can be seen, the values of the diffusion coefficients
determined by the present approach are an order of magnitude
different than the previously reported values by Riazi (1996),
Zhang et al. (2000), and Tharanivasan et al. (2004). This is not
surprising because, while the present approach is based on a rig-
orous phenomenological model, the accuracy of the previous stud-
ies is somewhat limited by their inherent simplifying assumptions
involved in their analytic interpretation methods. The accuracy of
the previous and the present results is also subject to the errors
associated with data measurement and/or processing techniques.
Temperature Dependence of the Diffusion Coefficient. Apply-
ing the Arrhenius equation (1889), the correlation of D with the
absolute temperature for the data of Sachs (1997) is obtained as
follows as shown in Fig. 6:
ED
ln D = ln D0 − , D in m2 Ⲑ s, T in °K, . . . . . . . . . . . . . . . . . (78)
RT
where ln(109 D0)⳱12.775 and ED/R⳱3,704.9 °K. In Eq. 78, D0 is
the preexponential constant (m2/s), and ED is the activation energy
required for diffusion (cal/mol), respectively; T (°K) is the absolute
temperature; and R (1.987 cal/mol–K) is the universal gas con-
stant. In contrast, Upreti and Mehrotra (2002) applied the follow-
ing empirical correlation for correlation of the diffusion coefficient:
ln D = A + BT, D in m2 Ⲑ s, T in °K. . . . . . . . . . . . . . . . . . . . . . (79)
Table 2 presents a comparison of the goodness-of-fit of the cor-
relations of the temperature dependence of the diffusion coeffi-
cient for CO2, CH4, C2H6, and N2 in Athabasca bitumen obtained
by the empirical equation (Eq. 79) of Upreti and Mehrotra (2002)
and the present Arrhenius equation (Eq. 78). Although the quality
of the correlation with the Arrhenius equation is slightly better
than that of the empirical equation (Eq. 79) of Upreti and Mehrotra
(2002), the Arrhenius equation provides a phenomenological
meaningful correlation (Fig. 7), which can be extrapolated beyond
the range of the experimental data. In contrast, the empirical equa-
tion of Upreti and Mehrotra (2002) can be used only within the
range of the data. Their equation is only an approximation, because

March 2006 SPE Journal 77

Fig. 6—Temperature dependence of the diffusion coefficient for
the CH4/water data of Sachs (1997).
it can be derived from the Arrhenius equation by means of a series
expansion of the temperature function truncated after the first-
order term (Civan 2004).
Conclusions
We conclude the following:
1. The analytical approach presented in this work provides
valuable insights into the mechanism of the equilibrium diffu-
sion process and offers an accurate interpretation method for
determination of the diffusion and mass-transfer coefficients of
gas for quiescent oil and brine, as well as drilling and comple-
tion fluids.
2. The flux continuity is proven to be the best choice for general
description of the surface/interface condition.
3. However, the general interface condition (Robin boundary con-
dition) expressed by the flux-continuity condition simplifies to a
prescribed point value condition (Dirichlet boundary condition)
when the interface-mass-transfer coefficient value approaches
infinity. The results of Fig. 2 show that the Dirichlet boundary
condition could also have been used to get approximately the
same parameter values as with the Robin boundary condition.
On the other hand, Fig. 4 indicates that the Robin boundary
condition is necessary to adequately describe the interface con-
ditions in general, because the Dirichlet boundary condition
would not describe the trends in these data.
78
Fig. 7—Temperature dependence of the diffusion coefficient for
the CO2, CH4, C2H6, and N2 in Athabasca bitumen data of Upreti
and Mehrotra (2002).
4. It is imperative to obtain accurate pressure-decline data in labo-
ratory experiments for accurate interpretation of the experimen-
tal data using the present approach.
5. The present methodology is proven practical and yields unique
and accurate values for both the diffusion coefficient and the
interface-mass-transfer coefficient.
Nomenclature
A ⳱ cross-sectional area of the test tank, L2
c ⳱ gas mass concentration of the gas/liquid solution, M/L3
C ⳱ gas molar concentration in the liquid, Mol/L3
D ⳱ gas diffusivity in the liquid, L2/T
H ⳱ height of the gas column, L
J ⳱ gas mass flux, M/L2–T
k ⳱ interface mass-transfer coefficient, L/T
L ⳱ height of the liquid column, L
M ⳱ molecular weight of gas, M/mol
p ⳱ pressure, M/L–T2
Q ⳱ cumulative gas mass, per unit cross section area,
dissolved in the liquid phase, M/L2
R ⳱ universal gas constant, ML2/mol–␪–T2
t ⳱ time, T
T ⳱ temperature, ␪
V ⳱ volume, L3
w ⳱ gas mass fraction of the gas/liquid solution,
dimensionless
x ⳱ distance measured from the gas/liquid interface into
the liquid phase, L
X ⳱ mole fraction of the dissolving gas in the gas/liquid
solution, dimensionless
Z ⳱ real-gas deviation factor, dimensionless
␤ ⳱ isothermal coefficient of expansion, dimensionless
␭ ⳱ root of Eq. 48, dimensionless
␳ ⳱ density, M/L3
␾ ⳱ fugacity coefficient of the dissolving gas in the
gas/liquid solution, dimensionless
Subscripts
D ⳱ dimensionless
g ⳱ gas
March 2006 SPE Journal
 LT ⳱ long-time
o ⳱ initial or reference state
r ⳱ reference measurement value
ST ⳱ short-time
Superscripts
* ⳱ equilibrium state
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SI Metric Conversion Factors
ft × 3.048* E–01 ⳱ m
ft2 × 9.290 304* E–02 ⳱ m2
psi × 6.894 757 E+00 ⳱ kPa
*Conversion factors are exact.
Faruk Civan is Alumni Chair Professor and the Brian and Sandra
O’Brien Presidential Professor in the Mewbourne School of Pe-
troleum and Geological Engineering at the U. of Oklahoma in
Norman. Previously, he worked in the Chemical Engineering
Dept. at the Technical U. of Istanbul, Turkey. Civan holds an
advanced engineering degree from the Technical U. of Istan-
bul, an MS degree from the U. of Texas at Austin, and a PhD
degree from the U. of Oklahoma, all in chemical engineering.
He has published extensively in technical journals, edited
books, and conference proceedings; presented seminars and
lectures at various technical meetings, companies, and uni-
versities; and taught short courses. Civan has received numer-
ous honors and awards, including five distinguished lectureship
awards and the 2003 SPE Distinguished Achievement Award
for Petroleum Engineering Faculty. He has served on numerous
AIChE and SPE technical committees and is currently a mem-
ber of the editorial boards of four engineering journals. Mau-
rice L. Rasmussen is the David Ross Boyd Professor Emeritus of
the School of Aerospace and Mechanical Engineering at the
U. of Oklahoma, Norman. e-mail: mbrasmusse@msn.com. His
research interests are in fluid mechanics and applied math-
ematics. He is the author of a book on hypersonic flow and
coauthor of a book on applied mathematics for engineers.
Rasmussen holds a PhD degree in aeronautics and astronau-
tics from Stanford U.
79