A New Mixing Rule for Petroleum
Mixture Compositional Processes
D.X. YOUNG
United Oil & Gas Consulting Ltd.
Abstract
A new mixing rule of a realistic vector form is proposed. It is
used for vapour-liquid equilibrium calculations of petroleum
mixtures with the commonly used Peng-Robinson (PR) and
Soave-Redlich-Kwong (SRK) Equations Of State (EOS). The
results are compared with those from the conventional calcula-
tions with the same EOS and the original matrix form of mixing
rule, and the experiment data obtained for the chosen petroleum
mixtures with and without added CO2.
The new vector form of mixing rule is a successful “trans-
form” of the old matrix form of mixing rule based on the idea of
component deviation from their pure-state, vapour-liquid equi-
librium behaviour when they are present in a petroleum mixture.
Such transformation will allow us to eliminate binary interaction
coefficients with the more practical component deviation coeffi-
cients for petroleum mixture phase equilibrium problems
encountered in compositional simulation and relevant chemical
engineering calculations.
The utilization of the new mixing rule has lead to results with
improved computation efficiency, convergence behaviour and
accuracy for the calculations performed. However, convergence
problems cannot be solved completely with the proposed mixing
rule as the problem does not stem from there only. Further
investigation results in a new critical criterion that has not been
satisfied by many EOS, including the PR and SRK EOS, on both
analytical and numerical basis for all pure components. Thus,
convergence problem has never been really solved no matter
how sophisticated mathematical methods have been employed to
get the “converged” results.
The new critical criterion is established with a newly devel-
oped three term cubic EOS, which can be easily reduced to
encompass many two term cubic EOS of similar forms as the PR
or SRK EOS. A discussion on the new EOS is given. With the
new EOS, it becomes obvious that the critical convergence prob-
lem is not purely a mathematical one, the EOS models them-
selves may have some inherent restrictions for the phase equilib-
rium computation schemes to work for complex mixtures when
the critical points are approached.
Introduction
The PR and SRK EOS have been in use for phase equilibrium
calculations for over twenty years since they were published(1, 2).
However some problems still exist for petroleum mixtures con-
taining more heavy fractions and near critical point conditions or
across phase boundaries(3). In some cases, it is even hard to get
converged results without considering their accuracy. Because
February 2000, Volume 39, No. 2
such problems have not been solved with satisfaction, reservoir
simulators that use EOS to model reservoir fluid compositional
behaviour are most likely to inherit the problems. When this hap-
pens in simulation, a lot of times, it is not clearly understood. The
reason that this is important is because reservoir fluid vapour-liq-
uid equilibrium states reflect its energy and petroleum recovery
potential.
Another problem with compositional reservoir simulators that
use an EOS model is that the computing time and storage require-
ment increase sharply with the number of components used for
each grid and iteration step, and soon become a restriction in a
simulation(4). Even with the new generations of computers, this is
still the case.
Many techniques have been developed to tackle convergence,
accuracy, computation time, and storage problems. Among these
are numerous lumping schemes(5, 6, 7) and highly sophisticated
mathematical optimization methods(8). In this paper, a new mixing
rule that can contribute a lot towards solving such problems is
used with the PR and SRK EOS. The rationale is to quantify the
phase behaviour deviations from their pure state behaviour for
each component present in a petroleum mixture when it is inter-
acting with the rest of the constituents.
The above conceived scheme is realized for phase equilibrium
computation of two reservoir fluids from different fields, for
which lab measurements on composition and saturation pressure
are conducted for the fluid samples alone and when various
amounts of CO2 are added.
The Mixing Rule
The new mixing rule is first introduced to improve computa-
tional efficiency of phase equilibrium calculations that use an
EOS by decomposing the binary interaction coefficients into com-
ponent deviation factors in a way that is suitable for petroleum
mixtures. The reasons for doing this are to overcome the draw-
backs of the binary interaction assumption for complex mixture
systems.
When we assume that binary interactions are valid for petrole-
um mixtures, we are inviting trouble for modelling such systems
although this might be the right thing to do at some point for rela-
tively simple mixture systems to establish certain methodology.
First, the basis is on very limited binary mixture experimental
data, which is extended to complex mixtures as an approximation.
However, in reality, we all know that naturally occurring reservoir
fluids are composed of thousands of hydrocarbon constituents.
Second, it is not always easy to control the binary interaction
coefficients, and a lot of times, such data may not be available at
all. Third, the limited binary interaction information may not be
comprehensive enough to incorporate all important factors that
35
TABLE 1: Reservoir fluids composition. Where Ki is the deviation coefficient for component i. If we
want Equation (7) to perform the similar function as Equation (5)
Res. Fluid Sample-1 Res. Fluid Sample-2 in EOS vapour-liquid equilibrium calculations, we can expand
Component (Mol%) (Mol%) Equation (7) and make the two equations equivalent by the
following:
H2S 5.86 0.00
CO2 0.30 2.97
N2 0.81 0.40 ....................................................................................(8)
C1 34.92 8.61
However, we should notice that the decomposed component
C2 11.46 7.39
deviation coefficient Ki in Equation (7) bears different meaning
C3 5.58 7.64 now and Ki = 1 represents no deviation for the component.
I- C4 1.28 0.95 As expected, the new mixing rule does not present any problem
N-C4 2.62 6.27 with respect to the fundamental thermodynamics. The justifica-
I- C5 1.32 1.59 tions for such modification may be partially attributed to the regu-
N- C5 1.44 3.84 lar changes of the physical and chemical properties of the con-
C6 2.63 4.06 stituents in a petroleum mixture.
C7 or C7+ 3.04 56.28 As the coefficient Ki in Equation (7) presents a vector form
C8 4.11
instead of the matrix form in Equation (5), obviously, the advan-
tages of using it are to increase computation efficiency and reduce
C9 4.09
the required storage. For a mixture system with n species, we only
C10 3.43 need n component deviation factors Ki compared to the previous
C11 2.60 n-by-n binary interaction coefficient matrix kij. When we imagine
C12 2.02 that this is for the computation of each grid and iteration of the
C13 1.99 simulation, its effect will be substantial.
C14 1.56 The proposed mixing rule is used to calculate the bubble point
C15 1.33 pressure and dew point temperature of two reservoir fluids with
C16 0.99 different CO2 concentrations. The two reservoir fluids are special-
ly chosen for the research project. Their compositions are given in
C17 0.89
Table 1. Sample-1 is a light sour crude, and 20%, 40%, and 60%
C18 0.81
CO2 in mole concentrations are added to the sample. Sample-2 is
C19 0.74 a relatively heavy crude, and 30%, 45%, and 60% CO2 are added
C20+ 4.18 to it.
The above-mentioned phase equilibrium calculations are per-
may contribute a lot to the vapour-liquid equilibrium state of a formed for the eight cases using the two crudes and six derived
petroleum mixture in the real engineering world because such data samples with the PR or SRK EOS to verify the validity of the new
are obtained for relatively ideal binary systems. Four, it causes mixing rule. The only difference in the calculations is the mixing
low computation efficiency for compositional reservoir and rules used. In one case, it is the original matrix form with binary
process simulations. interaction coefficients, and in the other, the new vector form with
The mixing rule proposed is for the numerator, aα, of the sec- component deviation factors. The results are presented in Table 2,
ond term in an EOS of a similar form as the PR or SRK EOS. It Table 3, and Table 4 along with the available experimental data
can be used to replace the corresponding parameter in such an for the specified calculations.
EOS for vapour-liquid equilibrium calculations. The PR and SRK As we can see from Table 2 or 3, the calculated bubble point
EOS have similar forms except the denominator of the second pressure results with the new mixing rule are in good agreement
term. Both EOS are commonly used for compositional process with the experimental data and the results from the conventional
calculations. Here we use the PR EOS given by Equations (1) – calculations. Table 4 compares the calculated dew point tempera-
(6) in standard form as the example to introduce the new mixing tures from the two schemes as there are no experimental data
rule as follows: available. Good consistency has been achieved as well.
One observation that is made when performing the above com-
putations is that the convergence behaviour of the compositional
phase equilibrium calculations is improved as an unexpected
................................................................(1) result of using the new mixing rule. This is indicated by the bub-
ble point pressure calculation for the case of sample-2 with 60%
CO2. For this case, the conventional calculation with the PR EOS
..........................................................................(2)
and the old mixing rule fails to converge, but the new scheme
using the same EOS and the new mixing rule works out quite well
.............................................................................(3)
as a result. With several other cases of high CO2 concentrations,
convergence problem is also observed for the conventional
scheme, but converged results are obtained after many trials. This
is not the case with the new scheme. However, a convergence
....................................(4)
problem does exist for the new scheme as we perform the calcula-
tion for the last case in Table 2 where the converged result is
achieved after some trials. The problem may have been attributed
.......................................(5) to the near critical point situation due to the very high CO2 con-
centration in the reservoir fluid.
...............................................................................................(6) In the calculations performed in this study, values for the com-
ponent deviation coefficients Ki are easy to control compared
For a mixture system with n components, the newly proposed with binary interaction coefficients. In general, values used for
mixing rule given by Equation (7) below can be used to replace light components have relatively large deviations from one.
Equation (5): Typical values used are between 0.92 – 0.99 for hydrocarbon
components with light components, such as methane and ethane,
having values close to the lower side. For a specific component,
.............................(7) only small variations in the Ki values are observed in different

36 Journal of Canadian Petroleum Technology

TABLE 2: Bubble point pressure calculation results.

Exp. Conventional New

Results Calc. Results Method
Cases (kPa) (kPa) (kPa)
Sample-1 18,609 18,533 18,588
Smp-1+20%CO2 21,043 20,960 21,091
Smp-1+40%CO2 26,745* 26,614 26,889
Smp-1+60%CO2 35,984* 38,176 32,950
Sample-2 3,902 3,709 3,827
Smp-2+30%CO2 6,881 6,840 6,991
Smp-2+45%CO2 8,267 8,225 8,225
Smp-2+60%CO2 9,198 not converged 9,266

Average error % 1.37% 0.87%

Note:
(1) * are Core Lab calculated bubble point results.
(2) The conventional calculation results are from the standard PR EOS and mixing rules.
(3) The new method results are from the PR EOS and the new mixing rule and the mixing rule given by Equation (6).
(4) The results are at temperature 220˚ F.

cases. The difference is normally within 0.02. For example, the Ki
values used for propane is between 0.97 and 0.99. This is actually
similar to the cases when using binary interaction coefficients. For
CO2, H2S, and N2, the deviation coefficients used a range from
0.82 – 0.91 with variations of about 0.02 for each individual com-
ponent in different cases. It should be pointed out that the compo-
nent deviation coefficients provided in this paper are the findings
of the pioneer simulation work. It is possible that these values
may change a bit if different grouping techniques and different
computer programs are employed when more extensive studies
are carried out in the future.
The Three Term Cubic EOS
The criticality problem may have existed as long as the history

TABLE 3: Predicted bubble point pressure.

Bubble point Predicted Bubble Point Pressure (kPa)

Sample-1 Sample-1+20% CO2
Temperature Old New Old New
Deg. C Method Method Method Method

15.6 12,562 12,569 12,211 12,307

37.8 14,472 14,493 15,051 15,162
71.1 16,816 16,851 18,478 18,602
104.4 18,533 18,588 20,960 21,091
137.8 19,685 19,747 22,615 22,739
171.1 20,312 20,367 23,518 23,642
193.3 20,464 20,512 23,746 23,863
226.7 20,298 20,333 23,559 23,649
260.0 19,691 19,726 22,780 22,822
293.3 18,643 18,664 21,415 21,401
315.6 17,699 17,706 20,119 20,084
329.4 19,009 18,947

TABLE 4: Predicted dew point temperature.

Bubble point Predicted Bubble Point Temperature (Deg. C)

Sample-1 Sample-1+20% CO2
Pressure Old New Old New
kPa Method Method Method Method

3,447 445 444 439.4 438.3

6,205 442 441 438.9 437.8
8,963 426 425 427.2 426.7
12,411 393 393 403.9 403.3
14,479 370 369 386.1 385.6
15,858 348 349 371.1 371.1
17,237 313 314 356.7 356.1
18,616 339.4 338.9
Note:
(1) Old method in Table-3 and Table-4 is the standard PR EOS and mixing rules. New method is the PR EOS and the new mixing rule.

February 2000, Volume 39, No. 2 37

of EOS for several hundreds of years, regardless of what kinds of
temperature or volume related corrections have been tried to
improve it. This is the fact caused largely by the imperfection of
all EOS and the mixing rules for extended mixture applications.
Numerous lumping schemes, property correlations, and math
techniques also come into the play. The same is true for the
vapour-liquid equilibrium calculations in this study.
To gain deeper insight into the critical convergence problem, .........................(13)
further efforts are devoted to it, and some important findings
come out with the help of a newly developed three term cubic To further reduce Equation (13), we choose b = 0, which is a
EOS. It reveals how the volume related correction for pure com- condition required by the new EOS at the critical point for all pure
ponents and mixtures could give rise to convergence problem components, to get:
when the critical point is approached.
As we know, uncertainties can be introduced into phase equi-
librium calculations that use an EOS, when the application of an
EOS is extended from pure components to mixtures to get the
approximate mixture parameters by mixing rules. However, to
make an EOS work near the critical point, such approach will fail
in most cases due to the extreme sensitivity of an EOS near the
critical point. For such mixture applications, the problem arises
mainly from the second mixing rule that appears as parameter b in ........................(14)
the denominator of an EOS of similar forms as the PR or SRK
EOS. The problem will become very clear as we present the new Where,
generalized three term EOS obtained on analytical basis:
.........................................................................................(15)

....................................................................................(16)

............................(9) ...............................................................................................(17)

In Equation (9), a, b, c, m, and n are treated as constants so far;
m and n are introduced to generalize the EOS and to adjust the
functional behaviour of the EOS. The use of m and n gives more
flexibility for α, which is a parameter similar to the α in the PR or
SRK EOS, to be correlated more reasonably; X and Y are inter-
mediate constants given by the restrictive relationships below:
...................................................................................(10)
We can notice that “c” has been eliminated from the EOS when
b is set to zero. Here we need to emphasize that b = 0 at the criti-
cal point is a very important finding that must be satisfied by the
new EOS on both analytical and numerical basis at the critical
point for not just one or two components, but for all pure compo-
nents, which is a tough condition that has not been met strictly by
any EOS on the same basis.
If we want Equation (13) to become a two term cubic EOS, we
can make the constant c equal to zero to arrive at:

....................................................(11)
...........................(18)

....................................................................................(12) Where,

As we can see, although a, b, and c are treated as constants, ..................................................................................(19)

they are not really independent of each other. This is a very
important characteristic of the new EOS that is not reflected in the
other EOS. Another important fact is that (Zc– b) in the first term
of the new EOS is used to replace the constant coefficient of the ...........................................................(20)
parameter b of the corresponding term in the PR or SRK EOS to
make the new EOS more generalized.
Equation (9) is in its complete generalized form, which is
seemingly complicated. But the interesting fact about the new ...........................................................................................(21)
EOS is that it can be reduced consistently. When we set c = 0, it
reduces to a two term EOS, and when (Zc – b) is set to a constant Again, we find that “a” has been eliminated in Equation (18)
close to what is used in the PR or SRK EOS (m = 0), we get new when c is set to zero. As we have mentioned earlier that the newly
EOS that are very close to the two EOS in form and performance. proposed EOS can generate EOS that are very close to the PR or
We will deal with these aspects in more detail as we start to SRK EOS. Here we will set an example when we choose the typi-
reduce the new EOS. cal values Zc = 0.3 and b = 0.22 to make (Zc – b) fall between
First, we will notice that m and n will disappear from Equation 0.0778 and 0.0866, which are the constant coefficients that are
(9) at the critical point. We can set m and n at different values to used in the PR and SRK EOS. The result of doing this is the fol-
try to better correlate the parameter α, which appears in the sec- lowing EOS in the same form as the two mentioned:
ond term of the EOS as the most appropriate place for such corre-
lation. To keep it simple, we only need to set m = 0 and n = 0 to
get the “normal” form of equation with the same a, b, c, X, and Y
below: .........................(22)

38 Journal of Canadian Petroleum Technology

 When we compare Equations (1) through (4) with Equation
(22), we see the minor difference for such an instance. This is not
just a coincidence if we analyse the values of typical critical com-
pressibility factors Zc and the general applicable range of an EOS,
but rather we are dealing with a more generalized EOS. The b
value used in Equation (22) and the required value at the critical
point may help us to understand the convergence problem and the
mixing rules better.
Now we will look into the EOS described by Equation (18) in
more detail. If we apply Equation (18) for some commonly found
components in a petroleum mixture at the critical points and allow
b to take different values, we will be able to find out that “b” has
to be zero in order for the EOS to work for all the pure compo-
nents at their critical points. When this criterion is enforced to
Equation (18), a two term EOS that will work at the critical points
for pure components is created:
............................(23)
Where,
........................................................................................(24)
.....................................................................................(25)
....................................................................................................(26)
When we compare Equations (18) and (23) with the PR or SRK
EOS, the difference is mainly caused by the requirement of setting
b = 0 at the critical point to satisfy the critical condition. This can
be verified on a rigorous numerical basis using analytically
obtained EOS applied for different components at the critical
points. We will be able to find out how sensitive the EOS will be
when the critical point is approached, and no longer rely on the
analytical EOS only.
If an EOS has not worked for the individual components that
are present in a mixture, it is not reasonable to expect it to
improve when it is extended to mixtures. Obviously, when the
mixing rule given by Equation (6) is used with the PR or SRK
EOS, it is less likely that they will produce terms close to those
given in Equation (23) at the critical point. Thus, poor conver-
gence performance and accuracy are expected near the critical
points for these EOS no matter how other masking factors may
also contribute.
The above-stated points are virtually true for all EOS of similar
forms. We can certainly use different mixing rules and lumping
schemes; again the point is whether the right EOS or mixture
parameters can be generated with these methods for the system
conditions. One implication that is still there is that single fixed
correction for the b constant in the new EOS or the b parameter in
the PR or SRK EOS under all system conditions may not always
work out as indicated by the difference of Equation (23) and the
two EOS mentioned.
Discussion
In the paper, we introduced the new mixing rule given by
Equation (7) on the basis of component deviation for petroleum
mixtures, and utilized it with the PR and SRK EOS for the initial
investigation for reservoir or chemical engineering processes
involving equilibrium or compositional behaviour. Its effective-
ness is supported by the comparable calculation results and avail-
able experimental data.
The significance of the new mixing rule may be clearly seen by
professionals who develop simulation models and simulator soft-
ware, and by engineers who have dealt with the binary interaction
coefficients with difficulty. In the real engineering world, it may
allow us to incorporate more practical factors that contribute to
February 2000, Volume 39, No. 2
compositional process behaviour. The possibility to extend it to
mixtures other than petroleum is not investigated.
As we know, in the literature, experiment and research for mix-
tures are conducted extensively on ideal binary pairs and some
ternary systems that yield very limited information. To verify the
new mixing rule, we may use modern lab measurement technolo-
gies for petroleum mixtures along with simulation tools. For
instance, experiments can be run by mixing the light components
of a petroleum mixture in vapour state and the heavy components
in liquid state without the light components in it.
The component deviation coefficients used in this paper are
generated by simulation match for the experimental data from the
specified reservoir fluids. The method is very effective and easy
to control as we perform the calculations. With today’s simulation
capabilities, component deviation factors will be easier to handle
as more research data flow out.
In general, the new mixing rule can yield results that indicate
equivalent or improved accuracy and convergence behaviour with
higher computational efficiency. The efficiency improvements are
mainly observed for the cases that are difficult to converge. For
these cases, the number of iterations to achieve a converged result
has about 70% reduction from around 30 iterations with the old
program to approximate nine with the modified program, when
the same real and pseudo-components are used. Thus, lumping
factor is excluded out of study.
The other mixing rule given by Equation (6) is not changed in
the calculations performed in this paper. However, its effect in
causing convergence problems is discussed with the help of the
newly developed three term generalized cubic EOS. The signifi-
cant finding is the new critical criteria required at the critical point
on both analytical and numerical basis. It is true that this is the
observation with the new EOS, but the clue it provides on conver-
gence problem has significant meaning for all the EOS that are
encompassed by the new generalized EOS.
It is author’s opinion that the new EOS can be shaped with
great flexibility for general or specialized applications, either for
vapour or liquid phase in liquid, two-phase or superheated
regions, and for common system conditions or localized applica-
tions. For petroleum mixtures, critical compressibility correlation
can be developed. These are not the topics of this paper.
Conclusions
1. A new vector form of mixing rule based on the idea of com-
ponent deviation from their pure state vapour-liquid equilib-
rium behaviour when they are present in a petroleum mix-
ture, has been proposed and utilized successfully with the
commonly employed PR and SRK EOS for reservoir fluid
compositional process phase equilibrium calculations. It
replaces the corresponding matrix form of mixing rule with-
out presenting any theoretical problem, and thus eliminates
the use of binary interaction coefficients with component
deviation factors. Its use for saturation pressure and temper-
ature calculations of the selected petroleum mixtures has
resulted in improved computation efficiency, convergence
behaviour, and accuracy. The proposed mixing rule provides
a more realistic treatment of the constituents of a petroleum
mixture for relevant reservoir and chemical engineering
problems. It reduces the required computation storage, and
its potential in increasing compositional simulation efficien-
cy will be expected to be enormous if applied successfully in
such a simulator.
2. The newly developed three term generalized cubic Equation
of State along with the newly established critical criterion on
both analytical and numerical basis, provides unique insight
into the critical convergence problem and possible solutions
to this tough existing problem.
NOMENCLATURE
EOS = Equation Of State
PR EOS = Peng-Robinson EOS
39
a, b, c = EOS parameters or new EOS constants
i, j = subscript index for component i or j Author’s Biography
kij = binary interaction coefficient for components i
and j Derek Young is a reservoir engineer with
KI = component deviation coefficient for component i United Oil and Gas Consulting Limited. He
Kij = 1 – kij worked as a senior reservoir engineer for
m, n = new EOS constants several oil companies and was involved in
P = pressure reservoir simulation and chemical process
Pc = critical pressure engineering simulation research before
R = gas constant joining UOG. He holds a B.Sc. degree in
T = temperature petroleum engineering, and studied for his
Tc = critical temperature M.Sc. and Ph.D at the University of
Tr = reduced temperature Wyoming in chemical and petroleum
V = molar volume engineering.
xI = mole fraction of component i
X = symbol
Y = symbol
Zc = critical compressibility factor
α = EOS parameter
ω = acentric factor

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Provenance—Original Petroleum Society manuscript, A New

Mixing Rule for Petroleum Mixture Compositional Processes
(97-116), first presented at the 48th Annual Technical Meeting,
June 8 – 11, 1997, in Calgary, Alberta. Abstract submitted for
review November 25, 1996; editorial comments sent to the
author(s) November 19, 1998; revised manuscript received
January 11, 1999; paper approved for pre-press February 16,
1999; final approval January 27, 2000.

40 Journal of Canadian Petroleum Technology