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Ind. Eng. Chem. Res.

1993,32, 1767-1771 1767

Comments on the Use of Quadrature in Selecting Pseudocomponents for


Multiple-Contact Processes
Kraemer D. Luks,' Edward A. Turek, and Tor K. Kragas
Amoco Production Company, Box 3385, Tulsa, Oklahoma 74102

Certain complex,multicomponent mixtures can be represented as continuous distributionsof species,


typically expressed as a function of one or more parameters (such as carbon number) or physical
properties. Rather than use a continuous distribution directly when performing flash calculations,
one often uses quadrature to choose a set of discrete components (pseudocomponents) to mimic the
distribution. In this paper we critically examine the validity of systematically updating the
(quadrature) identification of n pseudocomponents during a multiple-contact process, in order to
compensate for the changing compositional nature of the system. We show that updating procedures
can produce computationalresults for a multiple-contact process that diverge from those one obtains
using n pseudocomponents of fixed identification, where n is very large. As an illustration, the case
of a semicontinuous live oil repeatedly contacted with fresh COa is considered.

Introduction change in the limit B, but one can argue that a sensible
initial choice of B should remain appropriate throughout
It has been shown [e.g., see Cotterman and Prausnitz a multiple-contact process.
(1985, 19911, Cotterman et al. (1985a,b, 19861, Behrens
and Sandler (1988), and Shibata et al. (198711 that Matthews et al. carried out their continuous system
quadrature can be a very efficient way of specifying the description using two characterization variables: (1)dis-
pseudocomponents of the C7+portion of a live oil, providing tillation curve boiling point and (2) specific gravity or
one can accurately represent the distribution of the many Watson characterization factor. They employed a cu-
C7+ species present as a continuous function of some mulutiue boiling point temperature curve to describe their
parameter(s), say, carbon number. For example, given system, with temperature as the ordinate and cumulative
the simple exponential distribution weight fraction as the abscissa. The cumulative weight
fraction varies from 0 to 1in every step of the multiple-
F(I) = ae"'/(e4 - ea) = 0 when I < A, I > B (1) contact process and therefore permits one to use a
for a fluid portion with ita carbon number I limited to the Legendre-Gaussquadrature scheme once at the outset of
range A = 6.5 to B = 100.5, one can accurately represent the process to compute the quadrature points and weight
that portion by as few as four pseudocomponenta when factors; the fixed limits (0,l) of the cumulative weight
performing a single flash calculation. Du and Mansoori fraction eliminate the need to recompute these for later
(1986,1987) were the first, to our knowledge, to use the contactings. The characterization of the pseudocompo-
simple exponential distribution in phase equilibrium nenta changeswith successivecontactings,throughchanges
calculations,although Shibata et al. (1987) point out that in the pseudocomponent properties accompanying the
Vogel et al. (1983)earlier presented experimental evidence shiftingof the cumulative property curves. In other words,
supporting the use of the exponential form for C7+ mole although the locations of the pseudocomponent assign-
fraction distributions. menta along the cumulatiue property curve and their
The carbonnumber Ican be related to molecular weight associated weight fractions conveniently do not change
through with each contacting, the pseudocomponent properties
do.
MW = 14.01+ 2.0 (2) Setting aside any discussion of the relative merits of
The average carbon number for a given range (A,B) can choosing one set of characterizingparameters over another,
be expressed as a function of the exponential decay we judge that the description employed by Matthews et
parameter a: al. is equivalent in detail to a two-parameterdistribution.
In contrast, eq 1 is a one-parameter description. The
(I)= [ ( a A+ l)e"A - (aB + l)e41/[a(e4
In the limit B - -a, (I)
-
A + l/a. The higher the
molecular weight of the continuous portion, the smaller
(3) analysis that follows will focus on certain formal features
of Matthews' methodology versus traditional methods
using fixed identityfproperty pseudocomponents. The
analysiswill be formally,if not quantitatively,independent
a becomes, or equivalently, the "flatter" the distribution
eq 1becomes. of description. We will employ the one-parameter expo-
Recently, Matthews et al. (1991) have suggested that, nential function in eq 1in our computations. Ita simplicity,
in a multiple-contact process where the continuous portion/ which may properly be considered a quantitative liability,
phase composition is changing from stage to stage, one can in fact cause formal differences between Matthews'
should alter the description of the phase pseudocompo- methodology and more traditional strategies to be nu-
nents to reflect that change. In the context of the merically magnified. In summary, a recipe analogous to
distribution in eq 1above, alteration would be equivalent Matthews' can be constructed using the exponential
to changing the a parameter. It could as well mean a distribution eq 1, even if one must concede certain
computational advantages to the use of a cumulative
* Address correspondence to this author at Department of distribution. In the following section, such a computa-
Chemical Engineering, University of Tulsa, 600 S. College Ave., tional recipe will be constructed suitable for a distribution
Tulsa, OK 74104-3189. function such as presented in eq 1.
0888-588519312632-1767$04.00/0 0 1993 American Chemical Society
1768 Ind. Eng. Chem. Res., Vol. 32,No. 8, 1993

Formalism Table I. Molar Composition of Oil A Used in the Example


Calculations
One can redefine the carbon number variable I in the component mole fraction component mole fraction
distribution function as a reduced variable:
N2 0.0216 iC4 0.0188
y=a(I-A) (4) c1 0.1080 nC4 0.0338
COa 0.0187 iC6 0.0215
Similarly Ca 0.0520 nC5 0.0244
H2S 0.0024 CS 0.0457
C = CY(B- A ) (5) cs 0.0461 C7+ 0.6070
represents the upper bound of the reduced variable
function. Equation 3 can be reexpressed as contacting proms. Two situations were examined, where-
in the molecular weight of the C7+ portion of oil A was
(y) = 1 - Ce*/(l- e-‘) = cr((I) -A) (6) arbitrarily assigned to be either 149or 249. The first value
is close to that used by Matthews et al. (1991)for his CS+
MW is synonymous with (I)at fixed (A$) and directly mixture. The following multiple-contact processes were
yields a (and thus C). computed at 160 OF using fresh C02 as the contacting gas,
To select pseudocomponent carbon numbers and mole with the C7+ portion represented by eight (quadrature)
fractions for a continuous portion of a phase represented pseudocomponents:
by this distribution, one can apply finite Laguerre-Gauss 1. Fifteen contactings were made of the liquid phase,
quadrature, which is applicable to integrals of the type initially oil A having a C7+ MW of 149,with equimolar
amounts of C02 at 1500 psia, after which the equilibrium
S,‘f(z)e+ d~ (7) vapor phase was removed; four different values of the
carbon number upper bound B of the C7+ portion were
The quadrature weighting factors {wi)and the roots {xi) examined, 20.5, 40.5,60.5,and m, respectively. Carbon
of the pseudocomponents are functions of the reduced number lower bound A is fixed at 6.5in all computations.
parameter C. {Ii} depend directly on {xi]through eq 4. If 2. Fifteen contactings were made of the liquid phase,
the continuous portion of a fluid phase has a MW that initially oil A having a C7+ MW of 249,with twice the
varies with the number of process steps performed, then molar amount of C02 at 2500 psia, after which the
{wi]and (Ii)can in turn be varied with the steps through equilibrium vapor phase was removed; three different
C. Since it is understood that the properties of a values of the carbon number upper bound B of the C7+
pseudocomponentdepend on its carbon number,then they
-
will also vary with the steps.
-
In the limit C m (Le., B Q),given a fixed value of
A), the quadrature results {wj]and {xi)will be fixed at all
portion were examined, 60.5,80.5, and m, respectively.
Carbon number lower bound A is fixed at 6.5 in all
computations.
3. Fifteen contactings analogous to 1 were performed
process steps for the continuous portion of a phase. The
MW (equivalently the value of (I))of the continuous but with the eight C7+pseudocomponent carbon numbers
portion at each process step will determine a value of a (Le., properties) determined once, prior to the first
at that step, and consequently the {Ij]will vary with each contacting, and held constant.
step along with MW. This limiting scenario is mathe- 4. Fifteen contactings analogous to 2 were performed
matically simple, like Matthews’ which employs a cumu- but with the eight C7+pseudocomponent carbon numbers
lative distribution function accompanied by Legendre- (i.e., properties) determined once, prior to the first
Gauss quadrature. But it is not formally equivalent to contacting, and held constant.
the Matthews methodology. Matthews et al. were in As the MW of the liquid phase increased with each
essence able to achieve this degree of mathematical contacting in 1 and 2,the carbon numbers of the eight C7+
simplicity for arbitrary values of C; that is, they were able pseudocomponents were readjusted prior to the next
to impose a finite upper bound B on the carbon numbers contacting by finite Laguerre-Gauss quadrature to be
of the continuous portion at the outset and calculate their consistent with that MW and the (fixed) carbon number
Legendre-Gauss quadrature results once (initially), suit- upper bound B. In performing our computations, we
able for all later process steps. For finite B in the context empiricallyfound that our multiple-contactprocess results
of the exponential distribution in eq 1,one is required to did not vary significantly when we used six or more
recompute {wi)and (xi) at each step of the process. This quadrature components. Therefore, we arbitrarily used
is a computational inconvenience, of course. Of impor- eight components for our computations. When applying
tance here, however, is that this computation for a value Laguerre-Gauss quadrature to cases of more than six
of C that varies with each step, inconvenience aside, is pseudocomponents,we invoked quadruple precisionwhen
formally equivalent to that of Matthews et al., as B is generating the roots and weighting factors. We deemed
this necessary from comparisons of calculated roots and
maintained aa a finite, fixed parameter for the entire
multiple-contact process.
We will now compare the computational results of this
last recipe,cumbersomethough it may be, to those of more
-
weighting factors with literature tabulations for the case
C m (Abramowitzand Stegun, 1972). All computations
were performed using the same Redlich-Kwong equation
traditional strategies whereby the identity and properties of statedescription as employed in our earlier paper (Luks
of the pseudocomponentsare initiallyestablishedand then et al., 1990). It should be emphasized that the choice of
held fixed throughout the multiple-contact process. By equation of state is not crucial here, only that the same
this comparison, we will be able to evaluate the ramifi- equation of state description be used in comparative
cations of Matthews’ methodology relative to traditional computations.
methodologies within the framework of a common dis- Larger values of B as upper carbon number bounds were
tribution, that being the one in eq 1. employed for the computations for MW = 249 than for
those for MW = 149. MW = 249 corresponds to a carbon
Example Calculation
A live oil, ‘oil A” (described in Table I), with 60.7 mol
C - -
number of about 17.6,versus 10.5 for MW = 149. When
( B a),the normalized C7+mole fractions are the
same for all contactings, and thus quadrature only has to
5% C7+was chosen for the initial liquid phase of a multiple- be performed once; however, the properties of the
Ind. Eng. Chem. Flea., Vol. 32, No.8,1993 1769

e
460 I I
L
.-c1) Sliding (24W60.6)

Discrete (240/60 6)

al
Sliding (14W20.5)
Sliding (140/B -. -) 3
Discrete (149/20.6)
Discrete (140/B + m)
I I I I
60
0 3 6 9 12 16 0 3 6 9 12 16
Number of Contactings Number of Contactings
Figure 1. Comparieon of the liquid-phase molecular weight a~ a Figure 2. Comparison of the liquid-phase molecular weight BB a
function of the number of contactings for the sliding and discrete function of the numbr of contacting8 for the sliding and discrete
methods for two seta of initial CI+ molecular weight and parameter
B. -
meth~fortwo~teofinitialCI+molecular~ightandtheparame~
B 0,

pseudocomponents are changing with each contacting as 2oo


the carbon numbers change.
In their work, Matthews et al. performed a differential
pressure depletion calculation consisting of four steps at
533.2 K for a mixture of 30 wt 7% CO2 + 70 wt 7% c6+
mixture. Their c6+ mixture had a molecular weight of
about 145. The first depletion removed a substantial
portion of the pressuring gas, similar to what we experi-
enced with the light ends of the live oil in our computations.
It is not straightforward to assess how similar the multiple Sliding (149/20.5)
contact process calculations 1 and 2 above are to Matthew’ 50 -
oil depletion calculation. Such an assessment, however, 3
is not needed. The computationsperformed herein focus 3
on their methodology of adjusting pseudocomponent I I I 1
properties at each step of a process vis-a-vis more 0
traditional schemes using pseudocomponents with fued
properties. The comparison is made in a common frame-
work, the above-listed multiple-contact processes.

Discussion
For convenience, we will hereafter refer to the charac-
terization updating scheme used in calculations 1 and 2
as the sliding scheme, since the carbon numbers of the
remaining liquid-phase pseudocomponents in these cases 160
are adjusted (“slide”)to higher carbon numbers with each
-
contacting. This sliding will be most pronounced for the
case B m, as the freedom for the carbon numbers to
adjust to the changing value of MWl is not restricted by Discrete (140; B -. 4
a finite carbon number upper bound B. The character-
._
ization scheme where the carbonnumbers (and properties) Sliding (140; B -. m)
are fixed initially and held constant throughout the 60-
multiple contactings will be referred to as the discrete
scheme.
Figures1 and2compareMWlfortheslidinganddiscrete
computations for the cases of CI+initial MW = 149 for B 0 3 6 Q 12 15
= 20.5 and m, and C7+ initial MW = 249 for B = 60.5 and
m. The computations for MW = 249 with the different
Number of Contactings
values of E diverge with the number of contactings more Figurn 4. Comparison of the liquid-pham mam aa a function of the
dramatically than those for MW = 149.(There is a “kink”
in all the curves at contacting 1,more noticeable for C7+
initial MW = 249,which is caused by the first contacting
number of contactingn for the sliding and discrete methodn for two
seta of initial Cy+ molecular weight and the parameter B =, -
preferentially removing nearly a l l the volatile8 of the with MW = 249,especially over the fmt five contactings.
original live oil.) The same type of property divergence The divergences increase not only with the number of
(but not as pronounced) occurs when one computes the contactings but ale0 with the value of the upper carbon
CI+mass left in the liquid phase (Figures 3 and 4). The number bound B. For an initial C7+ MW = 149, for a
divergences between sliding and discrete results for MW particular computational strategy (sliding or discrete),
= 149 are very small in all the Figures 1-4 when compared the resulta for B 1 40.5 are virtually identical to those for
1770 Ind. Eng. Chem. Res., Vol. 32,No. 8,1993

0.5 0.5 I
1
Legend C Legend
.-50 0.4
Initial (148/20.6) Initial (249/60.6)
Sliding (16) - -
Sliding (16) - -
8 /--\
8 0.3 \ Discrete (16)

c
0.3 Discrete (161
c
2
0.2

x
3
s 0.1

0.0
1 2 3 4 5 6 7 8 1 2 3 4 5 6 7 8
C7+ Pseudocomponent C7+ Pseudocomponent
pigun, S, c7+mole fractions (normalized)for ininitialc,+molecular Figun, 7. C7+mole fractions(normalizsd)for an initial C7+molecular
weight of 149 and B = 20.5. Shown are the initial values, the values weight of 249 and B = 60.6. Shown are the initial values, the values
-
after 16 contactingafor the sliding and discrete calculations,and the
values for B a. values for B m. -
after 16 contactingafor the sliding and discrete calculations,and the

0.5 I I The distribution for the sliding case changes form with
Legend the number of contactings differently from that for the
discrete case. Bothstart with the same initial distribution
Initial (14W606) (shown), with all the pseudocomponents of the sliding
slifing(16) - - case experiencing increasing carbon numbers with the
Discrete (16) number of contactings. One effect of these carbon number
changes is a reduction in the volatility of the lighter C7+
Sliding (B -1
+
pseudocomponents, causing their normalized mole frac-
tions not to diminish as rapidly as in the discrete case.
The sliding pseudocomponent mole fraction distribution
thus becomes flatter with the number of contactingswhen
compared to the corresponding discrete distribution.
Since the pseudocomponents are changing identity
(carbonnumber) with each contacting for the sliding case,
one cannot strictly compare pseudocomponent masses
1 2 3 4 5 6 7 8
between contactings with the objective of quantitatively
C7+ Pseudocomponent examining a possible conservation-of-mass violation.
Fieurn 6. C7+ mole fractions (normalized)for an initialC7+molecular However, it was noted that the amount of mass in the
weight of 149 and B = 60.5. Shown are the initial values, the values heaviest pseudocomponents can and will increase for the
values for B a. -.
after 15 contactinge for the sliding and discrete calculations,and the sliding case when the limit B is finite. For example, this

-
B a at five contactings, and likewise for B 1 60.5 a t 15
contactings. For an initial C7+MW = 249,it appears that
occurred with the sixth through eighth C7+ pseudocom-
ponents for initial C7+MW = 149 when the upper carbon
number bound B = 20.5and 40.5,and with the f i i h through
eighth C7+ pseudocomponents when B = 60.5. This
one has to impose a bound B > 80.5 to accomplish this.
Given the above results, we wish to address two
questions:
disappears for the sliding case as B a. -
anomaly, which cannot occur with the discrete case,
In comparing Figures 5 and 6,there is not as much a
1. Why do the sliding and discrete results differ? shift in the normalized mole fraction curve peak with
2. Which result is "correct"? (It is recognized that pseudocomponent number for upper carbon number
whereas neither result may be "exact", one may be formally bound B = 60.5 as for B = 20.5. The sliding case
more correct than the other.)
Some preliminary insights to the first question can be
obtained by examining how the distribution of the
-
distributions for finite B's will be closer to that of the case
"Sliding (B m)" as B gets larger, which is logically to be
expected. The sliding distribution is flatter after 15
normalized C7+ mole fractions shifts as the coatactings contactings than the discrete distribution for B = 60.5, as
proceed. Figures 5 and 6 illustrate these distributions for before with B = 20.5.
the initial C7+ MW = 149, for B = 20.5 and 60.5, Figures 7 and 8,with the C7+ initial MW now equal to
respectively. Smoothed curves have been conatructed 249,are analogous to Figures 5 and 6. The differences in
through the eight normalized mole fractions in each case. the evolution of the pseudocomponent normalized mole
Interestingly, the initial mole fractions of the pseudocom- fraction distributions with contactings are more pro-
ponents that represent an exponentialdistribution exhibit nounced, which is consistent with the larger property
a maximum, which is at the second or third pseudocom- differences seen in Figures 1-4. Again, the distributions
ponent. For f i i t e valuesof B, both the discrete and sliding for the sliding cases are flatter than those for the discrete
mole fraction distributions shift in a logical manner, with cases. The dramatic divergences of results in Figures 1-4
the presence of the heavier pseudocomponents increasing
at the expense of the lighter ones. The "Sliding ( B 05)"
mole fraction curve is invariant with the number of
- are therefore not surprising.
We can now answer the fiist question as to why the
discrete and sliding results differ. The mechanics of the
contactings for the sliding computation, as pointed out discrete computation are straightforward. Given an
earlier. assumed initial exponentialdistribution of the C7+portion
Ind. Eng. Chem. Res., Vol. 32, No. 8, 1993 1771
0.5 I are already becoming prominent at five contactings and
1 are more sensitive to the C7+upper carbon number bound
B.

Nomenclature
A = lower carbon number bound
B = upper carbon number bound
C = upper bound of the reduced carbon number variable
F = distribution function
3
U
0.1 t' /
I /' \ \ --_ I
I = carbon number
MW = molecular weight
w = quadrature weighting factor
x = quadrature root
1 2 3 4 5 0 7 8 y = reduced carbon number variable
C7+ Pseudocomponent z = dummy variable
cy = exponential distribution decay parameter
Figure8. C7+mole fractions (normalized)for an initial C7+molecular
weight of 249 and E = 80.5. Shown are the initial values, the values Subscripts
after 15 contactinga for the sliding and discrete calculations, and the
values for E -m.
+
i = species
1 = liquid phase
of oil A, one gets a distribution of normalized C7+ mole
fractions which shifts with the number of contactings. The Literature Cited
distribution of these normalized mole fractions is not Abramowitz, M., and Stegun, 1. A., Eds. Handbook of Mathematical
consistent any longer with an exponential distribution after Functions with Formulas, Graphs, and Mathematical Tables;
the first contacting. The MWI information is derived Dept. of Commerce: Washington, DC, 1972; loth printing with
information and not used to adjust later C7+distributions. corrections, p 923.
In contrast, in the sliding property approach, the C7+ Behrens, R. A.; Sandler, S. I. The Use of SemicontinuousDescriptions
distribution is always designated to be exponential for the to Model the C7+ Fraction in Equation of State Calculations.
liquid phase (tobe contacted) and enters each equilibrium SPE Reservoir Eng. 1988,3,1041-1047.
Cotterman, R. L.;Prausnitz, J. M. Flash calculations for Continuous
contacting coupled to the MWIof the previous contacting. or Semicontinuous Mixtures Using an Equation of State. Znd.
This is an additional constraint on the computation that Eng. Chem. Process Des. Dev. 1986,24,434-443.
creates a bias in the computation, one that in the context Cotterman, R. L.;Prausnitz, J. M. Continuous Thermodynamics for
of multiple contactings causes divergences ( as illustrated Phase-Equilibrium Calculations in Chemical Procese Design. In
in Figures 1-4) between the computed results of the two Kinetic and Thermodynamic Lumping of Multicomponent Mix-
tures; Astarita, G.,Sandler, S., E&.; Elsevier: Amsterdam, 1991;
methodologies. pp 229-275.
We now address the second question concerning which Cotterman, R. L.;Bender, R.; Prausnitz, J. M. Phase Equilibria for
result is "correct". It is not just the contacting-to- Mixtures Containing Very Many Components. Development and
contacting constraint of a specified distribution (herein, Application of Continuous Thermodynamics for ChemicalProcess
Design. Znd. Eng. Chem. Process Des. Dev. 198Sa,24,194-203.
exponential) being applied that leads us to believe that Cotterman, R. L.; Dimetrelis, D.; Prausnitz, J. M. Design of
the sliding approach is flawed. Intuitively, it is an Supercritical-Fluid-ExtractionProcesses Using Continuous Ther-
appealing approach. However, as pointed out earlier, when modynamics. In Supercritical Fluid Technology; Penninger, J.
one uses six C7+pseudocomponents derived by quadrature M. L.,Radosz, M., McHugh, M. A,, Krukonis, V. J., Eds.; Elsevier:
techniques in the discrete approach for a problem con- Amsterdam, 1985b;pp 107-120.
sistingof 15contactings,one gets results that are essentially Cotterman, R. L.;Chou, G. F.; Prausnitz, J. M. Comments on "Flash
Calculations for Continuous or Semicontinuous Mixtures Using
identical with those that would be obtained using more an Equation of State". Znd. Eng. Chem. Process Des. Dev. 1986,
than six pseudocomponents, for example, using an in- 25,840-841.
definitely large number of pseudocomponents that could Du, P. C.; Mansoori, G. A. Phase Equilibrium Computational
be envisioned to approach infinity in number. Given the Algorithms of Continuous Mixtures. Fluid Phase Equilib. 1986,
premise that the initial exponential distribution correctly 30, 57-64.
represents the extremely large number of C7+ species in Du, P. C.; Mansoori, G. A. Phase Equilibrium of Multicomponent
Mixtures: Continuous Mixture Gibbs Free Energy Minimization
a "laboratory" system, then the discrete answer for n L and Phase Rule. Chem. Eng. Commun. 1987,54,139-148.
6 (--) is the correct answer to the multiple-contacting Luke,K. D.; Turek, E. A.; Kragas, T. K. Asymptotic Effecta Using
"laboratory" problem. The sliding approach produces an Semicontinuous vis-a-vis Discrete Descriptions in Phase Equi-
answer that does not asymptotically approachthis discrete librium Computations. Znd. Eng. Chem. Res. 1990,29,2101-2106.
answer for n 1 6 (+oJ). Matthews, M. A.; Mani, K. C.; Haynes, H. W. Continuous Phase
Equilibrium Thermodynamics for Sequential Operations. In
The calculation of Matthews et al. (1991)is not a severe Kinetic and Thermodynamic Lumping of Multicomponent Mix-
test of the methodology that they propose, and therefore tures; Astarita, G., Sandler, S., Eds.; Elsevier: Amsterdam, 1991;
any difficulty that may arise from it is not apparent. Their pp 307-324.
calculation is similar in severity to the computations for Shibata, S. K.; Sandler, S. I.; Behrens, R. A. Phase Equilibrium
the C7+ upper carbon number bound B = 20.5 in Figures Calculationsfor Continuous and SemicontinuousMixturea. Chem.
1 and 3 for MW = 149. Very little change in the Eng. Sci. 1987,42,1977-1988.
Vogel, J.L.;Turek,E. A.; Metcalfe, R. S.; Bergman, D. F. Applications
pseudocomponent carbon numbers takes place with each of Equations of State to Calculate Reservoir Fluid Properties.
contacting, and the sliding and discrete computationsare Fluid Phase Equilib. 1983,14,103-116.
essentially indistinguishable at five contactings. This is
not the case for a greater number of contactings and/or Received for review November 16, 1992
for higher C7+ MW's where the deviations in Figures 1-4 Accepted April 27,1993

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