Constantes de Equilibrio PDF

Tech n¡cal Publ¡cation
TP-22
Convergence Pressure and Vapor-Liquid

Equilibrium Ratios
Published by the
Gas Processors Association
June, 1999
6526 East 60th Street * Tulsa, Oklahoma 74145 Phone: 918/493-3872 Fax:
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Copyright Gas Processors Association

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No reproduction or networking permitted without license from IHS Not for Resale
~~ - ~
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"Copyright O 1999 by Gas Processors Association.

All rights reserved. No part of this report may be
reproduced without the written consent of the
Gas Processors Association."

Convergence Pressure and Vapor-Liquid Equilibrium Ratios
GPA Technical Publication

TP-22
Prepared by
Gas Processors Suppliers Association Editorial Review Board

6526 E. 60th Street
Tulsa, OK 74145
June, 1999
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Introduction
This Technical Publication, TP-22, serves to archive the GPSA Convergence Pressure Vapor Liquid1
Equilibrium Ratios (K-data) along with other K-data charts. The convergence pressure approach to handling1
composition dependency of K-values was omitted when the eleventh edition of the GPSA Engineering Data,
Book was published in 1998. The Editorial Review Board explained this change in the data book with the^
following statement:
Previous editions of this data book presented extensive sets of K-data based on the GPSA Convergence
Pressure Pk method. A component's K-data is a strong function of temperature and pressure and a weaker
function of composition. The convergence pressure method recognized composition effects in predicting K-
data. The convergence pressure technique can be used in hand-calculations, and it is still available as computer
correlations for K-data prediction.
There is now general availability of computers. This availability coupled with the more refined K-value1
correlations in modern process simulators, has rendered the previous GPA convergence pressure charts
outdated.
The convergence pressure method is presented in dual metric (SI) and English (FPS)units. This TP contains
the full explanatory text on convergence pressure from section 25 of the tenth Edition of the GPSA Engineering
Data Book (the blue books) supplemented with the SI information from the corresponding material from
section 18 in the 1980 SI Engineering Data Book (the green book). All of the standard charts are from the 1980
SI Engineering Data Book (the green book). In addition, other charts from the 1957 edition relating to acid gas
components in ethane and propane have been included.
For quick trouble-shooting and evaluation work a set of K-charts can be very helpful. They present an
illustration of the effect of temperature and pressure on K-values for light hydrocarbons. A composite set has
been retained in the eleventh edition of the data book for both the SI and FPS units.
The charts represent decades of careful comprehensive research directed by GPA and GPSA. Accordingly, the
Associations decided that they are to be retained as a resource available to the industry and academia.
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Also included in this TP are K-data for High-Boiling Hydrocarbons (Poettman charts), some hydrogen sulfide
binanes and hydrogen binaries,
The Equilibrium or K-value curves were first published in chart form by the NGAA and NGSMA (predecessors
to the present day GPA and GPSA) in the early 1950's. Much of the basic data was compiled in tabular form
under the direction of Dr. G. G. Brown, Dean of Engineering,University of Michigan. The data were taken
from numerous published articles and unpublished experimental data. From these tabular data the first charts to
be used by the industry were prepared by the Fluor Corporation Engineering Department under the guidance of
Blaine Kuist, C. W. Leggett and C.K. Walker. Most of the painstaking draftsmanship was done by Orville
McAdams, also of Fluor. Stuart Hadden developed the concept of convergence pressure, thereby making the
charts useful for predicting K-values in a mixture containing any number of components. The charts were first
published by the NGAA in 1955.

In anticipation of needing additional information to expand the data and improve the accuracy. NGAA
appointed the first Equilibrium Committee chaired by Elliott Organik, United Gas Corporation. Members of
the committee were C. L. DePreister, California Research Corporation; Karl Hackmuth, Phillips Petroleum
Company; James Kilmer, Stanolind Oil and Gas Company; H. H. Rackford, Humble Oil and Refining
Company; Bryon Woertz, The Pure Oil Company; and Charles Webber, Sun Oil Company.
In 1957 the charts were completely redrawn to provide data at lower temperatures and to increase the internai
consistency of the K-values. Karl Hackmuth guided the chart revision. By then Byron Woertz had assumed
chairmanship of the Equilibrium Committee. E.A. Gromatzky, The Texas Company; R. H. Jacoby, Pan
American Petroleum Company; Herbert L. Stone, Humble Oil and Refining Company; and C. J. Walters.
California Research Corporation had become members of the committee.
This committee continued to act as a clearing house for new equilibria data and correlation methods. In 1958
these charts were published as Tables of Coefficients for use with early computers. Robert Norman and
Brymier Williams presented a paper at the 57th Annual NGAA convention in Dallas April, 1958 that was the
basis for the initial work that developed these machine computations.
A set of equations was developed to represent each page in the Data Book. The NGAA prepared a
reproduction of the data from these charts in two forms - point cards and coefficient cards. The point cards
were IBM cards containing approximately 70,000 data points (pressure, temperature, composition and
convergence pressure) punches on 17,000 cards. The coefficient cards were IBM cards that contained the
coefficients for the equations used to empirically correlate the point data. This required only 432 cards because
each card contained seven coefficients. This drastically reduced the number of cards which in turn reduced the
computer storage space required.
Through the years the convergence curves have been modified and improved. They are still published in the
GPSA Engineering Data Book and represent decades of careful and comprehensive research directed by GPA
and GPSA.
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STDnGPA TP-ZZ-ENGL 1997 382qb97 00201178 1173 =
TP-22
EQUILIBRIUM RATIO (K) DATA Note that the critical data from these binary mixtures were
NOT used to adjust the critical loci of Figure 5 . Such an
The equilibrium ratio (Ki) of a component i in a multi- adjustment would necessitate complete cross-plotting and
component mixture of liquid and vapor phases is defined as the redetermination of all of the convergence pressure charts.
ratio of the mole fraction of that component in the vapor phase Use of Binary Charts - At temperatures below -100'F
to that in the liquid phase. [-73T],a light hydrocarbon system is most easily approximated
K , = - Yi as a pseudobinary. Determine the average molecular weight on
xi a methane-free basis; then interpolate the K-values between the
two binaries whose heavy component lies on either side of this
For an ideal system (ideal gas and ideal solution), this pseudocomponent. This calculation becomes poor for systems
equilibrium ratio is reduced to the ratio of the vapor pressure of with N2 content greater than 3 to 5 mole percent.
component i to the total pressure of the system.
The ternary methane-ethane-propane system is well
pi*
Ki = - defined.5 At temperatures below -75°F [-60°C], (except for the
P highest pressures 700-800 psia [4800-5500 kPa(abs)] at
This TP presents an outline procedure to calculate the liquid -75°F [-60"Cl and -100°F [-73"C]. if f=XE(Mp) /xECMi= ratio of
and vapor compositions of a two-phase mixture in equilibrium ethane mole fraction in the liquid phase of the ternary system to
using the concept of a pseudobinary system and the convergence the ethane mole fraction in the liquid phase of the methane-
pressure equilibrium charts. Discussion of CO;! separation. ethane system, then the ternary K-values can be calculated from:
alternate methods to obtain K values, and equations of state
follow. Finally, three sets of equilibrium rat¡:, charts are
log KM = log KM(P) [KM(P)IKM(E)1 Eq 3
presented:
K-values for specific binary systems

K-values of various components based on different log KP = log KP(M) log [KP(M)/KgME)l Eq 5
convergence pressures of hydrocarbon systems
Note that xE(MP) I xE(M), and KAo, denotes K-value of A in
K-values of pseudocomponents based on normal
boiling point and characterization factor the A-B binary system. These are found from pages 102 and
103. The infinite dilution KE(MP) and G,,,, are given on page
BINARY SYSTEMS DATA CHARTS 104.
The 1972 edition of the GPSA Engineering Data Book These generalizations can be made about the ternary K-
included for the first time several charts representing binary values:
combinations of N2,Cl. C,, C3,and n-C4. These data resulted Addition of propane increases the methane K-value and
from GPA-sponsored research at Rice University. Binary data decreases the ethane K-value.
with heavier components and acid gases have been added as Addition of ethane decreases the methane K-value and
revisions as they have become available. increases the propane K-value.
The propane K-value is highest when at infinite dilution
These charts are useful for low temperature (below - 100"F,
in the ternary (¡.e., a methane-ethane binary).
calculations. Below the critical temperature of
[-73"C]) The ethane K-value is highest when no propane is
methane (-1 16°F [-82"C]), the convergence pressure of a system
present (¡.e., a methane-ethane binary).
no longer has a real significance, since the K-values for heavy
components do not reach a value of 1.O. These generalizations can be extended to other ternary (or
Figure 1
Nomentclature
K = qulibrium ratio, y/x y = mole fraction in the vapor phase
L = ratio of moles of liquid to moles of total mixture Superscripts
N = mole fraction in the total mixture or system ' = pseudobinary
O = acentric factor = log Pv, - 1.o0 o0 = at infinite dilution
where. Pvr = reduced vapor pressure at Tr = 0.7
P = absolute pressure, psia [kPa(abs)] Subscripts
Pk = convergence pressure. psia [kPa(abls)] I = component
P* = vapor pressure, psia [kPa(abs)] c = critical
R = universal gas constant, (psia CU ft)Ab mole "R)[(kPa m3 ) /(kmole K)] M = methane
T = temperature, O R or OF [K or OC] E = ethane
V = ratio of moles of vapor to moles of total mixture P = propane
x = mole fraction in the liquid phase
____-
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Copyright Gas Processors Association 1

STD-GPA TP-ZZ-ENGL 1799 3824b99 0020479 30"
higher) systems: the heaviest component (propane in this case) is 0.674 v + 0.0674 (100 - v ) = 60
analogous to a "lean oil" in an absorber system. The methane- v = 87.8
ethane is acting in this case as a "natural gas" with the heaviest
The mixture consists of 87.8 moles of vapor and 13.2 moles
component (ethane) being preferentially absorbed into the "lean
of liquid.
oil" (propane), with the resulting effects on the K-values. The
liquid mole fraction of the middle (volatility) component is a
useful parameter. The user should be aware that the composition
K-VALUES CORRELATION BY
effect on K-values is very pronounced in the regions covered by
CONVERGENCE PRESSURE
the binary and ternary data systems. Accurate values can be
The convergence pressure chart representation of K-values.
obtained only by cross-plots of K-value versus composition.
used since 1957 by the GPA, provides a useful and rapid
Limiting conditions should be considered in the analysis and graphical approach for engineers. Within limits the values are
use of K-data. For example, the limits on a binary system are sufficiently accurate to satisfy many calculations required by the
defined by the vapor pressure of the pure components, as shown practicing engineer. Moreover. these charts are widely used in
by the Locus K G and Locus KSof page 102. The limits of a industry and are generally preferred over most nomographs.
ternary system are the binary systems. The charts included in this TP are a mixture of past and
The GPA/GPSA sponsors investigations iL systems of present, as shown in Figure 2.
interest to gas processors. Detailed results are given in the The Pk charts for methane, ethane, and propane are based on
annual proceedings and in various research reports and technical extensive cross plots of available experimental data. Properly
publications, which are listed in Section 1 of the Engineering used, they should represent both absorber oil and condensate
Data Book. systems adequately. Charts for components heavier than
Example 1 - Binary System Calculation propane are selected from previous editions, based on general
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experience as to whether the 1957 or 1966 edition of the

To illustrate the use of binary systerm K-value charts, Engineering Data Book gave the best results.
assume a mixture of 60 moles of methane and 40 moles of
The present convergence pressure charts do not have as
ethane at -125OF [-87"C] and 50 psia [345 kPa(abs)]. From the
chart on page 102, the K-values for methane and ethane are 10 many low temperature isotherms as in past editions. This is
and 0.35 respectively. This method is valid for either Ibmols or because no experimental data existed in these regions when the
charts were prepared. Calculations of systems at very low
kmols.
temperatures and at high convergence pressures do not have
Solution Steps much significance in hydrocarbon systems, and therefore should
not be shown.
From the definition of K-value, Eq 1 :
As an example, refer to Figure 5. Assuming methane as the
light componet and methylcyclohexane as the heavy, the critical
locus line indicates that the lowest possible temperature for a
3000 Pk is -50°F [-46OC]. This is about the practical limit in real
Y
G2= z =
0.35 systems; therefore, isotherms significantly below this would be
x c2 imaginary. This deletion of low-temperature isotherms is
intended to warn the user not to apply these charts beyond the
Rewriting
range of good practice.
The accuracy of the P, charts depends in part on how
--' yci - 0.35
'- xc1 carefully the convergence pressure has been determined. At
moderate to high values of operating pressurekonvergence
Solving pressure (ratio > 0.4), both accurate convergence pressure
determination and interpolation between P, charts can be made.
xcl = 0.0674 K-values from an equation of state are likely to be more reliable.
In the case of methane, interpolation between P, charts is a must
ycl = 0.674 to obtain accurate K-values. This is true to a lesser degree for
heavier components. The revised charts were back-calculated
Hence
from data and cross-plotted using Figure 5 as the basis of critical
locus; therefore, ali determinations of convergence pressure
xc2 = 0.9326 must be made from Figure 5.
yo = 0.326 If any other source of critical locus is substituted, the
revised charts will be less accurate in predicting the system
To find the amount of vapor in the mixture, let v denote of K-values. Recent binary data for the Cl-nC6, C1-nC,. C,-
moles of vapor. Summing the moles of methane in each phase nC6, Cz-nCIo, C3-nC6, and C3-nC7 systems allowed the addition
gives:
of their respective critical loci.

2
--A
Component Binary Convergence pressure, kPa (abc) [psia]

Data 5500 1 6900 10300 13800 20700 34500 69000
wo1 I [l@JJI [I5001 [2000] j [3000] [SOOO] (iO,OOO]
Nitrogen * O O O
Methane I
* V V V V V 1 V
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Ethylene I O O O I
Ethane i * V V V V V X X
Propylene I O O O
Propane * V V V V V X X
iso-B utane 0 O X X X X X I
n-Butane *t O O X X X X X
isoPentane I
O O X X X X X
I Octane I O i O 1 x l x I x I x X ~~
I
Nonane i x X X X X
Decane Q O X X X x , x
Hydrogen sulfide , X X
I
I
I
Carbon dioxide 1
* Binary data from Price & Kobayashi; Wichterle & Kobayashi; Stryjek. Chappelear. & Kobayashi; and Chen & Kobayashi
v Drawn for Data Book, 1972 Edition based on available data
0 Reused from Data Book, 1966 Edition Note: The charts shown in bold outline are published in the 1 1th
X Reused from Data Book, 1957 Edition edition of the data book. All charts shown in this Figure
t Prepared for Data Book. Second Revisions 1972Edition or revised are published in this Technical Publication (TP-22),as well
* * Limited to Cop concentrationof 1O mole percent of feed or less as the 10th Edition of the data book.
Method of Calculating Convergence Pressure binary K-data is recommended below the critical of methane (-
11
6'F [-82OC].
The vapor-liquid equilibrium K-value of each component in
a system is a function of the system temperature, system The convergence pressure of systems as encountered
pressure, and the composition of the vapor and liquid phase. For generally in natural gas processes is a function of the
natural gas processes, the convergence pressure can usually be temperature and the composition of the liquid phase. This
used as the parameter that represents the compasiton of the presumes that the liquid composition is known from a flash
vapor and liquid phase in equilibrium. The c.onvergence calculation using a first approximate guess for convergence
pressure is, in general, the critical pressure of a system at a given pressure. Therefore, the method of calculating convergence
temperature. pressure is an iterative procedure. This calculation procedure is
suggested.
At a given temperature, as the system pressure increases, the
K-values of ail components of the system converge to unity Step 1: Assume the liquid phase composition or make an
when the system pressure reaches the convergence pressure. In approximation. (If there is no guide, use the total feed
other words, it is the pressure for a system at a given temperature composi ton.)
when vapor-liquid separation is no longer possible. Naturally, it Step 2: Identify the lightest hydrocarbon component which
is equally impossible to have a vapor-liquid separation at a given is present at least 0.1 mole 480 in the liquid phase.
temperture i n which the system pressure is greater than the
convergence pressure. Step 3: Calculate the weight average critical temperature
and critical pressure for the remaining heavier components to
Although the convergence pressure charts include values for form a pseudobinary system. (A shortcut approach good for
methane, ...n-butane ai - 120°F [-84"C] and lower, the use of the most hydrocaròon systems is to calculate the weight average T,
only.)

3
~~~ ~
~
~
S T D I G P A TP-22-ENGL 1999 3 8 2 q b î 5 002OLi81 Tbö m
Step 4: Trace the critical locus of the binary consisting of When the convergence pressure so determined is beweein
the light component and pseudoheavy component. When the the values for which charts are provided, interpolation between
averaged pseudoheavy component is between two real charts may be necessary depending on how close the operating
hydrocarbons. an interpolation of the two critical loci must be pressure is to the convergence pressure.
made. If K-values do not change rapidly with P, ( P p > P ) then the
Step 5: Read the convergence pressure (ordinate) at the set of charts nearest to the calculated PI; m a y he used.
temperature (abscissa) corresponding to that of the desired flash Otherwise, a cross-plot of K values versus P,. all at constant
conditions, from Figure 5. temperature and pressure, must be constructed for interpolation.
Step 6: Using the convergence pressure determined at Step Aromaticity Corrections - These K-chrirrs for which Pk =
5 , together with the system temperature and systrm pressure, 800, 1000, and 2000 were based entirely on binary parafin
obtain K-values for the components from the appropriate hydrocarbon systems, while those for P, = 4000 and 10.000
convergence-pressure K-charts. were derived from early data on mixtures containing some
naphthenes (cycloparaffins) and aromatics. It is believed that
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Step 7: Make a flash calculation with the feed composition
small amounts of cyclic components added to mixtures of
and the K-values from Step 6, as shown in Figure 3.
paraffins do not seriously affect the K-values obtained from
Step 8: Repeat Steps 2 through 7 until the assumed and these charts. However, as the concentration of cyclics increases
calculated convergence pressures check within an acceptable the K-values are affected in a manner that is not fully accounted
tolerance, or until the two successive calculations give the same for by the convergence pressure variable.
light and pseudoheavy components check within an acceptable
tolerance.
Figure 3 SI
Example Flash Calculation at 4000 kPa (abs) and -30°C
-
Column
' I 2 3 1 4 1 5 6 1 7 1 8
Feed Gas Trial values of L Final L = 0.030 Merhane-free basis
:omponent I Composition
I
KI tor L = 0.02 L = 0.06 L = 0.04 1 Liquid 1 Vapor
m s s trac
Pk = 2000 Ni
Ni - Ni MW kg liquid
liquid
T,. K ' P,. kPa (absi
Ni 113800 kPaíabs) L+VKi .+VK, L+V& 7x9
0.90 I O 3.2 0.28549 0.29368 C.28952 3.1- 0.28749 , 0.91997
0.0106 1.14 0.00932 0.00937 c.00934 I . 13580 0.00933 0.01064 44.01 0.4106 0.0093 305.2 7382
0.0499 0.41 0.11830 O. 1 1203 O. 1 1508 0.42770 0.1 1667 0.01183 30.07 3.5083 0.079X 30S.J 4880
0.0187 0.097 0.16252 0.12369 o. 14047 O. 12409 O. I5070 0.01462 44.10 6.6459 0.1511 369.8 424s
0.0065 0.038 0.11356 0.06791 0.08499 0.06686 0.09722 0.00369 58.12 5.6504 o. 1284 408.1 36111
0.0055 0.024 0.10340 0.05451 0.01138 0.05328 0.08446 ~ 0.00203 58.12 4.9088 0.1 I I6 425.2 3797
0.0017 0.0088 0.05939 0.02490 0.03509 0.03854 0.04411 0.00039 72.15 3.1825 0.0723 460.4 3381
0.0019 0.0062 0.07286 0.02886 0.04135 0.03641 0.05276 0.00033 72.15 3.8066 0.0865 469.6 3369
0.0029 0.0019 O. 13265 0.04694 0.06934 0.03184 0.09107 O.WO17 86.18 7.8484 0.1784 507.4 3012
-
0.0023 O.ooo66 0.1 I140 0.03794 0.05661 0.03064 0.07506 0.ms 107.0 8.0314 O. 1826 554.5 261 I
2= 1.16889 0.79983 0.91317 I .O0887 0.99972 43.9929 1 .oooo 3542
'Avaagc of nC, + nC, properties End of flash calculation

-! Calculation to confirm PI. 448.6li
-273.2
175.4OC
Figure 3 FPS -
Example Flash Calculation at 600 psia and -20°F
Column
3 1 4 5 6 7 1 8
Trial values of ral L = 0.0210 Methane-free basis
__ - .._-._
:omponeni Composition
IT- -q-T
L=O.O2 I L=0.06
L+VKi L+VK,
L = 0.04
L+VK,
Ni
L+VK,
MW Ib liquid
la9
mass frac.
liquid
Tc. "U Pc. psia
i
~~
~
CI 0.9010 3.2m 0.28549 0.29368 0.28952 3.14060 0.28689 0.91 804

CO2 0.0106 1.13000 o.oO940 0.00945 0.00942 1.12649 0.00941 0.01063 44.01 0.4141 0.0093 557.6 1071.0
CZ 0.0499 0.4oooO 0.12112 0.11445 0.11769 0.4 I620 O. I 1989 0.04796 30.07 3.6052 0.08 I4 -549.6 706.5
c3 0.0187 O. 10500 0.15216 0.11783 O. I3281 o. I29 17 0.14478 0.01520 44.10 6.3846 0.1441 665.8 616.0
iC1 0.0065 0.01500 0.10140 0.06354 0.078 I3 0.07079 0.09183 0.00413 58.12 5.3370 o. I204 734.2 527.9
nC4 0.0045 0.03300 0.08598 0.04944 0.06278 0.0591 I 0.07613 0.00251 58.12 4.4247 0.0999 765.3 550.6
ic, 0.00 I7 0.01300 0.05192 0.02354 0.03239 0.03965 0.04288 0.00056 72. I5 3.0935 0.0698 828.8 490.4
nC3 0.0019 0.01000 0.06376 0.02738 0.03831 0.03673 0.02173 0.00052 72.15 3.7322 0.0842 845.5 4ö8.6
0.0029 0.00290 0.12696 0.04623 0.06778 0.02982 0.09724 0.00028 86.18 8.3805 0.1891 913.3 436.9
-
cb
T,+ 0.0023 O.WO55 0.1 I198 0.03801 0.05675 0.02754 0.08353 0.00005 107.00 8.9377 0.2017 998. I 378.7
Taala 1.11017 0.78354 0.88559 1.00431 0.99988 44.3096 I .oooo 813.11"R SOY.?
A v m g e of nC, inCKproperties End of flash calculation Calculation IO confirm Pk -459.7
-
-I 3M.I"F

4
The GPA has sponsored research to study these effects in A situation of reproducible sieady state condition> in ;1 piecc
absorber systems, and the experimental results of this work are of equipment does not necessarily imply that c l a s s i ~ i ~ l
published.' In general. the data show that the presence of thermodynamic equilibrium exists. If the steady composition
aromatics in paraffin mixtures serves to increase the K-values of differs from that for equilibrium, the reason can be the result of
the paraffins. time-limited mass transfer and diffusion rates. This wming is
made because i t is not at all unusual for flow rates through
HIGH BOILING OIL FRACTIONS equipment to be so high that equilibrium is not attained or even
closely approached. In such cases. equilihrium flash
At the end of the convergence pressure series of charts is calculations as described here fail to predict conditions in the
appended a small set of K-charts developed by Poettman and system accurately, and the K-values are suspected for this
Mayland2 for high boiling petroleum fractions. They are useful failure-when in fact they are not at fault.
for low pressure, high temperature flash calculations on heavy Eq. 6
Yi
Ki = -
oils, such as in the reboiler of an absorber oil stripper or an
atmospheric crude distillation tower, provided information on Xi
ASTM or IBP of the oil is available. At pressures below 100 L + V = 1.0 Eq. 7
psia [690 kPa (abs)] K s from these charts are fairly compatible
with those from the convergence pressure series, if a plot of K By writing a material balance for each component in the
vs. component boiling point is made. The reader is referred to liquid, vapor, and total mixture, one may derive the flash
White and Brown3 and Grayson and Streed4 for additional data. equation in various forms. A common one is.
N.
DATA FOR NONHYDROCARBONS xxi = zI = 1.0 Eq. 8
L + VK,
Hydrogen Sulfide Other useful versions may be written as
Since the hydrocarbon charts for Pk = 4000 were also
Eq. 9
eliminated, the Pk = 4000 chart for H2S was reduced to Pk =
3000 by simply adjusting the isotherms at pressures near 3000
psi. The H2S chart for Pk = 1000 was reused from the 1957 KiNi
xyyi= Eq. 10
edition of the Engineering Data Book. L + VK,
~
At the phase boundary conditions of bubble point (L = 1 .OO)

Nitrogen
and dew point (V = 1.00). these equations reduce to
The convergence pressure charts for N2 which are based
I;Ki Ni = 1.0 (bubble point) Eq. 11
largely on binary and ternary data from the University of Texas
were retained from the 1966 editon of the Engineering Data and
Book, as illustrated in Figure 2. mi/Ki = i .O (dew point) Eq. 12
--`````-`-`,,`,,`,`,,`---
Data for N2-CH4 and N2-C2H6 are given on pages 109- 1 1O. These are often helpful for preliminary calculations where
These data, and data on the ternary, show that the K-values in the phase condition of a system at a given pressure and
this system show strong compositional dependence. In this temperature is in doubt. If CK, Ni and LNi/K, are both greater
system, the component order is N2-CH4-C2H6,and the K-values than I .O, the system is in the two phase region. If XK,Ni is less
are functions of the amount of methane in the liquid phase. For than 1.O, the system is all liquid. I f If ZKi Ni is less than 1 .O,
example, at -190°F [-123"C] and 300 psia [2070 kPa(abs), the the system is ail vapor.
K-values vary from:
Example 2-FF'S - A typical high pressure separator gas is
N2 CH4 C2H6 used for feed to a natural gas liquefaction plant, and a
10.2 0.824* 0.0118 preliminary step in the process involves cooling to -20°Fat 600
3.05 0.635 0.035* psia to liquefy heavier hydrocarbons prior to cooling to lower
temperatures where these components would freeze out as
where * indicates the limiting infinite dilution K-value. See solids. Estimate the convergence pressure Pk.
TP-45for the data on this ternary.
Solution Steps - The feed gas composition, shown in
FLASH CALCULATION PROBLEM Figure 3-FPS,column 1, is similar to that used in the enthalpy
and entropy problems in Section 24 of the Engineering Data
To illustrate the calculation of multicomponent vapor-liquid Book. Pk is first estimated to be 2000 psia and K's are
equilibrium using the flash equations and the K-charts, a determined as in column 2. Then the flash equation 8 is solved
problem is worked out in detail below. for three estimated values of L as shown in columns 3, 4, and 5.
The variables are defined in Figure I. Note that the K-value By plotting estimated L versus calculated Exi, the correct value
fo L where Zxi = 1.00 is L=0.027,whose solution is shown in
is implied to be at thermodynamic equilibrium.
columns 6 and 7. The gas composition is then calculated using

--`````-`-`,,`,,`,`,,`---
yi = K,xi in column 8. This "correct" value is used for purposes 13) of the pseudo heavy component. calculate the mash averapt.
of illustration. It is not a completely converged solution, for xi = critical temperature and pressure using the T,, Irnd Pi,I I I
1.00431 and yi = 0.99988, columns 7 and 8 of Figure 3-FPS. columns 10 and 11; the results are shown at the bottom of those
This error will be too large for many applications. To check the columns. By referring to Figure 3-SI. the calculated T,' o t
convergence pressure assumption. the components heavier than 175.4"C is seen to fail between n-butane and n-pentane. and the
methane in the liquid are converted to a weight fraction basis as calculated P,' falls in line with the other paraffin hydrocarbons.
shown in columns 10 and 11 using the molecular weights in By interpolation, as follows. the critical pressure for the pseudo
column 9. Using this composition (column 1 1 ) of the binary, or the convergence pressure. may be calculated at -30°C
pseudoheavy component, calculate the weight average critical without actually sketching in a new locus:
temperature and pressure using the Tci and PCi in columns 12
and 13; the results are shown at the bottom of those columns.
By referring to Figure 5 , the calculated T c of 354°F is seen to
fall between n-butane and n-pentane, and the calculated P c falls All the Pks are read from the loci at -30°C and the prime
in line with the other paraffin hydrocarbons. By interpolation, as quantitites, Tcx' and Pkx'. refer to the pseudo binary. Thus.
follows, the critical pressure for the pseudobinary, or the
convergence pressure, may be calculated at -20°F without (448'6 - 425.2) (1 3800 - i 1700)+ 1700
actually sketching in a new locus: (469.6 - 425.2)
Eq. 13
23.4 (2100) + 11700 = 12800 kPa
44.4
All the Pks are read from the loci at -20°F and the prime 12800
quantitites, TCxand P'kx, refer to the pseudobinary. Thus = 1856 psia
6.895
-
(813.8 765.6)
(2000 - 1700) + 1700 This confirms the assumed Pk = 2000 closely enough for
P'k = this illustration. The more closely the operating pressure
(845.3 - 765.6)
approaches convergence pressure the more accurately the
48.2 calculated Pk must check the assumed Pk because in this region,
PIk= -(300) + 1700 = 1881 psia the K-values are most sensitive to the Pk value used.
79.7
Example 3-FPS- Dew Point Calculation
This confirms the assumed Pk = 2000 closely enough for
this illustration. The more closely the operating pressure As gas stream at 100°F and 800 psia is being cooled in a
approaches the convergence pressure the more accurately the heat exchanger. Find the temperature at which the gas starts i o
calculated Pk must check the assumed Pk because in this region, condense.
the K-values are most sensitive to the Pk value used.
Solution Steps - The approach to find the dew point of the
Example 2-SI- A typical high pressure separator gas is gas stream is similar to the last example. Assume a convergence
used for feed to a natural gas liquefaction plant, and a pressure of 1000 psia. The equation for dew point condition
preliminary step in the process involves cooling to -30°C at (CNi/Ki=l.O) is solved for two estimated dew point temperatures
4000 kPa (abs) to knock out heavier hydrocarbons prior to as shown in Figure 4-FPS. By interpolation. the temperature at
cooling to lower temperatures where these components would which LNi/Ki = 1.0 is estimated at -44°F. To check the
freeze out as solids. Estimate the convergence pressure Pk. convergence pressure, assume the corresponding saturated liquid
consists largely of the heaviest componet, propane. This agrees
Solution Steps - The feed gas composition. shown in
with the fact that the First condensed liquid droplet from any gas
Figure 3 SI, column I , is similar to that used in the enthalpy and
stream is the heaviest component in that stream. From Figure 5 ,
entropy problems in Section 24 of the Engineering Data Book.
the convergence pressure at -44°F for the pseudoheavy
Pk is first estimated to be 2000 psia (1 3800 kPa) and K's are read
component, propane, is 1240 psia. This is close to the assumed
off as in column 2. Then the flash equation 8 is solved for three
convergence pressure of 1O00 psia.
estimated values of L as shown in columns 3, 4 and 5 . By
plotting estimated L versus calculated L xi, the correct value of Example 3-SI -Dew Point Calculation
L where C xi = 1.00 is L = 0.030, whose solution is shown in
A gas stream at 40°C and 5500 kPa (abs) is being cooled in
columns 6 and 7. The gas composition is then calculated using
a heat exchanger. Find the temperature at which the gas starts to
yi = Kixi as in column 8. This "correct" value is used for
condense.
purposes of illustration. It is not a completely converged
solution. for xi = 1.0089 and yi = 0.99972, columns 7 and 8 of Solution Steps -The approach to find the dew point of the
Figure 3-SI. This error will bè too large for many applications. gas stream is similar to the previous example. The equation for
To check the convergence pressure assumption. the components dew point condition (ZNi/Ki = 1.0) is solved for two estimated
heavier than methane in the liquid are converted to a mass dew point temperatures as shown in Figure 4-SI. By
fraction basis as shown in columns 12 and i 3 using the interpolation, the temperature at which cNi/Ki = i .O is estimated
molecular masses in column 9. Using this composition (column at -4 1.4"C.

6
Figure 4 FPS
Dew Point Calculation at 800 psia
1
Column
1 -
2 -
3
-
Feed P, = loOO. T = -50°F P, = 1000, T = -40°F
Component Ni Ki -
Ni Ki -
Ni
Ki Ki
CH4 0.854 i .420 0.601 1.450 0.589
CO2 0.051 0.790 0.065 0.834 0.061
C2H6 0.063 0.440 0.143 0.480 0.131
C3H8 0.032 0.145 0.221 0.158 0.203
E= 1.o00 1.O30 0.984
k o 2calculated as 4K,-, G2
Linear interpolation: Tdew = -50 + 1-50 (-4011 -
Alternatively iterate until Z N i 6 = 1.O
Figure 4 SI
Dew Point Calculation at 5500 kPa (abs)
Column
1 -
2 - - 5
--`````-`-`,,`,,`,`,,`---
3 4
Feed Estimated T = -45°C Estimated T = -40°C
Component Ni Ki -
Ni Ki -
Ni
K; K:
L
CH4 0.854 2.73 0.313 2.75 0.31 1

CO2 0.051 0.866 0.059 0.9 1O 0.056
C2H6 0.063 0.275 0.229 0.300 0.21 o
C3H8 0.032 0.070 0.457 0.080 0.400
2= 1.o00 1 .O58 0.977
&o2 calculated as 4 QI G2
Linear interpolation: Tdew = -40 i-40- (-4511 - ( ~=-41.4"C ~ ~ ~ ~
Alternatively iterate until Z NiKi = 1 .O
Note that the heaviest component is quite important in dew Later, experience showed that at low concentrations of CO2, the
point calculations, since it essentially determines the rule of thumb
convergence pressure. For more complex mixtures, the
characterization of the heavy fraction as a pseudocomponent
such as hexane or octane will have a significant effect on dew
point calculations. could be used with a plus or minus 10% accuracy.
Developments in the use of CO2 for reservoir drive have led to
Carbon Dioxide extensive investigations in CO, processing. See the more recent
GPA research reports (listed in Section 1 of the Engineering
Early conflicting data on CO, systems was used to prepare Data Book) and the Proceedings of GPA conventions. The
convergence pressure (Pi, = 4000)charts for the 1966 Edition. reverse volatility at high concentration of propane and/or butane

has been used effectively in extractive distillation to effect CO2 hydrocarbon components are necessary in the Redlich-Kwong
separation from methane and ethane.z2 In general, CO, lies equation to predict the K-values accurately when high
between methane and ethane in relative volatility. concentrations of non-hydrocarbon components are present.
They are especially important in CO, fractionation processes.
Separation of CO2and Methane and i n conventional fractionation plants to predict sulfur
See Section 16, Hydrocarbon Recovery, of the 11th Edition compound distribution.
of the GPSA Engineering Data Book. The Chao-Seader correlation' uses the Redlich-Kwong
C02-Ethane Separation equation for the vapor phase, the regular solution model for
liquid-mixture non-ideality, and a pure-liquid property
See Section 16, Hydrocarbon Recovery of the 11th Edition correlation for effects of component identity. pressure. and
of the Engineering Data Book. temperature in the liquid phase. The correlation has been applied
Separation of CO2 and H2S to a broad spectrum of compositions at temperatures from -50'F
[-46"C] to 300°F [150°C] and pressures to 2000 psia [13.8
See Section 16, Hydrocarbon Recovery of the 1lth Edition MPa(abs)]. The original (P,T) limitations have been reviewed.]?
of the Engineering Data Book.
Prausnitz and Chueh have developed16 a procedure for high-
OTHER K-VALUE PROCEDURES pressure systems employing a modified Redlich-Kwong
equation for the vapor phase and for liquid-phase
Numerous procedures have been devised to predict K- compressibility together with a modified Wohl-equation model
values. These include state equations, combinations of state for liquid phase activity coefficients. Complete computer
equations with liquid theory or with tabular data, and program listings are given in their book. Parameters are given
corresponding states correlations. This section describes several for most natural gas components. Adler et al. also use the
of the more popular procedures currently available. It does not Redlich-Kwong equation for the vapor and the Wohl equation
purport to be all-inclusive or comparative. form for the liquid phase.6
State equations have appeal for predicting thermodynamic The corresponding states principlelo is used in all the
properties because they provide internally consistent values for procedures discussed above in that the behavior of all substances
all properties in convenient analytical form. Two popular state is assumed to follow the same equation forms and equation
equations for K-value predictions are the Benedict-Webb-Rubin parameters are correlated versus critical properties and acentric
(BWR) equation and the Redlich-Kwong equation. factor. An alternate corresponding states approach is to refer the
behavior of all substances to the properties of a reference
The original BWR equation17 uses eight parameters for each
substance, these properties being given by tabular data or a
component in a mixture plus a tabular temperature dependence
highly accurate state equation developed specifically for the
for one of the parameters to improve the fit of vapor-pressure
reference substance.
data. This original equation is reasonably accurate for light
paraffin mixtures at reduced temperatures of 0.6 and above.* The deviations of other substances from the simple critical-
The equation has difficulty with low temperatures, non- parameter-ratio correspondence to the reference substance are
hydrocarbons, non-paraffins, and heavy paraffins. then correlated. Mixture rules and combination rules, as usual,
extend the procedure to mixture calculations. Leland and co-
Improvements to the BWR include additional terms for workers have developed9 this approach extensively for
temperature dependence, parameters for additional compounds, hydrocarbon mixtures.
and generalized forms of the parameters.
"Shape factors" are used to account for departure from
Starling20 has included explicit parameter temperature simple corresponding states relationships, with the usual
dependence in a modified B W R equation which is capable of reference substance being methane. The shape factors are
predicting light paraffin K-values at cryogenic temperatures. developed from PVT and fugacity data for pure components.
The Redlich-Kwong equation has the advantage of a simple The procedure has been tested over a reduced temperature range
--`````-`-`,,`,,`,`,,`---
analytical form which permits direct solution for density at of 0.4 to 3.3 and for pressures to 4000 psia r27.6 MPa(abs)].
specified pressure and temperature. The equation uses two Sixty-two components have been correlated including olefinic,
parameters for each mixture component, which in principle naphthenic, and aromatic hydrocarbons.
permits parameter values to be determined from critical The Soave Redlich-Kwong (SRK)I3 is a modified version of
properties. the Redlich-Kwong equation. One of the parameters in the
However, as with the BWR equation, the Redlich-Kwong original Redlich-Kwong equation, a, is modified to a more
equation has been made useful for K-value predictions by temperature dependent term. It is expressed as function of the
empirical variation of the parameters with temperature and with acentric factor. The SRK correlation has improved accuracy in
acentric factor l9 and by modification of the parameter- predicting the saturation conditions of both pure substances and
combination rules. l 5 ~l 9 Considering the simplicity of the mixtures. It can also predict phase behavior in the critical region,
Redlich-Kwong equation form, the various modified versions although at times the calculations become unstable around the
predict K-values remarkably well. critical point. Less accuracy has been obtained when applying
the correlation to hydrogen-containing mixtures.
Interaction parameters for non-hydrocarbons with

Provided by IHS under license with GPA 8
~
STDmGPA TP-ZZ-ENGL 1799 3824b97 002048b 547' a
Peng and Robinson14 similarly developed a two-constant a=a,a

Redlich-Kwong equation of state in 1976. In this correlation, the
attractive pressure term of the semi-empirical van der Waals
equation has been modified. It accurately predicts the vapor
a, = 0.42747 (q)
pressures of pure substances and equilibrium ratios of mixtures.
In addition to offering the same simplicity as the SRK equation,
the Peng-Robinson equation is more accurate in predicting the m = 0.48 + 1.574 o - 0.176 02
liquid density.
In applying any of the above correlations, the original
critical/physical properties used in the derivation must be
b = 0.08664 (7)
inserted into the appropriate equations. One may obtain slightly Peng Robinson27
different solutions from different computer programs, even for
the same correlation. This can be attributed to different iteration
23- (1 - B) Z2+ (A - 3B* - 2B) Z - (AB - B* - B3) = O
techniques, convergence criteria, initial estimation values, etc.
Determination and selection of interaction parameters and
selection of a particular equation of state must be done carefully,
considering the system components, the operating conditons, etc.
EQUATIONS OF STATE
Refer to original papers for mixing rules for
multicomponent mixtures.
van der Waals"
23 - (1 + B) 2 2 + AZ - A B= O m = 0.37464 + 1.54226 o - 0.26992 a2
aP
A= -
R2T2 b=0.0778 >
:(-
bP
B= -
RT Benedict-Webb-Rubin-Starling(BWRS)20-25
27 R*T2, C D E
a= B,RT-A,-o+o-o
64 Pc P=-
V
+
T2 T3 T'l
b= -
RTC
pc
+ (bRT-a--$-)$+CX (a+$) 1
--`````-`-`,,`,,`,`,,`---
V6
Redlich-Kwong" - YN2
Z3 - Z2 + ( A - B - B2) Z - AB = O
v3
aP
A= -
~2~2.5
REFERENCES AND BIBLIOGRAPHY
B= - bP
1. Wilson, G. M., Barton, S.T., NGPA Report RR-2: "K-
RT
a = 0.42747 (+) R2T 2.5 Values in Highly Aromatic and Highly Naphthenic Real
Oil Absorber Systems," (197 I).
2. Poettman. F. H., and Mayland, B. J.. "Equilibrium
Constants for High-Boiling Hydrocarbon Fractions of
Varying Characterization Factors," Petroleum Refiner 28.
101-102, July. 1949.
Soave Rediich-Kwong (SRK)13
3. White, R.R., and Brown, G. G., "Phase Equilibria of
Z3- Z2 + (A - B - B2 ) Z - AB = O Complex Hydrocarbon Systems at Elevated Temperatures
aP and Pressures," Ind. Eng. Chem. 37, 1162 (1942).
A= -
R ~ T ~ 4. Grayson, H.G.,and Streed, C. W., "Vapor-Liquid
bP Equilibria for High Temperature. High Pressure Hydrogen-
B= - Hydrocarbon Systems," Proc. 6th World Petroleum Cong.,
RT
Frankfurt Main, III, Paper 20-DP7, p. 223 (1963).

5. Chappelear, Patsy, GPA Technical Publication TP-4, "Low Hydrocarbons and Their Mixtures,'' Chem. Eng. Prog. 47.
Temperature Data from Rice University for Vapor-Liquid 419-422 (1951); J. Chem. Phys. 8.334 (1940).
and P-V-T Behavior," April (1 974).
26. van der Waals, J., "Die Continuitat des Gasformigen und
6. Adler, S. B., Ozkardesh, H., Schreiner, W. C., nussigen Zustandes," Barth, Leipzig ( 1899).
Hydrocarbon Proc., 47 (4) 145 (1968).
27. Peng, D.Y., Robinson, D. B.. "A New Two-Constant
7. Chao, K. C., Seader, J. D., AIChEJ, 7,598 (1961).
Equation of State," Ind. Eng. Chem. Fundamentals 15. 59-
8. Bamer, H. E., Schreiner, W. C., Hydrocarbon Proc., 45 (6) 64 (1976).
161 (1966).
Leach, J. W., Chappelear, P. S..and Leland, T.W., "Use of
ADDITIONAL REFERENCES
9.
Molecular Shape Factors in Vapor-Liquid Equilibrium See listing in Section I of the Engineering Data Book for
Calculations with the Corresponding States Principle," GPA Technical Publications (TP) and Research Reports (RR).
AIChEJ. 14,568-576 (1968). Note that RR-64,RR-77, and RR-84provide extensive evaluated
10. Leland, T. W., Jr., and Chappelear, P. S.,"The references for binary, ternary. and multicomponent systems.
Corresponding States Principie-A Review of Current Also as a part of GPNGPSA Project 806. a computer data bank
Theory and Practice," Ind. Eng. Chem. 60, 15-43 (July is available through the GPA Tulsa office.
1968); K.C.Chao (Chairman), "Applied Another extensive tabulation of references only is
Thermodynamics," ACS Publications, Washington, D.C., available from Elsevier Publishers of Amsterdam for the work of
1968, p. 83. E. Hala and I. Wichterle of the Institute of Chemical Process
I l . Bamer, H. E., Pigford, R. L., Schreiner, W. C.. Proc. Am. Fundamentais, Czechoslovak Academy of Sciences, Prague-
Pet. Inst. (Div. Ref.) 46 244 (1966). Suchdol. Czechoslovakia.
12. Lenor, J. M., Koppany, C. R.. Hydrocarbon Proc. 46,249 Also, Hiza, M. J., Kidnay, A. J., and Miller. R . C.,
(1967). Equilibrium Properties of Fluid Mixtures Volumes I and II.
IFyPienum, New York, 1975. See Fluid Phase Equilibria for
13. Soave, Giorgio, "Equilibrium Constants from a Modified
various symposia.
Redlich-Kwong Equation of State," Chem. Eng. Sci. 27,
1 197-1203 (1972).
CHARTS FOLLOW AS LISTED BELOW
14. Peng, D.Y., Robinson, D. B., Ind. Eng. Chem.
Fundamentals 15 ( 1976). Convergence Pressure Charts:
80W to 10000# pages I l through 101
15. Spear, R. R., Robinson, R. L.. Chao, K. C., IEC Fund., 8
(1) 2 (1969). Binaries:
16. Prausnitz, J. M., Cheuh, P. L., Computer Calciilations for Pages 102 - 1 1 1
High-pressure Vapor-Liquid Equilibrium, Preiitice-Hall Methane-Ethane
(1968). Methane-Propane
Methane-Ethane & Methane-Propane Infinite Dilution
17. Benedict, Webb, and Rubin, Chem. Eng. Prog. 47,419
Methane-n-Butane
( 195 1 ).
Methane-n-Pentane
18. Wilson, G. M., Adv. Cryro. Eng., Vol. II, 392 (1966). Methane-n-Hexane
19. Zudkevitch. D., Joffe. J.. AIChEJ., 16 ( I ) 112 (1970). Methane-n-Heptane
Nitrogen-Methane
20. Starling, K. E., Powers, J. E., IEC Fund., 9 (4) 531 (1970).
Nitrogen-Ethane
21. Hwang, S . C., Lin. H.M.. Chappelear. P. S., and Methane-Carbon Dioxide
Kobayashi, R., "Dew Point Values for the Methane Carbon
Dioxide System," GPA Research Report RR-21 (1976). Poettmann Charts:
Pages 112 through 117
22. Price, B. C., "Looking at COz Recovery", Oil & Gas J., p.
48-53 (Dec. 24, 1984). 1957 Engineering Data Book
Hydrogen Sulfide-Ethane 118
23. Nagahana, K., Kobishi, H., Hoshino, D.,and Hirata, M.,
Hydrogen Sulfide-Propane 119
"Binary Vapor-Liquid Equilibria of Carbon Dioxide-Light
Hy drogen-Ethane 120
Hydrocarbons at Low Temperature," J. Chem. Eng. Japan
Hydrogen-Propane 121
7, No. 5, p. 323 (1974).
Hydrogen-Isobutane 122
24. Redlich, O.. Kwong, J. N. S., Chem. Rev. 44,233 (1 949). Hydrogen-n-Bu tane 123
Hydrogen-Octane through Dodecane 124
25. Benedict. M.. Webb, G. B., Rubin, L. C., "An Empirical Hydrogen-Benzene 125
Equation for Thermodynamic Properties of Light Hydrogen-Toluene
--`````-`-`,,`,,`,`,,`--- 126
10
--`````-`-`,,`,,`,`,,`---
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No reproduction or networking permitted without license from IHS 18 Not for Resale CONV. PRESS. 800 PSlA
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Tech n¡cal Publ¡cation

Convergence Pressure and Vapor-Liquid

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"Copyright O 1999 by Gas Processors Association.

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GPA Technical Publication

Gas Processors Suppliers Association Editorial Review Board

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Copyright Gas Processors Association

Copyright Gas Processors Association

K-values for specific binary systems

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experience as to whether the 1957 or 1966 edition of the

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S T D I G P A TP-22-ENGL 1999 3 8 2 q b î 5 002OLi81 Tbö m

'Avaagc of nC, + nC, properties End of flash calculation

CI 0.9010 3.2m 0.28549 0.29368 0.28952 3.14060 0.28689 0.91 804

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At the phase boundary conditions of bubble point (L = 1 .OO)

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E= 1.o00 1.O30 0.984

CH4 0.854 2.73 0.313 2.75 0.31 1

2= 1.o00 1 .O58 0.977

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STDmGPA TP-ZZ-ENGL 1799 3824b97 002048b 547' a

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PRESSURE, kPa (abs)

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S T D - G P A TP-22-ENGL 1999 I3829679 0020508 T30 II

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S T D - G P A TP-22-ENGL L999 II 3824b99 0020509 977 I

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