Separation and Purification Technology 36 (2004) 131–138

Separation of acetic acid and water by

complex extractive distillation
Zhigang Lei, Chengyue Li∗ , Yingxia Li, Biaohua Chen
The Key Laboratory of Science and Technology of Controllable Chemical Reactions, Ministry of Education,
Beijing University of Chemical Technology, Box 35, Beijing 100029, China

Received 11 December 2002; received in revised form 23 June 2003; accepted 24 June 2003

Abstract

A new separation method, complex extractive distillation, was put forward in this work for separating acetic acid and water.
Tributylamine was selected as the separating agent. The reversible chemical interaction between acetic acid and tributylamine
was verified through infrared spectra (IR) and mass chromatogram (MS) technique. The mathematics models of equilibrium (EQ)
stage with and without incorporating chemical equilibrium equations were, respectively, established to simulate the extractive
distillation column. From the comparison of simulated results with experimentally observed results, it was concluded that the
EQ stage model was accurate whether chemical equilibrium equation was incorporated or not because the chemical equilibrium
constant was small under the operation condition.
© 2003 Elsevier B.V. All rights reserved.

Keywords: Complex extractive distillation; Acetic acid; Water; Tributylamine; Equilibrium stage model

1. Introduction and easy to be operated, its energy consumption is

It is well-known that acetic acid is an important
raw material in the chemical industries. But in the
production of acetic acid, it often exists with much
water. As a high-purity of acetic acid is needed in in-
dustry, the development of effective methods for sep-
arating acetic acid and water is an urgent and very
important challenge. By now, there are three methods
commonly used for this separation, i.e. ordinary dis-
tillation, azeotropic distillation and extractive distilla-
tion [1–3]. Although the ordinary distillation is simple
∗ Corresponding author. Tel.: +86-10-64436787;
fax: +86-10-64419619.
E-mail address: licy@mail.buct.edu.cn (C. Li).
large and a lot of column trays are required. The num-
ber of column trays for azeotropic distillation is fewer
than that for ordinary distillation. But the amount of
azeotropic agent is great, which leads to much energy
consumption because the azeotropic agents must be
vaporized in the column. However, in the extractive
distillation process, the separating agents are not va-
porized and thus the energy consumption is relatively
little. Therefore, extractive distillation is an attractive
method for separating acetic acid and water, and has
been studied by some researchers.
In the extractive distillation, the selection of a suit-
able solvent is fundamental to ensure an effective and
economical design. The reported separating agents
[4,5] are sulfolane, adiponitrile, pelargonic acid,

1383-5866/$ – see front matter © 2003 Elsevier B.V. All rights reserved.
doi:10.1016/S1383-5866(03)00208-9
132 Z. Lei et al. / Separation and Purification Technology 36 (2004) 131–138

heptanoic acid, isophorone, neodecanoic acid, ace-

Nomenclature tophenone, nitrobenzene, and so on. It is evident that
å reaction volume (m3 ) the interaction between acetic acid or water and these
c number of components separating agents is mainly physical force including
C molar concentration in the liquid the van der Waals bonding and hydrogen bonding.
phase (kmol m−3 ) Herein, a new term, complex extractive distillation,
exp. experimental value is put forward, and a new solvent is selected as the
F feed flowrate (kmol h−1 ) separating agent.
H molar enthalpy (kJ kmol−1 )
Kp chemical equilibrium
L liquid flowrate (kmol h−1 ) 2. Mechanism of complex extractive distillation
M hold-up in the stage (kmol)
P stage pressure (kPa) If we select the solvent, tributylamine (bp:
Q heat duty (kJ h−1 ) 213.5 ◦ C), as the separating agent, then the following
r number of reactions reversible chemical reaction may take place in the
rj ratio of sidestream flowrate to non-aqueous solution:
interstage flowrate HAc + R3 N
R3 NH+ · − OOCCH3 (a)
R gas constant (kJ kmol−1 K−1 )
Rk,j reaction rate (kmol m−3 s−1 ) where HAc, R3 N and R3 NH+ · − OOCCH3 represent
S flowrate of the sidestream (kmol h−1 ) acetic acid, tributylamine and the salt or complex
t time (h) formed by the reaction, respectively. The complex
T temperature (◦ C or K) can dissociate in the aqueous solution:
v stoichiometric coefficient R3 NH+ · − OOCCH3 → R3 NH+ + − OOCCH3 (b)
V vapor flowrate (kmol h−1 )
x mole fraction in the liquid phase The reaction (a) may be reversible because weak acid
y mole fraction in the vapor phase (acetic acid) and weak base (tributylamine) are used
z mole fraction in the feed as reactants. That is, for the extractive distillation pro-
cess the forward reaction occurs in the extractive dis-
Greek symbol tillation column and the reverse reaction occurs in the
ν stoichiometric coefficient solvent recovery column. Therefore, this new sepa-
ration method is different from traditional extractive
Subscripts distillation, and based on the reversible chemical inter-
I component number action between weak acid (acetic acid) and weak base
j stage number (separating agent). So, we call this type of distillation
k reaction number complex extractive distillation.
salt product produced by the reaction A new substance, R3 NH+ · − OOCCH3 , is produced
1 water in this reaction, which can be verified by infrared
2 acetic acid spectra (IR) technique in the absence of water. The
3 tributylamine IR used was the type, Mattson Cygnus-100 (made in
USA) equipped with a KBr disk. The IR diagrams
Superscripts for different acetic acid concentrations in the solvent
F feed stream tributylamine are obtained and shown in Fig. 1, from
L liquid phase which it can be seen that a new characteristic peak
V vapor phase in the range of 1550–1600 cm−1 appears in the mix-
ture of acetic acid and tributylamine, and is assigned
to the carboxylic–salt functional group, –COO− [6,7].
This indicates that chemical reaction between HAc
and R3 N indeed takes place.
 Z. Lei et al. / Separation and Purification Technology 36 (2004) 131–138 133

Fig. 1. IR diagrams for the mixture of acetic acid and tributylamine. (1) Acetic acid; (2) acetic acid 10 wt.% + tributylamine 90 wt.%; (3)
acetic acid 20 wt.% + tributylamine 80 wt.%; (4) acetic acid 30 wt.% + tributylamine 70 wt.%; (5) tributylamine.

On the other hand, this chemical reaction is re- of the mixture of acetic acid 10 wt.% and tributy-
versible, which can be verified by the GC–MS. lamine 90 wt.% is illustrated in Fig. 2, where nos.
The instrument used was the type GCMS-QP5000 1 and 2 peaks denote acetic acid and tributylamine,
(Shimadzu, Japan). The total ion chromatogram (TIC) respectively.

Fig. 2. TIC of the mixture of: acetic acid 10 wt.% and tributylamine 90 wt.%.
134 Z. Lei et al. / Separation and Purification Technology 36 (2004) 131–138
So, it indicates that HAc, R3 N and the product pro-
duced by them can all be detected by the combina-
tion of IR and MS techniques. In general, the reaction
rate between weak acid and weak base is very quick.
So, the chemical reaction between HAc and R3 N may
be reversible. The further proof of reversible reaction
is supported by calculating the chemical equilibrium
constant in the following section.
In order to verify the effect of tributylamine as the
separating agent, the vapor liquid equilibrium (VLE)
was measured by experiment. Fig. 3 shows the equilib-
rium data for the ternary system of water (1) + acetic
acid (2) + tributylamine (3), plotted on a solvent free
basis. It may be observed that the solvent, tributy-
lamine, enhances the relative volatility of water to
acetic acid in such a way that the composition of the
more volatile component (water) is higher in the liq-
uid than in the vapor phase. The reason may be that
the interaction force between acetic acid and tributy-
lamine is stronger than that between water and tributy-
lamine because in the former the reversible chemical
1.00
0.80
y1
0.60
0.40
0.20
0.00
0.00 0.20 0.40 0.60 0.80
x1
Fig. 3. VLE curves on the solvent free basis for the ternary system
of: water (1) + acetic acid (2) + tributylamine (3) at 101.33 kPa.
(䉬) Solvent/feed volume ratio, 2/1; (䊉) solvent/feed volume ratio,
1/1; () no solvent.
reaction takes place. That is, water would be obtained
as the overhead product in the extractive distillation
column, and acetic acid and tributylamine as the bot-
tom product.
In terms of the mechanism of complex extractive
distillation, the following criteria should be satisfied
to ensure that this method can be implemented.
1. The chemical reaction is reversible. The reaction
product (here as R3 NH+ · − OOCCH3 ) is used as
carrier to carry the separated materials back and
forth.
2. One of the reactants (here acetic acid) is a low
boiling-point component. It can be easily removed
by distillation, so that the separating agent (here
tributylamine) can be regenerated and recycled.
3. There are no other side reactions between the sep-
arating agent and the component to be separated.
Otherwise, the separation process will be compli-
cated and some extra equipment may be added,
which results in no economy of this technique.
It is obvious that the system consisting of water,
acetic acid and tributylamine, meets these require-
ments. So, it seems to be advisable to separate wa-
ter and acetic acid by complex extractive distillation.
However, we should be cautious that not dialkylamine
(dibutylamine) and monoalkylamine (butylamine), but
trialkylamine (tributylamine) can be selected as the
separating agent because the reaction between acetic
acid and dibutylamine or butylamine is irreversible,
and some amides will be produced.
3. Chemical equilibrium constant
In general, the kinetic property of a chemical re-
action, which is carried out in a distillation column,
should be measured separately. However, it is very
difficult for us to obtain the chemical equilibrium
constant of this reaction between acetic acid and
tributylamine by experiment because the amount of
salt produced by them is not easy to be determined
1.00
by ordinary analysis.
By analyzing the reaction system, it is found that
the new group –NH is formed and the old group
–OH is disappeared during the reaction. This reac-
tion is exothermic and the heat generated can be ob-
tained from the reference [7], i.e. −2.17 kJ mol−1 . In
 Z. Lei et al. / Separation and Purification Technology 36 (2004) 131–138 135

addition, the ionization constant pKa of acetic acid Vj Lj+1

and tributylamine at 25 ◦ C can be found from [8], i.e. SVj
4.76 and 10.87, respectively. Therefore, the chemical
equilibrium constant KP of the overall reaction of re-
actions (a) and (b) in the aqueous solution at 25 ◦ C can Fj
Vapor
be deduced, and thus the relation of chemical equi- liquid
librium constant with temperature is expressed by the Qj Stage j Pj, Tj
following equation. Reaction


Csalt
2
261.01 SLj
Kp = = exp −4.6284 + (1)
CHAc CR3 N T

Vj-1 Lj
4. Mathematics model of complex extractive Fig. 4. Schematic representation of an EQ stage.
distillation

For the design of distillation process, two types of (7) Chemical reaction equilibrium is achieved in ev-
models have been developed: the equilibrium (EQ) ery stage (if chemical reaction is considered in the
stage model and the non-equilibrium (NEQ) stage EQ stage model). (8) Chemical reaction equilibrium
model [9–12]. However, building an NEQ model for is not included in every stage (if chemical reaction is
a distillation process is not as straightforward as it not considered in the EQ stage model).
is for the EQ stage model in which we need to sim- The equations that model EQ stages are known as
ply add an equation to take account of the effect of the MESHR equations [10]. MESHR is an acronym
chemical reaction equilibrium on a tray or section of referring to the different types of equation. The M
packing. As we know, the NEQ model is more com- equations are the material balance equations. The total
plicated than the EQ model. In the NEQ model, the material balance takes the form:
design information on the column configuration must dMj
= Vj+1 + Lj−1 + Fj − (1 + rjV )Vj
be specified, so that the mass transfer coefficients, dt
interfacial areas, liquid hold-ups, etc. can be calcu-  c
r 
lated. Therefore, for any new invented configuration − (1 + rjL )Lj + vi,k Rk,j εj · (2)
of the column, many experiments have to be done in k=1 i=1
advance to obtain the necessary model parameters. Mj is the hold-up on stage j. With very few exceptions,
Evidently, it is too tedious, and much time will be Mj is considered to be the hold-up only of the liquid
spent on the design of extractive distillation process. phase. It is more important to include the hold-up of
Fortunately, as pointed out by Lee and Dudukovic [9], the vapor phase at higher pressures. The component
a close agreement between the predictions of the EQ material balance (neglecting the vapor hold-up) is
and NEQ models can be found if the tray efficiency or
height equal to a theoretical plate (HETP) is known. dMj xi,j
= Vj+1 yi,j+1 + Lj−1 xi,j−1 + Fj zi,j
A schematic representation of the EQ stage model dt
is shown in Fig. 4. This EQ stage may represent a − (1 + rjV )Vj yi,j − (1 + rjL )Lj xi,j
tray or a section of packing. The assumptions used r

in this work are summarized as follows. (1) Opera- + vi,k Rk,j εj · (3)
tion reaches steady state. (2) System reaches mechan- k=1
ical equilibrium. (3) The vapor and liquid bulks are In the material balance equations given above, rj is
mixed perfectly and assumed to be at phase equilib- the ratio of sidestream flow to interstage flow:
rium. (4) Heat of mixing can be neglected. (5) Reac-
tions take place in the liquid bulk. (6) The condenser SjV SjL
rjV = , rjL = (4)
and re-boiler are considered as an equilibrium stage. Vj Lj
136 Z. Lei et al. / Separation and Purification Technology 36 (2004) 131–138

where vi,k represents the stoichiometric coefficient of is calculated by the modified Peng–Robinson (MPR)
component i in the reaction k, and εj represents the equation, and the sum of every vapor enthalpy multi-
reaction volume. plied by every mole fraction is the total vapor enthalpy.
The E equations are the phase equilibrium equa- The liquid phase enthalpy is deduced from vapor phase
tions: enthalpy and evaporation heat. Thermodynamic data
for this reaction system are taken from [16,17].
yi,j = Ki,j xi,j · (5)
The simulation of extractive distillation column was
The S equations are the summation equations: performed on a PC (Pentium 4, 1.5 GB). It took a
c c
few minutes for the EQ stage model for an extractive
  distillation column with 25 stages.
xi,j = 1, yi,j = 1· (6)
i=1 i=1

The enthalpy balance is given by 5. Comparison of experimental and simulation

results
dMj Hj
= Vj+1 Hj+1
V
+ Lj−1 Hj−1
L
+ Fj HjF
dt The experimental flow sheet of extractive distilla-
− (1 + rjV )Vj HjV − (1 + rjL )Lj HjL − Qj tion process with two columns, extractive distillation
(7) column and solvent recovery column, has been es-
tablished in the laboratory and illustrated in Fig. 5
There is no need to take separate account in Eq. (7) where components A (water) and B (acetic acid) to
of the heat generated due to chemical reaction since the be separated are, respectively, obtained from the top
computed enthalpies include the heats of formation. of two columns, and the solvent S (tributylamine)
The R equations are the reaction rate equations. Ac- is recovered in the solvent recovery column. The
cording to the assumption no. 7 given in Table 1, R is extractive distillation column, 30 mm in diameter,
equal to zero. That is to say, was composed of three sections: the rectifying sec-
tion (700 mm height), the stripping section (700 mm
R = Kp CHAc CR3 N − Csalt
2
=0 (8)
height) and the scrubbing section (200 mm height).
Under steady-state conditions all of the time The recovery column, 30 mm in diameter, was com-
derivatives in the MESH equations are equal to zero. posed of two sections, the rectifying section (600 mm
The modified relaxation method where the MESH height) and the stripping section (600 mm height). The
equations are written in unsteady-state form and are
integrated numerically until the steady-state solution
has been found, is used to solve the above equations (A) (B)
S
[13–15].
In the EQ model, The Wilson model is used for de-
S+B
scription of liquid phase non-ideality, while the ideal
equation of state is used for the vapor phase. The ex- 1 2
A+B
tended Antoine equation is used for calculating the va-
por pressure. The vapor enthalpy of every component

Table 1
The operation condition of extractive distillation column
No. Solvent/feed volume ratio Reflux ratio S
1 1.0 1.0
2 1.0 0.0
Fig. 5. The experimental flow sheet of extractive distillation process
3 2.0 1.0
with two columns: (1) extractive distillation column; (2) solvent
4 2.0 0.0
recovery column.
 Z. Lei et al. / Separation and Purification Technology 36 (2004) 131–138 137

two columns were all packed by a type of ring-shaped Table 2

packing with the size 3 mm (width) × 3 mm (height). Comparison of experimental and calculated values
The number of theoretical plate including a re-boiler No. Ttop (◦ C) Water concentration
and a condenser was determined by use of the at the top (wt.%)
n-heptane–methylcyclohexane system at infinite re- Exp. EQ1 EQ2 Exp. EQ1 EQ2
flux ratio for each column. The number of theoretical 1 99.9 99.7 99.7 99.74 98.83 98.95
plate of the extractive distillation column was deter- 2 100.2 99.8 100.0 99.81 98.15 97.04
mined as 25, and that of the solvent recovery column 3 99.6 100.0 99.6 99.77 99.63 99.19
as 20. The extractive distillation column was operated 4 99.9 100.5 99.8 99.86 98.36 98.05
at normal pressure, and the solvent recovery column
was operated at a reduced pressure of 0.080 MPa. The
models without (EQ1) and with (EQ2) incorporating
solvent is still recycled from the recovery column to
chemical equilibrium equations are listed in Table 2.
the extractive distillation column.
It can be found from Table 2 that:
Before the extractive distillation experiment was
run, the mixture of acetic acid 72.1 wt.% and water (1) high-purity of water can be obtained at the top of
27.9 wt.% was separated in the extractive distillation extractive distillation column in the case of small
column by ordinary distillation without adding any solvent/feed volume ratio and reflux ratio, which
solvent. The product was obtained at the top with the indicates that tributylamine is effective for the sep-
concentration of water 94.87 wt.% for the reflux ratio aration of water and acetic acid;
1.0, and 96.18 wt.% for the reflux ratio 4.0. (2) by comparison of the calculated results with the
In the extractive distillation process, the extractive experimental data, it can be seen that the EQ
distillation column is the key. The operation conditions stage model was accurate irrespective of whether
of extractive distillation column are given in Table 1, chemical equilibrium equation was incorporated
where the feed was supplied to the column at room or not. The reason may be that the value of chem-
temperature and normal pressure, and the concentra- ical equilibrium constant was small, about 0.02
tions of acetic acid and water were 72.1 and 27.9 wt.%, under the operation condition. This means that
respectively. At the same time, the solvent recovery this reaction is reversible, and the chemical in-
column is operated in batch way. The experimental teraction between acetic acid and tributylamine
data as well as the calculated results from the EQ stage is weak, which leads to no apparent influence of

Table 3
The calculated composition and temperature distributions along the extractive distillation column for the EQ1 and EQ2 models
No. x1 x2 x3 x4 T

EQ1 EQ2 EQ1 EQ2 EQ1 EQ2 EQ1 EQ2 EQ1 EQ2

1 0.0004 0.0002 0.4970 0.4645 0.5029 0.4711 0.0 0.0641 404.83 405.37
2 0.0029 0.0016 0.8910 0.8630 0.1058 0.0950 0.0 0.0403 393.75 393.84
3 0.0068 0.0039 0.9350 0.8997 0.0582 0.0628 0.0 0.0336 392.51 392.70
5 0.0301 0.0176 0.9168 0.9057 0.0531 0.0613 0.0 0.0155 391.41 391.98
7 0.1200 0.0743 0.8270 0.8510 0.0530 0.0599 0.0 0.0148 388.34 389.60
9 0.3430 0.2453 0.6015 0.6867 0.0553 0.0557 0.0 0.0123 382.65 384.33
11 0.6184 0.5097 0.3255 0.4277 0.0561 0.0430 0.0 0.0196 377.76 378.90
13 0.4862 0.5184 0.3006 0.3528 0.2133 0.1158 0.0 0.0131 378.06 378.57
15 0.4885 0.5876 0.3061 0.2832 0.2054 0.1048 0.0 0.0243 378.73 378.15
17 0.6334 0.6560 0.2318 0.2274 0.1348 0.0959 0.0 0.0206 376.89 376.67
19 0.6612 0.6903 0.2029 0.1835 0.1359 0.1188 0.0 0.0074 376.44 376.26
21 0.7236 0.7375 0.1386 0.1027 0.1378 0.1427 0.0 0.0172 376.44 374.79
23 0.7939 0.8499 0.0722 0.0422 0.1340 0.0965 0.0 0.0094 374.12 373.61
24 0.8717 0.8777 0.0328 0.0207 0.0955 0.0946 0.0 0.0070 373.30 373.11
25 0.9730 0.9693 0.0115 0.0103 0.0155 0.0203 0.0 0.0002 372.84 372.80
138 Z. Lei et al. / Separation and Purification Technology 36 (2004) 131–138
chemical reaction on solving the MESH equations
of distillation column.
In order to further investigate the difference between
the EQ1 and EQ2 models, the composition and tem-
perature distributions along the extractive distillation
column under the no. 1 operation condition are given
in Table 3, where subscripts 1, 2, 3 and 4 represent
water, acetic acid, tributylamine and salt produced by
the reaction, respectively. The tray is numbered from
the bottom to the top.
It can be seen from Table 3 that the calculated results
of EQ1 model correspond well with those of EQ2
model on a large part of trays. However, in the vicinity
of the feed tray, i.e. from nos. 9 to 15, the difference
of liquid composition distribution is evident, which
may be due to the relatively great influence of the feed
mixture on the chemical reaction between acetic acid
and tributylamine. So, the EQ1 model is more suitable
for the preliminary design of the extractive distillation
process disregarding the effect of chemical reaction.
6. Conclusion
A new separation method, complex extractive dis-
tillation, was proposed for the separation of acetic acid
and water. It was verified by the experiments that the
complex extractive distillation is effective for separat-
ing acetic acid and water if tributylamine is used as
a separating agent. Tributylamine is a chemically and
physically stable solvent and can be easily available in
the market. The separation mechanism of using trib-
utylamine is based on the reversible chemical interac-
tion between weak acid and weak base.
Moreover, the mathematics models of equilibrium
(EQ) stage with and without incorporating chemical
equilibrium equations were, respectively, established
to simulate the extractive distillation column. It has
been proved by experiment that the EQ stage model
is accurate whether chemical equilibrium equation is
incorporated or not in the model, due to the small value
of chemical equilibrium constant under the operation
condition.
It should be mentioned that although in this work
complex extractive distillation was only used for the
separation of acetic acid and water, it is not difficult
to extend to such systems as acid + water and base
+ water systems because similar reversible chemical
reactions can be used in the effective separations of
these systems.
Acknowledgements
The authors are grateful to China Petroleum and
Chemical Corporation for financial support of this
work.
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