Chemical Engineering and Processing 52 (2012) 21–27

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Chemical Engineering and Processing:

Process Intensification
journal homepage: www.elsevier.com/locate/cep

Steady-state simulation of a reactive internally heat integrated distillation

column (R-HIDiC) for synthesis of tertiary-amyl methyl ether (TAME)
A. Vanaki, R. Eslamloueyan ∗
School of Chemical and Petroleum Engineering, Shiraz University, Mollasadra Avenue, Shiraz, Fars 713481154, Iran

a r t i c l e i n f o a b s t r a c t

Article history: Tertiary-amyl methyl ether (TAME) is a very important fuel additive, which has attracted the attention of
Received 4 May 2011 many researchers. In this article, the synthesis of TAME by a reactive internally heat integrated distillation
Received in revised form column (R-HIDiC) is investigated. A complex mathematical formulation is developed for simulating the
13 December 2011
proposed reactive heat integrated distillation column (R-HIDiC), based on material balance, equilibrium,
Accepted 14 December 2011
summation of mole fractions and enthalpy balance (MESH) equations. The suggested model is used for
Available online 23 December 2011
simulating an R-HIDiC for industrial production of TAME. The performance of the proposed R-HIDiC
is compared to the conventional reactive distillation column which is usually used in TAME production
Keywords:
R-HIDiC
plants. The model verification has been performed using industrial data of the conventional TAME reactive
Reactive distillation distillation. The simulation results show that the total energy consumption of the proposed R-HIDiC is
TAME about 22% less than that of the conventional reactive distillation column.
Heat integration © 2011 Elsevier B.V. All rights reserved.
Energy saving

1. Introduction
Energy saving in industrial distillation columns is of great
importance, because the distillation columns consume a large pro-
portion of total energy of a plant. Among other methods, heat
integration of different sections of a column and/or integrating two
individual columns are usually used to design more efficient distil-
lation columns. In an internally heat integrated column, heat of hot
stages is transferred to the column cold stages. In this method, the
column is divided into two parts: (1) high-pressure (temperature)
section, and (2) low-pressure (temperature) section. The column
inside is designed to facilitate the heat transfer between high and
low pressure sections. This kind of column is usually called a heat
integrated distillation column (HIDiC). HIDiC basic concepts such as
its thermodynamic efficiency and its energy saving potentials can
be found in the references [1–5]. Gadalla et al. studied the internal
design of HIDiC towers [6]. In 2006, Olujic et al. worked on economic
aspects of HIDiCs [7]. Experimental results for the binary mixture,
benzene–toluene, proved the energy saving ability of this system.
Also, in a pilot study, it was shown that the binary HIDiC column
can be operated without using the condenser and reboiler [8]. This
astonishing result is due to the internal heat integration between
high and low pressure sections. Most of the previous papers have
∗ Corresponding author. Tel.: +98 711 2303071; fax: +98 711 6287294.
E-mail addresses: eslamlo@shirazu.ac.ir, reslamlou@gmail.com
(R. Eslamloueyan).
been focused on binary HIDiCs, and a few studies have also been
done on multi-component systems [9]. Fig. 1 illustrates schemati-
cally an internally heat integrated distillation column. The dashed
line in this figure implies that the condenser and reboiler can be
omitted in a certain ideal condition.
Fig. 2 shows the schematic of the internal section of a HIDiC
[7]. The internal pieces of the column are designed to allow heat
transfer between the column inner (rectification section) and the
outer sides (stripping section). The heat transfer between rectifi-
cation and stripping section causes the vapor condensation in the
rectification and liquid vaporization in the stripping sections.
Using the HIDiC configuration for reactive distillation is a new
research subject. The heat of reaction can improve the performance
of HIDiC. Indeed, exothermic reactions can be a source of heat for
liquid vaporization in stripping section, and the endothermic reac-
tions can cool the vapor stream in rectification, and generate more
liquid reflux in the column. This would lead to more heat integra-
tion energy saving.
Tertiary-amyl methyl ether (TAME) is an important fuel addi-
tive, which has attracted the attention of many researchers. TAME
is the product of the catalytic reaction between methanol and
isoamylenes (2-methyl-1-butene, 2M1B, and 2-methyl-2-butene,
2M2B). TAME synthesis includes three main reactions: (1) com-
bination of methanol and 2-methyl 1-butene, (2) combination
of methanol and 2-methyl-2-butene, and (3) isomerization of
2-methyl-1-butene. All side reactions such as dimerization of
methanol and production of TAA (tert-amyl alcohol) are usually
ignored. Some of the research papers related to modeling and

0255-2701/$ – see front matter © 2011 Elsevier B.V. All rights reserved.
doi:10.1016/j.cep.2011.12.005
22 A. Vanaki, R. Eslamloueyan / Chemical Engineering and Processing 52 (2012) 21–27

Nomenclature

a component activity
B bottom product molar flow rate (kmol h−1 )
c total number of components
D top product molar flow rate (kmol h−1 )
F feed molar flow rate (kmol h−1 )
h liquid enthalpy (kJ kmol−1 )
H vapor enthalpy (kJ kmol−1 )
L liquid molar flow rate (kmol h−1 )
P pressure (kPa)
Q heat load (kJ/h)
R reaction rate (kmol h−1 g−1 )
ri reaction rate (mol s−1 g−1 )
r total number of reactions
S side stream
T temperature (K)
U overall heat transfer coefficient (W m−2 K−1 )
V vapor molar flow rate (kmol h−1 )
Fig. 1. Schematic structure of HIDiC [7].
x mole fraction of liquid
y mole fraction of vapor
ε mass of catalyst (g) section (stages 5–23), and seven stages in the stripping sec-
 stoichiometric coefficient tion (stages 24–30). This column has two feed streams: (1) pure
methanol which enters into the 24th stage, and (2) pre-reactor
Subscripts: effluent which enters into the 28th stage. Table 1 gives the column
1B 2M1B feeds and product streams conditions [17].
2B 2M2B As shown in Fig. 4, the proposed R-HIDiC consists of two main
c coupling index sections: (1) the high pressure rectification section including top 23
F feed stages, and (2) the low pressure stripping section which contains
i component index seven stages from stage 24 to 30. In the R-HIDiC, the rectification
j stage index section has a smaller diameter and is placed inside the stripping
M methanol section so that the heat transfer between the two sections can be
m reaction index implemented. The TAME synthesis reactions occur in the rectifica-
T TAME tion section from stages 5 to 23. The rectifying and stripping are
respectively operated at 4 and 1 bars. The vapor stream from the
Superscripts: stripping section is compressed and transferred to the bottom of
E excess the rectification section. Also, the liquid outlet from the rectifica-
F feed tion is depressurized by a throttling valve before entering into top of
L liquid stripping section. All 7 stages of the stripping section are thermally
Sat saturation coupled with equal number of reactive stages. The heat transfer
V vapor area per stage is equal to 1 m2 . Overall heat transfer coefficient is
considered as 1000 W/m2 K for all stages. This value is in the range
of the reported heat transfer coefficients for HIDiCs [6]. This value
simulation of TAME reactive distillation process have been pre-
sented in the references [10–19]. In 1995, Rihko and Krause studied
kinetics of TAME synthesis reactions [20]. In 2000, Faisal and Datta
investigated TAME reactions thermodynamics [21].
As shown in Fig. 3, TAME is synthesized industrially in a reac-
tor followed by a reactive distillation column. The reactor effluent
enters into the reactive distillation column in order to complete
the TAME synthesis and TAME purification. The column bottom
product has more than 0.99 percent TAME, and its top product
consists of an azeotropic mixture of methyl–butene isomers and
methanol. The azeotropic mixture is transferred to another column
for methanol separation.
In this work, it is assumed that the reactive distillation column
of this process is replaced with reactive internally heat-integrated
distillation column (R-HIDiC). The proposed R-HIDiC is simulated
and its performance is compared to that of the reactive distillation.

2. System description

The conventional reactive distillation column used in the pro-

cess of TAME production has thirty equilibrium stages; four stages
in the rectifying section (stages 1–4), nineteen stages in the reaction Fig. 2. Scheme of HIDiC inside [7].
 A. Vanaki, R. Eslamloueyan / Chemical Engineering and Processing 52 (2012) 21–27 23

Fig. 3. Process flow diagram of TAME production in conventional reactive distilla-

tion [23].

is obtained through ignoring the heat transfer resistances of boiling

and condensation in the stages.
Various internal designs have been proposed for HIDiCs. In this
Fig. 4. R-HIDiC configuration for TAME synthesis.
work, a concentric configuration is used for the proposed R-HIDiC,
in which the high-pressure rectification section is surrounded by
the low-pressure stripping section. The suggested reaction rate equations are as following [17]:
−0.039aT + 0.609aM a1B
r1 = (RE1)
3. Reaction kinetics 0.128aT + aM
−0.161aT + 0.334aM a2B
TAME synthesis consists of two etherification reactions and one r2 = (RE2)
0.128aT + aM
isomerization reaction as shown below:
r3 = 3.177a1B − 0.381a2B (RE3)
Reaction1 : 2M1B + MeOH ⇔ TAME (R1)
where ai is the activity of component ‘i’, which is a function of
Reaction2 : 2M2B + MeOH ⇔ TAME (R2) temperature and composition.
Reaction3 : 2M1B ⇔ 2M2B (R3)
4. Mathematical model
where,
2M1B = 2-methyl-1-butene, C5 H10 Fig. 5 shows the variables used in the modeling of an equilibrium
2M2B = 2-methyl-2-butene, C5 H10 stage in the column. Heat transfer direction can be changed based
MeOH = methanol, CH3 OH on the stage position in the column. The stages have been numbered
TAME = tert-amyle methyl ether, C6 H14 O from top to down of the column.

Table 1
The feeds and products of TAME reactive distillation column.

Stream Methanol feed (F1) Pre-reactor effluent feed (F2) Top product (D) Bottom product (B)
Phase Liquid Liquid Liquid Liquid

Temperature (◦ C) 104.79 70 68.75 138.66

Pressure (bar) 4.1 4 4 4.05

Flow rates (kmol/h)

Methanol 215 165 297.81 Trace
2M1B 0 9.55 2.95 0.03
2M2B 0 83.94 16.5 0.78
TAME 0 157 0.047 230.24
n-Pentane 0 88.4 87.68 0.72
Iso-pentane 0 501.2 500.05 1.23
1-Pentene 0 38.06 37.97 0.09
2-Pentene 0 161.7 160.57 1.15
Total flow (kmol/h) 215 1196.1 1103.6 234.24
Total flow (kg/h) 6889 84,161 67,241 23,809
24 A. Vanaki, R. Eslamloueyan / Chemical Engineering and Processing 52 (2012) 21–27

Excess enthalpy HE is related to the activity coefficient  i as the

following:
 
∂(GE /RT )
H E = −RT 2 (E7)
∂T

GE c
= ˙i=1 xi ln i (E8)
RT
Summation of mole fractions in liquid and vapor phases of each
stage is equal to one as shown below:
c
˙i=1 xj,i = 1 (E9)
c
˙i=1 yj,i =1 (E10)

The liquid activity coefficients ( i ) are calculated

 based
 on
 ∅i  i
the UNIQUAC model [22]:ln i = ln xi + 0.5Zqi ln ∅i + i −
Fig. 5. Schematic of an equilibrium stage (heat transfer direction can be changed ⎛ ⎞
based on stage position in column).
 ∅i  
n
n 
n

xi j xj + qi (1 − ln 
) − qi
j=1 j ji
⎝ nj
ji ⎠where  i


k=1 k kj
j=1 j=1
The modeling equations consist of the material balance equa-
is the activity coefficient of component i, xi the mole fraction
tions (M), the equilibrium relations (E), the enthalpy balance
of component i, T the temperature (K), n the total num-
equation (H), and the summation of mole fractions (S) (MESH equa- j=1
tions) for each stage. No side stream is considered in the model. ber of components; j = 0.5Z(rj − qj ) − rj + 1; j = qi xi / qj xj ;
j=1 n
These equations are described in the following:
ij = exp − (aij + bij /RT); ∅i = ri xi / n rj xj ; Z = 10 is the coordina-
Total material balance on stage ‘j’: tion number; aij the non temperature dependent energy parameter
between components i and j (cal/mol K); bij the temperature depen-

r 
c
dent energy parameter between components i and j (cal/mol K); qi
Lj−1 + FjL + FjV + Vj+1 − Vj − Lj + i,m Rm,j εj = 0 (E1)
is van der Waals area parameter Awi /2.5e9; Aw is van der Waals
m=1 i=1 area; i is van der waals volume parameter Vwi /15.17; Vw is van
der Walls volume.
Component material balance on stage ‘j’ (c − 1 equations for each
Material and energy balances (E1–E3) are applied on reboiler
stage):
and condenser (total condenser and reboiler).
Lj−1 xj−1,i + FjL xj,i
F
+ FjV yj,i
F
+ Vj+1 yj+1,i − Vj yj,i The above-mentioned equations for all stages of the column
generate a set of nonlinear algebraic equations that are solved

r numerically for R-HIDiC by an appropriate algorithm. This algo-
− Lj xj,i + i,m Rm,j εj = 0 (E2) rithm is explained in the next section.
m=1
4.1. Solution algorithm
The last terms of Eqs. (E1) and (E2) are considered for chemical
reactions taking place in the reactive section of the column. To solve the system of nonlinear algebraic equations for the
Energy balance on stage ‘j’: modeling of the proposed R-HIDiC, the following input data are
specified for the column:
Lj−1 hj−1 + FjL hFj + FjV HjF + Vj+1 Hj+1 − Vj Hj − Lj hj + Qj = 0 (E3)
1. Top product flow rate and concentration.
Qj is the heat transfer between two coupled stages in R-HIDiC. 2. Reflux ratio.
This heat transfer is considered only in stages 24–30 and their cou- 3. Number of stages.
pled stages 17–23. The quantity of this energy is calculated by the 4. Column’s pressure.
following equation: 5. Feeds’ location, flow rate, composition, and condition.
6. Mass of catalyst on each stage.
Qj = Uj Aj Tcj (E4)
The initial guess of these variables is taken from conventional
where Tcj is the temperature difference between the jth stage
reactive distillation column [17]. As shown in Fig. 6 the solution
and its corresponding coupled stage.
algorithm has three steps. In the first step, k is equal to zero, and
Since the heat of formation is considered in the component
the modeling equations of the conventional reactive column are
enthalpies, heat of reactions does not appear explicitly in the heat
solved (by Newton–Rophson method). The results of this step are
balance equation.
used as the initial guesses for the next step as well as for making a
Phase equilibrium relations are based on ϕ– approach as
comparison between the conventional reactive distillation and the
shown below:
suggested R-HIDiC. In the second step, k is equal to 1, and the pres-
sure profile is set for the R-HIDiC. The stage equations will be solved
yi P = xi i PiSat (E5)
throughout the column (by Newton–Rophson method), while no
It is assumed that the vapor phase is an ideal gas, so the fugacity internal heat integration among the column stages exist. The tray
coefficient in Eq. (E5) is equal to 1. The mixture enthalpy has been equilibrium temperatures are calculated in this step, and are used
calculated according to the following equation: for estimating the heat transfer rate among the column stages in
the next step. After calculating the internal heat transfer rates, the
c modeling equations are resolved throughout the column stages. In
H = HE + xi Hi (E6)
i=1 the third step, k is equal to 2.
 A. Vanaki, R. Eslamloueyan / Chemical Engineering and Processing 52 (2012) 21–27 25

Fig. 6. Steady-state model solution brief flow chart.

After finishing the third step, the calculated bottom concentra-

tion is compared with the actual design concentration. If it does not
satisfy the error criteria, the column reflux ratio or total number of
stages can be adjusted to make the solution converge to the bottom
concentration spec. In this research, the reflux ratio has been cho-
sen as the adjustable parameter, and the total number of column
stages has been assumed to be equal to that of the conventional
reactive column.

5. Results and discussion

The solution algorithm, explained in the previous section, was

applied to the conventional reactive distillation column and the
proposed R-HIDiC. The conditions of the feed and the product
streams are the same for both column configurations. The industrial Fig. 7. The conventional reactive column pressure profile.
data are available for the TAME reactive distillation column, and
the modeling methodology is verified by using these data. In the
conventional reactive distillation column, pressure is 4 bars at all R-HIDiC operates at 4 bars up to 23rd equilibrium stage, and the
stages, and there is no internal heat integration among the stages. pressure is suddenly reduced to 1 bar after the stage 23.
The simulation errors for TAME molar fraction, temperature and the Fig. 9 shows the temperature profiles of the proposed R-HIDiC
total molar flow rate of the bottom product have been presented in and the conventional reactive distillation configuration. According
Table 2. As mentioned before, the top product conditions are fixed
as the column design specifications, and the column calculations
are started from the top of the column.
The results of the modeling verification indicate that the pro-
posed model has estimated the bottom product conditions with a
good accuracy.
Figs. 7 and 8 illustrate the difference between the pressure pro-
files of the conventional reactive column and the proposed R-HIDiC,
respectively. The conventional reactive distillation column oper-
ates in 4 bars with a linear pressure distribution. The proposed

Table 2
The relative absolute error percentages for the conventional reactive distillation.

Quantity Error (%)

Bottom TAME molar flow rate 5.60

Bottom product temperature 1.58
Bottom product molar flow rate 3.89 Fig. 8. R-HIDiC pressure profile.
26 A. Vanaki, R. Eslamloueyan / Chemical Engineering and Processing 52 (2012) 21–27

Fig. 10. The required molar reflux rates in the R-HIDiC and the conventional reactive
Fig. 9. Temperature profiles of the R-HIDiC and the conventional reactive column. column.

to this figure, the R-HIDiC operates at lower temperature for most

stages. The highest difference between the conventional and R-
HIDiC temperature profiles is related to the bottom stages because
of the lower operating pressures of these stages for the R-HIDiC.
The required reflux flow rates in terms of the TAME bottom con-
centrations have been illustrated in Fig. 10. As per this figure, the
reflux rate of the proposed R-HIDiC is lower than reflux that of the
conventional reactive column.
Composition profile of major components is shown in Fig. 11.
The figure does not show any difference in outlet composition
and reaction conversion of these components in comparison with Fig. 11. Composition profile in R-HIDiC and conventional reactive distillation col-
conventional reactive distillation column. However, the different umn.

Fig. 12. The temperature differences of the coupled stages.

Fig. 13. The heat loads of the coupled stages.

 A. Vanaki, R. Eslamloueyan / Chemical Engineering and Processing 52 (2012) 21–27
Table 3
The R-HIDiC and the conventional reactive column energy consumptions.
R-HIDiC
Condenser duty (kJ/h) 61e+06
Reboiler duty (kJ/h) 95e+06
Compressor duty (kJ/h) 93e+5
Total (kJ/h) 165e+06
profile and convergence manner is clear between two configura-
tions.
Fig. 12 illustrates the temperature differences among heat inte-
grated stages of the proposed R-HIDiC. Also, the heat loads of
the coupled stages are indicated in Fig. 13. The heat duties of
all the coupled stages are almost equal except for the last two
couples (i.e. 22–29 and 23–30). These are due to the higher
temperatures of the stages 29 and 30 in comparison to other
stages.
The energy consumptions in different equipment items of the
proposed R-HIDiC and the conventional reactive distillation col-
umn have been compared in Table 3.
As per this table, total energy saving achievement of the sug-
gested R-HIDiC compared to the conventional TAME reactive
distillation is about 22%. The energy consumptions of the reboiler
and the condenser of the proposed R-HIDiC are respectively 25.78%
and 27.38% less than those of the conventional TAME reactive
column. Although part of energy required in the R-HIDiC is the
work of the compressor that has higher quality compared to the
heat, it should be noted that the work of compressor is about
0.5% of the total energy supplied to the R-HIDiC. Hence, the com-
pressor cannot substantially influence the energy saving of the
R-HIDiC. On the other hand, the decrease of the condenser duty
is very useful in the regions where the shortage of water supply is
encountered.
6. Conclusions
A mathematical formulation based on the modeling equations
of reactive distillation columns has been developed for simulat-
ing a reactive heat integrated distillation column (R-HIDiC). The
suggested model has been employed to simulate an industrial
reactive distillation column for production of TAME. Also, the R-
HIDiC configuration has been simulated to replace the conventional
TAME reactive distillation. The proposed model and the solution
algorithm were verified by using the industrial data of the TAME
production process. The result of the simulation show that the total
energy consumption of the proposed R-HIDiC is about 22% less
than that of the conventional TAME reactive distillation column.
The total energy saving of the R-HIDiC is the outcome of 25.78%
energy saving in the reboiler, 27.38% energy saving in the con-
denser, and the energy consumption of the compressor added to
the proposed R-HIDiC. The energy saving of the R-HIDiC is due to
both heat integration and changes of pressure level in the strip-
ping and rectification sections. The percentages of the influences of
heat integration and pressure change depend on the type of com-
ponents in the fluid mixture, operating conditions, and the design
of the column. The reduction of the cooling water consumption in
the condenser is very important when the plant has to be installed
in the regions where water supply shortage is encountered. Also,
the simulation showed that the required reflux flow rate in the
R-HIDiC is approximately 50% less than that of the conventional
TAME reactive distillation. Although the proposed R-HIDiC is more
27
Conventional Difference (Abs) Reduction (%)
84e+06 23e+06 27.38
128e+06 33e+06 25.78
0.00
211e+06 46e+06 21.80
efficient than the conventional TAME reactive distillation, its oper-
ability and controllability performance may not be as easy as the
conventional reactive column. So the dynamic performance of the
TAME R-HIDiC should be studied in future research studies.
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