ARTICLE IN PRESS

G Model
CEP-5933; No. of Pages 10

Chemical Engineering and Processing xxx (2010) xxx–xxx

Contents lists available at ScienceDirect

Chemical Engineering and Processing:

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

Modeling, simulation and control of dimethyl ether synthesis in an industrial

fixed-bed reactor
M. Farsi, R. Eslamloueyan ∗ , A. Jahanmiri
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: Dimethyl ether (DME) as a clean fuel has attracted the interest of many researchers from both industrial
Received 26 December 2009 communities and academia. The commercially proven process for large scale production of dimethyl
Received in revised form 2 September 2010 ether consists of catalytic dehydration of methanol in an adiabatic fixed-bed reactor. In this study, the
Accepted 29 November 2010
industrial reactor of DME synthesis with the accompanying feed preheater has been simulated and con-
Available online xxx
trolled in dynamic conditions. The proposed model, consisting of a set of algebraic and partial differential
equations, is based on a heterogeneous one-dimensional unsteady state formulation. To verify the pro-
Keywords:
posed model, the simulation results have been compared to available data from an industrial reactor
Fixed-bed reactor
Heterogeneous model
at steady state conditions. A good agreement has been found between the simulation and plant data. A
DME reactor control sensitivity analysis has been carried out to evaluate the influence of different possible disturbances on
the process. Also, the controllability of the process has been investigated through dynamic simulation
of the process under a conventional feedback PID controller. The responses of the system to disturbance
and setpoint changes have shown that the control structure can maintain the process at the desired
conditions with an appropriate dynamic behavior.
© 2010 Elsevier B.V. All rights reserved.

1. Introduction
Dimethyl ether as a basic chemical product is mainly consumed
in industries as a solvent and propellant in various aerosol products
[1]. The similarity of some physical properties of DME, liquefied
petroleum gases and diesel fuel has presented DME as a clean fuel
that can be used in diesel engines, power generation, and other
purposes such as a substitute for LNG [2]. It can be produced from
a variety of feed-stock such as natural gas, crude oil, residual oil,
coal, waste products and bio-mass [3]. Although the commercially
proven technology for DME production is through dehydration of
pure methanol in an adiabatic fixed-bed reactor, many researchers
are working on the direct conversion of syngas to DME over a dual
heterogeneous catalyst [4].
DME can be produced in packed bed or slurry reactors. Although
slurry reactors have the advantage of better heat removal capa-
bility by coil or jacket and good productivity and good interface
contacting due to small solids particle size, they suffer from signif-
icant mass transfer resistance due to the use of inert liquid phases
such as waxy liquid [5]. At present, DME is commercially produced
through methanol dehydration using acidic porous catalysts in adi-
∗ Corresponding author. Tel.: +98 711 2303071; fax: +98 711 6287294.
E-mail addresses: eslamlo@shirazu.ac.ir, reslamlou@gmail.com
(R. Eslamloueyan).
abatic packed bed reactors [6]. Due to simplicity and lower costs,
adiabatic fixed bed reactors can be the first choice for catalytic pro-
cesses having low or intermediate heat of reactions [7]. However, in
case of highly endothermic or exothermic reactions, the problems
of reaction extinguishing or catalyst sintering may happen [8]. The
fluidized bed reactors have been suggested by some researchers
as a perfect reactor for DME synthesis [9,10]. Fluidized bed reac-
tors showed the better heat removal characteristics due to freely
moving catalyst particles in the bed. However, collision between
catalyst particles and the reactor wall causes loss of catalyst.
Simulation of packed bed reactors is not an easy task, since sys-
tems of nonlinear partial differential equations have to be solved
along with nonlinear algebraic relationships [11]. Modeling and
simulation of fixed-bed reactors have been done for many indus-
trial and pilot scales reactors. For instance, Shahrokhi et al. modeled
and simulated the dynamic behavior of a fixed bed reactor for
methanol production from syngas and proposed an optimizer to
maximization of the production rate [12]. Jahanmiri and Eslam-
loueyan modeled and simulated the isothermal fixed-bed reactor
for methanol production in industrial scale [13]. They calculated the
optimal temperature profile of the shell side to maximize methanol
production.
Fixed-bed DME synthesis reactors have been investigated
through a number of research studies. Lee et al. modeled and ana-
lyzed DME production from syngas in a fixed-bed reactor at steady
state condition [14]. Nasehi et al. simulated an industrial adiabatic

0255-2701/$ – see front matter © 2010 Elsevier B.V. All rights reserved.
doi:10.1016/j.cep.2010.11.013

Please cite this article in press as: M. Farsi, et al., Modeling, simulation and control of dimethyl ether synthesis in an industrial fixed-bed reactor,
Chem. Eng. Process. (2011), doi:10.1016/j.cep.2010.11.013
 ARTICLE IN PRESS
G Model
CEP-5933; No. of Pages 10

2 M. Farsi et al. / Chemical Engineering and Processing xxx (2010) xxx–xxx

Table 1 Table 2
The reaction kinetics and equilibrium constants. Equipment and catalyst parameters.

Parameter k = A(i)expB(i)/RT Parameter Value

A(i) B(i) Reactor

Catalyst density (kg m−3 ) 2050
k0 3.7 exp10 −1,05,000 Catalyst void fraction 0.2
KH2 O 0.84 exp−1 41,100 Specific surface area of catalyst pellet 673
KCH3 OH 7.9 exp−4 7050 Catalyst diameter (m) 0.3175 × 10−2
Ratio of void fraction to tortuosity of catalyst particle 0.066
Reactor Length (m) 8
fixed-bed reactor for DME production from methanol dehydration Reactor diameter (m) 4
at steady state condition, and showed that the difference between Bed void fraction 0.5
one and two dimensional models is negligible [15]. Omata et al. Catalyst density (kg m−3 ) 2010
Density of bed (kg m−3 ) 1005
studied DME production from syngas in a temperature gradient
Heat exchanger
reactor for overcoming both the equilibrium limit of the reaction Tube side diameter (m) 1.905 × 10−2
at high temperature and low activity of the catalyst at low tempera- Tube thickness (m) 2.11 × 10−3
ture [16]. Then, they optimized the reactor for higher CO conversion Shell diameter (m) 0.615
by a combination of genetic algorithm and neural networks. Fazlol- Overall heat transfer coefficient (W m−1 K−1 ) 325
Heat exchanger length (m) 4.57
lahnejad et al. investigated methanol dehydration in a bench scale
adiabatic packed reactor [17]. The reactor was packed with 1.5 mm
␥-Al2 O3 pellets as catalyst and operated at atmospheric pressure. the catalyst pellet and the reactor design specifications are sum-
They investigated the effects of weight hourly space velocity and marized in Table 2.
temperature on methanol conversion.
Although many research studies have been carried out on the
3. Process description
dynamic simulation and control of fixed bed reactors, we could not
find any work in this field for DME synthesis from methanol dehy-
DME production loop consists of an adiabatic packed bed reactor
dration. Fixed-bed catalytic reactors are often difficult to control
as well as a shell and tube heat exchanger as depicted in Fig. 1.
due to nonlinearity, process dead time and positive feedback of feed
The inlet feed to the reactor is preheated in the heat exchanger
preheating by the reactor effluent stream [18]. Jorgensen presented
through heat transfer to the outlet products from the reactor. The
a good review for dynamic modeling and control of fixed bed reac-
reactor product is transferred to DME purification unit, and DME is
tors [19]. Aguilar et al. developed a robust PID control law in order to
separated from water and methanol. Also, the unreacted methanol
control the outlet temperature of a fluid catalytic cracking reactor
is recycled to the reactor.
[20]. The controller is synthesized using an input–output lineariz-
The developed model of this process includes modeling equa-
ing control law coupled to a proportional-derivative reduced order
tions for both the reactor and the feed preheater.
observer to infer on-line the unknown heat of reaction. This control
strategy was robust against model uncertainties, noisy temperature
3.1. Reactor model
measurements and set point changes.
In this paper, we develop an unsteady heterogeneous model
In this study, a one dimensional heterogeneous model has been
for dynamic simulation of an industrial DME synthesis reactor and
considered for steady state simulation of the process. The basic
design a conventional feedback control system to maintain the inlet
structure of the model is composed of heat and mass conservation
stream temperature at the desired value.
equations coupled with thermodynamic and kinetic relations as
well as auxiliary correlations for prediction of physical properties.
2. Reaction kinetics
In the dynamic modeling of the reactor the following assumptions
have been considered.
The reaction equation of DME synthesis from dehydrogenation
of methanol is as the following.
- No heat loss to the surrounding from the reactor wall
2CH3 OH  CH3 OCH3 + H2 O, H298 = −23.4 (kJ/mol) (1) - Plug flow pattern and negligible concentration and temperature
variations in radial direction
In this work, the rate expressions have been selected from the
- Uniform temperature within each catalyst pellet (Biot num-
kinetic model proposed by Berćić et al. [21].
ber = 0.0125)
2
k · KCH ((CCH3 OH − (CC2 H6 O CH2 O )/Keq ))
3 OH
r= (2)
4 Biot number is a dimensionless number defined in conduction heat
(1 + 2(KCH3 OH CCH3 OH ).5 + KH2 O CH2 O )
transfer, and gives a simple index of the ratio of the heat transfer
where,
3138
ln (Keq ) = 086 log T + + 1.33 × 10−3 T − 1.23
T
× 10−5 T 2 + 3.5 × 10−10 T (3)

k = A(i) expB(i)/RT (4)

Ci is the molar concentration of component i in k1 , mol/m3 .
KCH3 OH and KH2 O are the reaction rate constant and the adsorption
equilibrium constant for methanol and water vapor, respectively,
which are tabulated in Table 1. Commercially, ␥-Al2 O3 catalyst is
used in methanol dehydration reaction. Also, the characteristics of Fig. 1. Process flow diagram of DME production.

Please cite this article in press as: M. Farsi, et al., Modeling, simulation and control of dimethyl ether synthesis in an industrial fixed-bed reactor,
Chem. Eng. Process. (2011), doi:10.1016/j.cep.2010.11.013
 ARTICLE IN PRESS
G Model
CEP-5933; No. of Pages 10

M. Farsi et al. / Chemical Engineering and Processing xxx (2010) xxx–xxx 3

Table 3 dTcold dT Do 
Feed specification of the industrial DME reactor. = −ug cold + U(Thot − Tcold ) (11)
dt dz  · Acold · Cp
Parameter Value
The overall heat transfer coefficient in the heat exchanger is
◦
T ( C) 260 calculated from
P (bar) 18.2
Mass flow rate (kg/s) 50.81 1 1 A ln(Do /Di ) A 1
= + i + i (12)
Mass fraction (%) U hi 2LKw Ao ho
Methanol 94%
Water 1% In Eq. (12), the heat transfer coefficient in the shell side (ho ) and
DME 5% the tube side (hi ) are calculated using the following equations [24]:

ho Do Cp 
 1/3
= 0.33(Re)0.6 (13)
kf k
resistances inside and at the surface of a body. For the Biot numbers
hi Di Cp 
 1/3   0.14
smaller than 0.1, the heat conduction inside the body is much faster = 0.023(Re)0.8 (14)
than the heat convection away from the surface, and the tempera- k k w
ture gradient is negligible inside of the body. To justify the first two
3.3. Auxiliary equation
assumptions, it should be notified the industrial reactor considered
in this study have insulation that causes the heat loss from the reac-
Auxiliary equations are used for prediction of the model param-
tor wall to the environment negligible in comparison to the heat
eters. In these equations i is the effectiveness factor which is
release in the reactor, and also because of high Reynold’s number
defined as actual reaction rate per particle to theoretical reaction
(about 10,000), the assumption of plug flow is reasonable. Further-
rate based on the external pellet surface concentration, which is
more, Nasehi et al. simulated the reactor at steady state condition
obtained from dusty gas model calculations [25]. It can be calcu-
by using a two-dimensional heterogeneous model with considera-
lated from the following equation:
tion of the heat loss from the insulation to environment [22]. The 
results of this simulation showed that the temperature difference ri dVp
between the reactor center and the reactor wall is at most 4 ◦ C. So, i =  (15)
Vp . ri 
the heat loss has a negligible influence on the simulation results in surface

one-dimensional plug flow model. In the heterogeneous model the physical properties of chemi-
The mass and energy balances for the gas and solid phase are cal species and overall mass and heat transfer coefficients between
expressed by the following equations: catalyst solid phase and gas phase must be estimated. The over-
Gas phase: all mass transfer coefficient between solid and gas phase has been
obtained from the correlation proposed by Cussler [26].
∂Ci ∂C
ε = −us i − kgi av (Ci − Cis
s
) (5)
∂t ∂z kgi = 103 (1.17Re−0.42 Sci −0.67 ug ) (16)
∂T ∂T In Eq. (16), the Sc is calculated for components along the reac-
g cpg ε = −us g cp + hf av (Tss − T ) (6)
∂t ∂z tor. Mass transfer diffusion coefficient for each component in the
Solid phase: mixture has been estimated by:
1 − yi
(1 − ε)
∂Cis s
= −kgi av (Ci − Cis ) + i Bs ri (7) Dim =  (17)
∂t (yi /Dij )

∂Ts Binary mass diffusion coefficient has been determined by the

(1 − ε)Bs cps = −hf av (Tss − T ) − i Bs (−H)ri (8) following equation [20]:
∂t

The pressure drop in the bed is calculated by Ergun equation 10−7 T 3/2 (1/Mi ) + (1/Mj )
[23]: Dij = (18)
3/2 3/2 2
P( ci + cj )
dp (1 − ε)2  · uc (1 − ε) · u2c
− = 150 + 1.75 (9) The overall heat transfer coefficient between solid and gas phase
l 2
d ε 3 d · ε3
(hf ) has been predicted from [27]:
The initial and boundary conditions for these equations are  −0.407
given below. Also, the feed specification of the industrial DME reac- hf
 C  2/3 0.458 udp
p
tor is reported in Table 3. = (19)
Cp  K εB 
  
Boundary conditions : C  = C0 , T  = T0 , P  = P0 The overall heat capacity in Eq. (19) depends on the temperature
Z=0 Z=0 Z=0
and composition, and is calculated using Eqs. (20) and (21):
 
Initial conditions : Ci  = Ciss , T  = Tiss Cp(i) = a + bT + cT 2 + dT 3 (20)
Z,t=0 Z,t=0

Cp = yi Cp(i) (21)
3.2. Heat exchanger model
Table 4 presents the values of a, b, c and d in Eq. (20).
There are no phase changes in the heat exchanger and this
unit is small in compare with the reactor unit. The shell and tube 4. Numerical solution
heat exchanger used for preheating feed stream is modeled at the
dynamic condition by the following equations: To solve the set of nonlinear partial differential equations (PDE)
obtained from dynamic modeling, the reactor length is divided into
dThot dT Di  equal discrete intervals, and by using finite difference method the
= −ug hot − U(Thot − Tcold ) (10)
dt dz  · Ahot · Cp PDEs are converted into a set of ordinary differential equations

Please cite this article in press as: M. Farsi, et al., Modeling, simulation and control of dimethyl ether synthesis in an industrial fixed-bed reactor,
Chem. Eng. Process. (2011), doi:10.1016/j.cep.2010.11.013
 ARTICLE IN PRESS
G Model
CEP-5933; No. of Pages 10

4 M. Farsi et al. / Chemical Engineering and Processing xxx (2010) xxx–xxx

Table 4 Table 5
Parameters of heat capacity coloration. Comparison of the steady state simulation results of the reactor with plant data.

a b c × 10−5 d × 10−9 Simulation Plant data Absolute

result error
DME 0.18 17.02 5.23 1.92
CH3 OH 21.15 0.07 2.59 0.29 DME exit mole flow rate (kmol/h) 2457 2506 1.95%
H2 O 32.24 0.002 1.06 3.6 MeOH exit mole flow rate (kmol/h) 940.6 937.7 0.31%
Outlet temperature (K) 652.2 644 1.27%

(ODE) in time domain. The set of equations are solved by 4th order
Runge–Kutta [28]. 6000
Before carrying out dynamic simulation, the stationary con-
dition of the system should be obtained through solving the DME
governing steady-state equations. The aim of performing steady 5000 MEOH
state simulation of the DME reactor is to determine the con- Water

Mole Flow (kmol hr-1)

centration and temperature profiles along the reactor at normal
operation. These steady state profiles are used as the initial con- 4000
ditions of the unsteady state PDEs. After rearranging the modeling
equations for the steady state condition, a set of ordinary differen-
3000
tial equation is obtained. This set of equations was solved by the
method of 4th order Runge–Kutta.
2000
5. Control structure

The main objective of the control system of DME reactor is to 1000

maintain the operating condition at the optimum designed state in
spite of probable disturbances. Since DME is produced through an
exothermic reaction in a fixed bed adiabatic reactor, the control of
feed temperature is crucial for keeping the conversion at its maxi-
mum level. The proposed control structure for a typical industrial
DME reactor is shown in Fig. 2. The reactor feed stream is preheated
in a shell and tube heat exchanger with the hot reactor effluent. A
bypass stream around this heat exchanger is manipulated to control
the reactor feed temperature. In this study, a conventional feedback
PID algorithm carries out the load rejection and set-point tracking
tasks.
6. Results and discussion
6.1. Steady state simulation
In this section, steady state simulation results of DME reac-
tor have been presented. Assuming an adiabatic tubular reactor
with plug flow pattern, the reactor has been simulated based on
a one dimensional heterogeneous model. Modeling validation is
done through comparing the simulation results with the industrial
0
0 1 2 3 4 5 6 7 8
Length (m)
Fig. 3. The profiles of mole flow rates of DME, Methanol and water along the reactor.
reactor data provided by Petrochemical Research and technology
Company which is a subsidiary of National Iranian Petrochemical
Company. Table 5 indicates the absolute errors of the steady-state
simulation results in comparison to available data of the industrial
reactor. This table shows that the proposed model has been able to
predict the exit concentrations and temperature very well.
Fig. 3 illustrates the molar flow rate of DME, methanol and water
along the reactor length at steady state condition.
The mole fraction of DME along the reactor in solid and gas phase
predicted by the heterogeneous model has been compared in Fig. 4.
Near the end of the reactor, where the reaction equilibrium is pre-
vailed, the difference between gas and solid phase concentrations
is vanished.

Fig. 2. Schematic of the control structure.

Please cite this article in press as: M. Farsi, et al., Modeling, simulation and control of dimethyl ether synthesis in an industrial fixed-bed reactor,
Chem. Eng. Process. (2011), doi:10.1016/j.cep.2010.11.013
 ARTICLE IN PRESS
G Model
CEP-5933; No. of Pages 10

M. Farsi et al. / Chemical Engineering and Processing xxx (2010) xxx–xxx 5

0.5 Table 6
Calculated average mass transfer and effective diffusion coefficients in the reactor.

DDME-mixture (m s−1 ) 0.1737 × 10−6

−1
0.41 DMeOH-mixture (m s ) 0.1745 × 10−6
Dwater-mixture (m s−1 ) 0.2685 × 10−6
kDME (m2 s−1 ) 0.0036
kMeOH (m2 s−1 )
Mole Fraction

0.0036
0.32 kwater (m2 s−1 ) 0.005

0.23

680
0.14
Gas Phase

Temperature (K)
Solid Phase 640

0.05
0 1 2 3 4 5 6 7 8 600
Length (m)

Fig. 4. DME mole fraction in solid and gas phase.

560

520
Also, the predicted temperature profile along the reactor 8
obtained from the simulation is shown in Fig. 5. The temperature 6 50
40
approaches to equilibrium temperature due to heat generation by 4 30
reaction, and remains constant. 2 20
Length (m) 10
The calculated average heat transfer coefficient between gas and 0
Time (sec)
0
catalyst phase (hf ) in Eq. (19) is about 1170 W m−2 K−1 . Also, the
average estimated viscosity and molar heat capacity of the reac- Fig. 6. Dynamic temperature profile along the reactor for 10 ◦ C step change in the
tion mixture are about 1.6 × 10−7 kg m−1 s−1 and 69.5 W mol−1 K−1 , inlet stream to the reactor.

respectively. The effective diffusion coefficients of components in

the mixture and mass transfer coefficients for components are
calculated along the reactor. The average effective diffusion and
average mass transfer coefficients of DME, MeOH and water vapor
in the mixture are presented in Table 6.
6.2. Open loop dynamic simulation
The open loop behavior of the reactor has been considered in
two levels. In the first level the behavior of the reactor without its
preheater has been studied. The second level investigates both of
the reactor and the related preheater as a heat integrated process.
To investigate the influence of disturbances on the dynamic
behavior of DME reactor, the feed temperature, pressure and com-
position have been considered as the main probable effective loads
of the system.
Figs. 6 and 7 indicate the step response of the system to 10 ◦ C
increase in the feed temperature. In Fig. 6, dynamic variation of
the temperature along the reactor length has been illustrated in
a three-dimensional diagram. Fig. 7 represents time variations of
DME concentration along the reactor bed.
As shown in Fig. 8, the response of the outlet temperature of
the reactor for this disturbance has a time delay about 15 s, and it
reaches to the new steady state point in 50 s.

660

625 0.5
DME mole fraction

0.4
Temperature (K)

0.3
590
0.2

0.1

555
0
8
6 50
40
4 30
520 2 20
0 1 2 3 4 5 6 7 8 Length (m) 10
0 0 Time (sec)
Length (m)
Fig. 7. Dynamic DME mole fraction profile along the reactor for 10 ◦ C step change
Fig. 5. Predicted temperature profile along the reactor. in the inlet stream to the reactor.

Please cite this article in press as: M. Farsi, et al., Modeling, simulation and control of dimethyl ether synthesis in an industrial fixed-bed reactor,
Chem. Eng. Process. (2011), doi:10.1016/j.cep.2010.11.013
 ARTICLE IN PRESS
G Model
CEP-5933; No. of Pages 10

6 M. Farsi et al. / Chemical Engineering and Processing xxx (2010) xxx–xxx

661

0.5
659

DME molefraction
0.4
Temperature(K)

0.3
657

0.2

655 0.1

0
8
653 6 50
40
4 30
2 20
Length (m) 10
0 0 Time (sec)
651
0 10 20 30 40 50
Time (sec) Fig. 10. Dynamic DME mole fraction profile for 0.05 step change in the methanol
and water vapor mole fractions of the inlet stream.
Fig. 8. The outlet temperature profile from the reactor to 10 ◦ C step change in the
inlet temperature.

652.5
The feed composition effect was studied by applying 0.05 step
changes in the mole fractions of both methanol and water vapor.
Figs. 9 and 10 represent dynamic responses of the reactor tempera-
651.5
ture and DME mole fraction profiles along the reactor, respectively.
The response of the reactor outlet temperature to the step
Temperature(K)

change in composition is shown in Fig. 11.

650.5
Applying 2 bar step change in the reactor inlet pressure gener-
ates the outlet temperature response shown in Fig. 12. As can be
deduced from this figure, the change in inlet pressure has no sig-
nificant effect on the temperature and consequently the product 649.5
composition of the reactor effluent.
The above mentioned results indicate that the feed temperature
and composition are the major process disturbances that should be 648.5
rejected by the designed control system.
In order to have a more realistic influence of inlet temperature
on the reactor dynamic response, we have also studied the response 647.5
of the reactor effluent temperature to a step change in the fresh feed 0 10 20 30 40 50
temperature to the preheater. The reactor output temperature and Time (sec)
DME mole fraction have been respectively shown in Figs. 13 and 14.
Fig. 11. The outlet temperature profile for 0.05 step change in the feed mole fraction.
According to these figures, increasing of the inlet feed temperature
to the heat exchanger will cause an increase in the reactor feed
temperature and consequently reactor outlet temperature. Due to
652.45

652.4
680
Temperature(K)
Temperature(K)

640 652.35

600
652.3
560

520 652.25
8
6 50
40
4 30 652.2
2 20 0 10 20 30 40 50
Length (m) 10 Time (sec)
0 0 Time (sec)

Fig. 9. Dynamic temperature profile for 0.05 step change in the methanol and water Fig. 12. The outlet temperature profile for 2 step change in the feed pressure.
vapor mole fractions of the inlet stream.

Please cite this article in press as: M. Farsi, et al., Modeling, simulation and control of dimethyl ether synthesis in an industrial fixed-bed reactor,
Chem. Eng. Process. (2011), doi:10.1016/j.cep.2010.11.013
 ARTICLE IN PRESS
G Model
CEP-5933; No. of Pages 10

M. Farsi et al. / Chemical Engineering and Processing xxx (2010) xxx–xxx 7

850 657

656
810

655

Temperature(K)
Temperature(K)

770

654

730
653

690
652

650 651
0 5 10 15 20 0 5 10 15 20 25 30 35
Time (min) Time (min)

Fig. 13. The outlet temperature profile for 10 ◦ C step change in the fresh feed tem- Fig. 15. Outlet temperature response for rejection of the disturbance by the closed
perature to preheater. loop control system.

temperature increase, conversion in the reactor decreases and this

cause a new equilibrium point for the process. But, variation of the
rector outlet temperature is lesser than the variation of the inlet
temperature.
6.3. Closed loop process simulation
Although packed bed reactors are distributed parameter sys-
tems, the output variables are usually measured at the process exit
streams. In order to control the inlet feed temperature to the reac-
tor, a feedback control loop as shown in Fig. 2 is designed based on
a conventional Proportional–Integral–Derivative (PID) controllers.
The PID control algorithm is usually used for the industrial control
systems. In this study, the PID controller has been tuned through
using Closed Loop Ziegler–Nichols method. This algorithm is one of
the most common methods for tuning PID controllers. The gain of
proportional controller is increased (from zero) until it reaches the
ultimate gain, at which the output of the control loop oscillates with
a constant amplitude. The parameters of the controller, i.e. the pro-
portional gain, reset time, and derivative value, are derived from the
ultimate gain and the sustained period of oscillation [29]. This type
of tuning creates a quarter wave decay ratio which is acceptable
for most systems. According to this procedure, the controller gain,
reset time and derivative constant estimated in this work are 9.6,
0.56 min and 0.14 min, respectively. To compare Ziegler–Nichols’
tuning method to other tuning rules, we have tuned the reactor
controller loop by using Luyben’s method [30]. This method have
smaller decay ratio, but it has slower response than Ziegler–Nichols’
method. According to Luyben method, the controller gain, integral
constant and derivative constant are 7.5, 2.45 min and 0.18 min,
respectively. Both methods were examined through their applica-
tion to the set point tracking of the reactor controller. According
to this investigation, Ziegler–Nichols’ method led to better con-
trol responses, so in this study the Ziegler–Nichols’ tuning rules
are applied.
In this section, the dynamic closed-loop behavior of the process
consisting of the reactor and preheater in response to predefined
disturbances and set point variation are presented and analyzed.

0.442 0.439

0.4388

0.432
DME molefraction

0.4386
DME molefraction

0.422 0.4384

0.4382

0.412
0.438

0.402 0.4378
0 5 10 15 20 0 5 10 15 20 25 30 35
Time (sec) Time (min)

Fig. 14. The outlet DME concentration for 10 ◦ C step change in the fresh feed tem- Fig. 16. Outlet DME concentration response for rejection of the disturbance by the
perature to preheater. closed loop control system.

Please cite this article in press as: M. Farsi, et al., Modeling, simulation and control of dimethyl ether synthesis in an industrial fixed-bed reactor,
Chem. Eng. Process. (2011), doi:10.1016/j.cep.2010.11.013
 ARTICLE IN PRESS
G Model
CEP-5933; No. of Pages 10

8 M. Farsi et al. / Chemical Engineering and Processing xxx (2010) xxx–xxx

300 668

250
664
Set point
Mole flow (mol sec-1)

Temperature(K)
200

150 660

100
656

50

0 652
0 5 10 15 20 25 30 35 0 10 20 30 40
Time (min) Time (min)

Fig. 17. Manipulated variable variations in case of load rejection. Fig. 18. The variation of the outlet temperature for set point tracking.

6.3.1. Load rejection 0.439

To observe the performance of the proposed control structure
and applied PID controller for the system, 15 ◦ C step change in the
temperature of the fresh feed to the preheater has been introduced
0.4382
to the process as the most influential disturbance. The closed loop
response of the process has been presented in Figs. 15 and 16. As
DME molefraction

can be seen from these figures, the load is completely rejected after
about 7 min using a PID controller. The variation of the manipu-
lated variable, i.e. bypass flow rate, has been represented in Fig. 17. 0.4373
The manipulated variable response has no sever oscillation and is
similar to the behavior of an appropriate control system.
The dynamic characteristics of the control loop response for
disturbance rejection are presented in Table 7. 0.4364

6.3.2. Setpoint tracking

The setpoint tracking capability of the propose control system
has been investigated by applying 10 ◦ C step changes in the set- 0.4355
point of the reactor inlet temperature. Figs. 18 and 19 indicate the 0 10 20 30 40
outlet temperature and DME mole fraction from the reactor. The Time (min)
outlet temperature approaches to the new setpoint with accept-
Fig. 19. The variation of the outlet DME mole fraction for set point tracking.
able speed and oscillations. In Fig. 20, the molar flow rate of the
bypass stream has been represented. This figure indicates that the
manipulated variable response for the servo problem has suitable 400
dynamic behavior and can be implemented easily by an ordinary
control valve.
Table 8 presents the dynamic characteristics of the control loop 320
response for the set point tracking. Table 8 shows that character-
Mole folw (mol sec-1)

istics response of controller is acceptable and proper in industrial

scale.
240

Table 7
Characteristics of the control loop response for disturbance rejection.
160
Time (min)

Rise time 4
Peak time 9.7
80
Settling time 17.3

Table 8 0
Dynamic properties of the closed loop response for setpoint tracking. 0 10 20 30 40
Time (min)
Overshoot 42%
Rise time (min) 3.8
Settling time (min) 19.8 Fig. 20. Variation of the bypass stream flow rate for set point tracking.

Please cite this article in press as: M. Farsi, et al., Modeling, simulation and control of dimethyl ether synthesis in an industrial fixed-bed reactor,
Chem. Eng. Process. (2011), doi:10.1016/j.cep.2010.11.013
 ARTICLE IN PRESS
G Model
CEP-5933; No. of Pages 10

M. Farsi et al. / Chemical Engineering and Processing xxx (2010) xxx–xxx 9

668 disturbance rejection and setpoint tracking so that it can control

the reactor in a time period of 20–30 min.

Appendix A. Nomenclature
664

av specific surface area of catalyst pellet (m2 m−3 )

Temperature(K)

Acold cross section area of cold side in heat exchanger (m2 )

660 Ahot cross section area of hot side in heat exchanger (m2 )
Ci molar concentration of component i (mol m−3 )
Cp specific heat of the gas at constant pressure (J mol−1 )
dp catalyst diameter (m)
Di tube inside diameter of heat exchanger (m)
656
Do tube outside diameter of heat exchanger (m)
activity:1.0
Dij binary diffusion coefficient of component i in j (m2 s−1 )
activity: 0.7
Dim diffusion coefficient of component i in the mixture
activity: 0.5
(m2 s−1 )
652
0 7 14 21 28 35 F total molar flow rate (mol s−1 )
Time (min) hf gas–solid heat transfer coefficient in reactor (W m−2 K−1 )
hi tube side heat transfer coefficient in heat exchanger
Fig. 21. Setpoint tracking response for different values of catalyst deactivation. (W m−2 K−1 )
ho shell side heat transfer coefficient in heat exchanger
(W m−2 K−1 )
As mentioned in the modeling section, the catalyst deactivation
k rate constant of dehydrogenation reaction
is not included in the model because of lack of deactivation rate
(mol m−3 Pa−1 s−1 )
correlation in open literature. However, it should be noted that the
kg mass transfer coefficient for component i (m s−1 )
worst condition for examining the capability of the control sys-
Keq reaction equilibrium constant for methanol dehydration
tem structure would be for the case of fresh catalyst in which the
reaction (mol m−3 )
reaction rate is at the highest level. Therefore, since the objective
Ki adsorption equilibrium constant for component i
of this work is to examine the controllability characteristics of the
(m3 mol−1 )
suggested control structure, very slow catalyst deactivation cannot
L reactor length (m)
affect the control system structure. To illustrate the influence of the
M molecular weight (g mol−1 )
catalyst deactivation on the control system response, the process
P total pressure (Bar)
has been simulated for three levels of catalyst deactivation, and the
r rate of reaction for DME synthesis (mol kg−1 s−1 )
controller responses are illustrated in Fig. 21.
R tube diameter in heat exchanger (m)
Re Reynolds number
7. Conclusion Sci Schmidt number of component i
T temperature (K)
In this study, an industrial DME synthesis reactor from dehydra- u superficial velocity of fluid phase (m s−1 )
tion of methanol has been simulated in steady and unsteady state ug linear velocity of fluid phase (m s−1 )
conditions. The reactor mathematical formulation is based on a U overall heat transfer coefficient (W m−2 K−1 )
rigorous one-dimensional heterogeneous model. Also, a feed-back V volume (m3 )
control system has been designed and tuned to control the reactor vci critical volume of component i (cm3 mol−1 )
inlet temperature. The comparison of the simulation results and the yi mole fraction of component i (mol mol−1 )
industrial data show that the proposed model can predict the reac- z axial reactor coordinate (m)
tor outlet temperature and concentrations with relative errors less
than 2%. Some important disturbances such as fresh feed tempera- Greek letters
ture, inlet reactor temperature, inlet pressure and feed composition  viscosity of fluid phase (kg m−1 s−1 )
have been applied to the process for investigating its open loop  density of fluid phase (kg m−3 )
dynamic behavior. Since the deactivation rate equation of the cata-
tortuosity of catalyst
lyst used in this study is not available in open literature, the catalyst ε void fraction
deactivation, which usually occurs very slowly in industrial reac-
tors, has not been included in the modeling. In fact, the objective
Superscripts
of this article is the investigation of controllability of the proposed
g in bulk gas phase
control system structure for DME reactor, and because the reactor
s at surface catalyst
control system responds very faster (about 30 min) than the cata-
o inlet conditions
lyst deactivation time (about 2 years), the catalyst deactivation has
i chemical species
no significant influence on the objective of this research. Anyway,
if experimental data or mathematical correlation for predicting the
deactivation of DME indirect synthesis catalyst becomes available References
later, inclusion of the catalyst deactivation rate will be an inter-
[1] T.A. Semelsberger, R.L. Borup, H.L. Greene, Dimethyl ether (DME) as an alter-
esting subject for future work. The dynamic characteristics of the native fuel, Journal of Power Sources 156 (2) (2006) 497–511.
open loop system have been used to design a PID controller for [2] V.V. Galvita, G.L. Semin, V.D. Belyaev, T.M. Yurieva, V.A. Sobyanin, Production
adjusting the preheater bypass flow rate in order to maintain the of hydrogen from dimethyl ether, Applied Catalyst 216 (1–2) (2001) 85–90.
[3] C. Arcoumanis, C. Bae, R. Crookes, E. Kinoshita, The potential of dimethyl ether
reactor inlet temperature at its setpoint. The suggested feedback (DME) as an alternative fuel for compression-ignition engines: a review, Fuel
closed loop system has shown a good performance for the cases of 87 (2008) 1014–1030.

Please cite this article in press as: M. Farsi, et al., Modeling, simulation and control of dimethyl ether synthesis in an industrial fixed-bed reactor,
Chem. Eng. Process. (2011), doi:10.1016/j.cep.2010.11.013
 ARTICLE IN PRESS
G Model
CEP-5933; No. of Pages 10
10 M. Farsi et al. / Chemical Engineering and Processing xxx (2010) xxx–xxx
[4] L. Makarand, R. Gogate, C.J. Kulika, A novel single-step dimethyl ether (DME)
synthesis in a three-phase slurry reactor from co-rich syngas Sunggyu, Chem-
ical Engineering Science 47 (13–14) (1992) 3769–3776. [18]
[5] J.W. Guo, Y.Q. Niu, B.J. Zhang, Macro kinetics study on DME synthesis from
syngas in slurry reactor, Natural Gas Chemical Industry 25 (2000) 4–7.
[6] W.Z. Lu, L.H. Teng, W.D. Xiao, Simulation and experiment study of Dimethly [19]
ether synthesis from syngas in a fluidized-bed reactor, Chemical Engineering
Science 59 (2004) 5455–5464.
[7] G.F. Froment, K.B. Bischoff, Chemical Reactor Analysis and Design, 2nd edn., [20]
John Wiley & Sons, New York, 1990.
[8] H.S. Fogler, Elements of Chemical Reaction Engineering, 2nd edn., Prentice-Hall,
1992. [21]
[9] Y.C. Ray, T.S. Jiang, C.Y. Wen, Particle attrition phenomena in a fluidized bed,
Powder Technology 49 (3) (1987) 193–206.
[10] Y. Petukhov, H. Kalman, A new apparatus for particle impact tests, Particle and [22]
Particle Systems Characterization 20 (4) (2003) 267–275.
[11] D.R. Parisi, M.A. Laborde, Modeling steady-state heterogeneous gas–solid reac-
tor using feed forward neural networks, Computer and Chemical Engineering [23]
25 (9–10) (2001) 1241–1250.
[12] M. Shahrokhi, G.R. Baghmisheh, Modeling, simulation and control of a methanol [24]
synthesis fixed-bed reactor, Computer and Chemical Engineering 60 (15)
(2005) 4275–4286. [25]
[13] A. Jahanmiri, R. Eslamlueyan, Optimal temperature profile in methanol synthe-
sis reactor, Chemical Engineering Communications 189 (6) (2002) 713–741.
[14] S.B. Lee, W. Cho, D.K. Park, E.S. Yoon, Simulation of fixed bed reactor for dimethyl [26]
ether synthesis, Korean Journal of Chemical Engineering 23 (4) (2006) 522–530.
[15] S.M. Nasehi, R. Eslamlueyan, A. Jahanmiri, Simulation of DME reactor from [27]
methanol, in: Proceedings of the 11th Chemical Engineering Conference, 2006. [28]
[16] K. Omata, T. Ozaki, T. Umegaki, Y. Watanabe, N. Nukui, M. Yamada, Optimization
of the temperature profile of a temperature gradient reactor for DME synthesis [29]
using a simple genetic algorithm assisted by a neural network: high-quality
transportation fuels, Energy & Fuels 17 (4) (2003) 836–841. [30]
[17] M. Fazlollahnejad, M. Taghizadeh, A. Eliassi, G. Bakeri, Experimental study
and modeling of an adiabatic fixed-bed reactor for methanol dehydration
Please cite this article in press as: M. Farsi, et al., Modeling, simulation and control of dimethyl ether synthesis in an industrial fixed-bed reactor,
Chem. Eng. Process. (2011), doi:10.1016/j.cep.2010.11.013
to dimethyl ether, Chinese Journal of Chemical Engineering 17 (4) (2009)
630–634.
E.M. Assaf, R.C. Giordano, C.A.O. Nascimento, Thermal runaway of ethylene
oxidation reactors: prevision through neural network, Chemical Engineering
Science 51 (11) (1996) 3107–3112.
S.B. Jorgensen, Fixed bed reactor dynamics and control: a review, in: Proceed-
ings of the IFAC Control of a Distillation Columns and Chemical Reactors, Oxford,
1986, pp. 11–24.
R. Aguilara, A. Poznyakb, R. Martınez-Guerrab, R. Maya-Yescasc, Temperature
control in catalytic cracking reactors via a robust PID controller, Journal of
Process Control 12 (6) (2002) 695–705.
G. Berćić, J. Levec, Intrinsic and global reaction rate of methanol dehydration
over Al2 O3 pellets, Industrial and Engineering Chemistry Research 31 (1992)
1035–1040.
M. Nasehi, R. Eslamloueyan, A. Jahanmiri, Simulation of DME synthesis reac-
tor from methanol, in: 11th National Iranian Chemical Engineering Congress,
Tehran, Iran, 2006.
J.F. Richardson, J.H. Harker, J.R. Backhurst, Chemical Engineering, vol. 2, 5th
edn., Butterworth–Heinemann, 1999.
A.P. Colburn, A method of correlating forced convection heat transfer data and
a comparison with fluid friction, Transaction on AIChE 29 (1933) 174–210.
G.H. Graaf, H. Choltens, E.J. Tamhuis, A.A.C.M. Beenackers, Intra-particle dif-
fusion limitations in low-pressure methanol synthesis, Chemical Engineering
Science 45 (4) (1990) 773–783.
E.L. Cussler, Diffusion Mass Transfer in Fluid Systems, Cambridge University
Press, United Kingdom, 1984.
J.M. Smith, Chemical Engineering Kinetics, McGraw Hill, New York, 1980.
J.R. Dormand, P.J. Prince, A family of embedded Runge–Kutta formulae, Journal
of Computational and Applied Mathematics 6 (1980) 19–26.
J.B. Ziegler, N.B. Nichols, Optimum settings for automatic controllers, ASME
Transactions 64 (1942) 759–768.
W.L. Luyben, Design of proportional integral and derivative controllers for inte-
grating dead-time processes, Industrial and Engineering Chemistry Research 35
(1996) 3480.