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I NTERNATIONAL J OURNAL OF C HEMICAL

R EACTOR E NGINEERING
Volume 6

2008

Article A113

The Optimization of an Ammonia Synthesis


Reactor Using Genetic Algorithm
Mohammad Taghi Sadeghi

Azam Kavianiboroujeni

Iran University of Science and Technology, sadeghi@iust.ac.ir


Iran University of Science and Technology, azamkavianiboroujeni@gmail.com
ISSN 1542-6580

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The Optimization of an Ammonia Synthesis Reactor


Using Genetic Algorithm
Mohammad Taghi Sadeghi and Azam Kavianiboroujeni

Abstract
An industrial ammonia synthesis reactor was studied in order to optimize its
operational conditions by means of increasing overall ammonia production. A heterogeneous, one-dimensional model and a two-dimensional rigorous model were
utilized to evaluate the process behavior. The simulation results of the two models
were compared with data from an industrial ammonia plant. The one-dimensional
model was found to be adequate for optimization purposes. Applying the Genetic Algorithm (GA) as a powerful method for complex problems, the model
was employed to optimize the reactor performance in varying its quench flows.
The optimal temperature profile along the fixed bed reactor was studied by changing independent variables including the quench temperature and the quench flow
rates. Optimization results show that the optimum quench temperature is about
615 K and that the optimum quench flows can enhance ammonia production rate
by 3.3%.
KEYWORDS: ammonia synthesis, fixed bed reactor, optimization, simulation,
genetic algorithm

The financial support of the Iran National Petrochemical Company-Research and Technology
Department is greatly acknowledged. Dr. M.R. Jafari-Nasr, head of the research group and Dr. A.
Taeb and Dr. V. Hadadi-Asl, head of the NPC-RT company are highly appreciated for their help.

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1. INTRODUCTION
Ammonia is produced via an exothermic reversible reaction of hydrogen and
nitrogen. The process takes place over an iron-promoted catalyst structure. The
reaction synthesis is straightforward with no side reaction between the
components. It gives a stable product that can be described by the overall reaction
of:
N2 + 3H2 2NH3

(1)

Ammonia is one of the most important chemicals produced having a wide


range of applications particularly in synthetic fertilizers production. That is why
modeling and simulation of the process has received considerable attention among
other industrial processes. Various models imitating different types of ammonia
synthesis reactors have been developed for design, optimization and control
purposes by Annable (1952), Eymery (1965), Murase (1970), Singh (1979) and
Upreti (1997). Optimum temperature trajectory along a tubular reactor length was
computed applying the Pontryagins Maximum Principle (PMP) by Murase
(1970). Lasdons Generalized Reduced-Gradient (LGRG) method was used to
calculate an optimal reactor length related to a special reactor top temperature by
Edgar (1988). Their objective function was different from Murases model
however, both researchers applied inappropriate expressions for calculation of
partial pressures of nitrogen, hydrogen and ammonia that are used to simulate the
temperature and flow rate profiles along the reactor. Moreover, Murases
formulation was employed with proper objective function having partial pressure
expressions of the components. Simple Genetic Algorithm (GA) in combination
with Gear package of Numerical Algorithms Group (NAG) librarys subroutine
D02EBF, was employed in optimization of the ammonia reactor. Mass flow rate
of nitrogen, feed gas temperature as well as reacting gas temperature were
specified at every 0.01m of the 10m long reactor. Reported results by Upreti and
Deb (1997) were completely different from the former results. Having the same
objective function a suitable formula was applied for reaction rate along the
reactor described by Babu and Angira (2005). The resulting three-coupled
differential equations were solved using the NAG subroutine with step sizes of
0.01 and 0.001. Quasi-Newton method was employed in optimization of the
system. All the above mentioned studies were focused on tubular ammonia
synthesis reactor however, not much works are available concerning the fixed bed
catalytic reactor.
In this paper, a mathematical model based on basic assumptions
describing the performance of a Kellogg ammonia synthesis reactor was
developed. Solving the resulted model equations, GA was applied to maximize

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International Journal of Chemical Reactor Engineering

Vol. 6 [2008], Article A113

the ammonia production at exit point of the fourth fixed bed inside the reactor.
This was done by varying the quench streams introduced between the catalytic
beds. The reactor configuration is described and modeling of the reactor with the
way of solving the differential equations as well as the reactor optimization
procedure is presented.

2. THE REACTOR CONFIGURATION


The axial flow reactor, shown schematically in figure 1, contains four catalytic
fixed beds and a vertical heat exchanger on its top. Syngas flows in spaces
between the two walls of the reactor. The heat transferred from the beds to the
syngas results in radial temperature gradient. The heat exchanger transfers the
heat of the hot reacted gas, coming from the fourth bed, to the syngas stream. The
hot gas flows inside the central cylinder and the heat exchanger tubes. The
preheated syngas enters the first catalytic bed. Each bed is filled with promoted Fe
catalyst. The outlet hot gas from each bed is mixed with a quench stream in order
to handle the temperature along the reactor. More description of the reactor is
given by Sadeghi (2004).

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Sadeghi and Kavianiboroujeni: Optimization of Ammonia Synthesis Reactor using Genetic Algorithm

Figure 1. Schematic view of the ammonia synthesis reactor

3. MATHEMATICAL MODELS
Two types of models were examined simulating the reactor including a one
dimensional as well as a two dimensional model.

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Vol. 6 [2008], Article A113

3.1. One-dimensional model


The one-dimensional model based on the following assumptions was developed to
explain the system behavior in a simple manner. The assumptions applied taking
into account simply axial changes along the ammonia synthesis reactor were as
following:

Steady state condition


One-dimensional heterogeneous model
Negligible diffusion of mass and energy in radial and axial directions
Constant gas density
Adiabatic catalytic beds

Basic equations include the energy and mass balance equations for
ammonia component along the reactor. The two equations can be derived as
below.
Considering an element of dx in axial direction of the bed by having the
bed area, mass balance equation in steady-state condition can be inscribed as
following equation:

uCA | x uCA | x + x + Ax( R NH 3 ) = 0

(2)

Dividing both sides by Ax and taking limit as x0 the following


equation can be derived by inclusion of nitrogen conversion:

R NH 3
dZ
=
dx 2 FNo2 / A

(3)

Similar to the mass balance equation, for an element of dx in axis


direction, the energy balance equation in steady-state condition can be written as:
A{ uC p T | x uC p T | x + x }+ Ax(H r ) R NH 3 = 0

(4)

Dividing both sides by Ax and taking limit when x0 results in the


following equation:
uC P

dT
+ (H r ) R NH 3 = 0
dx

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(5)

Sadeghi and Kavianiboroujeni: Optimization of Ammonia Synthesis Reactor using Genetic Algorithm

3.2. Two-dimensional model

In contrast, the more rigorous two-dimensional model was based on the following
assumptions:
Steady state condition
Intra-particle mass and heat transfer restrictions considered by a term
called effectiveness factor
Concentration and temperature of the gas flowing through the catalyst
beds are equal to the catalyst particle at each location.
Dispersion of mass and energy in radial direction are not negligible
Considering constant density along the reactor
Independent solution of the equations to the angular direction due to the
radial direction symmetry
The catalytic activity along the reactor is uniform and equal to unity.
Based on the above assumptions, the basic equations comprising energy
and mass balances for ammonia synthesis reactor can be derived. The energy and
mass balance equations for a cylindrical differential element of the catalytic bed
can be given as below:
k eff

2T
T 1
T
+ C p u
k eff
= b R NH 3 (H r )
2
x r
r
r

(6)

- Deff

2w
w 1
w
+u
Deff
= b R NH 3
2
x r
r
r

(7)

Boundary conditions are:


x =0

for all r

r = rin for all x

r = rout

T=T0

&

w=w0

w
=0
r

&

T
=0
r

for all x

(8)

w
=0
r

RNH3, used in the model was reported by Dyson and Simon (1968) as
following relation:

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RNH 3

= 2k K a2

aN2 (

Where ai =

ai =

a H2

2
a NH
3

) (

2
a NH
3

a H3 2

)1

Vol. 6 [2008], Article A113

(9)

fi
and the reference fugacity = 1 atm
fi 0

fi
= f i = y i i P
1

(10)

Empirical relations for fugacity coefficients of hydrogen, nitrogen and


ammonia are presented by Singh and Saraf (1979). Moreover, equilibrium
constant was derived by Gillespie and Beattie (1931).
LogK

= 2 .691122 LogT 5051925 10 5 T


7

+ 1 .848863 10 T +
T
2

2001 .6

(11)
+ 2 .689

Since the catalyst particles are not sufficiently small, interaction of kinetic
and transport effects may not be ignored. The effect of the resistance due to
diffusion is expressed by the effectiveness factor calculated from an empirical
relation as follows. The polynomial used for the Fe catalyst having the size of 610 mm, depends on the three parameters of temperature, pressure and nitrogen
conversion as noted by Gaines (1979).
= b0 + b1T + b2Z+ b3T2+ b4Z2+ b5T3+ b6Z3

(12)

The heat of reaction, H r , can be calculated using a formula presented


by Elnashaie et al. (1988) as the following:

846.609 459.734 106


P 5.34685T

= 0.54526 +
+
3
T
T

(13)

0.2525103 T 2 1069197106 T 3 9157.09

Gas density is calculated using Redlich-Kwong thermodynamic relation.


Shah (1967) gave different formula to estimate the specific heat for various
components. Since the bulk of gas does not flow in radial direction, Ergun
equation was employed to calculate the pressure drop of the bed:

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Sadeghi and Kavianiboroujeni: Optimization of Ammonia Synthesis Reactor using Genetic Algorithm

P = 2 u =

150(1 ) u
1 u2

1
.
75
3
d p2
3 dp

(14)

3.3. Numerical method

The partial-differential equations describing steady state behavior of the reactor


were discretized applying finite difference method to acquire ordinary differential
equations. The sets of model equations were solved employing a fourth order
Rounge Kutta method with step size of 0.01m. Depending on the node position
however, different numerical algorithms were applied. The resulting nonlinear
equations were solved using inverse matrix method with the step size of 0.01m.

4. SIMULATION RESULTS
Reactor specifications and operating conditions obtained from an operational
petrochemical ammonia plant used to simulate the Kellogg ammonia synthesis
reactor are given by Sadeghi (2004) as presented in Table 1.
Table 1: The plant data used for simulation of the ammonia synthesis reactor
Quench Temperature
Reactor ID
Reactor OD
First Bed Length
Second Bed Length
Third Bed Length
Fourth Bed Length
Syngas (feed) composition
yN2
yNH3
yH2
yCH4
yAr
Gas flow to first bed
First quench flow
Second quench flow
Third quench flow

650 K
0.18 m
1.48 m
1.1 m
2m
3m
4m
0.2363679
0.0269300
0.6567005
0.0597143
0.0202874
75000 kg/h
56500 kg/h
61000 kg/h
32000 kg/h

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Simulation results show that the reactor conditions vary within the four
beds. Figure 2 shows how ammonia concentration changes along the beds. The
discontinuities occurring in the profiles are due to the injection of the quench
flows between the beds. The quench flows reduce the ammonia concentration at
the end of each bed however, it will develop along the next bed. While the first
bed has the smallest length, it is responsible for most of the changes in
concentration. In contrast little change in the concentration is due to the fourth
bed which has the highest length.

Figure 2: Ammonia mole fraction along the reactor length


Similar trends along the reactor exist for temperature, nitrogen conversion
and ammonia concentration. Variation of the nitrogen conversion is shown in
figure 3. It shows that nitrogen conversion in the first bed is higher than the other
beds. This trend says that ammonia production decreases from first to fourth beds.

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Sadeghi and Kavianiboroujeni: Optimization of Ammonia Synthesis Reactor using Genetic Algorithm

Figure 3: Nitrogen conversion profile along the reactor


Simulation results were compared against experimental data obtained from
the industrial reactor of Khorasan petrochemical complex, located at Bojnourd,
north-east of Iran. Table 2 shows that there is a good agreement between
simulation results of the two-dimensional model and industrial data. Though,
agreement between simulation results using the one-dimensional model and
industrial data are also fairly well. This agreement justifies application of the onedimensional model for optimization purposes. Since the optimization procedure is
a time-consuming program, employing a simpler model with more agreeable
results would decrease the computational time.
Table 2: Comparison of simulation results with industrial data
Outlet Temperature (C)
Industrial data
One-dimensional model
Two-dimensional model

First bed
501.5
505.58
502.85

Second bed
490
494.77
491.88

Third bed
481.5
487.35
482.25

Fourth bed
475.3
482.56
476.45

5. OPTIMIZATION OF OPERATIONAL CONDITION


The syngas temperature significantly influences ammonia yield. In Kellogg
reactor, syngas temperature is controlled by quench streams. The streams are also

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International Journal of Chemical Reactor Engineering

Vol. 6 [2008], Article A113

important in preventing hotspots and keeping the reactor thermally stable.


Variations of flow and temperature of quench streams affect ammonia yield. An
increase in flow of injected quench between the beds may decrease or increase
reaction rate depending on the conversion. Ammonia production is favored by
high pressure and low temperature that increase the rate of forward reaction
however, high temperature condition is applied. The optimal temperature profile
along the reactor is obtained for two different conditions: Optimal temperature of
quench streams for given quench flows and optimal flows of quench streams for
given quench temperature. The objective function is to maximize ammonia
production rate at the end of fourth bed. In mathematical expression the terms can
be stated as follows:
Maximize: F = fout . yout

(15)

Where fout and yout are reactor outlet flowrate and ammonia mole fraction
respectively.
Constraints prevailing the system can be described as outlined below:
1. Hotspots along the reactor must be avoided. Hence temperature should be
under 800K as stated by Shahrokhi and Baghmisheh (2005).

T < 800K

(16)

2. Nitrogen conversion must have ascending approach while the reactor is


running in optimal profile. That means:
Z x<Z

x + x

(17)

3. Temperature of the outlet hot stream leaving the heat exchanger at the top
of the reactor must be more than the temperature of cold stream entering
the first bed.

(18)

Ti < To

In order to find the optimal quench flows as well as the optimal


temperature, an optimization problem was developed to maximize the objective
function while tacking into account the constraints.
Genetic Algorithm (GA) as a powerful and effective random search
optimization method have been successful in a wide variety of unconstrained and
constrained optimization problems. It presents several advantages with respect to

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Sadeghi and Kavianiboroujeni: Optimization of Ammonia Synthesis Reactor using Genetic Algorithm

traditional optimization techniques as described by Goldberg (1989), Michalewicz


(1996) and Mitchell (1996). It is a tool conceived by Holland (1965) that machine
can mimic selection mechanism of chromosomal processing in natural genetics.
The method searches for superior solution and not necessarily optimum solution
in the feasible region. Despite considerable advantages in constraint-handling, GA
requires a large number of fitness function evaluations and complex encodings or
mappings that increase computational time. However, new advances in computing
technologies have paved the way for using the algorithm on Personal Computers
(PC).
In this work, GA was employed to solve the constrained non-linear
optimization problem utilizing a dual core processor PC that needed to run for
several hours. In order to handle the constraints, all results were examined to be
within the feasible region. Calculations were repeated until all constraints were
satisfied. The repeating procedure for the optimization problem is shown in figure
4. The algorithm was also applied to optimize the temperature of the quench
streams.

Figure 4: Computing algorithm of the optimization problem


Figure 5 shows the values of ammonia production as the objective
function for a range of quench stream temperatures. It shows that the maximum

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International Journal of Chemical Reactor Engineering

Vol. 6 [2008], Article A113

ammonia production is at 650 K. The Genetic Algorithm parameters used to find


the optimal quench temperature are given in Table 3.
Table 3: Genetic algorithm parameters used to find optimal quench temperature
Population Size

50

Selection method
Crossover fraction
Mutation fraction

Roulette
.95
.05
Maximum generation
100

Figure 5: Ammonia production at the stream leaving the fourth bed for different
temperatures
The result shows that it is not possible to increase the amount of ammonia
production in the reactor by changing the quench temperature. An increase or
decrease in the quench temperature causes decline of ammonia production and
nitrogen conversion. Similar trend for nitrogen conversion profile in the reactor
was obtained.
Optimization of quench stream quantities is also studied with the aim of
enhancing the reactor performance. Ammonia production profile under optimal
condition for the fourth bed is depicted in figure 6. It shows the amount of
ammonia at the end of reactor in optimized condition has considerably improved
compared to normal operation reaching the value of 0.479. The Genetic

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Sadeghi and Kavianiboroujeni: Optimization of Ammonia Synthesis Reactor using Genetic Algorithm

Algorithm parameters used in finding the optimal quench streams are given in
Table 4.
Table 4: Genetic algorithm parameters used to find optimal quench configuration
Population Size
Selection method
Crossover fraction
Mutation fraction
Maximum generation

100
Roulette
0.8
0.2
200

Figure 6: Ammonia production at the stream leaving the fourth bed for normal
and optimum quench flows
Comparison of the results for normal versus optimum conditions confirms
that since the amount of inlet gas increases in optimum condition, temperature
would decreases. The value of temperature deviation enlarges along the reactor as
shown in figure 7.

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Vol. 6 [2008], Article A113

Figure 7: Temperature deviation along the reactor in optimized and normal


conditions
Moreover, nitrogen conversion in optimized condition is less than its
values in normal operation as shown in figure 8. While there is a little increase in
optimal condition, a considerable rise can be seen in normal condition. The lower
conversion in optimum conditions accompanied by lower temperature in the
fourth bed would imply deviation from equilibrium, allowing more reaction to
proceed.

Figure 8: Nitrogen conversion along the beds in normal and optimum conditions

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Sadeghi and Kavianiboroujeni: Optimization of Ammonia Synthesis Reactor using Genetic Algorithm

Applying the effectiveness factors to modify the reaction rate in optimal


condition along the bed, reveals different trends for the reaction rates in normal
and optimum conditions. The reaction rate increases in optimal condition
however, it slightly decreases in normal condition as shown in figure 9.

Figure 9: Different trends of reaction rates in normal and optimized conditions


Finally, Table 5 shows the amount of quench streams in normal and
optimum conditions. It shows how the amount of quench streams can be enhanced
in order to have an optimum operating condition.
Table 5: Comparison of quench streams in normal and optimum conditions
Streams
First quench stream
Second quench stream
Third quench stream
Total

Normal flow (kg/s)


15.69
16.96
8.89
41.54

Optimum flow (kg/s)


22.63
18.24
12.2
53.07

The total quench flows has increased by 1.28 times from 41.54 to 53.07
kg/s at the optimum flow condition. This results in the ammonia production to
increase from 0.4628 to 0.4786 kgmole/s that equals to 3.4% increase in each
pass. Ammonia concentration also enhances from 0.0836 to 0.0842. This
improves the daily ammonia production by 23,207.04 kg which is a substantial
amount in yearly production (8,470 tons per year).

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Vol. 6 [2008], Article A113

6. CONCLUSION
An industrial ammonia synthesis reactor has been numerically studied for
optimization of operational condition in order to maximize ammonia production
yield. The optimization problem includes two approaches. In first approach,
optimal temperature profile along the reactor was calculated among feasible
quench temperature. In the second approach, by changing quench flows between
the fixed beds optimal quench flows were obtained. The optimal temperature
trajectory along the reactor and optimal flows yield 3.3% additional ammonia
production during one pass of synthesis gas into the reactor.

NOMENCLATURE
A
C
Cp
Deff
dP
FN A

cross-sectional area of each bed, m2


concentration, kmol/m3
specific heat, kJ/kg.K
effective diffusion coefficient, m/s
catalyst diameter, m
nitrogen inlet mole flowrate, mol/s

f
fout
ID
k
K
OD
P
R
R NH 3

fugacity, atm
reactor outlet flowrate, mol/s
reactor inside diameter, m
reaction constant
equilibrium constant
reactor outside diameter, m
reactor pressure, atm
radial coordinate in reactor, m
reaction rate, kmol/kg catal.hr

T
u
w
x
yi
yout
Z

reactor temperature, K
velocity, m/s
mass fraction
axial coordinate in reactor, m
mole fraction of component i
ammonia mole fraction
nitrogen conversion

Greek letters

activity of component i
void fraction in catalyst bed

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b
r
i

effectiveness factor
dynamic viscosity, Pa.s
gas density, kg/m3
bed density, kg/m3
heat of reaction, kJ/kmol
fugacity coefficient of component i

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