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1 Introduction
Ammonia synthesis is the first stage in the
manufacturing of nitrous chemical products
(fertilizers, plastics, explosives, etc.). The direct
synthesis process, from basic gases (hydrogen and
nitrogen) needs a theoretical and experimental study
of the synthesis installation, in order to determine the
optimum working regimes. This is determined by:
1. The direct synthesis reaction N2 + H2 =NH3 is a
reversible exothermic reaction which must take
place at equilibrium to get a maximum
conversion rate.
2. The conversion rate depends of a series of
technological factors, the most important being:
temperature (the temperature increase leads to
ammonia decomposition, thus leading to
conversion rate decrease), catalyst activity
(which is decreasing in time because of catalyst
exhausting) and pressure. The maximum
ammonia concentration that can be obtained is
between 14% and 22% and depends of the
pressure and the temperature.
3. The synthesis columns are built with fixed
catalyst layer and there is no possibility to
control the temperature inside the catalyst layer.
To compensate this inconvenience, the columns
are built with multiple catalyst layers (Kellog
process), offering the possibility of introduction
of cold gas between the layers in order to reduce
the temperature and ammonia concentration at
the input into the next layer, thus increasing the
quantity of produced ammonia and the
conversion rate.
c
(
x
x
)
c j ( x a 0 x aj )
F
,
T
,
x
,
x
j
a
0
aj
2
a2
a2i
b2i
Celsius, that is preheated to 400 degree
Celsius
in
dt
1000
1000
u2 c K (T )V ( x , x ) C
the heat exchanger located at the column entrance.
Rj Tj
j Rj aj bj
Layer
The synthesis reaction thatCatalyst,
takes place
in2the catalyst
O
(2)
layers is highly exothermic. Thus, through flows F2,
N
F2, T2, xa0, xb0
dx
F
F
F3, and F4 introduced between catalyst layers atF a, T , x , xbj j c ( x x ) TRj c ( x x )
j b0
bj
j b0
bj
R3
0
a0
temperature T0, we get the following:
dtb0 1000
1000
R
Mixer 3 layers in order
-direct gas cooling between catalyst
c Rj K Tj (T j )V Rj ( x aj , xbj )
O
to maintain the optimum reaction parameters in the
(3)
F3, Ta3, xa3i, xb3i
L
new layer;
u3 dT j F j (c T c T E)
-reduction of the ammonia concentration in the gas
aj aj
pj j
Catalyst,
Layer
dt
1000
(4)
R
mixture (H2, N2, CH4, NH
the3equilibrium
3) below
H Rj K Tj (T j )V Rj ( x aj , xbj )
value, in order to allow the ammonia production
F3, T3, xa0, xb0
Mixer 4
u4
c) Mixer j
dTaj
F j 1
(c pj 1T pj 1 c pj T j )
dt
1000
FRj
(c p 0T0 c pj T j )
1000
V Rj 0,9 x aj
0.60648 x x 2
aj
bj
0, 479
0.60648 x x 2
aj
bj
xbj
0,521
3
xbj
(5)
(6)
25107.7
K Tj exp 27.751
Tj
(7)
were:
- j 1,4 FR1=0, F1 = 18860 Kmol/h, Fj = Fj-1 +
FRj;
- cj, cp0, cp1, cpj are thermal and mass coefficients,
- Tj (j=14) are temperatures in the catalyst layer j
V Raj
(8)
dz
FMN 0
b)
Heat accumulation inside the gas mix
and catalyst
dT j
dz
S
( H Ra )V Raj
FM c p
(9)
VRaj
K tj (T )
2
y*NH
y1H.52 y N 2
3
*3 *
p yH 2 y N 2 y NH 3
y NH 3
y1H.52
(10)
Equilibrium concentrations and constants can be
represented as a function of equilibrium conversion
rate xc and fugacity coefficients for N2, H2 and NH3.
Eventually we obtain an algebraic equation that
gives us the equilibrium conversion rate:
a2 xe2 2a1 xe a0 0
(11)
The real solutions of the equation represent the
maximum possible value for the conversion rate. At
the entrance in the new catalyst layer we determine
the conversion rate:
xj
xej 1F10
j
F10 FRi
(12)
and temperature
F c T
FRa c pjT1
T j m pm ej 1
( Fm FRa )c p
(13)
790
780
770
760
750
740
730
720
710
700
690
680
670
T [K]
Layer IV
Layer III
Layer II
Layer I
XA
0.02
0.04
0.06
0.08
0.1
0.12
0.14
0.16
0.18
0.2
0.22
F1 - F4
Fault detection
x(i)
Procedure
Pattern-search
F0
Subroutine
MODEL
F(i)
Fa(i)
F(i)
Subroutine OPTIM
T2 p T2m
DE T3 p T3m
T T
1 p 1m
F2
F F3
T
i
(14)
simulation.
Tgi
Fi
Real
Tg0
T2*
PI control
T3*
DE2
DE3
Detect
T3p
Process
Ft
AC2
Y1
Fault
Synthesis
AC1
PI control
DE1
T2p
Xc1
Y2
Synthesis
Xc1
Y3
Tgi
Process
Simulator
T1m
T2m
T3m
Tg0
Fault
display
5 Conclusions
The program allows the operators from the control
room to permanently evaluate the working
conditions and compare them with the optimal
values.
- It allows the permanent control of process
parameters.
- It allows the simple adaptation to the real optimal
working conditions.
References:
[1]. C. Crove, Chemical Plant Simulation, PrenticeHall, London, 1971.
[2]. E. Iancu, M. Vinatoru, Fault Detection and
Identification in Dynamic Systems , Craiova, Sitech,
Romania, 1999.
[3]. R Isermann, Supervision, fault detection and
fault diagnosis methods. An introduction, Control
Engineering Practice, 5(5), 1997, pp. 639 652.
Layer I
5.504
1
5.4763
Layer II
3.4673
0.514
3.40831
Layer III
2.01
0.635
1.992
Layer IV
0.5225
0.12793
0.5225
cpj
5.5048
3.4621
2.01
0.5225
cp0
0.2133
0.21229
0.11239
0.11229