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Dept. of Chemical Engineering, School of Chemical and Petroleum Engineering, Shiraz University, Shiraz 71345,
Iran
b Department of Chemical Engineering and Materials Science, University of California, Davis, 1 Shields Avenue,
Davis, CA 95616, United States
c Department of Chemical Engineering, Amirkabir University of Technology, Tehran, Iran
a b s t r a c t
Naphtha reforming is one of the most important processes in reneries in which high value-added reformate for
gasoline pool and aromatics such as benzene, toluene, and xylene are produced. It is necessary to establish new
naphtha reforming units and develop the traditional units to increase the efciency of the processes. In this study,
according to the recent progresses in the naphtha reforming technology, mathematical modeling of this process in
continuous catalyst regeneration mode of operation is accomplished in two dimensions (radial and axial) by considering cross ow pattern. In addition, a new catalyst deactivation model has been proposed and a new reaction network
model based on 32 pseudo-components with 84 reactions is investigated. Then, this model has been validated by
comparing with industrial data, and its results have acceptable agreement.
2013 The Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.
Keywords: Catalytic naphtha reforming process; Continuous catalytic regeneration; Two dimensional mathematical
modeling; Reaction network; Catalyst deactivation model.
1.
Introduction
1. Semi regenerative.
2. Cyclic.
3. Continuous regenerative (moving bed).
As shown in Fig. 1, 60% of total capacity of reforming process is the semi regenerative scheme, while the continuous
regeneration and the cyclic have 28% and 12% of total capacity of reforming, respectively (Antos and Aitani, 1995). Today,
due to many benets of continuous regeneration, all new
units are designed based on this technology and old units
are revamped to the continuous regeneration process or are
combined with this process. There are some advantages of
CCR process against traditional methods, such as producing
higher octane reformate even working with a low feed quality,
long time working of the process due to lack of shut down,
operating in the lower pressure by the low pressure drop,
Corresponding author at: Dept. of Chemical Engineering, School of Chemical and Petroleum Engineering, Shiraz University, Shiraz
71345, Iran. Tel.: +98 711 2303071; fax: +98 711 6287294.
E-mail addresses: rahimpor@shirazu.ac.ir, mrahimpour@ucdavis.edu (M.R. Rahimpour).
Received 26 April 2013; Received in revised form 11 September 2013; Accepted 14 December 2013
0263-8762/$ see front matter 2013 The Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.cherd.2013.12.012
Please cite this article in press as: Iranshahi, D., et al., Modeling of naphtha reforming unit applying detailed description of kinetic in continuous
catalytic regeneration process. Chem. Eng. Res. Des. (2014), http://dx.doi.org/10.1016/j.cherd.2013.12.012
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Notation
ai
aA
aCA
aCM
aM
Ar
C
CACP
CCA
CCM
Cj0
Cp
Cv
CT
dp
De
Ec
F
Fj
Ft
H
Hj
k
kCA
kCM
keff
kin
Kin
L
m
Mj
M
n
n1
n2
nA
nCA
nM
nCM
Nj
P
PAn
PACHn
PACPn
PH2
PIPn
PNPn
r
ri
catalyst activity
acidic function activity
acidic function activity for coke formation
metallic function activity for coke formation
metallic function activity
cross-section area of reactor in radial direction,
m2
concentration, kmol m3
alkyl-cyclopentane concentration, kmol m3
coke weight fraction on acidic function of catalyst, kg kg1
coke weight fraction on metallic function of catalyst, kg kg1
inlet concentration of component j, kmol m3
specic heat capacity at constant pressure,
kJ kmol1 K1
specic heat capacity at constant volume,
kJ kmol1 K1
total concentration, kmol m3
particle diameter, m
effective diffusivity, m2 s1
coke formation activation energy, J mol1
molar ow rate, kmol h1
molar ow rate of component j, kmol h1
total molar ow rate to the reactor, kmol h1
enthalpy, J mol1
enthalpy of component j, J mol1
thermal conductivity, W m1 K1
constant of deactivation equation for acidic
function, kg kg1 kPa1 n m1.5 kmol1.5
constant of deactivation equation for metallic
function, kg kg1 kPa1 n m1.5 kmol1.5
effective thermal conductivity, W m1 k1
reaction rate constant for reaction
equilibrium constant for reaction
length of reactor, m
number of reactions
molecular weight of component j, kg kmol1
mean molecular weight in the ow, kg kmol1
number of components
constant of deactivation equation
constant of deactivation equation
acidic function activity power number
acidic function activity power number
metallic function activity power number
metallic function activity power number
molar ux of component j, kmol m2 h1
total pressure, kPa
partial pressure of aromatic with n carbon, kPa
partial pressure of alkyl-cyclohexane with n
carbon, kPa
partial pressure of alkyl-cyclopentane with n
carbon, kPa
partial pressure of hydrogen, kPa
partial pressure of iso-parafn with n carbon,
kPa
partial pressure of normal-parafn with n carbon, kPa
radius, m
rate of ith reaction, kmol kg cat1 h1
rin
rCo
rCA
rCM
R
Ri
Ro
Sa
T
U
Uj
ur
yj
Greek letters
exit condition
numerator for reaction
numerator for component
number of carbon atom
total
Abbreviations
A
aromatics
alkyl-cyclohexane
ACH
ACP
alkyl-cyclopentane
CCR
continuous catalyst regeneration reformer
scaling factor
F
HC
hydrocarbon
IBP
initial boiling pint, C
IP
iso-parafn
normal-parafn
NP
RON
research octane number
Pt
platinum
tin
Sn
Please cite this article in press as: Iranshahi, D., et al., Modeling of naphtha reforming unit applying detailed description of kinetic in continuous
catalytic regeneration process. Chem. Eng. Res. Des. (2014), http://dx.doi.org/10.1016/j.cherd.2013.12.012
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2.
Kinetic model
An effective kinetic model of naphtha reforming must represent all the major types of reactions in the reforming process.
A kinetic model inherently satises both heat and material
balances; because it takes into account the stoichiometry of
the reactions. As discussed, the naphtha feedstock consists of
several hundred components and each of them takes part in
various reactions. Thus, presenting a detailed kinetics-based
model considering all components and reactions is infeasible. In past decades, many attempts have been made (Marin
et al., 1983; Froment, 1987; Ramage et al., 1987; Jorge and
Eduardo, 2000; Hu et al., 2003; Weifeng et al., 2006) to propose
a perfect kinetic model for naphtha reforming process by considering most kinetic lumps and reactions. Padmavathi and
Chaudhuri (1997) proposed appropriate model for naphtha
reforming kinetic, but in their model, some of the main lumps
and reactions have been ignored. Whiles in the reforming process, aromatics are the main products, 8-carbon aromatics
were not subdivided in details. In addition, some of the main
reactions such as dehydrocyclization of parafns to aromatics, isomerization and transalkylation of aromatics have been
ignored. In the proposed model, 8-carbon aromatics are subdivided to four lumps (ethylbenzene, para-xylene, meta-xylene
and ortho-xylene) and the variations of each of them are investigated. Also ignored reactions in Padmavathi and Chaudhuri
(1997) study, are characterized in Tables 19.
Proper kinetic modeling of reforming reactions is the key to
effective representation of the process over a wide operating
range. The rst effect of the kinetics of the reactions on the
product properties is the effect of operating variables on the
octane number (Taskar and Riggs, 1997). Therefore, by considering important kinetics in the reforming process and all of the
accomplished studies, in this study, a new reaction network is
proposed.
Parafns, naphthenes and aromatics are the different
hydrocarbon groups in the reforming feedstock. In the presented model, the naphtha feedstock has been subdivided
to naphthenes (alkylcyclohexanes: ACH, alkylcyclopentanes:
ACP), parafns (normal parafns: NP, isoparafns: IP), and aromatics (A) lumps with carbon numbers ranging from C6 to C9 + ,
this kinetic model consists of 32 pseudo components with 84
reactions. As shown in Fig. 2, in this model, all of the main
reactions are included, and the dened pseudo components
are related by major reforming reactions. In addition, rate constants in the proposed model are obtained by optimization,
so that deviation between output results of model and commercial data is minimized. In the following, main reactions in
the reforming process are discussed, and the reactions, rate
Please cite this article in press as: Iranshahi, D., et al., Modeling of naphtha reforming unit applying detailed description of kinetic in continuous
catalytic regeneration process. Chem. Eng. Res. Des. (2014), http://dx.doi.org/10.1016/j.cherd.2013.12.012
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(1)ACHn An + 3H2
C6
C7
C8
for An
for An
for An
for An
C9 +
a
r1n = k1n
PACHn
H (kJ (mol H2 )
E
RT
k1n = exp a
K1n
1
(kmol kg1
kPa1 ) K1n = exp A
cat h
E
R
18.75
20.70
17.89
19.15
18.66
18.71
20.38
19.50
19.50
19.50
19.50
19.50
19.50
19.50
59.90
60.23
60.37
60.32
60.13
60.40
61.05
68.73
208.47
64.50
65.10
64.74
68.70
66.05
= MXa
= OXa
= PXa
= EBa
PAn P3H
(kPa)
B
24.80 103
25.08 103
23.27 103
23.49 103
23.36 103
24.78 103
21.33 103
2.1.
catalyst (Antos and Aitani, 1995; Taskar and Riggs, 1997). The
reaction is endothermic and produces a sharp drop in temperature. The needed reaction constants for calculating the
reaction rate constants (k1n ) and equilibrium constants (K1n )
are presented in Table 1.
Dehydrogenation
Dehydrogenation reaction, due to produce high octane number aromatics, is a principal reaction in the reforming process
(Matar and Hatch, 2000). Octane number is gained at a loss
of volume, when a naphthene is converted to an aromatic
(Taskar and Riggs, 1997). This reaction is the fastest amongst
all the reforming reactions, thus reaches equilibrium very
quickly and is catalyzed by the metallic function of the
2.2.
Dehydrocyclization
H (kJ mol1 )
C6
C7
C8
C9 +
43.64
32.85
32.55
28.00
(3)ACHn + H2 IPn
C6
C7
C8
C9 +
(4)NPn ACPn + H2
H (kJ mol
a
C5
C6
C7
C8
C9 +
69.73
60.74
60.75
61.75
59.00
(5)IPn ACPn + H2
C5 a
C6
C7
C8
C9 +
33.11
33.11
33.11
33.11
9.12
8.95
8.34
8.12
PIPn
K3n
k3n = exp a
E
RT
1
(kmol kg1
kPa2 ) K3n = exp A
cat h
26.36
25.75
29.00
29.76
33.11
33.11
33.11
33.11
14.35
13.65
13.17
12.39
k4n = exp a
E
RT
1
(kmol kg1
kPa1 ) K4n = exp A
cat h
30.75
31.94
33.43
31.31
32.96
33.11
33.11
33.11
33.11
33.11
14.39
14.77
14.63
15.98
15.21
8.38 103
7.31 103
7.31 103
7.43 103
7.09 103
PACPn PH
2
K5n
k5n = exp a
E
RT
B
T
(kPa)
6.25 103
4.73 103
5.94 103
5.89 103
(kPa)
E
R
5.24 103
3.95 103
3.91 103
3.37 103
E
R
B
T
PACPn PH
2
K4n
1
(kmol kg1
kPa2 ) K2n = exp A
cat h
24.37
29.10
27.81
29.76
E
RT
k2n = exp a
E
R
52.00
39.30
49.40
49.00
PNP
K2n
H (kJ mol1 )
B
T
1
(kmol kg1
kPa1 ) K5n = exp A
cat h
H (kJ mol1 )
E
R
76.67
70.60
67.20
78.60
80.00
29.83
30.87
32.95
34.19
32.96
33.11
33.11
33.11
33.11
33.11
16.18
16.03
15.47
16.37
16.02
9.22 103
8.50 103
8.08 103
9.45 103
9.62 103
B
T
B
T
(kPa)
(kPa)
Please cite this article in press as: Iranshahi, D., et al., Modeling of naphtha reforming unit applying detailed description of kinetic in continuous
catalytic regeneration process. Chem. Eng. Res. Des. (2014), http://dx.doi.org/10.1016/j.cherd.2013.12.012
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PAn P4H
K6n
) k6n = exp a
E
RT
1
(kmol kg1
kPa1 ) K6n = exp A
cat h
B
T
(kPa)
E
R
66.50
63.20
16.87
17.17
18.86
18.86
35.73
35.21
7.99 103
7.60 103
= MX
= OX
= PX
= EB
56.51
56.95
56.70
59.66
59.29
17.32
17.89
17.01
16.96
18.90
18.86
18.86
18.86
18.86
18.86
34.13
34.21
34.16
34.63
33.56
6.79 103
6.85 103
6.81 103
7.17 103
6.36 103
(7)IPn An + 4H2
H(kJ (mol H2 )
C6 a
C7 a
C8 a
for An
for An
for An
for An
C9 + a
= MX
= OX
= PX
= EB
PAn P4H
K7n
) k7n = exp a
E
RT
1
(kmol kg1
kPa1 ) K7n = exp A
cat h
(kPa)
68.18
64.83
16.44
16.90
18.86
18.86
36.01
35.47
8.20 103
7.79 103
60.73
61.17
60.90
63.88
60.77
16.27
16.78
16.04
15.93
17.66
18.86
18.86
18.86
18.86
18.86
34.81
34.87
34.83
35.23
34.81
7.30 103
7.35 103
7.32 103
7.68 103
7.3 103
(8)ACPn ACHn
H (kJ mol1 )
C6
C7
C8
C9 +
17.10
27.90
29.20
31.00
(9)NPn IPn
PIPn
K9n
C4
C5 a
C6
C7
C8
C9 +
k8n = exp a
E
RT
E
R
15.11
24.73
25.78
26.13
23.81
23.81
23.81
23.81
5.20
6.63
6.83
7.16
E
RT
1
(kmol kg1
kPa1 ) K8n = exp A
cat h
9.23
6.94
9.86
6.45
13.95
21.00
PACPn
K8n
) k9n = exp a
H (kJ mol1 )
B
T
()
B
2.06 103
3.36 103
3.51 103
3.73 103
1
(kmol kg1
kPa1 ) K9n = exp A
cat h
B
T
()
E
R
25.08
24.89
24.70
24.15
25.54
24.48
26
26
26
26
26
26
0.80
1.17
0.69
1.27
0.04
1.09
1.11 103
0.83 103
1.19 103
0.76 103
1.68 103
2.53 103
n = 1a
n = 2a
n = 3a
n = 4a
n = 5a
n = 6a
a
E
R
Table 4 Rate constants and heat of reactions in isomerization of naphthenes and parafns.
B
T
H(kJ (mol H2 )
C6 a
C7 a
C8 a
for An
for An
for An
for An
C9 + a
OX
OX
MX
OX
EB
MX
PX
MX
EB
EB
PX
PX
PP
K10n
H (kJ mol1 )
10.50
17.60
12.60
10.84
11.89
0.71
k10n = exp a
E
RT
1 kPa1 ) K
(kmol kg1
10n = exp A
cat h
E
R
25.21
24.50
24.53
25.17
25.84
24.47
21.24
21.24
21.24
21.24
21.24
21.24
12.13
11.00
15.81
15.54
11.91
13.7
B
T
()
B
1.26 103
2.11 103
1.50 103
1.30 103
1.43 103
0.085 103
Please cite this article in press as: Iranshahi, D., et al., Modeling of naphtha reforming unit applying detailed description of kinetic in continuous
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n = 7a
n = 8a
a
T
OX
B
T
PX
A9+
PP PC
K11n
E
RT
k11n = exp a
1
(kmol kg1
kPa2 ) K11n = exp A
cat h
B
T
H (kJ mol1 )
E
R
16.20
09.16
16.68
15.48
21.24
21.24
16.41
15.28
1.95 103
1.10 103
()
2.3.
Isomerization
for n = 3
P3 + H2 P1 + P2
for n = 5
1
NP5 + H2 (NP4 + P3 + P2 + P1 )
P2
NPn
r12n = k12n
Pt E
1
k12n = exp a
(kmol kg1
cat h )
RT
n3
n
Pi
H2
3
15
5
NPn +
i=1
H(kJ (mol H2 )
65.20
53.60
49.50
47.80
47.26
46.69
46.61
46.15
C2 a
C3 a
C4 a
C5 a
C6
C7
C8
C9+
3
1
H2 (3P1 + P2 + P3 )
2
2
1
(13) for n = 5 IP5 + H2 (IP4 + P3 + P2 + P1 )
2
for n = 4
r13n = k13n
IP4 +
P
IPn
H(kJ (mol H2 )
C4 a
C5 a
C6
C7
C8
C9+
a
E
R
37.85
39.95
40.15
41.60
42.08
42.48
40.53
43.85
34.61
34.61
34.61
34.61
34.61
34.61
34.61
34.61
for n = 6 9 :
n3
n
Pi
H2
3
15
5
IPn +
k13n = exp a
Pt
40.30
45.30
37.40
41.85
36.00
35.65
E
RT
i=1
1
(kmol kg1
cat h )
E
R
36.15
41.57
40.53
41.57
41.51
42.93
34.61
34.61
34.61
34.61
34.61
34.61
Please cite this article in press as: Iranshahi, D., et al., Modeling of naphtha reforming unit applying detailed description of kinetic in continuous
catalytic regeneration process. Chem. Eng. Res. Des. (2014), http://dx.doi.org/10.1016/j.cherd.2013.12.012
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n
15
5
Pi
r14n = k14n
PACHn
Pt
k14n = exp a
E
RT
1
(kmol kg1
cat h )
i=1
H(kJ (mol H2 )
45.45
40.76
41.00
40.10
C6
C7
C8
C9+
for n = 5 :
ACP5 + 2H2
(15) for n = 6 9 :
E
R
42.15
44.70
43.90
44.15
34.61
34.61
34.61
34.61
r15n = k15n
1
(NP4 + P3 + P2 + P1 )
2
P
ACPn
Pt E
k15n = exp a
RT
1
(kmol kg1
cat h )
n
n
Pi
H2
3
15
5
ACPn +
i=1
H(kJ (mol H2 )
E
R
40.23
41.55
43.75
43.65
44.15
34.61
34.61
34.61
34.61
34.61
68.74
54.00
52.71
51.95
50.40
C5 a
C6
C7
C8
C9+
a
2.4.
Transalkylation
2.5.
Transalkylation is the reaction between two similar or dissimilar molecules involving transfer of an alkyl group. In
the alkyl-transfer reactions, shift of alkyl groups from one
ring to the other, depends on the number of alkyl groups
on the aromatic ring/s, the type of alkyl substituent/s and
the chain length (Roldn et al., 2004). In the proposed model,
transalkylation between aromatics is considered. Two toluene
rings can disproportionate to produce one benzene ring and
one Para xylene ring, in addition, two Ortho-xylene rings
disproportionate to produce one toluene and higher aromatics (A9 + ). These reactions are promoted by the catalyst
metallic function, and with increase in the reaction temperature, the conversion increases. It should be mentioned that
transalkylation occurs mainly in very severe conditions of
pressure (Roldn et al., 2004). Calculated constants for reaction rate in the transalkylation reactions are presented in
Table 6.
Hydrocracking
Breaking of carbon bonds in the reforming is called hydrocracking. Bonds breaking can occur at any position along the
hydrocarbon chain. This reaction by removing the low octane
number parafns and naphthenes from reformate and producing lighter hydrocarbons, such as methane, ethane and
propane, helps to improve the octane in the products (Matar
and Hatch, 2000). Hydrocracking is an irreversible reaction and
is favored at high temperature and high pressure, also is catalyzed by the acidic or metallic function of the catalyst (Antos
and Aitani, 1995; Matar and Hatch, 2000). Reaction constants
for hydrocracking of parafns and naphthenes are shown in
Tables 7 and 8, respectively.
2.6.
Hydrodealkylation
C7
C8
for An+1 = PX
for An+1 = EBa
C9 +
for Ak = OX
for Ak = T a
a
k16n = exp a
1
E
RT
1
(kmol kg1
kPa1.5 )
cat h
E
R
41.81
7.64
17.92
n
n1
42.32
20.02
5.57
5.55
17.92
17.92
n
n1
52.57
30.80
8.91
5.57
17.92
17.92
H(kJ (mol H2 )
1
2
1
2
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3.
Process description
recycle hydrogen gas and, after heating to the desired reaction temperature (798 K), it is sent to a series of reactors. The
specication of conventional process such as reactors, feed,
product and catalyst are shown in Table 10.
In the CCR process, spherical catalysts are used in the reactors to facilitate catalyst circulation by gravity. Coked catalyst
is withdrawn from the last reactor and sent to the regeneration unit, then, regeneration of the catalyst is performed as
the catalyst moves down in the regeneration unit on a continuous basis. Regenerated catalyst is added to the top of the
rst reactor to keep the efciency of process at the certain
level, and catalyst regeneration leads to reduction in operating cost, whiles, poor catalyst will lead to low product yields
and increase in operating expense. As shown in Fig. 4, catalyst ows vertically in the reactor; and the feed ows radially
through the catalyst bed (reaction side) of the reactor, thus
cross ow pattern exist in the reactors.
4.
Please cite this article in press as: Iranshahi, D., et al., Modeling of naphtha reforming unit applying detailed description of kinetic in continuous
catalytic regeneration process. Chem. Eng. Res. Des. (2014), http://dx.doi.org/10.1016/j.cherd.2013.12.012
ARTICLE IN PRESS
Table 10 Specications of reactors, feed, product and catalyst of plant for fresh catalyst.
Parameter
Numerical value
233637.01
216488.63
2.193
0.83
2nd reactor
798
550
1.25, 2.35
10.35
18
1st reactor
798
595
1.25, 2.19
8.50
12
Unit
3rd reactor
798
505
1.30, 2.53
12.1
25
kg/h
kg/h
4th reactor
798
460
1.3, 2.89
15.39
45
Naphtha feed ( C)
IBP
5%
10%
20%
30%
40%
50%
60%
70%
80%
90%
95%
FBP
81
91.2
93.2
96.9
101.1
105.7
111.4
117.6
124.5
132.7
143.1
150.5
159
1.8
0.3
0.3
220
680
0.36
mm
wt%
wt%
m2 /g
kg/m3
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Table 11 Catalyst functions on the main reactions in the proposed kinetic model (metallic (M) and acidic (A) functions).
Reactions
Agent
Reactions
r1n
r2n
r3n
ACHn An + 3H2
ACHn + H2 NPn
ACHn + H2 IPn
M
M+A
M+A
r9n
r10n
r11n
NPn IPn
RP
2R P + C
r4n
NPn ACPn + H2
M+A
r12n
NPn +
(n3)
3 H2
Agent
n
15
5
A
A
M
M or A
Pi
i=1
5
r5n
IPn ACPn + H2
M+A
IPn +
r13n
(n3)
3 H2
n
15
Pi
M or A
Pi
M or A
Pi
M or A
i=1
5
r6n
NPn An + 4H2
M+A
ACHn + n3 H2
r14n
n
15
i=1
5
r7n
r8n
IPn An + 4H2
ACPn ACHn
M+A
ACPn + n3 H2
r15n
n
15
i=1
An+1 + H2 Ak + Cm H2m+2
r16n
exp(Ec /RT)
Pn1 (H2 /HC)
n2
C0.5
ACP
(17)
where rCo , Ec , CACP , P and (H2 /HC)are the rate of coke formation
on the fresh catalyst, coke formation activation energy, alkylcyclopentane concentration, pressure and hydrogen over
hydrocarbon mole ratio, respectively. In addition, the rate of
reaction over a spent catalyst is calculated by multiplying the
catalyst activity on the dominant function and rate of reaction
over fresh catalyst.
ri = ai rio
(18)
If ni = 1 ai = exp(i CCi )
dai
= i ani i
dCCi
If ni =/ 1
ai =
1
(1 + (ni 1)i CCi )
(1/(ni 1))
(19)
(20)
where rCi and rC0 are coke formation rate of spent catalyst
i
on dominant function and rate of coke formation on dominant function of fresh catalyst, respectively. Similar to catalyst
activity in the reaction rate, catalyst activity in coke formation
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If
daCi
= Ci anCCi i
dCCi
nCi = 1
/ 1
If nCi =
1
(1 + (nCi 1)Ci CCi )
(1/(nCi 1))
(21)
5.
Mathematical modeling
6.
Numerical solution
7.
Model validation
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(22)ri = ai
rio
ai
ai
ai
ai
= aA
= aM
= mean(aA , aM )
= mean(aA , aM )
(23)ri = aM rio
(24)ri = aA rio
da
da
(25) dC M = M anMM
(26) dC A = A anAA
CM
nM = 1
CA
nA = 1
aM = exp(M CCM )
(27)
nM =/ 1
(28)
aM =
nA =/ 1
(1/(nM 1))
(31) dC M
CM
= CM
nCM = 1
(33)
nCM =/ 1
(35)rCo
M
8.
aA =
daC
aA = exp(A CCA )
1
(1 + (nA 1)A CCA )
(1/(nA 1))
daC
anCCM
M
(32) dC A
CA
nCA = 1
(34)
1
(1 + (nCM 1)CM CCM )
exp(Ec /RT)
M
Pn1 (H2 /HC)n2
kC
= CA anCCA
nCA =/ 1
(1/(nC 1))
M
C0.5
ACP
(36)rCo
A
1
(1 + (nCA 1)CA CCA )
kC exp(Ec /RT)
A
Pn1 (H2 /HC)n2
(1/(nC 1))
A
C0.5
ACP
The process of continuous catalyst regeneration is characterized by high catalyst activity, high quality reformate, and
high hydrogen purity. The results of the mathematical modeling for the CCR process are illustrated in the following. The
variations of parameters have been investigated in the dimensionless radial and axial coordinates for 3-D plots, also the
variations of some parameters have been investigated in 2-D
plots.
As can be seen in the results (Tables 14 and 15), satisfactory agreement can be observed between the simulated
Table 13 Mass and energy balances and auxiliary relations for CCR process.
Mass balance
Cj
Cj j = 1, 2, ..., n
1
1
ai
ij ri =
(Ar
)
(Ar ur Cj ) + b
Ar r
r
Ar r
t i = 1, 2, ..., m
m
(37)Dej
i=1
Cj ur
b
j = 1, 2, ..., n
ai
ij ri
=
+
(38)
r
r
ur r
ur
i = 1, 2, ..., m
m
Cj
Cj
i=1
Energy balance
T
1
(Keff Ar
) b
(39)
Ar r
r
b
(40) T
r = ur C C
m
T P
m n
i=1
(Hj vij ) ai ri
j=1
n
Nj
Hj
r
j=1
n
Cj
Uj
t
j=1
n
(Uj Hj )
Cj
t
j = 1, 2, ..., n
i = 1, 2, ..., m
j=1
(Hi ai ri ) i = 1, 2, ..., m
i=1
Velocity distribution
(41)
ur
ur
CT
ur
b
+
r
r
CT
r
Ct
n
m
j=1
ai
ij ri
j = 1, 2, ..., n
i = 1, 2, ..., m
i=1
Fj
z
j = 1, 2, ..., n
n
j=1
CP
P z
T
(45) T
z = C
T
FT
1
FT CP
150 (1)2
3
s2 d2
p
ur +
1.75 (1) 2
ur
s dp 3
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Molecular
weight
Input plant
(mole fraction)
86.178
100.205
114.232
128.259
86.178
100.25
114.232
128.259
84.162
98.189
112.216
126.243
70.135
84.162
98.189
112.216
126.243
78.114
92.141
106.168
120.195
106.168
106.168
106.168
2.016
16.043
30.07
44.097
58.124
72.151
58.124
72.151
Output
plant
(kmol/h)
0.0229
0.0292
0.0239
0.0156
0.0232
0.0314
0.0338
0.0244
0.0077
0.0084
0.0115
0.0018
0.0001
0.003
0.0065
0.0084
0.0012
0.0086
0.0109
0.0021
0.0026
0.0015
0.0016
0.0036
0.6226
0.0211
0.0231
0.0202
0.0106
0.0035
0.0073
0.0076
8.1.
Investigation of operating conditions during the
process
In this section, variation of operating conditions (pressure and
temperature) in CCR process is investigated. One of the advantages of the CCR process is the negligible pressure drop in the
reactors, which allows the use of smaller catalyst particles
with higher efciency. As shown in Fig. 6a, the variations of
pressure inside the reactors are slight, and sudden drops are
71.84
46.65
8.1
1.15
216.06
110.18
22.75
1.79
0.51
0.92
2.33
0.04
2.14
26
2.33
0.6
0.01
205.84
453.93
163.02
323.66
113.62
120.84
276.56
10071.31
398.53
399.16
352.36
189.21
71.06
140.75
149.21
Output model
(kmol/h)
Deviation
(kmol/h)
70.98
46
7.63
1.25
216.06
109.69
22.67
1.95
0.92
1.43
2.34
0.05
2.11
26.02
3.12
0.6
0.02
206.39
454.33
163.47
324.46
113.4
121.55
276.8
10090.82
396.64
397.72
351.69
189.93
71.69
139.38
149.49
0.86
0.65
0.47
0.1
0
0.49
0.08
0.16
0.41
0.51
0.01
0.01
0.03
0.02
0.79
0
0.01
0.55
0.4
0.45
0.8
0.22
0.71
0.24
19.51
1.89
1.44
0.67
0.72
0.63
1.37
0.28
Table 15 Comparison between predicted temperature, pressure and molecular weight with plant data.
Reactor number
1
2
3
4
Outlet temperature
Outlet pressure
Plant
Model
Plant
Model
Plant
Model
707
725
743
761
710.7
726.4
743.2
758.9
581
535
490
446
585.1
540.3
495.7
451.4
21.9
21.87
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8.2.
Catalyst investigation
8.3.
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Fig. 7 Coke concentration distribution in (a) metallic function, (b) acidic function and (c) total coke. (d) comparison coke
content in various length of reactors.
8.4.
Pseudo-components
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0.95
0.9
0.85
0.8
0.75
0.7
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
1
Z=0
Z=L/4
Mean
Z=3/4*L
Z=L
0.85
200
150
100
50
0.1
0.2
0.3
0.75
0.7
0.65
0.6
0.4
0.5
0.6
0.7
0.8
0.9
160
0.8
140
120
100
80
60
40
20
0.55
0.5
250
0.9
300
0.95
Z=0
Z=L/4
Mea n
Z=3/4*L
Z=L
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
8.5.
Physical properties
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a
900
700
600
500
400
300
200
100
0
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
M-xylene
O-xylene
200
P-xylene
150
100
50
b
1000
Ethylbenzene
800
700
600
500
400
300
0.4
0.5
0.6
0.7
0.8
0.9
0.8
0.9
0.9
A9+
Benzene
200
150
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
8.6.
Supercial velocity
Ur =
Rm T
PMA
(47)
12000
Molar flow rate along inner annulus of rea ctor
Mea n molar flow rate along radius of reactor
parameters. In this section, variations of these physical properties are illustrated in radial coordinates. Heat capacity
variations, is depicted in Fig. 15a. As previously mentioned,
the major reforming reactions are highly endothermic, thus,
temperature decreases in radial direction and due to direct
relationship between heat capacity and temperature, heat
capacity decreases in the reactors. As can be seen in Fig. 15a,
at the entrance of reactors heat capacity is high due to high
temperature, but endothermic reactions in the reactors cause
temperature drop. Consequently, reduction of heat capacity
can be observed in each reactor. The outlet stream of reactors is preheated via a furnace that causes sudden jumps in
the heat capacity plot. During the process, increase of temperature has a positive effect on the heat capacity, but due to
production of hydrogen, which has a very low heat capacity in
comparison of other components, downward trend occurs.
In the viscosity behavior, dominant agent is temperature of
components. Thus, during the process, the trend of viscosity
obeys temperature conditions. As shown in Fig. 15b, viscosity decreases along the radius of reactors due to temperature
reduction, and an ascendant trend can be observed during the
process, because the outlet stream of reactors is heated by
the furnace. One of the other signicant physical properties
in the naphtha reforming process is molecular weight, which
is affected by proceeding of the reactions. In Fig. 15c, molecular weight is depicted vs. radius of reactors. Molecular weight
decreases in the radial direction due to proceeding of reactions
and produce light products such as hydrogen and light ends.
0.7
Toluene
250
0.6
300
0
0.3
0.5
350
50
0.2
0.4
400
100
0.1
0.3
500
100
0.2
200
0.1
450
250
900
800
300
10000
8000
6000
4000
2000
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
Annulus Length(Radius) of reactor (Dimensionless)
0.9
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1800
Molar flow rate along inner annulus of rea ctor
Mean molar flow rate along radius of rea ctor
1600
1400
1200
1000
800
600
400
200
0
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
140
Heat capacity(KJ/Kmol.K)
130
120
110
100
90
80
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
-5
x 10
1.8
Viscosity(Kg/m.s)
1.75
1.7
1.65
9.
1.6
Supercial velocity can be varied with the changes of temperature (T), pressure (P), molecular weight (M) or cross section
area (A) at various radial positions. But supercial gas velocity
almost is unchanged at various axial locations because in the
axial direction the temperature and pressure gradient are very
small, cross section area is constant, and molecular weight
is almost unchanged in this direction. Consequently, supercial velocity along the various lengths of reaction side in each
radius is nearly constant. As shown in 3-D plot in Fig. 16, in
the radial direction, supercial velocity increases, because in
this direction pressure, temperature, molecular weight and
cross section area decrease. Although diminution in temperature causes reduction of supercial velocity, but the effect of
decrease in molecular weight, cross section area and pressure
are more. Consequently, according to Eq. 47, supercial velocity increases in the radial direction. Auxiliary correlations of
velocity distribution are presented in Appendix D.
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
0.8
0.9
30
25
20
0.1
0.2
0.3
0.4
0.5
0.6
0.7
Conclusions
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Reaction rate of pseudo-components based on activity of catalyst and reaction rate on the fresh catalyst can be obtained
by:
uz
ri = ai rio
rC
CCM
= M
z
uz
(A1)
CCM
= rCM
z
(A10)
ai = aA
ai = aM
ai = mean(aA , aM )
ai = mean(aA , aM )
(A2)
daM
= M anMM
dCCM
(A3)
(A4)
1
(1 + (nM 1)M CCM )
(1/(nM 1))
FCM
= rCM (B 2 r r)
z
(A6)
where FCM and rCM , are mass ow rate of coke and rate of coke
formation on the metallic function of catalyst. In addition, FCM
can be dened as:
.
(A7)
rCo M =
n2
C0.5
ACP
(A13)
(A14)
(A15)
1
(1 + (nCM 1)CM CCM )
(1/(nC 1))
M
To calculate the rate of coke formation on the metallic function Eqs. (A15) and (A13) must be replaced in Eq. (A12), then by
substituting coke formation rate in Eq. (A11), coke weight fraction on the metallic function (CCM ) could be calculated. With
same procedure, the rate of reactions that are catalyzed by
acidic site could be achieved, the results shown in Table 12. In
addition, required constants to calculate catalyst deactivation
rate and activity are presented in Table A.1.
(A12)
(A5)
(A8)
If nM = 1 aM = exp(M CCM )
If nM =/ 1 aM =
(A9)
To develop the mathematical model the derivation of governing equations (mass and energy balances) have been discussed
here. The mass balance for a control volume with length of dz
and cross section area of A is:
Input Output + Consumption = Accumulation
(B1)
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Value
1
nM
nCM
(B7)
kgcat
kgcoke
26
Ar = 2r dz
Dimension
Cj
1 (Nj Ar )
+ b
ai vij ri =
Ar
r
t
m
(B8)
i=1
kgcat
kgcoke
12.34
CM
nA
14.5
nCA
kgcat
kgcoke
Nj = Dej
Cj
r
+ Cj ur
(B9)
or
kgcat
kgcoke
10.18
CA
Cj
kCM
0.384
Nj Ar = Ar Dej
kCA
1.386
J
mol
4055
Ec
n1
0.94
n2
1.33
+ Ar Cj ur
(B10)
Cj
1
1
)
ai
(Ar
(Ar ur Cj ) + b
Ar r
r
Ar r
m
Dej
i=1
ij ri =
Cj j = 1, 2, ..., n
t
(B11)
i = 1, 2, ..., m
m
ai vij ri Ar
dr =
(B2)
i = 1, 2, ..., m
(Nj Ar )
r
dr + b
m
ai vij ri Ar dr =
nj
i=1
nj
1 (Nj Ar )
1
ai vij ri =
+ b
Ar
r
Ar dr t
Cj
ur Cj Ar
ur
1
Cj
(Ar ur Cj ) =
ur
Ar r
r
Ar r
r
=
ur Cj
r
ur
Cj
r
Cj
ur
r
ur Cj
r
ur
Cj
r
j = 1, 2, ..., n
ur
ai
ij ri = 0
+ b
r
i = 1, 2, ..., m
m
Cj
i=1
(Ar dr )
(B5)
Cj
r
Cj ur
j = 1, 2, ..., n
+ b
ai
ij ri
ur
ur r
i = 1, 2, ..., m
m
(B15)
i=1
Or
nj = Cj (Ar dr )
(B14)
(B4)
i=1
Cj =
(B13)
(B3)
nj
(B12)
i=1
nj j = 1, 2, ..., n
t
j = 1, 2, ..., n
1
ai
ij ri = 0
(Ar ur Cj ) + b
Ar r
i = 1, 2, ..., m
m
i=1
(B6)
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accumulation
of energy
Rate of
within the
Rate of
Rate of
energy leaving
to the system + the system
energy added
by conduction
system
by conduction
heat transfer
work done
by the
system on the
leaving
added to the
+ system by mass
ow into the
Rate of
ow of heat
from the
the system
Nj Ar Hj
j=1
Hj
Nj
Hi =
Hj
j = 1, 2, ..., n
(B17)
i = 1, 2, ..., m
n
Hj
T
n
Hj
Nj
(
r
n
j=1
j=1
(B18)
The term
n
Hj
Nj
j=1
n
Uj
Cj
j=1
n
(Uj Hj )
j=1
Cj
(B22)
(B23)
T
T
= CPj
r
r
(B24)
T
)
r
((Jj + Cj ur ) CPj
T
T
((Jj + Cj ur ) CPj ) ur (
Cj CPj )
r
r
n
j=1
j=1
n
Cj
j=1
)CPj ) = CT
CT
n
yj CPj = CT CP
Cj
t
= RT
(B25)
(B26)
j=1
(B27)
n
Cj
j=1
= RT
CT
t
(B28)
b
m
i=1
T
T
= CVj
t
t
(B29)
(B30)
CV = CP R
(B31)
Also:
n
Uj
ai vij ri +
Uj
CVj = CPj R
j=1
(B19)
j=1
Cj
j=1
Cj CPj ) = CT (
j=1
Uj
1
T
Hj
(Keff Ar ) +
Ar r
r
j=1
(Uj Hj )
Uj
n
Cj
(Nj Ar )
r
(B21)
j=1
Uj
j=1
(Uj Hj ) = Pvj = RT
n
1
T
1 (Nj Ar ) Hj
Hj
Nj
(Keff Ar )
Ar r
r
r
r
Ar
j=1
Uj
n
j=1
n
Cj
j=1
Cj
(vij Hj )
Nj Ar Hj )
j=1
n
Uj
j=1
Cj
j=1
Uj
nj
1
1
nj
Uj
+
Ar dr
Ar dr
t
t
Hj
j=1
j=1
1
T
1
(K Ar )
Ar r eff
r
Ar
n
i=1 j=1
r+dr
n
nj Uj )
ai vij ri
i=1
j=1
j=1
Cj
1
T
(Keff Ar ) b
(Hj vij ) ai ri
Ar r
r
b
m
Now we have:
surroundings
n
T
T
Keff Ar + Keff Ar
+
Nj Ar Hj
r r
r r+dr
j=1
n
Uj
n
Nj
j=1
(B16)
n
Hj
system
Rate of energy
j=1
Rate of energy
surroundings
1
T
(Keff Ar )
Hj
Ar r
r
heat transfer
Rate of
Hence:
Cj
Cj
j=1
n
Cj CVj
j=1
T
T
T
Cj CVj = (
Cj CVj )
=
t
t
t
n
j=1
j=1
(B32)
(B20)
r
n
Cj
Uj
j=1
n
j=1
Cj CVj ) = CT (
n
Cj
j=1
CT
)CVj ) = CT
n
yj CVj = CT CV
(B33)
j=1
Please cite this article in press as: Iranshahi, D., et al., Modeling of naphtha reforming unit applying detailed description of kinetic in continuous
catalytic regeneration process. Chem. Eng. Res. Des. (2014), http://dx.doi.org/10.1016/j.cherd.2013.12.012
ARTICLE IN PRESS
22
1
T
(K Ar ) b (
Ar r eff
r
ur CT CP
m
j=1
= 2Ri ure
n
(Cje )
(C5)
j=1
FT
= 2Ri ure CTe
z
Hi ai ri )
i=1
T
T
CT
= CT CV
RT
r
t
t
n
Fj
(B34)
(C6)
FT CP T|z FT CP T|z+dz +
And then,
n
(C7)
j=1
1
T
(Keff Ar ) b (
Hi ai ri )
Ar r
r
m
i=1
CT
T
T
ur CT CP
+ RT
= CT CV
r
t
t
(B35)
FT =
n
(C8)
Fj
j=1
Due to steady state conditions and low amount of conductive heat transfer in comparison with convective heat transfer,
therefore, heat transfer simplify to:
T
(Hi ai ri ) = 0
b
r
n
M=
ur CT CP
(B36)
n
T
b
(Hi ai ri )
=
r
ur CT CP
m
(B37)
i=1
Cp =
n
j=1
(C9)
FT
i=1
Mj Fj
j=1
Fj Cpj
j=1
(C10)
FT
n
Cje
((
j=1
CTe
)CPje ) = CTe
n
j=1
(C11)
FT CP T|z FT CP T|z+dz +
Fj |z Fj |z+dz + Fje = 0
(C1)
(C2)
j=1
(C12)
n
(C3)
(FT CP T)
= 2Ri ure CTe Cpe (Te T)
z
(C13)
CP T
(FT )
(T)
(CP )
+ FT CP
+ FT T
= 2Ri
z
z
z
(C14)
Then, to calculate total molar ow rate FT , the summation of recent equation for all pseudo-components must be
considered:
n
Fj
j=1
n
j=1
(C4)
1 T
1 CP
1 FT
1
+
+
=
2Ri
T z
CP z
FT z
FT CP T
ure CTe Cpe (Te T)
(C15)
Please cite this article in press as: Iranshahi, D., et al., Modeling of naphtha reforming unit applying detailed description of kinetic in continuous
catalytic regeneration process. Chem. Eng. Res. Des. (2014), http://dx.doi.org/10.1016/j.cherd.2013.12.012
ARTICLE IN PRESS
+
z
CP z
FT z
FT CP
2Ri ure CTe Cpe (Te T)
(C16)
z
CP z
FT
FT CP
ure CTe Cpe (Te T)
(C17)
Cj
r
Cj ur
ai
ij ri
+ b
ur r
ur
m
i=1
j = 1, 2, ..., n
i = 1, 2, ..., m
(D1)
Then the summation of recent equation for all pseudocomponents must be calculated
n
Cj
j=1
n
j=1
Cj
r
1 ur
Cj + b
ai
ij ri
ur r
ur
n
j=1
(D2)
j=1 i=1
CT
CT
CT ur
=
ai
ij ri
+ b
r
r
ur r
ur
(D3)
ur
CT
ur
ur
ai
ij ri
=
+ b
CT
r
r
r
CT
(D4)
j=1 i=1
n
j=1 i=1
ai
ij ri
=
+ b
r
r
CT
r
Ct
n
(D7)
j=1 i=1
To nd
CT =
CT
r
P
RT
(D8)
r
RT r
RT 2 r
(D9)
References
Aitani, A.M., 2005a. Catalytic naphtha reforming. In:
Encyclopedia of Chemical Processing.,
http://dx.doi.org/10.1081/E-ECHP-120039766.
Aitani, A.M., 2005b. Catalytic Naphtha Reforming. Science and
Technology. Marcel Dekker, New York.
Antos, G.A., Aitani, A.M., 1995. Catalytic naphtha reforming, 2nd
ed. Marcel Dekker, New York.
Barbier, J., 1986. Deactivation of reforming catalysts by cokinga
review. Appl. Catal. 23, 225243.
Bishara, A., Stanislaus, A., Hussain, S., 1984. Effect of feed
composition and operating conditions on catalyst
23
Please cite this article in press as: Iranshahi, D., et al., Modeling of naphtha reforming unit applying detailed description of kinetic in continuous
catalytic regeneration process. Chem. Eng. Res. Des. (2014), http://dx.doi.org/10.1016/j.cherd.2013.12.012
24
ARTICLE IN PRESS
chemical engineering research and design x x x ( 2 0 1 4 ) xxxxxx
Further reading
Perry, R.H., Green, D.W., Maloney, J.O., 1999. Perrys Chemical
Engineers Handbook, 7th ed. McGraw-Hill, New York.
Please cite this article in press as: Iranshahi, D., et al., Modeling of naphtha reforming unit applying detailed description of kinetic in continuous
catalytic regeneration process. Chem. Eng. Res. Des. (2014), http://dx.doi.org/10.1016/j.cherd.2013.12.012