Proreedings of the 42nd IEEE

Conferenm on Decision and Control

Maui, Hawaii USA, December 2003 FrE04-1
Modeling, Simulation and Optimization of Commercial Naphtha Catalytic Reforming Process
Yongyou Hu’, Hongye Su, Jian Chu

National Laboratory of Industrial Control Technologv, Institute ofAdvanced Process Control,

Zhejiang Universiry, Yuquan Campus, Haitgzhou, 310027, P.R.China
* CorrespondingAuthor eniail: ~l’hti!~iioc.iiu.edti.
cn

Abstract - A kinetics-based mathematic model for commercial
catalytic reforming process is developed to monitor and
optimize the process in this paper. The process model can
predict reaction temperature and concentration profiles of
each reactor, heater duties, catalyst deactivation, recycle gas
composition and octane number resulting from different
feedstocks or operating conditions. The lumping details of the
naphtha feed and reaction scheme are given. The reaction
model i s described by Hongen-Watson-type rate equations
with catalyst coking kinetics. Ihe nonlinear optimization
problem with process constraints is solved by the
Lagrange-Marquardt composite optimization algorithm. The
simulation and optimivltion results of the model validated for
three different commercial catalytic reforming processes are
presented.
1. INTRODUCTION
Catalytic reforming of naphtha is a very important
process in hydrocarbon processing industry for octane
improvement or as sources of aromatics and hydrogen. The
process model of catalytic reforming can be applied to
designing new processes, monitoring process performance,
troubleshooting, diagnosing faults, optimizing process and
process control [1][11][13]. Being those profitable
applications of process model, research on catalytic
reforming kinetics and process modeling has been
intensified by some institutes and companies involved [6].
The catalytic reforming of naphtha involves reactions
such as dehydrogenation, dehydrocyclization, hydrocrack-
ing, isomerizationand and hydrodealkylation. The naphtha
feed to reformer is very complex usually consisting of about
three hundreds Components with the carbon number range
from 5 to 9+. A detailed model considering all components
and reactions is infeasible, so a e m p t s had been made to
application, a simple but sound lirst-principle model of
catalytic reforming with 17 lumps involving only 17
reactions is proposed in this paper. The catalyst deactivation
due to coking is accurately considered in this model in
terms of the average deactivation function. The adsorption
of chemical lumps on the catalyst surface is also considered
here. The model kinetic parameters are benchmarked with
plant data. Process optimization based on kinetic model is
also studied on the commercial continuous catalyst
regeneration (CCR) reforming process.
2. PROCESS MODELING
The modem catalytic reforming is generally carried out
in theelfour fixed or moving bed reformers. The catalyst
used in reformer is commonly a bifunctional bimetallic
catalyst such as Pt-Re/Abq, F’t-SdAl~O~ providing the
metal function and the acid function. Figure 1 shows a
typical CCR reforming process flow sheet consisting of
four stacked reformers, a catalyst regeneration section, a
fued heater, a flash separator and a Cs+ recovery system.
2.1 Kinetic Reaction Model
The feed to the first reformer is generally cut from
straight run naphtha, of which the boiling point varies
depending on the type of reforming process and products.
In this model, the naphtha feed is characterized into PNA
(Paraffins, Naphthenes and Aromatics) lumps of each
carbon number from 6 to 9+ and light paraffins (Cl+).
The reforming reaction network undergone by all 17 lumps
is shown in Figure 2.
In this reaction network, dehydrogenation of naphthenes
to aromatics is the most rapid of all reforming reactions and
.
is catalyzed by the metal function ofthe catalyst. This

split naphtha into kinetic lumps and some notable models

had been developed in past decades [3] [5] [SI [11-13].
Generally, detailed models are theoretically sound but
quite complicated. Especially, normal and branched R
paraffis, or five and six-membered ring naphthenes were
distinguished in most of reported models except for Smith’s
model[lZ], which is difficult for application in some plants
because of costly analysis of components and getting
enough plant data for parameter estimation difficultly. On
the other hand, too complex lumping scheme will
drastically increases the number of estimated kinetic
parameters and the difficulty for the convergence of relative Fig. I A f7ow diagram for CCR reforming process -UOPPlatforming
algorithms. Considering the convenience of model

0-7803-7924-1/03/$17.0002003 IEEE 6206

 (4)
P- %A
+- * The reaction rate coefficients of (1) - (4) obeying the
Arrhenius law can be written as
koJ.exPC-€, I RT).P: I @ ,j = 1 - 4
(5)
l r ,j = 5 - 1 7
k,, .exp(-E, I RT) .EqJ
where the adsorption term for the metal function, @andfor
the acid function,l'can be defined in [14].

@ = 1+ P,,+ K ~ . P , / P : , K',=2.7Mpn-I,
K:( = 48.1 Mpn
Fig.2 Reaction scheme for naphtha reforming

reaction favors the formation of aromatics and increases the l- +

1 Kc3- .Pc I f h + K , .PpI Ph +K ,PNI Ph +K .PA,
octane number of reformate. Dehydrocyclization of Kc5- =107,K, =21.9,Kh, =659,KA =703Mpa-'
paraffins to naphthenes is a comparatively slow reaction but
very important for increasing the yield of aromatics. The Note that the six equilibrium constants of adsorption were
hydrocracking of paraffins and hydrodealkylation of
acquired hy studying the reforming of Q hydrocarbons and
aromatics are minor, much slower reactions forming less
valuable products than others. Generally, the reforming here we extend them to other hydrocarbons with different
reaction rates can be represented by first-order kinetics [I I ] . carbon number.
To best describe the reactions, here the Hougen-Watson The reaction equilibrium constant K,, in (I) and (2)
Langmuir-Hinshelwood adsorption model is employed. can be calculated by the following thermodynamic relation,
Corresponding rate equations are presented below. K, = exp(-AG, IRT),j = 1 8 - (6)
Dehydrogenation The rate equation for hydrogen balance is
N, t . A , + 3 H 2 j = 6 , 1 , 8 , 9 + 4 8 17
rJ = dYMI d (VcI FHC)= k, . (Y, -YA, I K,,), j = 1 4 - dY,, l d ( y l F w ) = 3 C r +E?-E? (7)
(1)
JII ,=5 ,+

-
Dehydrocyclization
+
4 N i H,,i = 6,7,8,9 +
r, = dY,, I d ( t IFH(.)= k, .(U,, -Y,v I Ken,),j = 5 -8
Under the normal reformer operating conditions, radial
and axial dispersion effects were found to be negligible [13].
For radial flow reactoq the global material and enthalpy
balance equations are given by
(2)
Hydrocracking

where Pis a vector of molar flow rates including seventeen

lumps and H2.
I
The pressure drop in radial flow reactor can be omitted
&+HZ - 1 1 4 ( P , + P 6 + ~ C , + C , ) for it is far smaller than that in axial flowreactor. The Ergun

- i= I equation [4] is adopted to predict the total pressure drop in

5 axial flowreactor.
P,, + H , 1l4(P, + P, + 5 + c C , )
j=,

rJ = dY, I d V C /FHc)= k,,'yP,,i =5 - 9 + , j = 9-13

(3 ) The free energy AG, in (a), heat of reaction AH,and
Hydrodealkylation e,,
specific heats in (8) are taken from API data book [ 2 ] .
A,+H,+% t C , , $ + H , - q +q 2.2 CatalystDeactivation Model
During the running of reformers the catalyst gets
.%++Hi+ 4 + c * , 4 + + H z * 4 + G
deactivated by coke deposition blocking the active sites and
r, = dY,,Id(< IF,.)= k , . yAj,i = 7 - 9t,j = 14-17 reduces the selectivity of catalyst and the products yields.

6207
For predicting the behavior of such reactions subject to Being the specific configuration of radial flow reactor
catalyst deactivation, the coking rate equation is also
included in the kinetic model. Generally, both the reforming
and coking reactions decrease exponentially with coke
deposited on the catalyst [9][141 The modified rate
equations by introducing a deactivation functionf are
rj = r ; . f , O < f < I , j = l - l 7 (10)
where r,: is the jth reaction rate at fresh catalyst. The
coking rate equation and deactivation function of catalyst
are as follows [9].
dCK
?-<(I)=-= r,‘ . f (1 1)
d
f = exp(-a. CK) (12)
d e r e r; is the coking rate at fresh catalyst correlated with
feed composition, hydrogen partial pressure and reforming
severity. For convenience, we suppose that is equal at Fig. 3 The cnnIiguration ofradial flaw m c b r
any point of reactor and can be written as
rc~= k, .exp(-~, /WAIT/ 4 . 4 .f;: ,( T /T,)E ~ ,.~ ~(1 3) shown by Figure 3, the oil gas flows radially through the
where = L H ~ V. fie corresponding parameters can be catalyst bed and the reforming reactions undergo all
estimated from experimental or plant data. catalysts with different coke content along the axial
fiereforming operation varies with time on stream, so direction almost at the same time. If we divide averagely
r; is a nonlinear function with r. B~ substituting equation reactant into N sections along axial coordinate of each
reactog the material balance equation of (8) can he
(12) into (1 1) and integrating it, we can get
modified as
CK(r) = (lla) In(l + a . sr:(t)df) (14)
.-=
dFlN 2pR’H K,.f/N
0
dR fi. LHSV . V<
This equation can be applied only to the semi-regenerative (17)
unit of which the reformers are normally fixed beds. For dl/N 2pR.H
CCR, all reformers are moving bed and radial flow reactors. -- - fN, K;?IN
The catalyst with coke are moved continuously and slowly
dR LHSV.Vc
through the reactors, withdrawn from the last reactor,
regenerated in a regeneration section, and returned to the
first reactor as fresh catalyst. Obviously, the coke content
on catalyst increases with residence time of catalyst or axial
coordinate of the reactor, h (the axial coordinate of the inlet
of first reactor is supposed to zero). The correlation of coke
with h and f for CCR is given by

CK(h, 1) = (I/a).ln(l+ a . sT’

1-,*
<
(r)d),O h 5 H,,,,O 5 fh 6 f,,

(15)
with

J
H,, = O , H , , = c H , , j = l , . . . , n
1-3

The corresponding deactivation function given by (12) is

described by

f(h, I ) = I/( 1 s
+ a. r; (r)dt)
rWA
(16)

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separator model which is fairly straightforward and is with four radial flow reactors using P t - S d M ~ O catalyst,
,
illustrated in relative reference book [7], resolving the producing BTX (Benzene, Toluene, Xylene).
process model will involve successive substitution and the
direct substitution method is enough effective. TABLE 1. OPERATING CONDlTlONS
Case1 Case2 Case3
3. PARAMETER ESTIMATION Number ofreactors 4 4 4
Total catalyst (m’) 25.21 227.69 80.1
Considering catalyst deactivation, ( 5 ) can be modified as Catalyst loading ratio (wth)
RI 10.5 IO 15
ko, .exp(-E, I RT). 4qt
. f la2,j =1-4 RI 18.1 15 20
(26) IL 23.0 25 25
k,, ‘exp(-E, I RT). 6:.f i r ,j = 5 - 1 I Ri 48.4 50 40
Feed flow rate Fpm, 34000 359960 104450
If we estimate E, k, q for all seventeen reactions, there Latent ammatin (@A) 30.8 54.1 43.1
will be fifty-one kinetic parameters to be estimated in total &WC molar ratio gm) 3.34 1.76
3.716.9
and it is very difficult to estimate them synchronously. To LHSV (I&) 1.85 1.1 1.78
decrease the number of estimated parameters, we modify WAIT cc) 481.7 514 524.7
(26) further into Reaction Ressun M a ) 1.3 0.9 0.35
Separationtemperame (“0 40 36 60
Separation Resun (Mpa) 1.05 0.73 0.24
ki, .exp(-EjlRT).P, flQ2,j=1-4
k, = { (27)
ki, exp(-Ej/ RT). P$. f /I‘,j = 5-1 7 TABLE 2. COMPARISON OF PREDICEDAND ACTUAL VALUES
where k:, = ko, .exp(-AE, I R T ) . . Usually E, q casc 1 Case 2 casc 3
A n u P n d A c t u P n d A c h r M
reported by different literatures for the specific catalyst are Componenls in the reaElant ( e h )
similar, so A E,, Aq, are also small and it is acceptable to H> 9.56 9.94 7.67 7.15 6.30 6.10
consider k:, a constant for specific reaction and reformer. Cl
~. 3.49 4.02 1.86 2.40 0.13 1.03
The parameters E ; q’ are taken from [I51 in this model and Q 6.20 6.68 4.60 4.35 1.83 2.01
C3 9.38 9.80 8.98 8.17 2.73 3.50
only seventeen parameters k: are to be estimated as soon G 10.71 10.70 10.51 9.74 3.50 3.70
as catalyst deactivation functionf is acquired. By this way, C5 3.62 2.54 7.92 10.02 6.42 6.87
the difkiculty for parameter estimation is decreased greatly. Intotal 33.40 33.74 33.87 33.68 15.22 17.11
PI. 4.20 5.02 4.30 3.83 10.04 9.24
The procedure of parameter estimation is done by P; 10.38 10.23 2.63 2.55 4.87 4.59
minimization of the sum of the squares of the deviations Pt 6.95 6.59 0.22 0.21 1.11 0.82
between plant and calculated values of key variables such P9+ 2.81 2.43 0.00 0.03 0.15 0.20
In total 24.34 24.27 7.15 6.62 16.17 14.85
as compositions of components, outlet temperatures of N6 0.25 0.56 0.42 0.59 0.33 0.40
reformers. It is an unstrained optimization pmhlem and the NI 0.24 0.04 0.24 0.08 0.19 0.05
objective function forthis model is NI 0.20 0.08 0.03 0.01 0.04 0.04
Ng+ 0.04 0.10 0.00 0.00 0.00 0.00
Lntotal 0.73 0.18 0.69 0.68 0.56 0.49
AS 1.72 1.7i 4.84 5.39 5.58 5.36
A7 8.47 1.99 14.01 13.86 15.57 16.05
As 11.96 11.64 15.90 16.08 21.63 22.19
As+ 9.82 9.92 15.87 15.54 18.97 17.85
where S, m are the number of plant data samples and Intotal 31.97 31.27 50.62 50.87 61.15 61.45
focused components respectively. Many effective
optimization algorithms can be applied to solve the problem
AT C
s 61
RI 55 105 106 110 117
and the Marquadt optimization method [lo] is adopted RI 23 36 65
U3 14 IS 39
here. RA 16 17 17
Intotal 114 123 226
4. PROCESS MODEL VALIDATION
The operation and performance data samples for several RI (Mpa)0.15 0.14 -
Liquid yield (wth)
months of the commercial reforming processes, which are 90.54 90.20 75.8 76.5 86.0 86.4
firstly reconciled by material balance, are used to purity of recycle gas (vol.% B)
estimate k: . 86.3 85.7 86.2 85.7 89.1 90.4
Yield of ammatics (wth)
The operation conditions and simulation results of three 45.58 46.04 65.5 65.54 68.9 68.7
cases are summarized in Table 1 and Table 2, respectively. RON 87.2 87.5 - - - -
Case 1 is a fixed bed semi-regenerative reforming with two
stages of recycle-gases and using Pt-RelAlzO3 catalyst,
-
Coke content on the catalyst(wtO4
- 5.2 5.4 3.8 4.0
Heater Duty (GJh)
producing high-octane gasoline. The research octane I* - 6.71 - 57.65 - 29.13
number (RON) of gasoline is predicted by regressive model 2nd - 8.66 -
-
78.46 - 47.90
3rd - 5.87 47.74 - 28.11
Case 2 and 3 are both UOP CCR Platforming processes 4th - 3.21 - 26.60 - 18.07

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 CPU time on an IBM PC with Pentium 4 1.7GHz, 256M
Overall, of all cases the obtained agreement is
satisfactory in view of the scatter observed generally in
plant data. Hence allowing us to conclude that the lumping values and their gradients
and reaction schemes in this model are adequate reasonable.

5 . PROCESS OPTIMIZATION
Process optimization is noticeable and profitable
applications for kinetic model to improve the process
performance and maximize unit profitability. Optimizing
decision variables such as WAIT, HzMC and reaction
pressure can be achieved by rsolving he optimization
problem with process constraints described below
min J ( X ) = -AY = f , ( X )
(29)
g,(*)=c, -CK 2 0
Sf. g2(X)=c*-x2 2 0 (30)
g;@) = c 3 - € C 2 0
where B=[wAIr,H,/HC,P],CK=f,(X),EC=f,(X)
The objective function is aromatics yield (AY) representing
the unit profitability for the product values of BTX are
much larger than the energy cost. Process constraints are
mainly coke coking, capacities of recycle hydrogen
compressor and heaters. Obviously, it can be converted into
an unconstrained optimization problem by introducing the
Lagrange function
3
minL(2,I)=f(X)-CI;g,(X) (31) in each parameter separately and the results of the
i=l
where X is a vector with six elements including three
decision variables and three residual variables with which
the constrained inequalities are converted into equalities,
1 )is a Lagrange multiplier of corresponding constrained
inequality. The first-order necessary condition of this
optimization problem is VL = 0 , which can be replaced by
solving the following unconstrained optimization problem
with Marquardt method for the special formation of
objective function.
To perform the procedure of process optimization, a
simulator of process must be included to calculate the
objective and constraint values and their gradients for the conditions
optimizer. Figure 4 gives the optimization procedure by
means of a simple block sketch.
It has been proved that the so-called Lagrange-Marquardt
method is very effective for solving this NLP problem with
lower dimensionality. The computing of process model is
most time-consuming and it is necessary to choose an
optimization method that required fewer functional
evaluations for convergence. The advantage of Lagrange-
Declswn VanablCS
Fig. 4 Process optimization prccedure
DDR memory required for solving the NLP problem with
this method is only about 30-90 seconds depending on the
initial values of input variants. Table 3 gives the
optimization results of key operation conditions to
maximize the aromatics yield under specific naphtha feed.
As is shown in Table 3, the optimized process variables
can bring a potential increase of aromatics yield by 2.2
percent in weight. However, the actual result is subject to
the accuracy of kinetic parameters of the reaction model. A
study on kinetic parameter sensitivity is performed to assess
the impact of errors in some of main parameters: activation
energy, E, pressure exponent, q and deactivation constant,
a on the aromatics yield. A 10% relative error is introduced
sensitivity analysis are given in Table 4. Obviously, Table 4
indicates that the optimization result is not sensitive to the
uncertainty of model parameters.
6. CONCLUSIONS
A rigorous process model is developed for simulation and
optimization of commercial naphtha catalytic reformers.
The lumping scheme of the model greatly decreases the
analysis requirements and makes it easy to acquire lots of
plant data for parameters estimation. The model along with
deactivation function of catalyst can monitor the reformer
performance with time on stream. The simulation results
illustrate that agreements between model predictions and
plant observations are satisfactory for all cases. By applying
the model, it is possible to optimize the operating
TABLE 3. OpThlIzAnONRESULTS FOR
KEY PROCESS VARJABLES
Feed (th): 104.05 LHSV (Ih): 1.78
Latent " a t i c s (MA)): 49.1 Catalyst tupe: Pt-SdAkQ
Catalystdislrihutim(MA): RI: R2: R 3 R4 = 15: 20: 25: 40
Conslsaint Current Optimization
Process variable \dUe value result
WAn eo - 525 527.7
HI/HC (moVmol) -<-3 0 2.55 2.71
-
~

Marquardt method is to solve only one unconstrained Rcadonpressure (Mpa) 0.35 0.39
optimization problem rather than several these problems for Coke content (MA) 5 6.0 4.90 6.0
Heater capacities (GJh) 5 135 122.5 135
other methods such as Penalty Function method, SQP. The
Aromatics yield (MA) - 65.22 67.45

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 TABLE 4. S E N S l T ” ANALYSIS OF MODEL PARAMETER m =adsorption term for the metal fmction ofcatalyst
Parameterwith Aromatics LossofAmmaties r =adsorption term for the acid function ofcatalyst
10% m r yield (MA) yield (MA)*
q of dehydrocyclization 61.54 -0.09
f =deactivation fimction
q ofhydrocracldng 67.2 0.25 e ’ =void h t i o n of reactor he4 dim'
E of dehydrogenation 67.5 -0.05 m =vismity, pa.s
E of dehydracyclization 67.3 0.15 rc = catalyst density, Irgim’
E of catalyst colring 61.3 0.15
= nuid density, kg/ d
Deactivation constant. a 67.5 -0.05 r/
R = cross section of reactor, d
* Lass of AromaIics yield is Aromatics yield calculated by the model
with parameter error -us Aromatics yield (67.45%) calculated by the Superscripts
0 = mmposition exponent
model without any parameter enor.
of reforming process such as WAIT, reaction pressure, b. rl = presswe e+n&

HdHC, catalyst load ratio. c =relative t e m p z ” exponcnt

Subscripts
i.j =lump or reaction number
ACKNOWLEDGEMENT I,. ...9 + = carbon atom number
This work is supported by the National outstanding
Youth Science Foundation of China (NOYSFC: 60025308), REFERENCES
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