Beruflich Dokumente
Kultur Dokumente
Engineering
Science,
CATALYTIC
Pergamon
Press.
REACTIONS
Printed
in Great Britain
IN TRANSPORT
REACTORS
K. C. PRATT
Department of Chemical Engineering and Chemical Technology, Imperial College, London SW7 2BY,
England
(Received 21 August 1973)
Abstract-By
assuming plug flow of both gas and solids phases, and simple kinetics, a model of the
transport reactor has been prepared which accounts for the unsteady state behaviour of the catalyst
particles. Computational results are presented to show the influence of the major variables. As in a
steady state analysis, the Thiele modulus serves to indicate the catalyst effectiveness.
1. INTRODUCTION
2. THE MODEL
We shall consider a system in which both particulate and gas phases are in plug flow. The catalyst
particles are spherical and of uniform size. For
simplicity, we assume that only a single reaction is
occurring, and that this reaction is first order, irreversible, and isothermal.
Considering an element of the reactor, if there is
no volume change during the reaction, a mass balance for the reacting component in the gas phase
leads to
747
Under the usual conditions of operation, experimental evidence suggests that axial diffusion can be
neglected[5], thus Eq. (1) becomes
u*_
dl
30(1-a)
Ry-
ac
arlrzR.
(2)
It should be noted that while the above results consider steady state operation in the gas phase, the
particles themselves do not attain steady state.
The mass balance equation for the particles is
E aC #C
--=2----D at
ar
Equations (2) and
ously subject to the
(a) At the entrance
cles are filled with
2 ac
rar
kc
D
C(O,r)=O
OSrSR.
(4)
748
K. C.
cu
PRAIT
and
&Y
(5)
$+,O)=O.
M=~Q
mass transfer
c(t, R) = c(l).
resistance
30(1-o)
R
a
ac
arh
Equations
(3)-(S) are solved
Transforms[8], the solution is
using
(8)
groups given by
DL
p_U(1-4
u
(7)
(18)
in the particles
= l-ficotfi.
(19)
m=R&
(21)
The group C#Jwill be recognised as the Thiele Modulus of the catalyst particles.
Finally, by making use of Eq. (7), we obtain the
concentration of the reacting component in the gas
phase as a function of the dimensionless length l/L,
Laplace
(22)
F, is given by Eq. (16).
3. COMPUTATIONAL
P =1+&&(1-o)-2u
(Y
--
&+&lJxo)
URZp,2
I( m
(10)
= I-(k,R)cot(kR),
(11)
RESULTS
Using an iterative technique, the first 10 eigenvalues of the transcendental Eqs. (17) and (18) were
found for 5 values of rk2, namely, 1000, 100, 10, 1,
O-1, and 5 values of P; 0~1,0~05,0~025,0~01,0@05.
In practice, the series in Eqs. (15) and (22) converged rapidly, and only the first 4 eigenvalues were
used. A representative set of results is contained in
the figures accompanying this paper.
and
k;=-T epPn+ k
(12)
(13)
lZ2
4. DISCUSSION
In Figs. 1 and 2, conversion is plotted as a function of the parameter M, for various values of c$
and P. As the catalyst particles are not at steady
state, the quantity (1 -C/C&~
does not, strictly
speaking, represent the conversion. However, as
the volume of the reactor occupied by catalyst is
y. = 7
Thus the concentration
is given by
and
F
=1+?p-y.+~y.2
2
2x.
6P xn
05)
I
0
(17)
20
40
60
80
I
loo M
M, for
749
0025
P.005
,o_
am
0005
08
06
04
02
COnV
lr,,:
0
200
400
600
800
1000 M
o-
0 025.
P-0 05
02
04
06
OS
1O"L
0 5IlL~Ol
I
P=&&
(23)
06
t
where p is the catalyst circulation ratio (weight of
catalyst circulated/weight of gas). Figure 3 isolates
the influence of catalyst circulation ratio, and demonstrates the diminishing return from increasing
catalyst circulation at conversions greater than 80
per cent.
From the designers point of view, a family of
curves similar to Figs. 1 and 2 would be the most
useful. Having selected the catalyst (hence d), and
the desired conversion, the designer can then determine corresponding values of reactor length and
catalyst circulation.
The optimum combination
would be determined by external factors, such as
power requirements, regeneration, and space limitations.
0.01
a02
0.03
0.04
02
0 L-
03
02
02
04
06
06
10 r/R
o a
a05 p
750
K. C.
TIC
-0-i .
IiL.01
02
0.6 0.3
0.4 -
04
05
06
02-
PRATT
08
10
I
02
04
06
06
r/R
IO
OS-
liL.0 1
02
06:
03
04.
04
02
04
06
08
10
r/R
display radial concentration profiles within the particles at various stages of their passage through the
reactor. Values of 4 range from 100 to 0.1. Consideration of steady state effectiveness factors [93, indicates that for values of 4 greater than about
unity, the rate is diffusion controlled. Examination
of Figs. 5-g shows that similar criteria will apply to
the unsteady state case treated here. The transition
from diffusion to reaction control over the range of
values of 4 is striking. For 4 = 100, it is clear that
only a fraction of the available catalyst is being utilised, while for 4= 0.1, the almost uniform concentration profiles indicate virtually full use of available active surface.
Some difficulty was experienced in obtaining
convergence of the series in Eq. (15) for very small
values of l/L, even when the number of eigenvalues used was increased. Since xn and y. are not
751
cu
c
D
E
k, P
k
1
L
M
P
r
r
t
t:
x.9 Y
concentration
of reactant in the reactor, g
mole/cm3
concentration
of reactant at reactor entrance, g mole/cm3
concentration of reactant in catalyst particle,
g mole/cm
effective diffusion coefficient of reactant in
the catalyst particles cm2/sec
axial dispersion coefficient cm*/sec
roots of Eqs. (11) and (12)
first order rate constant per unit volume of
catalyst pellet, set-
length along reactor, cm
length of reactor, cm
dimensionless group defined by Eq. (19)
dimensionless group defined by Eq. (20)
radial co-ordinate, cm
radius of catalyst particles, cm
time, set
particle velocity, cmlsec
interstitial gas velocity, cm/set
roots of Eqs. (17) and (18)
Greek symbols
a voidage in reactor
p
c
pp
ps
catalyst circulation,
voidage of catalyst
gas density, g/cm3
bulk density of a
g/cm
& Thiele modulus for
g catalyst/g gas
particle
single catalyst
particle,
REFERENCIZS