33 Modeling the Slugging Fluidized Bed Reactor J. R A G H U R A M A N
and Ο. E . P O T T E R
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Department of Chemical Engineering, Monash University, Clayton 3168, Victoria, Australia
In some industrial, and nearly all pilot-plant, fluidized bed reactors the aspect ratio is such that slugging behaviour can be expected, as Davidson and his co-workers have suggested. Scale-up therefore frequently involves a jump from slugging-bed behaviour to freely bubbling bed behaviour. Slugging behaviour occurs when the bubbles present in the bed have diameters approaching that of the vessel. By 'freely bubbling' is meant that there are many bubbles present, each bubble being of a diameter much less than that of the vessel. Fryer and Potter (1,2,3) have compared the counter-current backmixing model with experimental results and the predictions of other models and have demonstrated that the countercurrent back mixing model is appropriate to the freely bubbling bed and has advantages over other models which have been proposed. Raghuraman and Potter (4) have extended the concepts of the countercurrent backmixing model to the slugging fluidized bed, basing the analysis on the solids m i x i n g model o f Thiel a n d Potter (5,6). C o m p a r i s o n o f the predictions o f the new model w i t h t h e experi m e n t a l d a t a o f Hovmand and D a v i d s o n ( 7 , 8 ) and Hovmand, Freedman and D a v i d s o n ( 9 ) shows better a g r e e m e n t w i t h e x p e r i m e n t t h a n i s exhibited by the t w o - p h a s e model o f Hovmand and D a v i d s o n . In t h i s p a p e r an e x t e n s i o n o f t h e new model i s d e s c r i b e d . T h i s e x t e n s i o n o f t h e model h a s t h e a i m o f f a c i l i t a t i n g a d e t a i l e d d y n a m i c i n v e s t i g a t i o n o f t h e s l u g g i n g f l u i d i z e d bed r e a c t o r whether o f t h e c a t a l y t i c t y p e o r o f t h e t y p e e x h i b i t i n g r e a c t i o n between g a s and s o l i d a s i n m i n e r a l r o a s t i n g and f l u i d i z e d bed combustion. The e x t e n d e d model r e p o r t e d h e r e s e e k s t o d e s c r i b e t h e c y c l i c v a r i a t i o n s w h i c h o c c u r due t o s l u g g i n g i n a s t e a d y s t a t e c a t a l y t i c system. A l t h o u g h t h e s t u d i e s c o m p l e t e d and p r o p o s e d have d i r e c t a p p l i c a t i o n o n l y t o s l u g g i n g f l u i d i z e d bed r e a c t o r s t h e r e w i l l be i n s i g h t s g i v e n i n t o t h e b e h a v i o u r o f f r e e l y b u b b l i n g beds. P o t t e r (10) h a s r e c e n t l y r e v i e w e d t h e m o d e l l i n g o f f l u i d i z e d bed reactors. © 0-8412-0401-2/78/47-065-400$05.00/0
Weekman and Luss; Chemical Reaction Engineering—Houston ACS Symposium Series; American Chemical Society: Washington, DC, 1978.
33.
RAGHURAMAN
Slugging Fluidized Bed Reactor
AND POTTER
401
Model o f D a v i d s o n and C o - w o r k e r s Hovmand and D a v i d s o n (8_) p r o p o s e d a t w o - p h a s e model a n d compared t h e p r e d i c t i o n s o f t h a t model w i t h t h e e x p e r i m e n t a l d a t a o f Hovmand a n d D a v i d s o n (7_) a n d Hovmand, Freedman and D a v i d s o n (9). The model assumes c o - c u r r e n t p i s t o n - f low o f b u b b l e g a s (U-U ^) a n d d e n s e - p h a s e g a s ( U ^ ) , w i t h t o t a l m i x i n g o c c u r r i n g when s l u g s c o a l e s c e . This latter a s s u m p t i o n has n o t been j u s t i f i e d a s y e t . The new model r e t a i n s t h e a c c o u n t o f g a s - e x c h a n g e g i v e n by Hovmand a n d D a v i d s o n ( 8 ) . Gas e x c h a n g e due t o d i f f u s i o n and b u l k - f l o w a r e a d d i t i v e .
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2_ = ±
^mf U
Dm
In e q u a t i o n
1/2
1
+
mf
1
+
£
mf
J
D
is slug-length.
f o r t h e s l u g , g i v e n by : 1/9
L S
S
(1)
I J
(1) m i s a s h a p e - f a c t o r 4V
Λ ]
Γ
π
495
-
°·
I i s surface
,..(2)
+ 0.061
D
integral
tabulated
in Table I .
Table I Value of Surface Integral I L /D s
I
0.3
0.5
1.0
2.0
3.0
4.0
5.0
0.13
0.21
0.39
0.71
0.98
1.24
1.48
The a u t h o r s a l s o g i v e a n e x p r e s s i o n f o r g a s - e x c h a n g e w h i c h t a k e s i n t o a c c o u n t i n t e r a c t i o n between d i f f u s i o n and b u l k - f l o w b u t recommend f o r use t h e g a s - e x c h a n g e r a t e c a l c u l a t e d by e q u a t i o n ( 1 ) . The s l u g - r i s e v e l o c i t y , w i t h r e s p e c t t o s t a t i o n a r y s o l i d s a h e a d , i s g i v e n by Kehoe a n d D a v i d s o n ( 1 1 ) U
=
s
and t h e r i s e v e l o c i t y o f c o n t i n u o u s l y g e n e r a t e d s l u g s U
SA
U-U
f
,.(3)
0.35 ( g D ) '
+ 0.35 ( g D )
i s g i v e n by:
:
(4)
The e x c h a n g e c o e f f i c i e n t , Q/V , i s used by D a v i d s o n a n d c o - w o r k e r s f o r g a s e x c h a n g e between t h e s l u g and t h e r e s t o f t h e b e d , o r dense p h a s e . The New M o d e l , T i m e - A v e r a g e d T h i e l and P o t t e r ( 4 , 6 ) have shown t h a t m i x i n g o f s o l i d s i n r o u n d - n o s e d s l u g g i n g beds c a n be a c c o u n t e d f o r by a s s u m i n g t h a t t h e s l u g i s f o l l o w e d by a wake o f w e l l - m i x e d s o l i d s w h i c h t a k e s up a b o u t t w o - t h i r d s o f t h e i n t e r s l u g m a t e r i a l . The r e m a i n d e r o f t h e i n t e r - s l u g m a t e r i a l i s i n piston-flow. Thus t h e model a d o p t s t h e g a s - e x c h a n g e r a t e a s g i v e n i n e q u a t i o n ( 1 ) b u t c o n s i d e r s i t a p p l i c a b l e t o gas e x c h a n g e between
Weekman and Luss; Chemical Reaction Engineering—Houston ACS Symposium Series; American Chemical Society: Washington, DC, 1978.
CHEMICAL REACTION ENGINEERING—HOUSTON
402
wake and s l u g , Q/V~ being r e l a b e l l e d K^. So f a r as gas-exchange between wake and tne p i s t o n - f l o w region i s concerned, t h i s i s considered t o be determined by the s o l i d s movement, allowance being made f o r gas flow U ^ , with respect t o s t a t i o n a r y s o l i d s . The s o l i d s phase flows i n and out of the wake, which i s of vo I urne f V at a volumetric r a t e , U This exchange can be expressed i n terms of an exchange c: o e f f i c i e n t , namely the volume of s o l i d s phase exchanged with the wake per u n i t s l u g volume per u n i t time, (IL πΟ /4)/V^. If there were no flow of gas through the s o l i d s phase, then the gas-exchange r a t e would be (ε U π ϋ / 4 ) / ν . Following Stewart and Davidson (12) the flow out of the s l u g nose and i n a t the base of t h e s l u g w i l l be U ^ -nD /4. So, the net volume of gas exchanged between the p a r t i c u l a t e p i s t o n - f l o w U J πϋ /4. region and the wake per u n i t time w i l l be (U ε mf mf ç
r
2
$
f
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z
ζ
c
(U
S
mf 4 V
U )πϋ mf
ζ
χ
,(5)
r
If the f r a c t i o n of the bed-volume occupied by slugs i s ε^, then
...(6) B
V
2
+ TD(wD /4)
s
where Τ i s the r a t i o of mean i n t e r - s l u g spacing t o column diameter. Therefore, equation (5) may be a l t e r n a t i v e l y presented : (1-ε > Β
Κ
CP
TD ε
,(7)
υε ,- U S mf mf ο
Β
#
Figure 1 i l l u s t r a t e s the gas-exchange process. For f i r s t - o r d e r s t e a d y - s t a t e chemical r e a c t i o n , the m a t e r i a l balances on reactant gas, on a time-averaged b a s i s , a r e as f o l lows : dO,
Slug
Β U GB dz
Wa ke
U G
K
BC
K
CP
(C
,(8)
)ε
C " °Β Β
dCç c
dz
( C
C
P
) £
C B
+
K
k
Pi ston-flow reg ion
5
U GP dz
K
( C
C
CP C " P
) e
B "
k
( C
C
BC B " C
f
ε
) £
B ,(9)
C
w Β C 1
ε
- Β
Π +
ν ...(10)
Here the wake f r a c t i o n i s given by : f
2
w
= wUD /4)TD/V S c
Weekman and Luss; Chemical Reaction Engineering—Houston ACS Symposium Series; American Chemical Society: Washington, DC, 1978.
...(11)
33. w
RAGHURAMAN
is the
and
of
the
estimated
conditions
U
GB
=
U
GP
=
Ζ
=
material
and Potter
which
to
by Raghuraman
403
i s we I I - m i x e d
be 0 . 7
*
0.2.
and Potter
(4_).
The
...(12)
=
U
U
and
At
inter-slug
by T h i e l
are given
average,
where
Slugging Fluidized Bed Reactor
POTTER
proportion
has been
boundary
On
AND
+
GB
U
-
U
U
, mf
U
U
m f -
o,
ε
c
+
GC
U
U
GC =
Vmf GB
,f,,(U-U
mf w = c
B
GP
...(13)
,)
mf
...(14)
0
...(15)
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and U
-
The
exit
The
New M o d e l ,
at
reacting
The
cycle
slug
slugs
obtain flow
time
Figure
at
of
assumed
that
becomes
piston-flow
when
slug
New s l u g
formation is
distributor moment on.
of
Since
again 0
of
top
the bed a t
from
i n t e r s lug
it 0
one-third.
risen
by o n e - t h i r d
reached
the top of
In
of
we
7
)
from t h e bed from
non-reacting
time.
here
1
follow
region
the top of
with
(
Only
for
the
comparison
model
of
Hovmand a n d
to
rise
a
t h e bed and s l u g s
above
are
cycle
in the top
it
above
is
seen
detach
also
a
1
Figure
at
being
2 this
τ / 3 , slug
0
the
i n t e r s lug
spacing
t h e bed and b u r s t s ,
is
as
necessarily
t
= 0
from
the
an
is
α
a new
to
forming,
α
at
the
2 and s o
integral remains
detaching
fraction
=
section
renumbered
amount
t h e new s l u g
piston is
produce
renumbered
in general,
fractional
when
that
is
It
calculation.
itself
has detached, 1;
to
are not
in the
the bed
and
the top.
bursting
account
in
conditions
a s t h e wake
and a t
i s no s l u g
to
situations
Special
t h e flow
2,
the
cycle
1,
of
through each
the top.
not contain,
the time
At t
of
slug
to
regions,
form
is approached
zero
progressive
to
into
from
the distributor.
mately
at
the f i r s t
= 0
this
bed t o
the two-phase
the
Figure
t h e bed does
number of
t
In
f o r the slug
+
and a t
Form
At the beginning
is just about
detachment
- - ·
fluidized
and slug
taken to
C
data.
there
and t h i s
numbered
C
mf
:
and the p i s t o n - f l o w
bursts
since
in
Referring
U
by
admitted
behind
mixing. phase
...(16)
t h e bottom
during
C
are presented
TD/U^.
shows
C
p
the bed i s
and r i s e
a
G C
Cyclic
version,
a r e formed
U
the steady-state
gas is
2
=
0
the fluidized
Thus
at
t h e bottom
regimes
slug,
+
i s the time
a r e formed
C
the slug,
i.e.
is admitted
renumbered. as
C
GB B
solutions
length
)
= C
c
and the experimental
inter-slug new
of
the time-averaged
Davidson
G B
is given
in which
steady-state
with
U
C
U
=
bursts.
state
and then
final
H
t h e bottom
the slug
initial
C
-
Mechanistic
t h e wake
formation
gas
U
gas concentration
slug,
where
(
= H,
U
each
+
P
Ζ
At
an
C
GP
is all
a n d s Iug 5
illustrated,
at
the
itself
approxi slugs has a
later.
Weekman and Luss; Chemical Reaction Engineering—Houston ACS Symposium Series; American Chemical Society: Washington, DC, 1978.
have just
moment
CHEMICAL REACTION ENGINEERING—]
4*i
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Β
wTD f
**0
I
i=^-wJTD
Figure 1. Slugging fluidized bed. (A) well-mixed wake region; (B) piston-flow region.
β β β β aβ β a β ft
ft
ft
ft
β β β β β β β β β β β β f.Wr
Figure 2. The mechanistic model portrayed over one time cycle
Weekman and Luss; Chemical Reaction Engineering—Houston ACS Symposium Series; American Chemical Society: Washington, DC, 1978.
33.
RAGHURAMAN
405
Slugging Fluidized Bed Reactor
AND POTTER
The l e n g t h o f t h e w e l l - m i x e d r e g i o n b e h i n d a s l u g i s wTD. T h e r e f o r e a t t i m e W T , f r a c t i o n w o f a new s l u g 0 h a s f o r m e d a n d t h e l e n g t h o f t h e i n t e r - s l u g m a t e r i a l b e h i n d s l u g 1 i s wTD. As the r e s t o f t h e i n t e r - s l u g m a t e r i a l , behind s l u g 1, f a l l s into p l a c e , a p i s t o n - f l o w r e g i o n i s commenced u n t i l a t t = τ the s i t u a t i o n has r e t u r n e d t o t h a t d e p i c t e d f o r t = 0~.
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+
Due t o t h e f r a c t i o n o f TD r e m a i n i n g a t t h e t o p o f t h e b e d , t h e t o p s e c t i o n i s o u t o f p h a s e w i t h t h e f o r m a t i o n o f new s l u g s at t h e bottom of the bed. Thus, r e f e r r i n g t o Figure 2, a t time t = τ/3 the top-most slug bursts, l e a v i n g a l e n g t h TD o f p a r t i c u l a t e phase o r i n t e r - s l u g m a t e r i a l , l y i n g above s l u g 4 w h i c h h a s now b e c o m e t h e t o p - m o s t s l u g . As t i m e i n c r e a s e s t o WT, t h e l e n g t h o f t h i s i n t e r - s l u g ( o r s h o u l d we now s a y "above-slug") material decreases. A t WT t h e new w a k e r e g i o n b e h i n d s l u g 1 i s complete. A t τ the p i s t o n - f l o w region behind s l u g 1 i s a I so complete and the s l u g detaches. At the top of the bed, the length o f i n t e r - s l u g m a t e r i a l w i l l have f a l l e n t o o n e - t h i r d o f TD. T h e b e h a v i o u r now r e p e a t s i t s e l f a n d i s t h u s c y c l i c a l . T h e m o d e l b r i e f l y d e s c r i b e d a b o v e i s now c o n s i d e r e d f r o m a chemical reaction point of view. Fresh r e a c t a n t gas i s s u p p l i e d at a steady flow U and of t h i s flows c o n t i n u a l l y through the b e d w h i l e d J - U ^ ^ a c t s g r a d u a l l y t o r a i s e t h e b e d a b o v e t h e new s l u g a n d , i n a s e n s e , o n l y e n t e r s t h e b e d , a s r e a c t a n t i n t h e new s l u g a t t h e moment o f i t s d e t a c h m e n t . The s t e a d y - s t a t e results p r e s e n t e d here have been a p p r o a c h e d from an i n i t i a l s t a t e i n which t h e bed i s c y c l i n g a s above w i t h no r e a c t a n t gas p r e s e n t , t h e p r o c e s s s t a r t i n g when t h e e n t e r i n g g a s i n s t a n t a n e o u s l y h a s i t s reactant concentration adjusted to C . are and
C o n s i d e r a g e n e r a l c e l l , j . C e l ? s , as d e p i c t e d i n F i g u r e 1, counted from t h e bottom upwards, so t h a t (j+1) i s above c e l l ( j - 1 ) below i t . Material
Balances
on general
j
cell
SI ug 0
^
=
Wake
^BcS-Vj dC
m f
+
M f
p
1
•••
(18)
.
•••
^ B C ^ C - V j
V ^ J - ^ e . j + l *
+ k f
(19)
w C C
P i s t o n - F l o w Region o f P a r t i c u l a t e Phase Since piston-flow o b t a i n s , a c c u m u l a t i o n terms c a n , i n t h i s c a s e , be i g n o r e d a l t h o u g h q u a l i f i c a t i o n s w o u l d b e made t o t h i s s t a t e m e n t i f space permitted. However t h e r e remains a d i s t a n c e - v e l o c i t y l a g w h i c h needs t o be t a k e n i n t o a c c o u n t . If ζ i s t h e length dimension and ζ = 0 a t t h e bottom o f the w e l l - m i x e d wake,
Weekman and Luss; Chemical Reaction Engineering—Houston ACS Symposium Series; American Chemical Society: Washington, DC, 1978.
CHEMICAL
406
jnf
REACTION ENGINEERING—HOUSTON
dC, P
...(20)
+ kC . =0 P,j,z
Z
'J'
n
dz
and -kz
exp
,(21)
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"mf Note t h a t C earlÎ e r .
.
p
i s r e l a t e d t o C , j , 0 a t time
z
[z/(U -U /ε^)]
p
s
mf
M a t e r i a l Balances on Ce I I 1 The slug-balance i s the same as equation (18). The wake and p i s t o n - f l o w regions are no longer of constant dimensions but of dimensions which vary with time. The wake begins t o form immediately and when i t has grown t o f u l l s i z e , the p i s t o n - f l o w region commences t o form. Wake
ε ,f 0 = - E U xw
. f 4r ( t c . j + K ( C _ - C _ ) C " C 1 "ΒΓ W T dt ΧΓ
W
B pV
D
k f U X + (υ ε mf o S mf ο
U JC mf Ρ
w tc
D
e,2
xw
p 1
(22)
CI
P i s t o n - f l o w Region This region commences t o form a t time wx and the region extends from ζ = 0 t o ζ = [(t/x)-w]TD. Equation (21) a p p l i e s with t h i s p r o v i s o . M a t e r i a l Balances on Top-most Region When a slug reaches t h e top of the bed and b u r s t s , i t leaves behind a well-mixed wake region and p i s t o n - f l o w region and i t i s assumed t h a t flow i s p i s t o n - f l o w t h e r e a f t e r . This material f a l l s around the r i s i n g top-most slug and of course disappears e n t i r e l y a t the moment of slug b u r s t i n g , only t o be replaced by the i n t e r - s l u g m a t e r i a l b,elow t h e b u r s t i n g s l u g . Equation (21) a p p l i e s . When 0 < t £ ατ, the top-most region decreases in length from ζ = aTD t o ζ = 0; when ατ 4 t