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BRANE
SCIENCE
Mrnal
ELSEVIER
Abstract
Sherwood-number relations for prediction of the mass-transfer coefficient for developing concentration boundary-layer
have been obtained for laminar flow-regime from first principles. The common flow-modules, namely, rectangular channel,
tubular and radial cross-flow are considered. The relationships developed include the effect of suction through the membrane.
Relevant relations for estimation of mass-transfer coefficient for cross-flow reverse osmosis and ultrafiltration are formulated.
The Sherwood-number relations developed are compared with the standard correlations to quantify the effect of the suction.
The proposed Sherwood relations are used in conjunction with the osmotic-pressure model to predict the permeate flux in
reverse osmosis and osmotic-pressure governed ultrafiltration.
Keywords: Mass-transfer coefficient; Suction; Laminar flow; Osmotic pressure: Cross flow; Reverse osmosis; Ultrafiltration
1. Introduction
The design of pressure driven membrane-separation
processes, like reverse osmosis (RO) and ultrafiltration
(UF), are generally based on the mass-transfer coefficient (k) for the relevant flow-configuration and flowregime. The mass-transfer coefficients used for such
purposes are usually derived from the correlations
obtained from heat-mass-transfer analogies. The maj or
drawbacks of the use of such Sherwood-number correlations with regard to RO/UF are: (a) they are derived for flow through a non-porous conduit; hence,
the effect of suction cannot be considered; (b) changes
in properties like viscosity and density due to concentration polarization near the membrane surface cannot
*Corresponding author,
0376-7388/97/$17.00
1997 Elsevier Science B.V. All rights reserved.
PII S0376-7388(96)00313-4
120
The mass-transfer correlations for membraneseparation processes were reviewed in detail [5,6].
It was concluded, in both of the reviews, that the
present correlations need to be modified in light of
their limitations discussed earlier. In fact, it was
suggested that mass-transfer correlations should be
developed, based on experimental techniques, namely,
the velocity-variation technique or osmotic-pressure
model [5-7]. Each technique has its own disadvantages which were discussed in detail [5,6].
Another alternative method, which was quite successfully employed in our earlier work [8-11] on UE
includes the development of a second correlation for
concentration polarization in terms of polarized layerresistance along with a standard mass-transfer correlation like the Leveque correlation for laminar flow in
a channel or Colton's correlation in a stirred cell [3].
But such approaches are solute and system specific. In
addition, it is difficult to work with two correlations
simultaneously.
The role of suction in mass transfer through porous
membranes is very important. It has been identified
earlier [5,6] that the effect of suction on mass-transfer
coefficient is two-fold. First, it enhances the mass
transfer from the surface to the bulk; and, second, it
stabilizes the laminar-flow condition in the conduit by
delaying the laminar-to-turbulent transition (typically,
critical Reynolds number is shifted from 2100 to 4000
in the presence of suction [6]).
Therefore, it seemed possible that a generalized
mass-transfer relation may be obtained theoretically
for laminar flow from first principles. The present
work aims to develop a generalized mass-transfer
relation, including the effects of suction over a developing concentration boundary-layer. Such relations
can be coupled with the osmotic-pressure model to
predict permeate flux for osmotic-pressure governed
UF and also for RO. Further, the theoretical work is
extended to include all the flow modules, usually
encountered in membrane-separation processes,
namely, rectangular channel, tubular and radial
cross-flow configurations.
I
.
I
.
. . . . . .
Vw (x)
Non-permeating section
Top Disk
Feed
y=2h
2h
Membrane
B o t t o m Disk
Permeate
2. Theory
In this section, an attempt has been made to develop
a generalized mass-transfer-coefficient relation from
I
h
x=0, y=0
V V c = V(DVc)
(1)
(2)
where
Rr
(8)
From this point onwards, estimation of the masstransfer coefficient for different flow modules is presented separately.
Oc
Oc
02c
u Ox - Vw~y -= D Or~.
(9)
r/= y
(5)
(6)
c*(rl) = c/co
(11)
1-
(13)
(7)
(10)
or,
Oc
VwCmRr + D ~ y = 0 at y = 0
~c
(4)
Oc
VwCm + D-~y = VwCp at y = 0
c=c0aty=
A similarity solution for Eq. (9) is obtained by defining a dimensionless variable (lumped parameter),
(3)
121
3uoy
h
(14)
122
can be rewritten as
Vw
= A1
(15)
O.42Alrlld~
dc*
(r?2 + A 1 ) dr/
(16)
(17)
and
dc*
d---~+A1Rrc* =
(26)
d2c *
d~72 -
Ii = f o ~ e X p [ - ~ -
0 at ~7 = 0
(18)
k(c m -
(19)
1) = - D
( U0 ) 1 / 3 ( d c * ~
hxD
\d~/n= 0
(28)
k(K2 c*07)=Klfo~lexp(-~-A97)d~+K2
(27)
y=0
_ / u0 ,~1/3
l) = - t g ~ , ~ )
K1
(29)
or
where
:
A1Rr
K1 -/(2 --
(20)
1 -- A1RrI1
1
(21)
1 - A 1RrI1
(30)
41/3
Sh(x*) = ~
(Re Sc de/L)U3(x*) -1/3
and,
11 = f0 e x p ( - ~T]3 - Alr/)dr/
(22)
S-h =
Vw : -1fo L Vw(X)dx :
f uoD2) l/3 a
1.5 ~ , ~ - - )
(23)
Now, for a rectangular channel, the equivalent hydraulic diameter can be defined by:
de = 4h
(24)
(25)
Sc=#/pD.
(31)
/0'
Sh(x*)dx* = 2.381 ( R e S c d e / L ) l / 3
Ii
(32)
Oc
oc
O (rOC
UOx- Vwor -- r Or \ Or/
(33)
123
1-
(34)
[ ( )21
1-
(35)
(36)
fo '~exp (
84'3
A~O)d6+K4
9
"'
(41)
where
K3-
(42)
A2Rr
1 - A2Rrl2
1
K 4 - 1 - A2Rrl2
(43)
and
12 =
exp
~A?0 dO
(44)
1/3(x*)-1/3
(45)
(46)
(37)
(38)
where
( xD ~1/3
A2 = Vw\uod---Sj
(39)
OC
02C
(47)
3Qy
u(r, y) - 47rrh2
(48)
124
as~
) 1/3
= y ~
41/3
Sh(r*) = ~ (Re Sc h/R)l/3(r*) -2/3
(58)
(49)
d~
(50)
where
V w ( 7 ( h ; D ) 1/3
r2/3
A3 = ~- - -
(51)
f0"
Vw = - ~
Vw(r)rdr
(52)
(53)
~3
c*(~) = K, f ~ e x p ( - ~
-- A3~) d~ + g 6
(54)
(59)
(60)
(61)
(62)
(63)
where
K5 -K6 --
A3Rr
1 - A3Rr13
1
(55)
(56)
1 - A3Rr/'3
and
/3=f0
ec
~3 _ 0'42"X3~) d~
exp ( - ~-
(57)
125
I
lg
where
z_~7r :
//
t/
71-m - - 71-p
(68)
i3
i2/"
~4
(67)
-)
13"" 223"
[3"
0 ~rTwn~n~;
0
2
10
/~ 1,2,3
(64)
(69)
(65)
(70)
Cp) :
_o(c)
\~'J,:0
(71)
In terms of average Sherwood number and non-dimensional flux (Pew) from Eqs. (27) and (71), one can
obtain
Pe,~.
S~h(1
= Rr
- co/cm)
(72)
(66)
126
parameter (Pew), can be in the range 1-500. Sherw o o d - n u m b e r profiles along the c h a n n e l length, for a
rectangular cell, for different operating conditions, are
shown in Fig. 3a. Similar profiles for tubular and
radial m o d u l e s are depicted in Fig. 3b and Fig. 3c,
respectively. Such profiles were generated from
600 ~1
400
500
400
300
i,\
~I~~\
r/?
20O
20O
-----2222
.....
100
2
0
0
0.0
0.2
0.4
0.6
0.8
1.0
"'llll''''l"ll'J''tlrl'll'T''lll''ll'''l'''li'i~''l''''~llll
0.0
1.2
0.2
0.4
x/L
O~
X
0.8
1.0
1.2
600
400
200
Ij I P i l l
0.0
II I~ [ I , , , , 1 1
0.2
I[11 JIIIIl~[,llla
0.4
0,6
r
II I I I '
0.8
1.0
I 1 ~ 1 el
1.2
Fig. 3. (a) Variation of local Sherwood number along the channel length for different values of suction, for a rectangular cross-flow cell. 1:
Pew=0; 2: Pe,,=50; 3: Pew=100; 4: Pew=200; and 5: Pew=300. Solid lines are for Re Sc dJL=lO 3 and dashed lines are for Re Sc de/L=-lO5.
(b) Variation of local Sherwood number along the module length for different values of suction, for a tubular module. 1: Pew=0; 2: Pew=50; 3:
Pew=lO0; 4: Pew=200; and 5: Pew=300. Solid lines are for Re Sc d/L=lO 3 and dashed lines are for Re Scd/L=lO 5. (c) Variation of local
Sherwood number along the channel radius for different values of suction, for a radial cross-flow cell. 1: Pew=0; 2: Pew=50; 3: Pew= 100; 4:
Pew=200; and 5: Pew=300. Solid lines are for Re Sc h/R-lO 3 and dashed lines are for Re Sc h/R=lO 5.
the figures that the Sherwood number decreases sharply near the entrance and then gradually for the rest of
the conduit. Local Sherwood number increases with
an increase in the suction (as Pew increases). This
leads to an increased mass transfer from the surface to
the bulk, in agreement with the qualitative description
of the effects of suction on mass-transfer coefficient by
Gekas and Hallstrom [6]. At higher Re Sc d J L , the
Sherwood number is larger for the same suction. For
127
5
q 4
100
200
300
Pe~
C
400
500
100
200
300
Pew
400
500
2
3
i00
200
300
Pew
400
500
Fig. 4. (a) Variation of ~/S'hno suction with Pe,~ for different Re Sc de~L, in a rectangular cell. 1: Re Sc de/L=103; 2: Re Sc de/L--104; 3:
Re Sc dJL=105; and 4: Re Sc dJL=lO 6. (b) Variation of Sh/Sh,o suctionwith Pew for different Re Sc dJL in a tubular module. 1: Re Sc d~
L=103: 2: Re Sc d/L=104; 3: Re Sc dlL=105; and 4: Re Sc d/L=lO 6. (c) Variation of Sh/Shno suctionwith Pe,~, for different Re Sc dJL, in a
radial cross-flow cell. 1: Re Sc h/R=103; 2: Re Sc hIR=104; 3: Re Sc h/R=105; and 4: Re Sc h/R=lO 6.
128
15
10
09
'
2000
I000
3000
Re
Fig. 5. Variation of dimensionless flux (Pew) with Re for RO
system. Solid lines are predicted flux and symbols are the
experimental data of Merten et al. [15]. l: L/de=5.0; 2: L/
de=16.56; 3: L/de=30.O; 4: L/de=60.0; 5: L/de=150.0; and 6: L/
de=300.0.
129
35
~ . . .9
Water/~Flux
i i
//
"
~
0 /'/O//
25
q)
o
/ , ~ ->, .s-a-5.
. ~ ".,
.........
3 :::fl::::::
.:A
.:!.S
:.:.
-~
, ~
!:'~ . ::::::{:%%...A. . . . . . .
/.S:j'cb . .......
/ / /
//(~
.'.:~l
.,',-::--'"
i 3
':~:.
,,* ,,q?.-'
"
is_,
+ 1 0 ~ / / ~
I i
300
150
450
i,
600
p i J i
25
35
Pe,~
18
/
[ i
Experimental
+10~/
15
AP (kPa)
"~"
I i
4. Conclusions
v
/ /~///105g
C
"U
,//
I I I I I I t l t l l r l l l I ' l l l l l l t
I I 1 1 1
0
4
e~
Experimental Flux x lO m3/m2.s)
12
5. List of symbols
A1,2.3
B1
c
C*
130
de
d
h
11.2.3
k
K1,2,3,4,5,6
L
Lp
PEG
Pew
Q
F
/-
R
Re
RO
Rr
Sc
Sh
Sh
U
Uo
Vw
!)w
V
x
x
Y
UF
Diffusivity, m 2 s -1
Equivalent diameter, m
Diameter of the tube, m
Half-channel height, m
Integral defined by Eqs. (22), (44) and
(57), respectively
Mass-transfer coefficient, m s -1
Constants defined by Eqs. (20), (21),
(42), (43), (55) and (56), respectively
Channel length, m
Membrane permeability, m 3 N-1 S-1
Polyethylene glycol
Wall peclet number
Volumetric flow-rate, m 3 s - t
Radial coordinate, m
Dimensionless radial distance, (r/R)
Cell radius, m
Reynolds number
Reverse osmosis
Real rejection, (1 - Cp/Cm)
Schimdt number
Local Sherwood number
Average Sherwood number
Axial velocity, m s -1
Average bulk velocity, m s-1
Velocity, m s -1
Average permeate flux, m 3 m -2 s -1
Local permeate flux, m 3 m 2 s-1
Transverse velocity, m s-1
Axial distance, m
Dimensionless axial distance, (x/L)
Normal distance, m
Ultrafiltration
Greek symbols
AP
An
71"
P
#
A1,2,3
Pressure differential, Pa
Osmotic pressure differential, Pa
Osmotic pressure, Pa
Parameter defined by Eq. (10)
Parameter defined by Eq. (37)
Density, kg m -3
Viscosity, Pa s
Parameter defined by Eq. (49)
Pew/(Re Sc de[L)1/3, Pew/(Re Sc d/L) 1/3
and Pew/(Re S c h/R) 1/3, respectively
Subscripts
m
o
p
Appendix
(A1)
(A2)
where 7r is in Pa and c is in g ml i.
The osmotic pressure for PEG was calculated from
Flory's equation [4,20].
References
[1] C. Kleinstreuer and M.S. Paller, Laminar dilute suspension
flows in plate and frame ultrafiltration units, AIChE J., 29
(1983) 529.
[2] C.R. Bouchard, P.J. Carreau, T. Matsuuara and S. Sourirajan,
Modeling of ultrafiltration: predictions of concentration
polarization effects, J. Membrane Sci., 97 (1994) 215.
[3] S. Bhattacharjee, A. Sharma and P.K. Bhattacharya, Surface
interactions in osmotic pressure controlled flux decline during
ultrafiltration, Langmuir, 10 (1994) 4710.
[4] S. Ganguly and P.K. Bhattacharya, Development of concentration profile and prediction of flux for ultrafiltration in a
radial cross flow cell, J. Membrane Sci., 97 (1994) 287.
[5] G.B. van den Berg, I.G. Racz and C.A. Smolders, Mass
transfer coefficients in cross flow ultrafiltration, J. Membrane
Sci., 47 (1989) 25.
[6] V. Gekas and B. Hallstrom, Mass transfer in the membrane
concentration polarization layer under turbulent cross flow. I.
Critical literature review and adaptation of existing Sherwood
correlations to membrane operations, J. Membrane Sci., 80
(1987) 153.
131