Modeling of a radial flow hollow fiber module and estimation

of model parameters using numerical techniques

Abhijit Chatterjee, Aruj Ahluwalia, S. Senthilmurugan, Sharad K. Gupta*
Department of Chemical Engineering, Indian Institute of Technology-Delhi, New Delhi 110016, India
Received 24 September 2003; received in revised form 7 October 2003; accepted 12 January 2004

Abstract

A numerical solution is developed for modeling as well as predicting the performance of a radial flow hollow fiber reverse osmosis (HFRO)
module. The three-parameter Spiegler-Kedem (S-K) model is used for describing the mass transport across the membrane. The solution
proposed considers pressure drops in both permeate and bulk streams and includes concentration polarization. The numerical solution uses
finite difference method. Two limiting cases of the system of equations are used to arrive at analytical solutions and check the validity of the
numerical solution. The simulation of the above three-parameter membrane model is compared with a two-parameter membrane model and
an analytical solution available in literature and the significance of the third membrane parameter, the reflection coefficient, is investigated in
detail. It is found that when the reflection coefficient is decreased from its maximum value of one, the permeate flow rates are higher and the
permeate concentration differs substantially from that reported by the two parameter membrane model of Sekino [J. Membr. Sci. 85 (1993)
241]. Under the simulation conditions investigated (1 > > 0.9), the maximum difference in the permeate flow rates between the two can
be as large as 14% while the differences in the permeate concentrations can be as large as 4431%.
The mass transfer coefficient and the membrane model parameters are determined by using an optimization techniquethe Simplex Search.
The data for phenol separation obtained on a laboratory scale B9 HFRO experimental setup and the experimental data available in literature
are used for the estimation of the model parameters as well as the mass transfer coefficient in the B9 module. These estimated parameters are
then used to predict and compare performance at some other operating conditions. The theoretically predicted and the experimental values
for both present and previous studies are found to be in good agreement. The analysis of the phenol separation data clearly shows the two
parameter membrane transport model used in previous studies may not be sufficient for accurate design and analysis of a radial flow hollow
fiber system for many solute-membrane systems. Finally, the mass transfer correlation for the shell side of the hollow fiber module is also
developed and compared with the correlation available in literature.

Keywords: Reverse osmosis; Hollow fiber module; Modeling; Parameter estimation; Spiegler-Kedem model; Finite difference

1. Introduction water output of all membrane geometries besides offering

Reverse osmosis (RO) has become a popular method for
water purification. The major advantage of the process is
its ability to perform direct separation at ambient conditions
and allowing separation of heat sensitive materials. RO is
currently being extensively used in the production of potable
water, production of industrial water, treatment of domes-
tics as well as industrial wastewater, and in food process-
ing. Common membrane configurations employed for RO
are plate and frame, tubular, spiral wound, and the hollow
fiber configurations. Hollow fiber modules offer the largest
the highest surface area per unit volume of the system. De-
velopment of a reliable mathematical model for description
of hollow fiber reverse osmosis (HFRO) modules is a highly
desirable goal since not only does it allow us to analyze the
transport properties of a HFRO system, it is also useful in
design and finding the optimal network when HFRO mod-
ules have to be arranged in networks of several units [1].
Many research workers have studied the design and anal-
ysis of HFRO modules over the years. Most of the solu-
tions available in literature are approximate solutions [3-6].
Gupta [7] developed analytical design equations by using the
solution-diffusion (S-D) model for tubular, plate-and-frame
and spiral wound modules. The mass transfer coefficient
 A. Chatterjee et al. /Journal of Membrane Science 236 (2004) 116
was assumed to be constant and the pressure drops were ne-
glected. Furthermore, the membrane was assumed to be a
high rejection membrane. Unlike the analytical design equa-
tions developed by others, these equations are simpler to use
and can be applied for all values of the mass transfer coef-
ficients. Gupta [8] extended the above design equations for
radial flow hollow fiber modules. These equations for single
solute RO system having high rejection coefficient mem-
brane predict the dimensionless length and the averaged so-
lute permeate concentration for a given solvent recovery.
El-Halwagi et al. [9] analyzed the performance of HFRO
system by coupling mass and momentum transfer on the
fluids inside and outside the hollow fiber and membrane
transport expressions. The model equations were solved nu-
merically and experimental data was used for transport pa-
rameter estimation and model validation. They used the
Kedem-Katchalsky model for membrane transport but ne-
glected the concentration polarization.
Starov and coworkers [1,2] developed a mathematical
model for various hollow fiber geometries and then used
this to optimize the performance of these modules. How-
ever, their analysis assumed that the osmotic pressure and
the concentration polarization on the feed side of the mem-
brane are negligible. They further assumed that the equiva-
lent annulus or free surface model where feed flows parallel
to fibers can be applied and that the Darcey's equation is
valid for calculating the trans-module pressure drop. In real-
ity, the osmotic pressure and the concentration polarization
in RO may not be negligible. Furthermore, the equivalent
annulus model requires that all the fibers are subjected to
the same operating conditions, which is clearly not the case
for a radial flow hollow fiber module. Therefore, the above
model may predict optimization trends but it cannot be used
for accurate design and analysis of a radial flow hollow fiber
module.
Ohya et al. [10] conducted experimental studies on a Du
Pont B9 hollow fiber module to determine its RO character-
istics. The average mass transfer coefficient and the solute
diffusivity were calculated by numerically solving the gen-
eral equations for radial flow hollow fiber system. In this
study the mass transfer coefficient was assumed to be con-
stant and the pressure drops in both shell side and in the fiber
were neglected. Furthermore, the solution-diffusion model
was assumed to be applicable for describing the mass trans-
port across the membrane. Tweddle et al. [11] used sim-
ilar approach and derived a analytical solution following
the Kimura-Sourirajan analysis to analyze the ROGA spi-
ral wound module and the Du Pont B9 Permeator with the
systems of sucrose and NaCl.
Recently, Sekino [12] reported the numerical solution
of a radial flow hollow fiber module. The two-parameter
solution-diffusion model was used for describing mass
transport across the membrane. The permeate pressure drop
in the fiber bore and the pressure drop of the bulk solution
within the shell and concentration polarization were taken
into account. The differential equations were solved using
a finite difference scheme, taking into account local varia-
tions in flow rate, concentration and pressure. The systems
modeled were the Toyobo Hollosep modules (HA 8130 and
HR 8355).
The objective of this work is to extend the analy-
sis of Sekino by using the three-parameter, non-linear,
Spiegler-Kedem (S-K) model for describing the mass trans-
port in the hollow fibers. The three-parameter model has
been shown in literature [15,16] to be more accurate model
for describing the mass transport processes in the RO mem-
branes. The Toyobo Hollosep module and the Du Pont B9
Permeator are simulated and the significance of the reflec-
tion coefficient on product flow rates and concentration is
analyzed. The results are compared with the two-parameter
solution-diffusion model used by Sekino [12] and the an-
alytical solution proposed by Gupta [8]. A method for
estimating the membrane performance parameters and the
mass transfer coefficient parameters from a given module
data is also developed. This method is then used to analyze
the phenol separation data for B9 radial flow HFRO module
and the various other module data available in literature.
2. Hollow fiber modules
2.1. The Du Pont B9 permeator
Du Pont introduced a series of non-cellulosic membranes
including aromatic polyamide membranes to fabricate B9
and B10 modules. These hollow fibers have an asymmetric
structure with volume fluxes as much as ten times those of
homogeneous membranes. The configuration of these mod-
ules is similar to shell and tube heat exchangers where hol-
low fibers extend axially along a fiber glass shell and are
sealed at both ends on the shell side. The fiber bores are
sealed at one end and open at the other to allow the product
(permeate) to flow out and be collected. The feed enters a
porous central feeder tube and flows outwards radially over
the fibers. The concentrated solution, due to solute rejection
at the membrane surface, is removed from the outside sur-
face of the shell. Thus, the flow in the shell is mainly radial
while the flow inside the fibers is axial.
2.2. The Toyobo Hollosep module
Unlike the Du Pont B9 and B10 Permeator, the Toyobo
Hollosep fibers are cross-wound around a core tube. The
fibers are made of cellulose triacetate. These are covered
with epoxy and are vertically sliced on one side, from which
the permeate flows out. The main advantage of this configu-
ration is the large surface area afforded by the denser packing
of fibers in the radial flow arrangement. Two kinds of mod-
ules are available, one for separation of brackish water and
the other for seawater. The difference lies in the fact that in
case of seawater, the concentration of salt is higher and the
feed inputs at a much higher pressure. The feed concentra-
 A. Chatterjee et al. /Journal of Membrane Science 236 (2004) 116
tion and the feed pressure ranges for both systems are given
as 0.5-10 kg/m3 for brackish water and 3 0 ^ 5 kg/m3 for sea
water, and 1-4 MPa for brackish water and 5-6.5 MPa for
sea water.
3. Theory
3.1. Modeling
The permeate flow rate and solute concentration obtained
for a given hollow fiber module can be predicted by solving
a set of equations which describe the mass transfer inside
the membrane. These equations namely, the membrane
transport model, concentration polarization model, local
solvent and solute mass balances are all applicable at any
point within the Permeator. The system of coupled partial
differential equations is solved numerically using the finite
difference method.
Fig. 1 shows both how the bulk (reject) and permeate
streams flow through a Du Pont B9 module and how a grid
can be created to carry out the method of finite differences.
The radial direction (r-axis) and the axial direction (z-axis)
are divided into 'm' and 'n' segments, respectively. Here,
the axial direction refers to the axis of the hollow fiber along
the permeate flow direction. The same is applicable for a
Hollosep module as well, where the fibers are wound around
the feeder tube.
The following assumptions have been made in the devel-
opment of our analysis:
Permeate
Grid points
z=0
central(ffie.
Cer,
Bulk
stream
Fig. 1. Finite difference mesh construction for a Du Pont B9 hollow fiber module.
The bulk stream flows radially outward and there is suf-
ficient axial mixing in the bulk stream. This implies that
the bulk flow variables are only dependent on r and it al-
lows us to replace the partial derivative terms that appear
in the material balance equations and the pressure drop
equation with ordinary derivatives.
The element chosen for finite difference analysis within
the permeator is much larger than the fiber dimen-
sions. Hence, for all practical purposes the shell side
of the membrane can be assumed to be a continuous
phase.
Membrane structure is uniform throughout the module.
All model parameters within the permeator are constant.
There is no variation in bulk flow properties along the
circumferential direction.
The permeator is in operation for sufficient time and
steady state has been achieved.
Solution contains only one solute and a solvent (binary
solution).
Film theory is applicable within the membrane module.
Fluid properties and diffusivities remain constant inside
the module.
Perfect mixing in the radial direction on permeate side
fluid
3.2. Membrane transport equations
The Spiegler-Kedem model is used to describe the mass
transfer inside the membrane. The model equations for per-
meate flux and solute rejections are given below.
Reject
feeder if
Permeate stream
 A. Chatterjee et al. /Journal of Membrane Science 236 (2004) 116

3.2.1. The permeate flux equation and

: - ( A P - a An) (1) A f RT
P Jy=-\AP-
p L
where (11)
RT
Tt = (2) Eq. (11) gives an expression for Jv where the only other
c
variables are Pb, Pp and cb, F and can be written in terms
and of Jv. An expression of this form for Jv is easier to solve,
as discussed in subsequent sections.
AP = pb- (3)
3.2.4. Equations for the pressure drop
3.2.2. Equation for rejection by the membrane The pressure difference across the membrane which
The true rejection at a particular point inside the mem- is used in Eq. (1) for obtaining the permeate flux varies
brane is given by throughout the membrane because of friction losses. The
inside hollow fiber and bulk/retentate side streams pres-
__ (4) sure drop can be estimated using Hagen-Poiseuille and the
1-oF cm
Ergun's equation, respectively. These equations are given
where below:
Hagen-Poiseuille equation:
1 -a
F = exp -Jv (5) dPp 32/x
= V p
(12)
mdz ~ ^
The hydrodynamic permeability, A, the solute permeability,
Pm and the reflection coefficient, are the three parameters Ergun's equation:
of the Spiegler-Kedem model.
The expression for Jv can be rewritten in terms of the bulk dPb /150(1-e) 1.75(1 - )v2r
(13)
~dr~
and the permeate variables as
V
A ( RT Here, dp = 6/av = 1.5do is the mean particle diameter and
Jv=-((Pb- Pp) ~ RT - cp) (6)
bp Mw vr is the superficial velocity within the module on the bulk
side along the radial direction.
where
Cm Cr> 3.2.5. Material balance
(7) The material balance equations for both solute and solvent
cb -
streams within the membrane are given below.
3.2.3. Concentration polarization model Permeate stream:
Accumulation of the solute on the membrane surface leads
2jtr +&z 2jtr Ar6vp\z=z = 2jtr Arg6vpJv\z=z
to the development of a concentration polarization layer. z=z

This phenomenon can be mathematically described using Hence,

the film theory as
= Jv such that vp|z=0 = 0,
A Do
(14)
Cm Cn < 2r <
= exp (8) Z 2

-c p 2 2 2
Here, = di N/(D o - Di ), = (4do/di2)(L/Lm) and the
The mass transfer coefficient used in Eq. (8) may be ex- length of a hollow fiber is given as, L = Lm2 + 4(rW)2.
pressed as a function of the Reynolds and Schmidt numbers. Bulk stream solute concentration:
Sh = aRebSc1/3 (9) _Ar 2rLvr|r = 2nrAr6vp\z=L

Equations of the same form are used in literature for esti- Hence,
mating the mass transfer coefficients. In a particular case
for Toyobo Hollosep modules Sekino et al. [13] had derived d(rvr) r
(15)
a = 0.048 and b = 0.6. dr ~ Lv z=L
By combining the Eqs. (4) and (8), we obtain
subject to
cb
Cn = (10)
vr|r=Di/2 = vf, for 0 < z < L
 A. Chatterjee et al. /Journal of Membrane Science 236 (2004) 116

Likewise for the solute, Step 8: Obtain Fi,j, faj and cbi,j from Eqs. (5), (8)
and (10), respectively.
d(rvrcb) r
(16) Step 9: Solve vri+1 and cbi+1 by using forward difference
z=L representation of Eq. (15) and (16), unless i + 1 > m. for
subject to solving cbi+1 the value of cbi,n defined as ratio between the
total solute flux and solution flux through the membrane
cb|r=Di/2 = cf, for 0 < z < L along the axial direction of finite element "i".
Step 10: Calculate the value Qp and cp as follows:
Differentiation of Eq. (12) and subsequent substitution into
Eq. (14) leads to m-\
Qp = (18)
=0
32/xt dz z=0
(17)
32/x
M? lit

The above Eqs. (1)(17) are solved numerically by the finite m-\

difference method with each of the variables being expressed

as a discrete value. Since the permeate flow variables vary
only along the z-axis while the bulk flow terms vary along the
r-axis, the equations are solved sequentially by proceeding
from r = Di/2 to Do/2 while solving all the z-axis dependent
difference equations at a particular radial grid location. The
bulk flow terms at r = Di/2 are known, Pb = Pf, cb = cf
and vr = vf.
3.3. Algorithm for the solution of the Spiegler-Kedem
model
The Eqs. (1)(17) are solved by the finite difference
method and the differential equations are discretized fol-
lowing the method of Sekino [12]. The algorithm used to
simulate the performance of a hollow fiber module when
all the Spiegler-Kedem model parameters and the constants
appearing in the mass transfer correlation are known, is
given below.
Step 1: Obtain the Spiegler-Kedem model parameters,
dimensions of the membrane and the input feed flow rate,
concentration and pressure.
Step 2: Form the grid for carrying out method of finite
differences.
Step 3: Repeat steps 4-9 for "i" (along the radial direction)
going from 1 to m (the radial grid point n = Di/2, rm =
Do/2).
Step 4: For j = [1, n], calculate Jvi,j by assuming feed is
pure water and fiber bore pressure is in atmosphere, as an
initial estimate for Jvi,j. Calculate vpi,n from Eq. (14) using
numerical integration.
(19)
3.4. Limiting cases for checking the validity of the
numerical solution
Since the system of coupled equations involved in model-
ing a HFRO are complicated in nature, one way of checking
the validity of the solution is to compare the numerically ob-
tained solution with analytical solutions for particular limit-
ing cases. It was concluded that if Jv is estimated correctly
then all other variables that are directly or indirectly depen-
dent on Jv can be estimated easily. Two limiting cases were
considered.
3.4.1. Case A: analytical solution for pure feed
An analytical solution can be obtained for systems with
low solute concentration, cf and where the epoxy seal thick-
ness, 4 is small. This solution may also be valid if the re-
jection of the solute is poor and the concentration difference
across the membrane, cb - cp is negligible. Eliminating the
osmotic pressure term in Eq. (17), we obtain,
(20)
subjected to
Pp ^p = 0, rp z=LPatm
dz z = o

Step 5: Solve for the system of linear equations for Pp The solution for this equation is
by applying central difference method to Eq. (7).
Pb - Pp cosh(Kz)
Step 6: Estimate Jvi, j for j = [1, n] from Eq. (17), where (21)
r\y Patm cosh(KL)
ki can be calculate from correlation Eq. (9). Calculate vp
as mentioned in step 4. As with Pb, q,^. and vri,j can be and hence,
replaced by cbi and vri since they only vary radially.
A cosh(Kz)
Step 7: Repeat steps 5 and 6 till values of Ppi,j and Jvi, j a m (22)
converge at all points at radial index "i". p t ) cosh(KL)
 A. Chatterjee et al. /Journal of Membrane Science 236 (2004) 116

where values when pure water is passed through the module at a

feed pressure of 7 bar at 25 ml/s. For this case, the value
K= of K is 1.4749 m " 1 . The comparison for the numerical and
analytical values for Jv as a function of position is shown in
Fig. 2. The numerically obtained solution for total permeate
Normally, the pressure drop in the bulk stream is small be-
flow rate, Qp was equal to 11.163 ml/s, which is same as the
cause of the high porosity of the membrane. Hence, Pb may
solution using the limiting case A.
be approximated by Pf. The permeate flow rate per unit area
If 4 for the HFRO module is small, one can estimate the
or in other words the flow velocity at z = L is
pressure drop because of the epoxy sealing from the equation
-Pat given below:
'P z=L
(23)

Since the solute is in very low concentration or absent, the ^^epoxy = /2 ^P Az (25)
same value of vp is applicable throughout the membrane. z=L
Therefore, the total permeate flow rate, Qp for a module with
fiber configuration same as in a Du Pont B9 HFRO module 3.4.2. Case B: analytical solution for : , F > 0
is given by For the special case where Jv is large, then
1 -a
F = exp -Jv 0 (26)
f f 2prJv dzdr v
Di/2 0
A (Pf - Patm) 1 1
tanh(KL) (24) 0 (27)
r K <p exp(Jv/k)
For a Du Pont B9 HFRO with hydrodynamic permeability The expression for Jv in Eq. (11) can be simplified to
10 2
being 7 x 10" kg/(m s), do = 91 (xm, di = 44 (xm, N =
383,820, Do = 0.1016 m, A = 0.025 m, L = 0.254, the A cosh(Kz)
(28)
expression obtained above was used to check the numerical Jv= [Pb " cosh(KL)
p

0 425
- Analytical solution
o Numerical solution

0.42
f

0.415 /

| 0.41 /

?
7
><

1
^ 0.405

1 >

0.4

0.395

0.39( ) 0.05 0.1 0.15 0.2 0.25 0.3

Z (axial coordinate)

Fig. 2. Comparison of permeate flux obtained from numerical and limiting case A analytical solution.
 A. Chatterjee et al. /Journal of Membrane Science 236 (2004) 116

where 3.5. Numerical method for parameter estimation

RT An initial guess for each of the model parameters to be

r
\-a Mw estimated is used to initialize the estimation of parameters.
The predicted exit permeate flow rates and concentrations
The same module specifications as in case A were used obtained based on the initial guess are compared with exper-
with A = 70 x 10" 1 0 kg/(m2 s), Pm = 10" 1 0 m/s, = 0.5, imental values. In case the values chosen for the parameters
a = 0.048 and b = 0.6. For this case, K is 4.664 m " 1 . Feed were not correct, the values are refined so that the predicted
conditions were taken as 3 bar, 23.65 ml/s and 3000 ppm with and experimental permeate conditions are as close as possi-
Mw as 94 and a numerical solution was obtained. At these ble.
feed conditions and parameter values, the retentate radial Algorithm:
velocity becomes very small just before exiting the module
at i = m. This makes the mass transfer coefficient small at (a) Obtain the initial set of guesses for the parameters.
i = m. For the conditions we have chosen, the above criteria (b) Evaluate the error at all h experimental data points. De-
are satisfied with F ~ 0, while the largest value for 1/ is fine the error as:
0.02 at z = 0. At i < m, the conditions (26) and (27) are not
satisfied hence Eq. (28) cannot be used for these i values. In p,esti c,p,esti
order to check the numerical solution, it is assumed that the
error -- p,esti
QP,
+ 1 - C,p,esti (29)

solution till i = m -1 is correct and we compare Jv obtained i=1

numerically with that obtained from Eq. (28) using the reject
flow rate, pressure and concentration values at i = m. Fig. 3
shows this comparison. It is because of the non-zero values
of 1/ close to z = 0 that a very small deviation can be
observed in the Fig. 3, otherwise the agreement is excellent.
(c) Minimize error by adjusting the parameter values with
help of an optimization technique till error is below a
tolerance value.
The simplex search method [14] was used to estimate the
parameters from a given set of data.

1.2 1

Numerical so luttofl
O Limiting case analytical solution
1.1 -

/
1 - jr

0.8 -

L
0.7

_ _ -
0.6,
r
o

0.5 \
0.05 0.1 0.15 0.2 0.25 0.3
z (Axial coordinate)

Fig. 3. Comparison of permeate flux obtained from numerical and limiting case B analytical solution.
 A. Chatterjee et al. /Journal of Membrane Science 236 (2004) 116

4. Results and discussion Table 1

Specifications of Toyobo Hollosep membranes

4.1. Analysis Characteristics Membrane for Membrane for sea water

brackish water
Figs. 4-6 depict the behavior of leaky membranes ( < do (m) 160 x IO- 6 163 x IO- 6
1) versus the perfectly rejecting membrane ( = 1) as ap- di (m) 77 x IO- 6 70 x IO- 6
A (kg/(m2 s Pa)) 9.8 x 10-1" 2.89 x 10-1"
plied to the brackish water system while Figs. 7 and 8 de-
Pm (m/s) 2.51 x IO- 8 8.12 x 10-1"
pict the same for seawater using a Toyobo Hollosep Mod- A (m) 0.04 0.04
ule. The specifications for the Toyobo Hollosep module are A (m) 0.19 0.19
given in Table 1. The dependence of permeate flow rate L(m) 0.99 0.99
and solute concentration on feed conditions namely feed 4 (m) 0.07 0.07
2 2
flow rate or recovery, feed concentration and feed pressure
have been studied by keeping two constant and varying the
third feed variable, the recovery, A, has been set as 0.6
and 0.3 for brackish and sea water respectively in Figs. 5, are hence a direct comparison between the three and the
6 and 8. Pf and Cf have been set as 30 bar and 1.5kg/m3 two-parameter model.
for brackish water and 55 bar and 35kg/m3 for seawater In all plots for Qp, we find that as the reflection coeffi-
when they have to be kept constant in Figs. 4-8. For = cient decreases, the permeate flow rates are higher. This
1, the three-parameter Spiegler-Kedem model reduces to is evident from the fact that a leaky membrane allows more
the two-parameter solution-diffusion model. These figures solute and water to flow through leading to an overall in-

8.00 60.00

7.50 - - 50.00

7.00 - -- 40.00

8
6.50 - - 30.00 x

6.00 - - 20.00

5.50 - - 10.00

5.00 0.00
35

Fig. 4. Variation of Permeate characteristics with feed flow rate for brackish water.

30,00

?oo-
- 25 00
B.50- vT] X
5.00- -.-B-I H
0=0.98 20,00
5 50- - - * - 0-0.^5
xo-9.9
5 00- - 15.00
A
-- . _
4.50-
- 10.00
4.00-

3 50
- 5,00
-- +
3.00-

0,00

3
C, (kglm )

Fig. 5. Variation of Permeate characteristics with feed concentration for brackish water.
 A. Chatterjee et al. /Journal of Membrane Science 236 (2004) 116

10.00 30.00

3.00 -
- 2 5 00
e.oo -

7.00 - - 20.00

6.00 -
-1500 x
5.00- d

4.00 - - 10.00

3.00 -
- 5.00
2.00 -

1.00 0.00
10 15 20 25 30 35 40
P, (bar)

Fig. 6. Variation of permeate characteristics with feed pressure for brackish water.

-3 0L

0 Of
5 10 15 20
4 a
Qf x 10 (m /s)

Fig. 7. Variation of permeate characteristics with feed flow rate for sea water.

2.00 -T 8.00

1.S0 -
7.00

1 60 -
6.00
1.40 -
5.00 3
Jj? 1.20 -
8
*o 1 00 - I 4 00 K
5 0.80 - 3.00

0.60 -
2.00
0.40 -
1.00
0.20 -

0.00 - O.00
27 29 31 33 35 37 39 41 43
Ct(kg/m3)

Fig. 8. Variation of permeate characteristics with feed concentration for sea water.
10 A. Chatterjee et al. /Journal of Membrane Science 236 (2004) 116
crease in permeate flow with decreasing . The reflection
coefficient is a measure of how imperfect (leaky) the mem-
brane is. The maximum difference between the Qp values
for leaky membrane and perfectly rejecting membranes is
6% for brackish water and 14% for seawater. This also ex-
plains why a similar increase in permeate concentration is
observed with decreasing in all plots for Cp/Cf. Here, the
maximum differences in Cp/Cf values for leaky membrane
and perfectly rejecting membranes are of the order of 362%
for brackish water and 4431% for seawater. The percentage
variation in seawater is greater because here the values of
Cp/Cf for perfectly rejecting membranes are very small in
magnitude.
From Figs. 4 and 7, we find that as the feed flow rate in-
creases, the permeate concentration declines. This is because
a greater feed flow rate implies that mass transfer coeffi-
cient, k, becomes larger, hence the concentration polariza-
tion approaches closer to its asymptotic value of one. This
results in the solute concentration gradient across the mem-
brane becoming smaller, while the permeate flux increases,
thereby leading to an overall decrease in the solute permeate
concentration.
The variation of Cp/Cf with changing feed concentration
(Figs. 5 and 8) is particularly interesting. When is 1 or
perfect rejection is assumed, Cp/Cf increases with increas-
ing the feed concentration. As decreases, the above trend
is reversed to an extent. This is because the solute flux is
strongly dependent and increases with the difference in the
solute concentrations of the feed and permeates. The sol-
vent flux on the other hand is reduced by large concentra-
tion differences across the membrane because of the osmotic
pressure term. This kind of scenario would lead to a steady
increase in the permeate concentration with increasing feed
concentration as observed for = 1. The reversal of this
trend at low is due to the increase in the overall flux which
causes the dilution of the permeate stream. Reduction of
10.00
Fig. 9. Ratio of permeate to feed concentration vs. feed pressure for brackish water: comparison of solution-diffusion model and model of Gupta et al.
permeate concentration in Fig. 9 with feed pressure is be-
cause of the higher permeate flow rate as is evident from
Eq. (1). As the permeate flow rate increases, the bulk solute
concentration gradually increases. This explains the shape
of the graph in Fig. 8 for = 1. Increased solute concen-
tration and low (for example, = 0.9), leads to higher
fluxes through the membrane thus increasing the permeate
concentration.
A comparison of the plots for = 1 and lower val-
ues from Figs. 4-11 show that there are substantial differ-
ences between the solution-diffusion and Spiegler-Kedem
membrane transport models and that one should use the
Spiegler-Kedem model for design and analysis of a RO sys-
tems.
4.2. Analytical solution of the solution-diffusion model vs.
numerical solution
Figs. 9-11 compare the analytical solution provided by
Gupta and the exact numerical solution. Fig. 9 shows that
the analytical solution gives lower values of the permeate
concentration. The differences are as high as 36%. The main
reason for these differences is because the analytical solution
neglects pressure drops in both permeate and feed streams.
Since the pressure drop in the fiber bores can be as large as
9 atm, the variations in the net pressure differences across the
membrane are substantial. Another reason for the differences
is the fact that the analytical solution assume constant mass
transfer coefficient through out the module, which may be
reasonable only for low recoveries (<0.4). The recoveries
considered here are 0.6 and larger. This restricts the accuracy
of the analytical solution. Similar trends are observed for
varying feed concentration and varying feed pressures. We
can conclude from this discussion that the consideration of
pressure drops gives a much clearer picture of the separation
process and must be employed for modeling.
Solution Diffusion Model - x - Model of Gupta et al
 A. Chatterjee et al. /Journal of Membrane Science 236 (2004) 116 11

7- Solution Diffusion Model -Model of Gupta et. al.

B-

5 -

4 3-

2-

10 15 20 25 30
Qf*104(m3/s)

Fig. 10. Permeate flow rate vs. feed flow rate for brackish water: comparison of solution-diffusion model and model of Gupta et al.

9.0D
Solution Diffusion Model - x - Model of Gupta et al

3
C, (kg/m )

Fig. 11. Ratio of permeate to feed concentration vs. feed concentration for brackish water: comparison of solution-diffusion model and model of Gupta
et al.

4.3. Results of parameter estimation
Experimental data obtained from literature on Du Pont
B9 Permeator and Toyobo Hollosep module for various op-
erating conditions were used to obtain parameters of these
systems using our parameter estimation program. The hy-
drodynamic permeability, A is determined from the perme-
ate flow rate obtained for a module with pure water. The es-
timations are first carried out for three sets of experimental
data of Sekino [12], Tweddle et al. [11] and Ohya et al. [10].
Sekino [12] obtained experimental data on NaCl system
on a Toyobo HA8130 module and presented these in the
graphical form in their paper. We used this data and the mem-
brane characteristics and the mass transfer coefficient given
by them to predict the membrane performance as shown in
Table 2. It may be noted that the membrane parameters given

Table 2
Experimental data for Toyobo Hollosep module: parameters provided by Sekino

P f (bar) Q f (xl0 4 m 3 /s) C f (kg/m3) Qp (xl0 4 m 3 /s) Q p (xl0 4 m 3 /s) Error in C p (kg/m3) C p (kg/m3) Error in
reported predicted Qp (%) reported predicted C p (%)
30.00 12.90 0.53 7.74 7.54 2.58 0.020 0.019 4.00
30.00 11.74 1.46 7.04 6.93 1.56 0.056 0.059 -5.46
30.00 8.71 4.93 5.23 5.04 3.63 0.230 0.229 0.43
30.00 4.92 10.00 2.95 2.85 3.39 0.710 0.717 -0.99
1
A = 9.8 : kg/(m2 s Pa), Pm = 2.51 x 10~8 m/s, = 1, a = 0.048 and b = 0.6.
12 A. Chatterjee et al. /Journal of Membrane Science 236 (2004) 116

Table 3
Estimating all model parameters with A known

P f (bar) Q f (xl0 4 m 3 /s) Cf (kg/m3) Q p (xl0 4 m 3 /s) Q p (xl0 4 m 3 /s) Error in C p (kg/m3) C p (kg/m3) Error in
reported predicted Qp (%) reported predicted C p (%)
30.00 12.90 0.53 7.74 7.56 2.33 0.020 0.020 2.10
30.00 11.74 1.46 7.04 6.98 0.85 0.056 0.057 -1.75
30.00 8.71 4.93 5.23 5.15 1.53 0.230 0.231 -0.30
30.00 4.92 10.00 2.95 2.98 -1.02 0.710 0.709 0.08

Predicted: Pm = 2.684 x 10- 8 m/s, = 0.99999, a = 0.0473, b = 0.4166. Fixed: A = 9.8 x 10- 10 kg/(m 2 sPa).

by them were calculated on a test cell where the flow condi-
tion were such that the effect of concentration polarization
could be neglected. Furthermore, the mass transfer coeffi-
cients were obtained from literature correlation [13]. As can
be seen the maximum error is around 5% in permeate con-
centration and 3.63% in permeate flow rate. The same ex-
perimental data is used in Table 3 to predict simultaneously
the membrane parameters (Pm, ) and mass transfer corre-
lation constants (a, b) using the present numerical procedure
given in Section 3.4. The maximum error now reduces to
2.1% in permeate concentration and 2.33% in permeate flow
rate which shows the validity of our parameter estimation
program.
The data reported by Tweddle et al. [11] (Table 4) is for
fixed pressures drop of 2758 kPa and only four data points
are available for NaCl system on a Du Pont B9 hollow fiber
module. Since only few data points are available, it was as-
sumed that the parameters of mass transfer coefficient are
already known and only the membrane parameters Pm and
a were calculated from our parameter estimation program.
Once again the experimental and the predicted value of the
permeate concentration and the flow rates are in good agree-
ment.Now consider the data reported by Ohya et al. [10]
(Table 5) for B9 hollow fiber system. Since in this case large
numbers of data are available, here we see that the net error
is much lower and better distributed when we compare the
results presented in Table 4. The experimental data are in
good agreement. This also validates our model.
The experimental data of Sekino et al., Tweddle et al. and
Ohya et al., are all for NaCl-water system and our param-
eter estimation program shows that for these systems the
reflection coefficient is one and therefore for these systems
the two parameter model of Sekino et al. is sufficient. How-
ever, the significance of the reflection coefficient can not
neglected for a large number of other systems as has been
seen in the previous Sections 4.1 and 4.2. There are several
studies available in literature on small membrane test cells
where it has been shown that for many systems the value of
reflection coefficient is less than one. For example, Murthy
and Gupta [15] reports that for a NaCN system the reflection
coefficient is 0.97 while Murthy and Gupta [16] reports that
for phenol water system, the reflection coefficient is 0.90 for
cellulose acetate membrane.To further investigate the impor-
tance of the reflection coefficient the experiments for separa-
tion of phenol were carried in a laboratory scale B9 Du Pont
HFRO module, the hollow fiber membrane material is aro-
matic polyamide and the data obtained was analyzed. The
phenol concentration was experimentally determined by us-
ing the HPLC with reverse phase column. The B9 module
specifications used in the present study are shown in Table 6.

Table 4
Estimation of parameters for Du Pont Permeator using Tweddle's data

(bar) gf(xl04rn3/s) C f (kg/m3) Qp (xl0 4 m 3 /s) Qp (xl0 4 m 3 /s) Error in C p (kg/m3) C p (kg/m3) Error in
reported predicted Qp (%) reported predicted C (%)
28.593 2.06 1.974 1.39 0.0 6.24 0.09 0.10 -11.71
28.593 1.63 4.112 3.0 1.07 3.04 0.24 0.26 -5.97
28.593 1.86 8.19 0.92 0.874 5.02 0.46 0.45 1.92
28.593 1.96 15.65 0.62 0.572 7.68 1.28 1.00 22.08

Predicted: Pm = 1.628 x 10~8m/s, = 0.999989. Fixed: A = 4.8 x 10" 10 kg/(m 2 sPa), a = 0.0408, b = 0.6.

Table 5
Experimental data for Du Pont B9 module: estimating all model parameters with A known

Pf (bar) Q f ( x l 0 4 m 3/s) C f (kg/ m 3 ) Q p (xl0 4 m 3 /s) Qp (xl0 4 m 3 /s) Error in C p (kg/m3) C p (kg/m3) Error in
reported predicted Qp (%) reported predicted C p (%)
27.30 1.25 3.50 0.93 0.97 -3.77 0.42 0.44 -4.31
27.50 1.04 2.78 0.88 0.91 -3.55 0.51 0.52 -2.38
21.30 1.88 3.50 0.96 0.87 9.11 0.27 0.26 2.23
22.30 1.04 3.30 0.79 0.77 1.70 0.50 0.45 9.15
22.30 0.83 3.10 0.70 0.70 0.51 0.57 0.59 -3.50

Predicted: Pm = 2.2506 x 10~8 m/s, = 0.9999736, a = 0.0536, b = 0.6741. Fixed: A = 5 x 1 0 - 1 kg/(m2 s Pa).
 A. Chatterjee et al. /Journal of Membrane Science 236 (2004) 116 13

Table 6 and then these estimated parameters were used for the pre-
Specifications of Du Pont B9 permeator diction of separation data in Table 8. The maximum errors
Characteristics B9 module of Ohya B9 laboratory scale in prediction of the permeate flow rates and permeate con-
et al. used in present study centration are less than 13 and 5%, respectively for the data
do (m) 84 x 10~6 91 x 10~6 in Table 7 which was also used for parameter estimation.
di (m) 42 x 10- 6 44 x 10- 6 However, the maximum errors increase to 14 and 11%, re-
A (kg/(m2sPa)) 5 x 10- 1 0 7.322 x 10- 1 0 spectively when these same estimated parameters are used
N 6.6 x 105 383820
for prediction of the data given in Table 8.
A (m) 0.0254 0.025
Do (m) 0.1 0.1016 The phenol separation data was also analyzed by using
L(m) 1 0.254 the solution-diffusion model of Sekino et al. For this, it was
s(m) 0.08 0.02 assumed that the reflection coefficient was equal to one and
W0 0 0
the same parameter estimation program was used to deter-
mine the solute permeability and the mass transfer parame-
ters. For the separation data given in Table 7, the estimated
The past studies for phenol separation [17] on flat membrane solute permeability and the mass transfer coefficient param-
test cell have shown that the rejection of phenol is highly eters are shown in Table 9. Though the mass transfer param-
dependent on the pH of the solution and are reasonable only eters remain the same, the value of the estimated solute per-
at high pH. Therefore, the experiments were carried out at meability is much higher at 22.79 x 10~8 m/s. Using these
pH = 9.1. The hydrodynamic permeability of the membrane parameters, the permeate flow rates and the concentrations
was determined by using the pure water permeability data. are predicted and are compared with the experimental re-
The experimental data for phenol separation at various oper- sults in the same Table 9. As can be seen from this table,
ating feed flow rates, pressures and feed concentrations are the maximum error for permeate flow rate and concentra-
presented in Tables 7 and 8. The data in Table 7 was used tion are 12.85 and 26.31%, respectively. The same estimated
for the parameter estimation of the Spiegler-Kedem model parameters were then used to predict the phenol separation

Table 7
Analyzed data for phenol separation in laboratory scale experimental setup Du Pont B9 module using S-K model

Pf (bar) (x 106 m3/s) Cf (x 103 kg/m3) Qp (xl0 6 m 3 /s) Qp (xl0 6 m 3 /s) Error in C p (xl0 3 kg/m 3 ) Cp (xl0 3 kg/m 3 ) Error in
reported predicted Qp (%) reported predicted Cp (%)
4.61 14.79 14.26 6.30 7.00 -11.10 10.87 11.36 -4.54
4.61 25.56 13.65 6.20 7.00 -12.90 10.33 10.01 3.11
5.99 25.67 14.36 9.30 9.69 -4.14 11.17 10.87 2.70
4.65 19.11 49.08 6.28 7.07 -12.65 37.50 37.46 0.10
6.03 19.44 49.29 9.20 9.76 -6.09 38.45 39.49 -2.72

Predicted: Pm = 9.69 x 10" 8 m/s, = 0.538, a = 0.0487, b = 0.593. Fixed: A = 7.322 x 10"lkg/(m2 sPa).

Table 8
Permeate characteristics predicted using parameters estimated in Table 7 using S-K model

(bar) gf(xl06rn3/s) C f (xl0 3 kg/m 3 ) Qp (xl0 6 m 3 /s) Qp (xl0 6 m 3 /s) Error in C p (xl0 3 kg/m 3 ) Cp (xl0 3 kg/m 3 ) Error in
reported predicted Qp (%) reported predicted Cp (%)
5.53 14.53 26.94 8.83 8.79 0.48 20.95 21.26 -1.46
5.87 18.97 25.84 8.64 9.45 -9.37 19.61 19.13 2.42
5.87 24.52 26.37 9.14 9.45 -3.39 20.24 18.29 9.65
4.89 22.82 35.95 6.83 7.54 -10.41 27.40 24.57 10.35
4.49 15.74 25.98 5.94 6.76 -13.87 19.74 18.89 4.33

Table 9
Analyzed data for phenol separation in laboratory scale experimental setup Du Pont B9 module using S-D mode

Pf (bar) gf(xl06rn3/s) C f (xl0 3 kg/m 3 ) gp(xl06rn3/s) Qp (xl0 6 m 3 /s) Error in C p (xl0 3 kg/m 3 ) Cp (xl0 3 kg/m 3 ) Error in
reported predicted Qp (%) reported predicted
4.61 14.79 14.26 6.30 7.00 -11.06 10.87 9.64 11.33
4.61 25.56 13.65 6.20 7.00 -12.85 10.33 8.1 21.61
5.99 25.67 14.36 9.30 9.68 -4.11 11.17 8.23 26.31
4.65 19.11 49.08 6.28 7.06 -12.47 37.50 30.92 17.54
6.03 19.44 49.29 9.20 9.74 -5.9 38.45 31.24 18.76

Predicted: Pm = 22.79 x 10~8m/s, a = 0.0483, b = 0.596. Fixed: A = 7.322 x 10"lkg/(m2 sPa).

14 A. Chatterjee et al. /Journal of Membrane Science 236 (2004) 116

Table 10
Permeate characteristics predicted using parameters estimated in Table 9 using S-D model

(bar) gf(xl06rn3/s) C f (xl0 3 kg/m 3 ) Q p (xl0 6 m 3 /s) Q p (xl0 6 m 3 /s) Error in Cp (xl0 3 kg/m 3 ) Cp (xl0 3 kg/m 3 ) Error in
reported predicted Qp (%) reported predicted
5.53 14.53 26.94 8.83 8.78 0.56 20.95 19.03 9.16
5.87 18.97 25.84 8.64 9.44 -9.3 19.61 16.47 16.03
5.87 24.52 26.37 9.14 9.44 -3.32 20.24 15.34 24.21
4.89 22.82 35.95 6.83 7.53 -10.32 27.40 21.62 21.11
4.49 15.74 25.98 5.94 6.76 -13.8 19.74 17.23 12.73

Table 11
Permeate characteristics predicted using parameters estimated in Table 5

P f (bar) Q f (xl0 4 m 3 /s) C f (kg/m3) Qp (xl0 4 m 3 /s) Qp (xl0 4 m 3 /s) Error in C p (kg/m3) C p (kg/m3) Error in
reported predicted Qp (%) reported predicted C p (%)
26.50 1.65 3.50 0.97 1.05 -8.11 0.27 0.30 -12.06
27.50 1.02 3.20 0.89 0.88 1.58 0.70 0.57 18.92
23.30 1.02 3.50 0.75 0.78 -3.82 0.48 0.50 -3.67
21.50 1.67 3.50 0.91 0.86 5.56 0.29 0.29 1.28
22.00 1.25 3.50 0.84 0.81 3.21 0.41 0.38 9.08

data shown in Table 8 and the predicted results are shown
in Table 10. The overall maximum error for the permeate
flow rate and concentration are 10.32 and 24.21%, respec-
tively. When the results of Tables 7 and 8 are compared
with the results of Tables 9 and 10, respectively we find that
the errors between the reported and the predicted values of
the permeate concentration for the solution-diffusion model
are significantly higher than those for the Spiegler-Kedem
mode while the errors for the permeate flow rate are nearly
the same. It may be further noted that the mass transfer co-
efficient parameters obtained for phenol separation for both
two parameter solution-diffusion model and three parame-
ter Spiegler-Kedem model are nearly the same as obtained
by the parameter estimation of Ohya data shown in Tables 5
and 11 and of Tweddle et al., data shown in Table 3 as the
flow pattern in these modules are similar. This again val-
idates the present model and clearly shows that for many
systems the solution-diffusion model used by Sekino et al.
may not be sufficient to accurately describe the membrane
performance of a radial flow hollow fiber module.
The estimated value of the reflection coefficient for
phenol-water system is 0.538 for the present B9 hollow
fiber polyamide membrane whereas the value of reported
by Murthy and Gupta [16] is 0.9 for cellulose acetate mem-
brane. Clearly, the membrane transport parameters such as
the reflection coefficient are function of both solute-solvent
system as well as the physical properties of the membrane.
Similar results have also been reported by Wadely et al.
[18] and Moresi et al. [19].
5. Conclusions
The mathematical model of Sekino [12] for a ra-
dial flow hollow fiber is extended by replacing the
solution-diffusion model for membrane transport by a
non-linear Spiegler-Kedem model. While Sekino modeled
the Toyobo hollow fiber model, the present model can be
used for both Toyobo as well as Du Pont hollow fiber
module. The main difference between the two models is
the introduction of third membrane parameter namely the
reflection coefficient. The results obtained for different val-
ues of the reflection coefficient, , are compared with those
obtained equal to one where the present model reduces
to model of Sekino. It is found that as the reflection coeffi-
cient is decreased from its maximum value of one, the total
permeate produced is much higher and also the concen-
tration of the permeate solution differs substantially from
that reported by the solution-diffusion model. The effect of
increasing the feed pressure along with decreasing the re-
flection coefficient causes at first a decrease in the permeate
concentration, then an increase at very high pressures.
The results of the present model for the reflection coeffi-
cient equal to one are also compared with the analytical solu-
tion proposed by Gupta [8]. The analytical solution neglects
the pressure drop in the permeate streams and this is respon-
sible for giving lower permeate rates and permeate concen-
tration. Since the mass transfer coefficient and the pressure
difference across the membrane are assumed to be constant,
the analytical solution is not valid for high recoveries.
The membrane performance parameters as described by
the three-parameter Spiegler-Kedem model are estimated
from the experimental data on Toyobo and Du Pont hollow
fiber modules. Since the experimental data is obtained for
NaCl system for which the solution-diffusion model is suffi-
cient for describing the membrane mass transport across the
membrane, the parameters evaluated from the present model
are not very much different from the results obtained by the
model Sekino et al., To further validate the present model,
the experimental data for phenol separation were obtained
 A. Chatterjee et al. /Journal of Membrane Science 236 (2004) 116 15

on a B9 hollow fiber module and the present model was used

to analyze the data. These results clearly show that the two e volume fraction of module available to bulk
parameter model used by Sekino et al. may not be sufficient side fluid
for accurate design and analysis for many solute-membrane concentration polarization
systems. Furthermore, the present parameter estimation pro- viscosity (kg/(m2 s))
gram can also be used for developing the mass transfer cor- V VantHoff factor
relation in the radial flow hollow fiber modules. Tt osmotic pressure (Pa)
constants appearing in Eq. (14)
p density (kg/m3)
a reflection coefficient
Nomenclature
a coefficient in mass transfer correlation Subscripts
av surface-volume area of particle b bulk/retentate side
A hydrodynamic permeability (kg/(m2 s Pa)) exp experimental
b exponent of Reynolds number in mass est estimated
transfer coefficient f feed
c,C solute concentration of stream (kg/m3) th grid point along radial direction
di, do inside and outside diameter of hollow j jth grid point along axial direction
fiber(m) P permeate
dp specific surface diameter (m)
b diffusion coefficient (m2/s)
i, D inside and outside diameter of fiber bundle,
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