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processes

Suhan Kim, Eric M.V. Hoek*

Department of Civil and Environmental Engineering, 5732-G Boelter Hall, University of California,

Los Angeles, CA 90095-1593, USA

Tel. +1 (310) 206-3735; Fax +1 (310) 206-2222; email: hoek@seas.ucla.edu

Abstract

Accurate prediction of concentration polarization (CP) phenomena is critical for properly designing reverse

osmosis (RO) processes because it enhances trans-membrane osmotic pressure and solute passage, as well as

surface fouling and scaling phenomena. The objective of this study was to compare available analytical CP models

to a more rigorous numerical CP model and experimental CP data. A numerical concentration polarization model

was developed to enable local description of permeate flux and solute rejection in crossflow reverse osmosis

separations. Predictions of channel averaged water flux and salt rejection by the developed numerical model, the

classical film theory model, and a recently proposed analytical model were compared to well-controlled laboratory

scale experimental data. At operating conditions relevant to practical RO applications, film theory and the numerical

model accurately predicted channel-averaged experimental permeate flux and salt rejection data, while the more

recent analytical model did not. Predictions of local concentration polarization, permeate flux, and solute rejection

by film theory and the numerical model also agreed well for realistic ranges of RO process operating conditions.

Keywords: Concentration polarization; Reverse osmosis; Film theory; Modeling; Membranes

1. Introduction

Concentration polarization (CP) is one of the

most important factors influencing the performance of membrane separation processes [1]. Prediction of solute concentration polarization is

crucial for designing reverse osmosis processes,

*Corresponding author.

understanding surface fouling phenomena [25].

For example, accurate description of local variations in permeate velocity, solute rejection, and

concentration polarization are required to predict

the onset of surface scale formation by sparing

soluble minerals [6]. However, some debate lingers among membrane scientists and engineers

0011-9164/06/$ See front matter 2005 Elsevier B.V. All rights reserved.

doi:10.1016/j.desal.2005.05.017

112

concen-tration polarization in reverse osmosis and

other semi-permeable membrane separations like

nano-filtration and ultrafiltration [7].

Concentration polarization is governed by

solute properties, membrane properties, and hydrodynamics [810]. It is influenced by both axial

and transverse flow fields, which are in turn influence by concentration polarization [1113]. The

coupling of momentum and mass transport makes

simultaneous solution of the NavierStokes, continuity, and convection-diffusion equations computationally intensive even for simple systems [13,

14]. Although concentration polarization in

reverse osmosis processes under laminar flow conditions can be rigorously modeled [15,16], these

accurate numerical solutions have little bearing

on real membrane separations in spiral wound elements with complex hydrodynamics due to feed

spacers [1719]. However, these relatively idealized

CP models are important for proper interpretation

of laboratory scale mechanistic studies, especially

those focused on elucidating fundamental mechanisms governing fouling and scaling phenomena.

Early CP models were limited to semi-empirical mass transfer analogies of heat transfer

correlations, which were developed to describe

stagnant film layer formation in conduits with

impermeable walls [20]. Stagnant film models are

fundamentally ill-suited to accurately describe all

mechanisms of concentration polarization in

crossflow membrane filtration processes because

these models assume uniform concentration along

the filtration channel wall and do not account for

the impact of permeate convection on the film

layer thickness. Despite these limitations, film

theory is simple, analytical, and (reasonably) accurate for most reverse osmosis separations. Further,

film theory can be extended to describe CP

phenomena in spacer-filled RO modules, which

is of tremendous value in practical process design

and evaluation.

Recently, a model was proposed [21], which

attempts to capture the fundamental interplay

between concentration polarization layer development and a locally varying permeate flux (in a

closed form analytical solution) by making use

of the retained solute concept [22]. This model

describes two dimensional convective-diffusive

solute transport without complex computational

effort, and hence, can be used to predict local concentration polarization and permeate flux in

spacer-free reverse osmosis flow channels. The

retained solute model appears an attractive alternative to film theory and is simpler than numerical

techniques, but it has not been subjected to

rigorous analysis or comparison to well-controlled

experimental data. A more rigorous numerical

convection-diffusion based concentration polarization model was developed for comparison with

the retained solute and film theory models. Predictions from all three models were compared to

experimentally-derived permeate flux and observed salt rejection data. The accuracy, limitations, and applicability of each model for RO

processes are discussed.

2. Theoretical

2.1. Analytical film theory (FT) model

A film theory approach to describe concentration polarization was developed by Michaels

and others [810]. Film theory simplifies a complex transport problem to a one-dimensional masstransfer problem by assuming axial solute convection near the membrane surface is negligible.

Integrating the one dimensional (transverse) convection-diffusion mass balance from the membrane surface out to a finite mass boundary (film)

layer thickness, , yields the relationship between

concentration polarization and permeate flux. The

result is

cw c p

v

= exp w

cb c p

D

(1)

the bulk and permeate solute concentrations, respectively, vw is the permeate water velocity at the

channel wall, and D is the solute diffusion coefficient.

A procedure for estimating the convective

diffusion layer thickness in a channel with soluble

or rapidly reacting walls forms the basis of most

film theory models [23]. For fully developed

laminar flow in a thin rectangular channel, the

film layer thickness is described by

( x)

h

= 1.475

x

x

2/3

1/ 3

umax h

(2)

channel half-height, and umax is the maximum

crossflow velocity at channel center. Assuming

constant diffusivity, a local mass transfer coefficient is described by

1/ 3

D

1 3u D 2

k ( x) =

=

( x ) 1.475 2h x

1/ 3

D 2

= 0.538 w

x

113

transfer coefficient is expressed as

1/ 3

D 2

k = 0.807 w

L

(4)

for laminar flow in a thin channel commonly

reported in terms of a Sherwood number, e.g.,

1/ 3

Sh = kd H / D = 1.85 ( ReScd H / L ) [9].

In reverse osmosis processes, the driving force

for permeation is the difference between the

applied pressure, p, and the transmembrane

osmotic pressure, m. Thus, the permeate flux is

described by

vw = A ( p m )

(5)

membrane. The transmembrane osmotic pressure

is given as

m = f os ( cw c p ) = f os Ri cw

(3)

(=Q/2hW), W is the channel width, Q is the

volumetric feed flow rate) and w ( = 3u / h) is the

wall shear rate [24,25]. A key limitation of applying film theory to membrane separations is the

assumption that the transverse component of convection (permeate flux) does not influence the

boundary layer thickness, .

The channel averaged mass transfer coefficient, k , derives from integrating the local flux,

vw(x), given by Eqs. (1) and (3) assuming the membrane, permeate, and bulk concentrations, as well

as the permeate and crossflow velocities remain

constant along the channel length, L. This assumption is unrealistic for large scale RO systems, but

reasonable for short membrane channels where

(6)

of membrane and fos is a coefficient that converts

molar salt concentration to an osmotic pressure

via an appropriate expression [26]. vant Hoffs

equation gives fos = 2RT for NaCl (R is the universal gas constant and T the absolute temperature), which is accurate for dilute concentrations.

Provided with the system operating parameters

(p, u , T), solution and solute characteristics (cb,

D), and membrane properties (A, Ri), the wall concentration, cw, is the only unknown parameter

linking concentration polarization, permeate flux,

and observed rejection (Ro = 1 cp/cb). The wall

concentration can be solved for when Ri is known

from [5]

cw

v

= 1 Ri + Ri exp w

cb

k

(7)

114

The retained solute model attempts to account

for the interplay between solvent permeation,

solute retention, and concentration polarization.

The coupling of water permeation and concentration polarization becomes more complex in

crossflow filtration when the local variation of CP

is considered along the filtration channel. An

analytical concentration polarization model was

previously developed to describe the combined

influences of colloidal particle diffusion, crossflow velocity, and permeate flux in crossflow

ultrafiltration using the concept of retained solute

[21].

At steady state, the concentration of retained

solute in the CP layer satisfies the following condition, assuming negligible axial transport

vw ( x ) C + D

C

=0

y

(8)

coordinates, respectively, vw(x) is the permeate

flux at x, and C indicates the concentration of

retained solute (the actual solute concentration in

the polarization layer is cb + C) [22]. At steady

state, the longitudinal solute flux at any point x

along the channel is equal to the total amount of

solute rejected by the membrane from the inlet to

the location x, that is

w yCdy = Ro cb vw ( x ) dx

0

(9)

and x is a dummy integration variable.

Using Eqs. (5), (8) and (9) a closed-form

analytical expression for the local permeate

velocity can be written as

vw ( x ) =

AF 0

(1 + 6F

X / Ns3 )

1/3

1/3

1/ 2

4

2

+

+

2

3

+

F

X

N

1

6

/

s )

(

(10a)

1/ 3

1/ 2

4

2

+

2

3

(1 + 6F X / Ns )

with F =

p 0

0

(10b)

1/ 3

and N s =

1 1 D 2 w

A 0 L

(10c)

pressure difference between feed and permeate

sides of the membrane (0 = fos (cb cp) = fosRocb),

X is the dimensionless longitudinal distance, x/L,

and F and Ns are the dimensionless driving force

and dimensionless membrane resistance, respectively [21]. The salt concentration on the membrane surface can be derived from vw(x) via

Eq. (5), that is

cw ( x ) =

p vw ( x ) / A + f os (1 Ro ) c0

f os

(11)

model is attractive because it accounts for the

fundamental interplay between concentration

polarization and permeate flux in a closed form

analytical solution.

2.3. Numerical convectiondiffusion (CD) model

We have developed a new concentration polarization model accounting for the two-dimensional

The velocity field is composed of axial (feed) and

transverse (permeate) components. In principle,

the velocity profile can be obtained by complete

solving the NavierStokes and the continuity

equations; however, a Poiseuille flow profile is

classically assumed if the permeation velocity is

small and does not significantly alter the axial flow

profile [15]. An additional complication arises

because both velocity components influence

concentration polarization of rejected salt ions.

Simultaneously, concentration polarization reduces

permeate flux, which in turn alters the polarization

layer characteristics. A complete description of

the process requires solving the fully coupled

NavierStokes, continuity, and convectiondiffusion equations.

In order to simplify the coupled momentum

and mass transport problem, the axial velocity

profile is assumed independent of concentration

polarization in our model. The axial (u) and

transverse (v) components of velocity are expressed as [15]:

r2

u ( x, y ) = umax ( x ) 1 2

h

r2

3

= u ( x ) 1 2

2

h

r2

r

v ( x, y ) = vw ( x ) 3 2 ;

h

2h

hvw ( x )

115

compared to the channel height, which enables

the transverse velocity within the boundary layer

to be held constant and equal to the permeate

velocity at the wall, vw(x).

Conservation of mass is considered in two

regions of the crossflow filtration channel. One

region is above the boundary of the CP layer

and the other is within the CP layer. Fig. 1 shows

the domain for solving the mass balance problem.

At steady state, solute and solvent mass should

be conserved everywhere. Since the height of

concentration polarization layer is much smaller

than the channel height, solvent mass is considered

above concentration polarization layer, that is

Q ( x ) = Q ( x + x ) +

x +x

vw ( x )Wdx

(13)

at x and x + x, respectively, and vw(x) is the permeate flux at x. The solute mass balance above

concentration polarization layer is described as

Q ( x ) cb ( x ) = Q ( x + x ) cb ( x + x )

x +x

(12a)

(12b)

= Re w 1

rectangular channel (r = y h) and is kinematic

viscosity of water. As indicated, Eq. (12b) is valid

when the wall Reynolds number based on the

permeation velocity is much smaller than unity.

A further simplification used in our model is that

vw ( x )Wcb ( x ) dx

(14)

where cb(x) and cb(x + x) are the bulk concentration at x and x + x, respectively. By solving

Eqs. (13) and (14) simultaneously, cb(x) is proved

constant and denoted as cb.

Solute mass should be conserved within concentration polarization layer as well, that is,

vw ( x ) c ( x, y ) + D

c ( x, y )

y

= vw ( x ) c p ( x )

(15)

within concentration polarization layer. Eq. (15)

is a form of convectiondiffusion equation and

its solution can be written as

116

Fig. 1. The problem domain used in developing the numerical convection diffusion model for a laboratory scale crossflow

membrane filter without mesh feed spacer. Feed water flows from left to right along the channel length and some portion

of water flows through the membrane.

v ( x)

c ( x, y ) = cw ( x ) c p ( x ) exp w

y

D

(16)

+ c p ( x ) ; y ( x )

At steady state, axial and transverse input and

output should be balanced in the problem domain

within concentration polarization layer as shown

in Fig. 1, that is

( x )

u ( x, y ) c ( x, y ) y

0

at x

( x )

u ( x, y ) c ( x, y ) y

0

at x +x

= cb c p ( x )

x +x

vw ( x )dx

(17)

The integrations in Eq. (17) are solved numerically using the trapezoidal rule. The concentration profile starting from an arbitrary (initial)

wall concentration is solved for by Eq. (16). As

the transverse coordinate (y) increases, the concentration decreases due to solute back transport by

convection and diffusion. The extent of the CP

boundary layer thickness is defined as the position

when the concentration, calculated from Eq. (16),

equals the bulk concentration. Concentration

polarization layer thickness is defined as the

distance from that position to the channel wall.

Above the CP layer, all the concentrations are

equal to the bulk concentration.

Since the initial wall concentration is an

arbitrary value, an iteration process is required.

This is performed by solving Eqs. (12), (16) and

(17) simultaneously to obtain the salt concentration locally in the channel. Once the local salt

determined, the local permeate flux can be calculated from Eq. (5) and the osmotic pressure from

Eq. (6). Provided with the system operating parameters (T, p, u ), solution and solute characteristics (cb, D) and membrane properties (A, Ri),

concentration polarization, permeate flux, and permeate concentration can be predicted. All mass

conservation equations above assume constant and

equal density and viscosity in feed, retentate, and

permeate solutions.

3. Experimental

3.1. Membrane and reagents

A commercial RO membrane designated as

XLE (Dow-FilmTec Corp., Edina, MN) was used

in this study. Upon receipt from the manufacturer,

the membrane was immersed in de-ionized water

(Milli-Q Synthesis, Millipore, Billerica, MA) and

stored at 5C. Deionized water was changed daily

for the first two weeks and subsequently changed

about every two weeks. Salt stock solutions were

prepared using ACS grade NaCl (Fisher Scientific;

Pittsburgh, PA) dissolved in de-ionized water.

3.2. Crossflow membrane filter

The crossflow membrane filter (CMF) used in

fouling experiments was a modified version of a

commercially available unit (Sepa CF, Osmonics,

Inc.; Minnetonka, MN). A schematic illustration

of the experimental apparatus and a complete

description of modifications are provided elsewhere [27]. The crossflow membrane filter was

rated for operating pressures up to 6895 kPa

(1000 psi), and had channel dimensions of 14.6 cm,

9.5 cm, and 1.73 mm for channel length, width,

and height, respectively. Membrane surface area

was 1.39102 m2 and cross-sectional flow area

was 1.64104 m2.

3.3. Pure water permeability

At the start of each fouling experiment, de-

117

overnight at constant temperature of 25C to allow

for membrane compaction and other unknown

causes of flux decline inherent to laboratory-scale

recirculation systems. After stable flux was

achieved, pure water permeability was determined

by measuring pure water flux over a range of

applied pressures. The relationship governing the

pure water flux is

vw = Ap

(18)

from a linear regression of the measured pure

water flux and applied pressure data.

3.4. Concentration polarization, salt rejection and

osmotic pressure

After membrane permeability was determined,

an appropriate volume of stock NaCl solution was

added to provide the desired feed ionic composition. Flux and crossflow were set at the desired

values for each fouling experiment and the system

was allowed to equilibrate up to 24 h to ensure

stable performance. Temperature was maintained

at 25C by a recirculating chiller. Experiments

were conducted with 27 (333) combinations

of cb (10, 20, and 50 mol/m3 NaCl), p (689, 1034,

and 1379 kPa), and u (0.017, 0.042, and 0.068 m/s;

290, 590, and 1170 as Reynolds number) at

unadjusted pH of 5.8 0.2.

Due to concentration polarization of rejected

ionic constituents, the driving force for permeation

is the difference between the applied pressure (p)

and the transmembrane osmotic pressure (m).

During electrolyte equilibration, observed salt

rejection (Ro) was determined from feed (f) and

permeate (p) conductivity measurements (Ro = 1

p/f).Conductivity of NaCl solutions was

determined linear over the range of ionic strengths

used.

Intrinsic salt rejection (Ri = 1 cp/cw) was determined from the calculated salt concentration at

the wall (cw), and the measured permeate concen-

118

pressure was first calculated using Eq. (5). Then,

cw was calculated using the experimental permeate

concentration (cp) from the conductivity measurement as in Sutzkover et al. [28].

4. Results and discussion

4.1. Comparison of CP modulus predicted by

models

Prediction of observed salt rejection and permeate water flux at any applied pressure and

crossflow rate are dependent on the concentration

polarization modulus (=cw/cb), intrinsic salt rejection, and intrinsic water permeability. Once the

CP modulus, rejection, and permeability are known,

the channel averaged permeate flux may be predicted from Eqs. (5) and (6). Observed salt rejection is then predicted from the intrinsic salt rejection and known feed salt concentration. Hence,

the variable CP modulus combined with intrinsic

water permeability and salt rejection determines

RO process performance. Table 1 lists experimentally determined intrinsic salt rejections and

CP moduli, plus CP moduli predicted by the FT,

RS, and CD models.

According to results in Table 1, CP modulus

increases with increasing applied pressure, decreasing Reynolds number, and decreasing bulk

concentration. All model and experimental results

are in qualitative agreement. Higher applied pressure and lower crossflow rate make the CP modulus larger by increasing permeate convection and

decreasing shear rate (mass transfer), respectively.

At the same applied pressure and crossflow rate,

the permeate flux decreases with increasing bulk

concentration because the feed solution osmotic

pressure is larger. Salt rejection increased with

applied pressure and crossflow, but decreased with

increasing ionic concentration.

All three models underestimated the CP modulus at the lowest operating pressure. At the intermediate pressure, the FT and CD models were

quite accurate, but the RS model dramatically

FT and CD models overestimated the CP modulus,

whereas the RS model underestimated CP again.

All three models were increasingly accurate as

ionic concentration increased. At a given applied

pressure, the accuracy of all models improved at

higher crossflow.

The overall average prediction errors by the

FT, RS, and CD models were 4.0 10.4, 37.8

7.9, and 2.1 10.0%, respectively, where the

value represents the standard deviation of all percent differences. A negative percentage error

means that the average predicted value is smaller

than the experimental one. The RS model consistently underestimated the CP modulus by as

much as 51%, while the FT and CD models never

deviated by more than 29 and 26%, respectively.

The numerical CD model was most accurate, but

the predicted CP moduli by the FT model were

also quite reasonable.

4.2. Accuracy of models for predicting flux

The predictive accuracy of the FT, RS, and CD

models were tested by comparison to experimental

flux data. Fig. 2 shows channel averaged permeate

flux produced by model predictions and experimental measurements. For the FT model, the

channel averaged permeate fluxes were predicted

directly. For the RS and CD models, the channel

average fluxes were determined by integrating the

locally predicted permeate flux over the entire

channel. All predicted and measured flux data

increased as applied pressure increased, as Reynolds number increased , and as feed concentration

decreased. Higher applied pressures induce a

larger driving force for permeation. Higher Reynolds number flows enhance mass transfer, which

causes a smaller CP modulus and osmotic pressure

drop resulting in a larger relative permeate flux.

Increasing bulk salt concentration causes a higher

osmotic pressure drop, which results in a smaller

permeate flux.

As shown in Fig. 2, fluxes predicted by the FT

and CD model are quite close to the experimental

50 (1170) 94.1% 1.42 1.37 -3.5% 1.09 -23.2% 1.40 -1.4% 96.1% 1.70 1.72 1.2% 1.18 -30.6% 1.76 3.5% 97.1% 1.99 2.13 7.0% 1.35 -32.2% 2.17 9.0%

20 (1170) 95.9% 1.89 1.60 -15.3% 1.18 -37.6% 1.66 -12.2% 97.0% 2.17 2.12 -2.3% 1.33 -38.7% 2.19 0.9% 97.5% 2.54 2.73 7.5% 1.60 -37.0% 2.80 10.2%

10 (1170) 96.6% 2.43 1.73 -28.8% 1.22 -49.8% 1.80 -25.9% 96.9% 2.38 2.29 -3.8% 1.38 -42.0% 2.39 0.4% 97.3% 2.76 3.04 10.1% 1.71 -38.0% 3.13 13.4%

93.7% 1.48 1.41 -4.7% 1.10 -25.7% 1.44 -2.7% 96.0% 1.83 1.83 0.0% 1.23 -32.8% 1.87 2.2% 97.0% 2.23 2.30 3.1% 1.47 -34.1% 2.33 4.5%

CD % err

50 (590)

p = 1380 kPa

EX FT % err RS % err

95.9% 2.01 1.71 -14.9% 1.20 -40.3% 1.76 -12.4% 96.9% 2.39 2.32 -2.9% 1.42 -40.6% 2.39 0.0% 97.5% 2.87 3.07 7.0% 1.82 -36.6% 3.12 8.7%

Ri

20 (590)

CD % err

96.5% 2.57 1.86 -27.6% 1.25 -51.4% 1.96 -23.7% 97.0% 2.69 2.59 -3.7% 1.51 -43.9% 2.68 -0.4% 97.4% 3.21 3.53 10.0% 2.00 -37.7% 3.59 11.8%

p = 1035 kPa

EX FT % err RS % err

10 (590)

Ri

93.0% 1.62 1.54 -4.9% 1.15 -29.0% 1.57 -3.1% 95.4% 2.09 2.04 -2.4% 1.39 -33.5% 2.07 -1.0% 96.6% 2.72 2.67 -1.8% 1.82 -33.1% 2.67 -1.8%

% err

50 (290)

CD

95.7% 2.31 1.98 -14.3% 1.31 -43.3% 2.04 -11.7% 96.8% 2.97 2.85 -4.0% 1.76 -40.7% 2.89 -2.7% 97.5% 3.89 3.92 0.8% 2.51 -35.5% 3.88 -0.3%

p = 690 kPa

% err RS % err

20 (290)

EX FT

96.4% 2.91 2.27 -22.0% 1.39 -52.2% 2.34 -19.6% 96.9% 3.49 3.35 -4.0% 1.95 -44.1% 3.40 -2.6% 97.6% 4.68 4.89 4.5% 2.96 -36.8% 4.79 2.4%

Ri

10 (290)

c b (Re)

Table 1

Predicted and experimental CP moduli

119

120

28

24

RS model

Experiment

FT model

RS model

CD model

20

16

<

10 mol/m

<

20 mol/m

<

50 mol/m

Experiment,

FT model,

CD model

12

10 mol/m >

3

20 mol/m >

8

3

50 mol/m >

4

400

600

800

1000

1200

1400

1600

(a) Crossflow Reynolds number = 290

28

Experiment

FT model

RS model

CD model

24

<

10 mol/m

<

20 mol/m

<

50 mol/m

20

16

Experiment,

FT model,

CD model

12

10 mol/m >

20 mol/m >

50 mol/m >

4

400

600

800

1000

1200

(b) Crossflow Reynolds number = 590

1400

1600

28

Experiment

FT model

RS model

CD model

24

121

3

<

10 mol/m

<

20 mol/m

<

50 mol/m

1400

1600

20

16

Experiment,

FT model,

CD model

12

10 mol/m >

3

3

20 mol/m >

50 mol/m >

4

400

600

800

1000

1200

(c) Crossflow Reynolds number = 1170

Fig. 2. Channel averaged permeate fluxes determined experimentally (circles) and predicted (lines) by film theory (FT),

retained solute (RS), and convection diffusion (CD) models plotted as a function of applied pressure and salt concentration for crossflow Re of (a) 290 (b) 590 (c) 1170. Constant experimental and simulation conditions employed were

temperature and pure water permeability of 298 K and 2.151011 mPa1s1. Solution pH was 5.80.2.

appear significantly off scale. Although the slope

of pressure-flux predictions by the FT and CD

models is not identical to the experimental data,

the slope of RS model prediction gives a less

accurate slope. The average prediction errors of

the FT, RS, and CD models were 2.0 3.6,

21.9 12.1 and 0.5 3.6%, respectively. These

errors were less than those of the CP modulus

predictions. The CP modulus prediction errors

result in the deviation of predicted osmotic pressure from the real value. The osmotic pressure is

used to predict the channel average permeate flux

with the pure water permeability and transmembrane pressure using Eq. (5). When channel

average values are compared, the prediction errors

were significantly reduced. The FT and CD

models appear to be most accurate for the highest

most realistic set of conditions for practical RO

membrane desalination processes. It appears that

the FT and CD models reasonably predicted permeate flux of the experiments performed.

4.3. Accuracy of models for predicting rejection

Observed salt rejection cannot be predicted by

the RS model because it is an input parameter for

the model. The observed salt rejection may be determined experimentally or by a non-equilibrium

thermodynamic model [29]. Since the bulk concentration (cb) is an input for all models, observed

salt rejection (Ro = 1 cp/cb) is determined by predicting permeate concentration (cp). The permeate

concentration is determined from the product of

salt passage and the salt concentration on the

membrane surface, cp = (1 Ri) cw.

122

and CD models and was determined experimentally for every set of operation conditions simulated. Since the intrinsic rejection is known, the

observed salt rejection predictions are solely dependent on the accuracy of predictions of CP

modulus. In Figs. 3a and 3b the predictions of

observed salt rejection by the FT and CD models

are plotted against experimental data. The average

prediction errors of the FT and CD models were

0.2 0.1 and 0.3 0.9%, respectively. Hence,

1.0

(a)

FT model

0.9

0.8

0.7

0.6

0.6

0.7

0.8

0.9

1.0

0.9

1.0

Experiment

1.0

(b)

CD model

0.9

0.8

0.7

0.6

0.6

0.7

0.8

Experiment

Fig. 3. The comparison between experimental and observed salt rejection (Ro) by (a) film theory (FT) model

and (b) numerical convection-diffusion (CD) model. The

experimental and simulation conditions are the same as

those for Fig. 2.

give reasonably accurate prediction of salt rejection, as well as CP modulus and permeate flux.

4.4. Sources of errors in modeling CP, rejection

and flux

Potential sources for deviations between model

predictions and experimental results include entrance, exit, and side wall effects as well as density

differences for high salinity feed and low salinity

permeate solutions. For example, the entrance

length, over which a full developed parabolic flow

profile forms, is predicted by Lu = 0.08Reh,

where Re = u ( 2h ) / [30]. For Reynolds numbers

of 38, 191, 380 and 1910, Lu/L is 0.02, 0.09, 0.18

and 0.91 for the crossflow channel geometry used

in this study. Hence, the assumption of a fully

developed parabolic profile at the inlet is not satisfied for any experimentally employed conditions,

and is a source of common error for predictions

by all three models.

The analytical retained solute model is based

on a concept introduced by Song and Elimelech

[22] to describe particle concentration polarization

in membrane filtration processes. Use of the retained solute concept enabled analytical solution

of a two-dimensional convection-diffusion mass

balance applicable for crossflow membrane filtration. This approach worked well to predict the

limiting flux during ultrafiltration of nanoparticle

suspensions [31]. However, the RS model did not

accurately predict concentration polarization

phenomena for the reverse osmosis experiments

reported in this study. A possible explanation for

the inaccuracy of the retained solute model in

predicting concentration polarization is provided

below.

At the membrane surface, net solute mass

transfer by convection and diffusion is equal to

the solute flux through membrane, that is,

c

vw cw + D = vw c p

y y = 0

(19)

Eq. (19) can be transformed by substituting c = cb

+ C, where C is the excess solute concentration at

the membrane surface or the retained solute concentration, into Eq. (19) yielding

( cb + C )

vw ( cb + Cw ) + D

= vwc p

y

y =0

(20)

Here Cw is the excess concentration at the membrane surface. Since the bulk concentration (cb)

is constant, the derivative is zero.

Rearranging the left hand side of Eq. (20) and

applying the definition of retained solute, i.e.,

Eq. (8), yields

C

vw cb + vwC + D

= vw c p

y y = 0

(21a)

or

C

vw C + D

= vw c p vwcb

y y = 0

(21b)

mass balance for the concentration polarization

domain. According to Eq. (21b), this term does

not equal zero at the membrane surface (y = 0), as

specified in the development of Eq. (8), because

the bulk and permeate concentrations are significantly different and non-negligible in RO

separations. This means that Eq. (8) cannot be used

as a boundary condition at the membrane surface.

However, the assumption that Eq. (8) is true

just at the membrane-solution interface is the key

step in deriving an analytical solution to the

integral in Eq. (9) and, ultimately, arriving at the

closed form analytical solution. The assumption

is acceptable if the bulk and permeate concentrations are approximately equal and if both are

negligible compared to the concentration at the

membrane surface (wall) as is the case for

123

However, in RO separations the solute wall concentration is only slightly elevated over the bulk;

hence, the bulk concentration is not negligible.

The lack of mass conservation is likely the primary

source of error in predictions by the RS model;

however, the retained solute model does more

realistically simulate the fundamental interplay

between permeation, crossflow, rejection, and

concentration polarization than does film theory.

Thus, the retained solute model offers significant

conceptual insight into concentration polarization

phenomena in all crossflow membrane processes.

4.5. Applicability of film theory for RO processes

Film theory models are widely preferred by

process engineers for their simplicity and reasonable performance predictions. The data of Figs. 2

and 3 demonstrates that the film theory model

predicts permeate water flux and salt rejection

nearly as well as a more rigorous numerical convectiondiffusion model. For the experimental

conditions tested, the FT model was less accurate

than the CD model at low fluxes, but slightly more

accurate at the higher fluxes examined for all

crossflows and salt concentrations. Although this

is counter-intuitive, the film theory neglects the

effect of solute permeation through the membrane,

which may suppress the boundary layer thickness

at high fluxes.

Since film theory has been shown to give

reasonable predictions of CP, flux, and rejection,

it is of interest to further compare the FT and CD

models across an array of operating conditions,

membrane properties, and solution chemistries

likely to be encountered in real applications. In a

new set of simulations, constant conditions assumed were temperature, water permeability (A), and

salt rejection (Ri) of 298 K, 1.121011 mPa1s1,

and 97%. Table 2 summarizes the simulation conditions that were varied and Fig. 4 compares channel averaged permeate flux and observed salt

rejection data predicted by both models.

124

Table 2

Simulation conditions for the comparison of FT and CD models

#

Re

p, kPa

cb, mol/m3

30

10

11

38

912

50

191

912

50

380

912

50

1910

912

50

191

576

50

191

1580

50

191

2930

50

191

912

10

191

912

100

191

912

500

191

912

1000

1.0

(a)

(b)

25

FT model

FT model (m/s)

0.9

20

15

10

0.8

0.7

5

0

10

15

20

25

30

0.6

0.6

0.7

0.8

0.9

1.0

CD model

CD model (m/s)

Fig. 4. The comparison between the film theory (FT) and the numerical convection-diffusion (CD) model predictions for

(a) channel averaged permeate flux and (b) observed salt rejection. Constant simulation conditions employed were temperature, water permeability, and salt rejection of 298 K, 1.121011 mPa1s1, and 97%. Table 2 summarizes the simulation conditions that were varied. Crossflow hydrodynamics were varied within the laminar range (Re < 2100).

the laminar range (Re < 2100). Permeate fluxes

employed were in the range frequently used in

real operations and higher. Salt concentrations

ranged from fresh water conditions to about twice

the molarity of seawater. Permeate flux and observed salt rejection data predicted by both models

are well-matched according to the data in Fig. 4.

Overall there was a difference of 3.5 2.8%, where

the FT model consistently over predicted the permeate flux and salt rejection because it under predicted the CP modulus.

4.6. Using film theory to predict local concentration polarization

Accurate prediction of local concentration

reverse osmosis processes because, for example,

it enables prediction of the onset of scaling by

sparing soluble minerals. The FT model may be

used to predict the local concentration polarization

modulus, cw/cb, via

cw ( x )

v ( x )

= 1 Ri + Ri exp w

cb ( x )

k ( x )

(22)

by the CD model, k(x) is the local mass transfer

coefficient predicted by Eq. (3), and cw(x) and cp(x)

denote local wall and permeate concentration,

respectively.

CD model was used as an input for CP modulus

predictions by the FT model because film theory

can not predict the local flux and CP modulus independently. It is more common to assume a constant permeation velocity when applying film

theory to RO processes; however, this has no effect

on the local film layer thickness, but does subtly

influence the local solute rejection. Also, simulations were performed for the geometry of the lab

scale filter used in the experiments of this study.

Hence, the assumption of a constant bulk concentration introduces little error because the recovery

in this system ranges from about 0.11.0%.

Clearly, a separate mass balance for the axially

varying retentate concentration must be performed

for systems with significant recovery [26].

Figs. 5 and 6 describe local CP modulus (cw(x)/

cb) predicted by FT and CD model for various

inlet permeate fluxes and crossflow Reynolds

numbers. The difference between each predicted

factor increases as the initial flux at the membrane

12

11

CP modulus (cw/cb)

10

9

125

decreases (Fig. 6). Film theory works well when

CP factor is small (e.g., higher crossflow Reynolds

number and lower operating pressure). At permeate fluxes below 7.5410 6 m/s (~16 gfd,

gallons per square foot per day), the FT model

accurately predicts local concentration polarization. The key source of error at higher fluxes

relates to independence of the boundary layer

thickness from permeation. Considering most RO

applications employ fluxes smaller than 7.54

106 m/s, it appears reasonable to apply film theory

based concentration polarization models.

5. Conclusions

A two dimensional, numerical convectiondiffusion mass balance model was developed to

enable more fundamental description of concentration polarization phenomena in reverse osmosis

processes. Predictions by two analytical concentration polarization models and the numerical

p

FT model CD model

576 kPa

912 kPa

1580 kPa

2930 kPa

8

7

6

5

4

3

2

1

0.0

0.2

0.4

0.6

0.8

1.0

x/L

Fig. 5. Prediction of local CP moduli depending on different applied pressures using the film theory (FT) and the numerical convection-diffusion (CD) models. Constant simulation conditions employed were temperature, water permeability,

and salt rejection of 298 K, 1.121011 mPa1s1, and 97%. Simulation conditions employed were combinations #2, 5, 6,

and 7 in Table 2. Crossflow hydrodynamics were varied within the laminar range (Re < 2100).

126

CP modulus (cw/cb)

Re FT model CD model

38

190

380

1900

1

0.0

0.2

0.4

0.6

0.8

1.0

x/L

Fig. 6. Predicted local CP moduli depending on different crossflow Reynolds numbers using the film theory (FT) and the

numerical convectiondiffusion (CD) models. Constant simulation conditions employed were temperature, water permeability, and salt rejection of 298 K, 1.121011 mPa1s1, and 97%. Simulation conditions employed were conditions 14

in Table 2.

model were compared to experimental RO separation performance data. The three models allowed

the prediction of local solute concentration polarization, permeate water flux, and permeate salt concentration given inputs of operating parameters,

filter geometry, and membrane properties. Predictions by film theory and the numerical convectiondiffusion model compared favorably to experimental data and to each other, providing accurate and consistent predictions of observed water

flux and salt rejection. An important result of this

study is the validation of film theory as a simple

and reliable indicator of concentration polarization

phenomena in reverse osmosis separations, particularly for mechanistic studies of fouling and

scaling conducted in laboratory scale crossflow

membrane filters. Further, the use of film theory

based concentration polarization models in real

RO processes appears justified given the specific

operating conditions of high crossflow and low

flux used in most practical applications.

Acknowlegements

The research described above was performed

while Dr. Suhan Kim was a postdoctoral fellow

at University of California, Riverside. Partial

financial support for this work was obtained

through a post-doctoral fellowship from the Korea

Science and Engineering Foundation (KOSEF) for

Dr. Kim. Additional support was obtained from

the California Department of Water Resources

through the Desalination Research Innovation

Partnership (DRIP), which is managed by the

Metropolitan Water District of Southern California.

Symbols

A

C

cb

cp

Concentration of retained solute, molm3

Solute concentration in the bulk, molm3

Solute concentration in the permeate,

molm3

cw

molm3

D Solute diffusion coefficient, m2s1

dH Channel hydrodynamic parameter, m

F Dimensionless driving force

fos Osmotic coefficient, Pamol1

h

Channel half-height, m

k

Mass transfer coefficient, ms1

k Channel averaged mass transfer coefficient, ms1

L

Channel length, m

Ns Dimensionless membrane resistance

p

Pressure, Pa

Q Axial flow rate, m3s1

R Universal gas constant,

= 8.314 Jmol1K1

Ri Intrinsic salt rejection of membrane

(e.g., Ri = 1 cp/cb)

Ro Observed salt rejection (e.g., Ro = 1

cp/cb)

r

Distance from center line of a rectangular channel, m

Re Reynolds number (e.g., Re = ud H / )

Sc Schmidt number (e.g., Sc = v/D)

Sh Sherwood number [e.g.,Sh = kd H / D =

1.85 (ReScdH/L)1/3]

T

Absolute temperature, K

u

Axial components of velocity filed, ms1

u Bulk average crossflow velocity, ms1

umax Maximum crossflow velocity at channel

center, ms1

v

Transverse components of velocity filed,

ms1

vw Permeate water flux, ms1

X Dimensionless longitudinal distance,

xL1

x

Axial coordinate, m

x Dummy integration variable

y

Transverse coordinates, m

Greek

m

Feed conductivity, Sm1

p

w

127

Wall shear rate, s1 (e.g., w = 3u / h )

Viscosity of water, Nsm2

Kinematic viscosity of water, m2s1

Osmotic pressure difference between

feed and permeate sides of the membrane,

Pa (e.g., 0 = fos (cb cp) = fosRocb)

m Transmembrane osmotic pressure, Pa

References

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