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Desalination

journal homepage: www.elsevier.com/locate/desal

in ultraltration

Debasish Sarkar a, Debojyoti Chakraborty b, Mithu Naskar a, Chiranjib Bhattacharjee b,

a

Department of Chemical Engineering, University of Calcutta, Kolkata, India

b

Department of Chemical Engineering, Jadavpur University, Kolkata, India

H I G H L I G H T S

Performance characterization of the module in ultraltration of BSA

Average permeate ux enhancement is 0.06 10 6 m3 m 2 s 1 per unit kPa rise of TMP.

Mathematical model to predict the steady permeate ux

Maximum absolute deviation of the model is well within 7%.

a r t i c l e i n f o a b s t r a c t

Article history: Design, characterization and modeling of a novel radial ow membrane (RFM) module is reported in the present

Received 31 March 2014 study. The module has been investigated in ultraltration of bovine serum albumin (BSA) with a 30 kDa

Received in revised form 16 September 2014 polyethersulphone (PES) membrane under steady state. The proposed semi-empirical, steady state model was

Accepted 17 September 2014

validated under different parametric conditions of transmembrane pressure and bulk concentration. The

Available online xxxx

model may be viewed as an extension of the well known osmotic pressure model in conjugation with

Keywords:

SpieglerKedem black box model and a system specic, steady state solute balance equation. Model empiricity

Ultraltration was introduced primarily to account for unknown entranceexit effects and effects of membrane roughness on

Radial ow hydrodynamic prole. The empirical parameter was evaluated by minimizing a global objective function. The

Steady state maximum absolute deviation of the model with respect to the experimental data of permeate ux was found

Mathematical model to be well within 7%.

Permeate ux 2014 Elsevier B.V. All rights reserved.

Rejection

eld assisted ltration have been proposed to counter fouling phenom-

Membrane separation technology is an energy efcient downstream enon. Recently, in a review article, Hilal et al. [12] have presented a root

process either to separate valuable components from an intermediate cause analysis and necessary remedial techniques of fouling in details. It

process stream or to treat the far downstream efuents in order to has been also established that to limit the membrane fouling, concen-

meet the discharge standards [13]. However, rapid ux decline due tration polarization must be reduced to its lowest possible threshold

to (i) reversible concentration polarization and (ii) irreversible mem- [13].

brane fouling restrict the growth of membrane based techniques as an It is well recognized that high membrane shear arrests the growth of

alternative to the conventional energy intensive separation processes. polarized layer and the therefore enhances the permeate ux. To create

These non idealities triggers higher energy consumption and addition- a high membrane shear, it is necessary to circulate the uid at high

ally reduce the effective membrane life [4]. In general, concentration po- speed i.e. in the range of 36 m s1 [14] in a standard cross ow module.

larization can be partially controlled by the use of periodic pulsation, This leads to a higher pumping cost. Over the last two decades, different

electric eld, gas sparging or ultrasound [510]. On the other hand, types of cross ow modules with varied geometry and/or shear enhanc-

membrane fouling is a complicated physicochemical phenomenon, ing accessories were proposed [1520]. Alternative to passive enhance-

which leads to an irreversible loss of membrane permeability [11]. ment strategies, active use of external force elds, for example

ultrasound to enhance the permeate throughput are also reported [21,

Corresponding author. 22]. Dynamic shear enhanced (DSE) modules, which consist of rotating

E-mail address: cbhattacharyya@chemical.jduv.ac.in (C. Bhattacharjee). or reciprocating parts like rotating, spinning or vibrating disks and/or

http://dx.doi.org/10.1016/j.desal.2014.09.020

0011-9164/ 2014 Elsevier B.V. All rights reserved.

D. Sarkar et al. / Desalination 354 (2014) 7686 77

membranes were introduced in late 1980s to further intensify the 0.045 m) was operable in the pH range of 210 and temperature range

membrane shear independent of feed ow rate [2327]. However, the of 554 C.

specic membrane surface area (m2 m3) of even the most advanced

DSE module is practically insignicant compared to the standard cross 2.2. Filtration system

ow units. For example, in a typical plate and frame module (the oldest

cross ow unit commercialized), the surface to volume ratio is around The present module was designed to ensure smooth radial ow of

350500 m1, whereas the same for the well known hollow ber mod- the feed over a at circular membrane. Therefore, the corresponding ki-

ules is as high as 700013,000 m 1 [28,29]. Naturally the permeate nematic pattern must either be source or sink ow type. The primary

throughput becomes much higher in cross ow devices compared to drawback of sink ow is the heavy impact of incoming radial jets over

the equivalent DSE units of same size. Instead of several advantages, en- the central region. This may create ow reversal and may hinder the

hanced axial pressure drop in a cross ow module leads to a progressive outow of the retentate. Accordingly, source ow type feed inlet and

reduction of transmembrane pressure. Therefore, it is necessary to retentate withdrawal system was chosen for the present work. Fig. 1

introduce a cross ow design with reduced pressure drop so as to opti- represents the sectional view of the module along with the snapshots

mize the membrane area usage in terms of uniform TMP distribution. of the membrane holder and the top lid. The membrane holder is a per-

It is well known that in a radial ow channel with central inlet and forated disk through which permeates ows out. This also acts as a me-

peripheral outlet (source ow type), the pressure drop is lower than a chanical support of the membrane. Permeate can be collected through a

rectangular/cylindrical conduit of same internal volume and surface radial tube tted below the holder. The feed is delivered to the module

area. Based on this idea, the present work has been undertaken in an at- through a central opening on the top lid. Just below the opening, a circu-

tempt to develop and characterize a radial ow module in ultraltration lar impingement plate of 0.016 m radius (ri) is xed to top lid in order to

of bovine serum albumin (BSA). Moreover, a semi-empirical model was avoid the feed jet impact on the membrane. Essentially, the feed enters

proposed to simulate the present radial ow membrane (RFM) module the module through a narrow channel of 0.001 m depth between the

under steady state. impingement plate and the top lid. The retentate ows out of the mod-

ule through nine peripheral holes of diameter 0.005 m, drilled through

2. Materials and methods the lid. The clearance between the top lid and the membrane (zt) is

0.014 m, as shown in Fig. 1. An O-ring was used to x the membrane

2.1. Materials over the porous membrane holder. This eventually reduces the effective

diameter of the membrane diameter (ro) to 0.041 m. For the present

Bovine serum albumin (BSA) with an average molecular weight work, the RFM module, made of SS-316 was fabricated by Concept

of 66,000 g mol 1 was supplied by E. Merck, Mumbai, India. Moist, International, Kolkata, India as per the specied design. SS-316 was

semi-permeable, asymmetric polyethersulphone (PES) membrane selected as the material of construction.

with a molecular weight cut off (MWCO) of 30 kDa was obtained from The schematic of the entire ltration bench is shown in Fig. 2. The

Spectrum Medical Industries (USA). The at disk membrane (diameter: feed tank is tted with a coolant circulation system. The feed is

Fig. 1. Sectional view of the radial ow membrane (RFM) module (insert showing the photograph of the module internals).

78 D. Sarkar et al. / Desalination 354 (2014) 7686

design (CCRD) was carried out because CCRD takes all the curvatures

of the response surface i.e., parametric interactions into account [31].

Thirteen experimental runs were performed with varying TMP (223.31

to 368.69 kPa) and feed concentration (5.86 to 34.14 kg m3). Corre-

sponding data of permeate ux were used to determine an adjustable

parameter of the proposed model as discussed later. Additionally, in

order to extract the dependence of permeate ux on TMP and C0 over

an extrapolated parametric space, 25 experimental runs were designed

with varying TMP (196.2, 244.6, 294.3, 347.4 and 392.4 kPa) and feed

concentration (5, 10, 20, 30 and 40 kg m3). One parameter at a time

was subjected to variation, while the other was held constant to extract

the true nature of the dependence. A constant retentate ow rate of

6.4 10 6 m3 s 1 was maintained throughout all the experimental

runs in order to restrict the number of effective process parameters

within two. The operating temperature of the present study was

30 1 C. Each experiment was conducted in triplicate to ensure

repeatability.

3. Theoretical development

The main objective of the model is to simulate the steady state var-

iations of three major process variables, namely (i) the permeate ux

( J) (ii) radially averaged membrane surface concentration C m and

(iii) the permeate concentration (CP) with the applied transmembrane

pressure (TMP) and feed concentration (C0). Therefore, three simulta-

n o

neous equations of the form f i J; C m ; C P 0 are necessary.

Fig. 2. Schematic of the ltration bench. i1; 3

From the well known osmotic pressure model [32] and the Spiegler

delivered to the module by a single acting piston pump. The TMP and Kedem black box formulation of the membrane based on irreversible

the ow rate can be adjusted by operating the back pressure regulator thermodynamics [33], two simultaneous equations, out of three, may

(BPR) and the bypass valve (V1) respectively. be directly obtained. In order to get the third equation, a steady state

solute balance within the concentration boundary layer is to be derived.

2.3. Analysis The assumptions made for the model formulation are as follows:

1. The ow is steady, incompressible and turbulent.

The concentration of BSA in BSA/water solution was measured by a 2. Solute concentration is independent of angular coordinate (),

Hitachi dual beam UVvisible spectrophotometer (Model No. U-2800, i.e. C = C(r, z).

tted with UV solution software) by the principle of absorbance assay 3. Feed and retentate are Newtonian uids. This assumption may be

at 280 nm [30]. The solution pH was monitored by a Systronix make justied in terms of dilute feed concentration (=40 kg m3).

digital pH meter. 4. Diffusive transport of solute along radial direction is negligible com-

pared to convection.

2.4. Experimental procedure 5. Axial permeation velocity is small enough compared to the radial

velocity.

Prior to all experimental runs, the membrane was subjected to water 6. Concentration boundary layer is well within the viscous sub layer of

compaction nearly for 2 h at a transmembrane pressure (TMP) of 600 the fully developed momentum boundary layer.

kPa, which is higher than the highest operational TMP of the present

study. This was followed by the actual experimental runs. Permeate 3.1. Steady state concentration prole

ux was measured by the direct method. According to this method,

for a permeate volume of V, collected over a xed time interval t, For solute with low diffusivity (like BSA in the present study),

Schmidt number (Sc) is quite large and since c Sc3 , thickness of

1

the respective ux value may be calculated as J A1 Vt , where A is the ef-

fective membrane surface area. Flux values were recorded at an internal the concentration boundary layer becomes negligible compared to the

of 10 min. Essentially t 10 min. The observed rejection, dened as momentum boundary layer. Considering assumptions 5 and 6, the

Ro 1 CC P0 , where C0 is the feed concentration, was calculated measur- axial velocity component (vz) within the thin concentration boundary

ing the corresponding steady state permeate concentration (CP) of a layer may be regarded equal and opposite to the permeate ux [34] as

specic run. A particular run was continued until three successive ux the z axis is vertically upward (Fig. 1). So

readings were equal. Once an experimental run was over, the mem-

brane was thoroughly cleansed with distilled water to remove any de- vz J: 1

posits. The water ux was checked again to ensure the same hydraulic

resistance of the membrane. For all the runs, the feed solution was pre- On the other hand, the radial velocity component (r) may be

pared and maintained at the neutral pH, far from the isoelectric point of expressed in terms of free stream radial velocity (V0) and the dimen-

BSA (pH 4.71). This was done in order to reduce the solute adsorption sionless axial distance from the membrane ( z/) according to the

led irreversible membrane fouling. Solute concentration in the feed approximate formulation proposed by Lin [35]:

tank was continuously monitored and make-up solution was periodi-

cally added to maintain C0 at its set point.

In order to extract the dependence of permeate ux on two process

r V 0 f : 2

parameters, namely the TMP and C0, a 22 central composite rotatable

D. Sarkar et al. / Desalination 354 (2014) 7686 79

However, for the present study, the velocity prole expression is Substituting the velocity components, vr and vz from Eqs. (6) and (1)

required only within the viscous sub layer (assumption 6). From the respectively, the following form is obtained:

universal velocity prole of turbulent ow [36], the radial velocity

distribution within the viscous sub layer can be expressed as a linear 1 Az C 2 C

C J D 2: 8

function of z: r r r z z

r : 3

(i) at r r i ; C C 0 for all z 9a

Analytical expression of the wall shear stress (w) for a conned C

radial jet has been reported by Glauert as a function of V0 and [37]. (ii) at z c ; 0 for all r 9b

z

The proposed form was exactly in accordance with the well known Z r

Blasius law [37]: 1 0

(iii) z 0 ; C C m 2 2 C r; z2rdr 9c

r 0 ri ri

0:25

2

w 0:0225V 0 : 4

V 0

where C m is the radially averaged membrane surface concentration.

Since the thickness of concentration boundary layer is practically negli-

Using this expression, the variation of turbulent boundary layer gible compared to the same of its hydrodynamic counterpart, variation

thickness () with the radial distance was solved by Watson [38] as of the radial velocity component along the axial direction may be

1 neglected. Accordingly, the axially averaged radial velocity, vr over the

14zt =5 concentration boundary layer can be calculated as

0:205 r: 5

Q

Z c

1

vr r vr z; r dz: 10

Combining Eqs. (3), (4) and (5) and noting that V 0 Q c

2rzt , the ex- 0

Using the expression of vr(z, r) as in Eq. (6), vr may be expressed as

z

vr r; z A 2 6 A c

r vr : 11

0:84 2 r2

where A 7:97 103 Q z Q

. To develop the solute concentration

t

c

As c Sc3 , the nal working form of vr can be obtained using

1

prole in the RFM module, an annular control volume between

[r, r + r] and [z, z + z] is considered as shown in Fig. 3. Neglecting Eq. (5), after introducing an empirical correction factor (k) as

the diffusive transport along radial direction (assumption 4), the steady 1

state solute mass balance over the differential control volume yields Ak zt 5 1 13

vr Sc : 12

2 Q r

C C

C2rzvr jr C2rzvr jrr D 2rzD 2rr

z z z zz It may be noted that in the present module, the effective membrane

vz Cjz 2rrvz Cjzz 2rr 0 7 radius is only 0.041 m. Therefore, the entrance and exit effects cannot be

1 rvr C C 2 C fully neglected. However, incorporation of these effects in the respective

vz D 2: momentum balance equation gives rise to severe complication, such

r r z z

that the analytical solution of the velocity prole becomes impossible.

The relation between wall shear stress and hydrodynamic boundary

layer thickness, as in Eq. (4) is generally accepted, but in case of mem-

brane separation processes, w is reported to be additionally dependent

on membrane roughness, porosity and on entranceexit effects [39]. Ac-

cordingly, the correction factor k, as used in Eq. (12), may be inferred to

compensate for the errors introduced due to (i) entrance-exit effects,

(ii) effects of membrane properties (roughness, porosity) on velocity

prole and (iii) lack of coefcient data in the relation between c

and . So the nal expressions of pertinent velocity components, to be

used in the solute mass balance equation are

vz J 13a

and

a

vr 13b

r

1

zt 5 13

where a Ak

2 Q Sc . Using these expressions, Eq. (7) may be

modied to a much simpler form compared to Eq. (8), which is as

follows

Fig. 3. Different incoming and outgoing uxes over the annular shell between r to r + r 1 aC C 2 C

J D 2: 14

and z to z + z (not in scale). r r z z

80 D. Sarkar et al. / Desalination 354 (2014) 7686

h

The respective boundary conditions remain unchanged, as in Eq. (9). Combining Eqs. (19) and (20) m C m and P = (CP), whereas

Eq. (14) can be solved by the standard variable separation method. The

= m P], the equation of the desired functional form, f 2

solution can be represented as

J; C m ; C P ; 0 is obtained.

C r; z m2 e 2e 1 e 15 1 9:22 10

3

C m C P

m1 RT 4

1 P 5 C m C P

m1 5 2

MW 3:01 10 C m C m C P C P 2

J 0

p

p

Rm

J J 4D

2

J

J 2 4D

where m1 2D m2 ; 2D . is equivalent to the single 21

effective eigen value of Eq. (14). It may be noted that can be evaluated

using the following equation, which is an outcome of the third boundary

condition (Eq. (9c)). 3.4. SpieglerKedem black box model: Formulation of f 3 J;C m ; C P ; 0

h 2 2 i

Permeate ux for UF, NF and RO membranes can be described by the

2aC 0 e2ar0 ri 1 m z m m z

Cm e 2 t 2 e 1 t 16 standard SpieglerKedem black box model [33]. The model relates the

2 2 m m1

r 0 r i 1 2 real rejection (Rr) to the permeate ux through solute permeability

m1 (PS) and osmotic reection coefcient () as process parameters

CP 1 F

Rr 1 22

However, C m is unknown

n beforehand. Sooin order to solve for , three Cm 1 F

equations of the form f i J; C m ; C P 0 ; i 1; 3 as stated previ- n o

ously, are required. where, F exp 1

P

J

. Eqs. (16), (18), (21) and (22) can be simulta-

S

3.2.

Solute mass balance at the membrane surface: Formulation of

different parametric conditions of TMP and feed concentration (C0).

f 1 J;C m ; C P ; 0

4. Simulation technique

Under steady state, the net solute ux through the membrane must

be balanced by the Fickian back diffusion ux. Accordingly, the solute

4.1. Estimation of process parameters

balance equation at the membrane surface becomes

C ical values of different process parameters (appearing in Eqs. (16), (18),

J C m C P D 17

z (21) and (22)), which are D, Rm, , Ps, , and k.

z0

The solute diffusivity (D) may be evaluated by the following empir-

r

ical correlation [41].

where, C C z 1

0 C r; z2rdz is the radially averaged solute

r20 r2i ri 1

9

concentration at any D 2:74 10 M Pol3 23

axial location. Combining Eqs. (15), (16) and (17),

the nal form of f 1 J; C m ; C P ; 0 is as under

For BSA, the average molecular weight is around 67,000 g mol1. Ac-

r2

cordingly the diffusivity was estimated to be 6.74 1011 m2 s1,

2A

i

Dm2 C 0 e m z m z

e2A 0 i 1 e 1 t e 2 t :

2

r r

2

which is fairly close to the respective diffusivity value reported by

J 18

m2 2 2 Opang and Zydney [42]

1 r 0 r i

m1 2A The osmotic reection coefcient () and solute permeability (PS)

were evaluated by the well known iterative method of Nakao and

Kimura [43]. For the present solutemembrane combination the values

were found to be 0.894 and 2.47 107 m s1 respectively.

3.3. Osmotic pressure model: formulation of f 2 J;C m ; C P ; 0 The hydraulic resistance of the membrane was determined by

making a series of water runs with the present radial ow cell after

In any standard UF process, the osmotic pressure at the membrane allowing the initial membrane compaction. The mean Rm, estimated to

surface cannot be neglected because of high polarization effects. So be 1.69 1012 m1 from different experimental runs, was used in the

the permeate ux may be evaluated by the phenomenological equation present study. The density and viscosity of BSAwater solution depends

of osmotic pressure model [32], described as primarily on the solute concentration.

The reported correlations at 30 C [40], as used in the present study

are as follows

P

J 19

Rm 4 0 2 3 3

1:00021 2:856 10 C 10 kg m 24

sistance of the membrane. Regarding the evaluation , the following 0

4 0 2 3

0:94 0:21C 1:329 10 C 10 Pa s: 25

empirical correlation of as a function of solute concentration (BSA as

used in the present study) is used [40]

The hydrodynamic parameter (k), introduced to account for

(i) entrance-exit effects, (ii) effects of membrane properties on velocity

RT 3 2 5 3

prole and (iii) lack of coefcient data in the relation between c and

C 9:22 10 C 3:01 10 C : 20

MW was impossible to estimate analytically. Therefore, the same was

D. Sarkar et al. / Desalination 354 (2014) 7686 81

estimated by minimizing the sum of the mean square error between the 5. Results and discussion

experimental and model predicted permeate ux values under different

parametric conditions. Accordingly, the model may be regarded as a 5.1. Fixing the adjustable parameter (k)

single-adjustable parameter, semi-empirical, steady state model of the

present RFM module. The only adjustable parameter of the model (k) was evaluated by

minimizing the global objective function, dened in Eq. (26). It was

4.2. Simulation algorithm found that a single k value of 0.37 resulted in a minimum E(k) =

6.24 10 4 (dimensionless), which is the average of normalized

The simulation scheme to obtain the steady state values of permeate square error for 13 experimental data points according to the CCRD

ux (J), membrane surface concentration C m and permeate concen- scheme. The parameter (k) was introduced in the velocity prole equa-

tion primarily to account for the entranceexit effects and the effects of

tration (CP), under different parametric conditions is shown in Fig. 4.

membrane properties on velocity prole as mentioned earlier. There-

Eqs. (16), (18), (21) and (22) are simultaneously solved using the stan-

fore, k must be primarily dependent on TMP and on C0 to some extent.

dard predictorcorrector Newton method with a suitable tolerance. As

The present module was fed through a narrow channel of thickness

mentioned previously, the only adjustable parameter of the model, k

0.001 m, where from the radial jet had to suddenly expand over the

was determined by minimizing the following global objective function

full axial span of zt. At the outlet, the retentate ow was again subjected

E(k), dened as

to a sudden contraction from zt to the diameter

of the peripheral holes,

!2 i.e., 0.005 m. As axial to radial span ratio r0 zr

t

i

of the present module

1X n

J i;model was 0.56, the entrance and exit effects must be dependent on the re-

Ek 1 26 spective TMP. Effects of feed concentration on entrance and exit velocity

n i1 J i;exp

proles might be negligible. On the other hand, a change in C0 would

lead to a change in membraneuid interaction through density and

where, n is the total number of data points marked by different TMP viscosity effects. So in true sense, the parameter k is inferred to be

and C0. It is evident from the denition that the function E(k) actually dependent on TMP and C0. However, the dependence was weak; other-

represents the sum of the normalized square error between the exper- wise a single adjusted k value would not have resulted into a minimum

imental and model predicted permeate ux over the entire parametric E(k) of 4.08 104. In order to conrm the nature of the dependence,

space of the present study. The direct search technique with accelera- the same k value (= 0.37) was used to simulate the permeate ux,

tion [44] was used to determine the optimum value of the parameter membrane surface concentration and permeate concentration over an

k. A small tolerance limit of 0.001 for E(k) was used as a stop criterion extrapolated parametric space marked by TMP [196.2 kPa, 392.4

of direct search algorithm. C m C 0 , CP = 0, J P

Rm

C 0

, = 1 and kPa] and feed concentration [5 kg m3, 40 kg m3]. Over the extrap-

k = 1 were the initial values/guess values used in the present study. olated space, E(k) was found to be 6.24 104, which clearly conrms

the apprehended nature of dependence. The contribution of end effects

(entrance and exit effects) or the effects of membrane roughness on k

cannot be predicted separately because of the gross empiricity inbuilt

in the denition of the same parameter.

at different bulk concentration. As evident from the osmotic pressure

model, the permeate ux was observed to increase with TMP. On the

other hand, because of higher osmotic pressure differential, the ux

exhibits a decreasing trend with C0. In both of the cases, the variation

J

was nearly linear. For example, at C0 = 20 kg m3, TMP was found to

be 5.89 107 m3 m2 s1 kPa1 over the TMP range of [196.2 kPa,

294.3 kPa], whereas the same was 5.02 10 7 m3 m 2 s 1 kPa1

over the next higher range i.e. [294.3 kPa, 392.4 kPa]. Similar trend

was observed with respect to C0, though the respective prole was

slightly nonlinear. As a result, the contour plot of the steady permeate

ux becomes marginally nonlinear (Fig. 5 insert). This is exactly consis-

tent with the trends predicted by osmotic pressure model. According to

Eq. (19), the steady ux has to be a linear function of TMP, provided ,

and Rm remains constant. However, is nonlinear in terms of C m and

C m is supposed to increase in a complex, nonlinear fashion with C0. This

may be attributed to the phenomenon of concentration polarization. It

is well known that any UF process is marked by the presence of severe

polarization resulting a sharp concentration gradient between the

membrane surface and bulk uid. Hence the average membrane surface

concentration (C m ) must be a nonlinear function of C0. Subsequently,

the permeate ux becomes essentially nonlinear with respect to C0.

Still the degree of nonlinearity is pretty low, as indicated by the contour

plot. This may be explained once again in terms of osmotic pressure

model in conjugation with the empirical functionality between

and C (Eq. (20)). Eq. (20) reveals that the ratio of quadratic to

Fig. 4. Flow chart showing the steady state simulation scheme for permeate ux, linear term is in the order of 102 C. As the experimental range of C0

membrane surface concentration and permeates concentration of RFM module. was 540 kg m3 of BSA in the present study, which may be marked

82 D. Sarkar et al. / Desalination 354 (2014) 7686

Fig. 5. Variation of the steady state permeate ux with TMP at different bulk concentration (inserts showing (i) contour plot of J as a function of TMP and C0 and (ii) parity diagram of

experimental and model predicted permeate ux).

as lower side values of C0, the contribution of quadratic term becomes variation of Rr with TMP at different C0 over the extrapolated parametric

negligible compared to the linear one. Essentially the steady ux may space, as mentioned earlier is shown in Fig. 6. As expected, the real re-

be justied to be a nearly linear function of C m . On the other hand, the jection shows an increasing trend both with TMP and C0. For example,

nonlinearity between C m and C0 is negligible at low C0 owing to a at C0 = 5 kg m3, real rejection was observed to increase from 0.78 to

small thickness of the polarized layer. As a consequence, variation of 0.82 (=5.1%) for a change of TMP from 196.2 kPa to 392.4 kPa. Similarly

the steady ux with respect to TMP and C0 becomes approximately at TMP = 392.4 kPa, the same quantity exhibits an increase of 13.2%

linear as indicated by the contour plot (Fig. 5). with a change of C0 from 5 to 40 kg m3. In standard ultraltration pro-

The parity diagram, as shown in the insert of Fig. 5, other than the cesses, at increased TMP and/or C0 the solute rejection increases rapidly

contour plot, clearly points out that the proposed model can predict leading to a growth of the polarized layer.

the variation of steady ux with TMP and C0 with reasonable accuracy. The layer acts as an additional mass transfer resistance promoting

A closer investigation reveals that the average value of the normalized further growth. However, the monotonicity levels off to a steady state

s

2

n J

value due to the tangential velocity led membrane shear and the Fickian

j1 1 iJj:model back diffusion. Generally in a cross ow module, the membrane shear is

standard deviation, dened as n1

i j;exp

for the present

primarily dependent on the feed/retentate ow rate. Similarly in the

study was found to be 0.025, which is well within the acceptable limit. 9

present module, a monotonic relation between w and Q (w Q 5 )

may be established from Eqs. (4) and (5). It is to be noted that the

5.3. Steady state real rejection as a function of TMP and C0 present study was conducted at a xed retentate ow rate of Q =

6.4 10 6 m3 s 1. Effect of C0 on w through may be assumed to

Real rejection, as described by Eq. (22) is an important parameter be negligible small as the study was conducted with dilute feed solution

to characterize the performance of any membrane separation unit in (C0 : 5 to 40 kg m3). Additionally, w has got no specic functional

general. Compared to the observed rejection, dened as Ro 1 CC P0 dependence on TMP, which can be justied from Eqs. (4) and (5). There-

(where, C0 is the bulk uid concentration), real rejection is not marked fore, a negligibly small variation of w over the parametric range of the

by the phenomenon of concentration polarization and hence indicates present study may be conrmed. On the other hand, the solute rejection

the true separation efciency of the membrane. The model predicted by the membrane surface, due to the higher rate of transport from the

D. Sarkar et al. / Desalination 354 (2014) 7686 83

Fig. 6. Model predicted real rejection as a function of TMP at different C0 (inserts showing the variation of experimental and model predicted permeate concentration with TMP at

different C0).

bulk is expected to increase monotonically with TMP and C0. Accordingly whereas only 18% change of CP was observed for C0 change from 30

the approximate linear increasing trend of Rr with the two process param- to 40 kg m 3.

eters of the present study becomes evident as indicated by Fig. 6.

In order to establish the validity of the proposed model, experimental

5.4. Variation of the effective eigen value equivalent term of Eq. (9)

CP values were compared with the corresponding model predictions at

different TMP and C0. Insert of Fig. 6 illustrates the respective variations

The parameter , equivalent to the effective eigen value of Eq. (9),

with TMP at different C0. For all the experimental data points, the nor-

s

2 was obtained by solving Eqs. (16), (18), (21) and (22) along with J, C m

n

j1 1 CPiPij;model

C

and Cp. was observed to be strongly dependent on TMP and C0. There-

malized standard deviation, dened as C P n1

j;exp

, was fore, may be represented as function of these two parameters. In order

as low as 0.078, which clearly indicates the validity of the proposed to decipher the respective functional form, response surface methodol-

model. The gure also reveals that CP exhibits a sluggish exponential ogy (RSM) was adopted with the previously mentioned 22 central com-

growth with TMP at different bulk concentrations. The trend may be ex- posite rotatable design (CCRD). Standard regression models, which

plained in terms of growth saturation of the polarized layer at higher side include (i) linear, (ii) quadratic, (iii) 2FI, and (iv) cubic were tested to

values of TMP. However, the growth saturation does not mean a constant represent the response () as a function of independent/regressor vari-

mass transfer resistance, with respect to the solvent (water) as well as ables. The software package of Design Expert (version 8.0) was used for

the solute. For solvent, it may attain a constant value, leading to a near the present RSM analysis. From the t summary, multivariable quadrat-

linear increase of solvent ux (J) with TMP. But in case of the solute, ic regression model was chosen to be the optimum in representing the

the resistance may go on increasing, exactly counter balancing the effect variation of . Cubic and quartic models were also tested to t the

of enhanced driving force (TMP). For example, at TMP = 196.2 kPa, present data, though the test parameters did not show any signicant

C P has increased by 129% for a change of C 0 from 5 to 10 kg m 3 , improvement over the chosen quadratic model. The corresponding

Fig. 7. (a) Parity diagram of for quadratic regression model. (b) Contour plot of as a function of TMP and C0.

84 D. Sarkar et al. / Desalination 354 (2014) 7686

parity diagram, as shown in Fig. 7(a) also justies model selection. The shear rate arrests the growth of the polarized solute layer and thereby

nal working equation of , as a function of TMP and C0 becomes increases the permeate ow. Naturally, the permeate ux is expected

to be higher in any DSE modules compared to the most advanced

4

2:28757 0:037577 TMP0:40838 C 0 6:00 10 TMP cross ow unit. However, the specic ltration areas of DSE modules

6 2 3 2

C 0 6:73907 10 TMP 8:70657 10 C0: 27 are insignicant in relation to the simplest cross ow modules. For ex-

ample, the specic surface area of the reported RDM modules is only

The model F value of 2079.4 implies the model is signicant. More- 3.62 m2 m 3, whereas the same for the present RFM module is

over, high values of R2 (=0.99) as well as adjusted R2 (=0.99) repre- 60.55 m2 m3. Therefore, the gross permeate ow becomes higher in

sent the gross validity of the regression model. It is well known that case of cross ow devices. On the other hand, in case of electric eld en-

R2 always increases as more terms are added to the model, whereas ad- hanced cross ow ltration, the maximum steady state permeate ux

justed R2 statistic often decreases upon adding unnecessary terms. For was reported to be 4.44 105 m3 m2 s1 at a TMP of 635 kPa [47],

the present model, up to two decimal places equality of R2 and adjusted which is only 11.1% higher than the maximum ux of the present

R2 conrms the presence of signicant terms only. Moreover, adequate study. For air sparged ultraltration experiments, using a tubular mem-

precision (signal to noise ratio N 4 is desirable) of 140.583 suggests that brane module with human serum albumin (HSA) as the test media, the

the model equation can be used to navigate the entire parametric space. reported maximum value of permeate ux was 7.3 105 m3 m2 s1

So the overall predictive capability of the quadratic regression model [48], though the bubble size and frequency have strong inuence on the

based on these criteria seems to be quite satisfactory. The contour permeate ux. From the foregoing discussion, it becomes clear that the

plot, representing the variation of is shown in Fig. 7(b). However, a performance of the proposed RFM module is comparable with other

complete characterization of the response cannot be done only with cross ow and DSE units. Moreover, the RFM module is devoid of the

the contour/response surface plots. Therefore a more formal canonical complicated internal arrangements necessary for gas sparging, electric

analysis was carried out to reveal the true nature of the response. The eld or rotating membrane.

model equation (Eq. (27)) may be represented in a more compact form

T

b0 Xb XBX 23 6. Conclusion

" #

b12

b11 The present investigation illustrates the design, performance charac-

where X = [TMP C 0] T , b = [b1 b 2] and B b12

2 . The eigen

2 b22 terization and modeling of a new cross ow module. The module has

values of the matrix B for the present system are [0.0001 0.0087] T. been named as radial ow membrane (RFM), owing to the directional-

ity of ow. In the present study, bovine serum albumin (BSA) was sep-

This implies that the response surface must pass through a mini- arated from its synthetic aqueous solution using the present module

1

hmum, though the corresponding

i stationary point, Xs 12 B b tted with polyethersulfone (PES) membrane of 50 kDa MWCO. The

3

7177:5 kPa 223:9 kg m is far outside the region of exploration. steady state performance of the proposed module was investigated

under different transmembrane pressure (TMP) and feed concentration

5.5. Performance comparison with other membrane modules (C0). A maximum permeate ux of 4.0 105 m3 m2 s1 was obtain-

ed at TMP = 392 kPa C0 = 5 kg m3. In general, an average permeate

A legion of studies on ultraltration of BSA and using different mod- ux enhancement of 0.06 10 6 m3 m 2 s 1 per unit kPa rise of

ules with different types of membrane was reported. Performances of TMP was recorded over the parameter range of the present study. Addi-

some of them in terms of operating conditions and the respective steady tionally, a single parameter, semi-empirical model was proposed to

state permeate ux are reviewed here in comparison to the proposed simulate the RFM module. The only adjustable parameter of the pro-

RFM module and are presented in Table 1 [40,4548]. Amongst the posed model was introduced primarily to account for the unknown

other studies, the highest permeate ux as reported by Sarkar et al. entranceexit effects and the effects of membrane properties (rough-

[40] was 2.0 10 4 m 3 m 2 s 1 in the ultraltration of BSA ness, porosity) on velocity prole. The respective parameter was

using a standard rotating disk-membrane (RDM) module. This is evaluated by minimizing a global objective function equivalent to the

followed by the permeate ux obtained from a single stirred cell sum of the normalized square error between the experimental and

(= 11.11 10 5 m 3 m 2 s 1 ) [46]. It may be noted that both the the model predicted permeate ux under steady state. The maximum

studies were conducted in standard DSE modules in which membrane absolute deviation of 7% establishes the gross validity of the model in

shear can be increased independent of feed ow rate. The enhanced simulating the steady state performance of the RFM module.

Table 1

Comparison of the proposed RFM module with the reported DSE and cross ow modules in terms of permeate ux.

(m3 m2 s1)

Standard cross ow cell C0: 20 kg m3 Polyamide/BSA 1.25 105 Wang and Tang [45]

TMP: 1240 kPa

Stirred cell C0: 0.6 kg m3 Polysulfone/BSA 11.11 105 Gell and Davis [46]

TMP: 71 kPa

Electric eld enhanced rectangular C0: 0.11.5 kg m3 Polyphenylene ethersulfone/BSA 4.44 105 Sarkar et al. [47]

cross ow channel TMP: 220635 kPa

Velocity: 0.060.18 m s1

Electric eld: 01000 V m1

Tubular cross ow module with air C0: 4.5 kg m3 Polyvinylidene uoride/human 7.3 105 Li et al. [48]

sparging facility TMP: 101.32 kPa serum albumin (HAS)

Rotating disk-membrane module C0: 130 kg m3 Polyethersulphone/BSA 2.0 104 Sarkar et al. [40]

TMP: 294882 kPa

Stirrer speed: 5.230.9 rad s1

Membrane speed: 5.230.9 rad s1

Radial ow membrane module C0: 540 kg m3 Polyethersulphone/BSA 4.0 105 Present study

TMP: 196.2392 kPa

D. Sarkar et al. / Desalination 354 (2014) 7686 85

Nomenclature p permeate

a parameter dened by Eq. (13b) pol polymer

A parameter dened by Eq. (6) 0 bulk

B coefcient matrix dened by Eq. (23)

b vector dened by Eq. (23)

b0 parameter dened by Eq. (23) Superscript

C solute concentration (kg m3)

C' solute concentration (gm cm3) T transpose

C average solute concentration (kg m3)

Cm average membrane surface concentration (kg m3)

CP permeate concentration (kg m3)

C0 feed concentration (kg m3) References

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