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*

B.V. Babu and Suresh Gupta

Department of Chemical Engineering

Birla Institute of Technology & Science

Pilani 333031 (Rajasthan) India

Abstract

The kinetic behavior of a fixed-bed adsorber can be explained and the characteristic breakthrough curve of

the adsorption phenomena can be obtained through mathematical models. In the earlier models, the

kinetics is explained using a mathematical model that takes into account of external and internal masstransfer resistances with a nonideal plug flow behavior. The variation of fluid velocity along the column is

an important aspect, which has not been accounted so far. In the present study, a mathematical model is

proposed for explaining the kinetic behavior of adsorption phenomena incorporating the fluid velocity

variation along the column length also. Internal mass-transfer resistances due to pore diffusion mechanism

are considered in the model. The proposed mathematical model for fixed-bed adsorption is solved

numerically and compared with earlier model reported in literature. The results show that the breakpoint is

obtained earlier which represents the realistic behavior in adsorption phenomena. Initially the sharp front of

the breakthrough curve is seen followed by broadening of tail of the breakthrough curve. Simulations are

carried out using the present model for a systematic parametric study. The effects of various important and

influencing parameters such as flow rate, bed height, inlet adsorbate concentration and particle diameter on

breakthrough curve are studied in detail.

Keywords: adsorption; modeling; pore diffusion control; breakthrough curve; mass transfer

1. Introduction

Use of adsorption contacting systems for industrial and municipal wastewater treatment

has become more prevalent during recent years [1]. The process of adsorption of the

components of a fluid mixture flowing through a packed bed of an adsorbent porous

material is the basis of several important applications in chemical engineering. These

include continuous separation processes for large-scale applications such as bulk

separations [2], and also chromatographic processes for both analytical and preparative

purposes [3]. As a consequence of this applicative interest, a great amount of work has

been devoted to the modeling of these processes [4].

* Corresponding Author: Assistant Dean - ESD & Head of Chemical Engineering Department, B.I.T.S.,

PILANI-333031 (Rajasthan) INDIA.

Email: bvbabu@bits-pilani.ac.in;

Home Page: http://discovery.bits-pilani.ac.in/discipline/chemical/BVb/index.html;

Phone: +91-01596-245073 Ext. 205 / 224;

Fax: +91-01596-244183;

Nomenclature

aP

Cb

Cs

Cbo

DL

DP

kf

column length, m

qm

qs

radial coordinate, m

time, sec

Vo

Vi

axial coordinate, m

Greek letters

bed porosity

The key parameters for design of an adsorption system are the process parameters that are

used for modeling the system for predicting the quality of effluent under a wide range of

operating conditions [5]. In most of the large-scale processes, relatively large porous

particles (50-1,000 m in diameter) are used to reduce pressure drop and sorbent cost.

Intraparticle diffusion is usually the rate-limiting step in these systems and it controls the

sharpness of breakthrough curves [6]. One of these models describes diffusion as the

mechanism occurring in the fluid phase with a distributed adsorption along the pore

walls, i.e., the pore diffusion model [7]. For low-affinity solutes in macroporous sorbents,

pore diffusion is usually the dominant intraparticle diffusion mechanism [8].

Pore diffusion model has been used for predicting the kinetics of fixed bed adsorption

process [6,9,10,11]. These models take account of both external and internal masstransfer resistances as well as of nonideal plug flow along the column. The above models

have not incorporated the fluid velocity variation along the bed, which makes a

significant effect on breakthrough curve. In the present work, the effect of operating

variables on the process of fixed-bed adsorption is studied. Furthermore, the kinetics is

studied using a mathematical model that takes account of both external and internal masstransfer resistances, nonideal plug flow along the column and the variation of fluid

velocity along the column.

2. Mathematical Modeling

Before discussing the assumptions needed for model formulation, we first introduce the

physical process considered in this model. Convection along the column axial direction

and axial dispersion are the mass transport mechanisms in the bulk phase. Molecules

from the bulk interstitial phase are transported via axial convection and Fickian diffusion

(film diffusion) onto the particle surface. Inside the particle, molecules can diffuse into

the inner portion of particle via surface diffusion, pore diffusion, or both. This study

focuses on understanding the mechanism in pore diffusion.

Bautista et al. [9] proposed the kinetic mechanism for the adsorption of -amylase from

Aspergillus oryzane in a fixed bed. The model takes account of both external and internal

mass-transfer resistances as well as of nonideal plug flow along the column. They did not

consider the fluid velocity variation along the bed to predict the behavior of breakthrough

curve. In the present study this model is modified by considering the variation of velocity

along the column.

To formulate a generalized model corresponding to the pore diffusion mechanism,

following assumptions are made:

1. The system operates under isothermal conditions.

2. The equilibrium of adsorption is described by Langmuir isotherm, a nonlinear

isotherm.

3. Intra-particle mass transport is due to Fickian diffusion, and it is characterized by the

pore diffusion coefficient, DP.

4. Mass transfer across the boundary layer surrounding the solid particles is

characterized by the external-film mass transfer coefficient, kf.

5. The linear velocity of the liquid phase varies along the column.

6. The macro porous adsorbent particles are spherical and homogeneous in size and

density.

Based on the preceding assumptions, for the control volume, Adz (Figure 1), for limiting

situation z

DL

2C

q

C

C

p

b +V

b + C V + b + 1

=0

b z

p

z

t

t

z 2

(1)

V

C b ( z , t ),

dz

Cb +

C b

z

(C bV )

dz ,

z

C b

2C b

+

dz

z

z 2

C b = C bo

z = 0, t = 0

(2)

Cb = 0

0 < z L, t = 0

(3)

The contour conditions at both ends of the column are given by the following equations

DL

C b

= V0 (C bo C b ), z = 0, t > 0

z

C b

= 0,

z

(4)

z = L, t 0

(5)

The following equation was used to estimate (dV/dz), the variation of velocity of bulk

fluid along the axial direction of the bed. For liquid adsorption, assuming the liquid

density to be constant, then the total mass balance gives

q p

V

= (1 ) s

z

t

(6)

V = V0 ,

z = 0, t > 0

V

= 0,

t

(7)

z = L, t > 0

(8)

q p

t

3k f

(C b C s )

ap

(9)

The intra-pellet mass transfer is due to the diffusion of adsorbate molecules through the

pore. The macroscopic conservation equation is given as

c

q

2 c 2 c

+ (1 p ) p

= Dp

+

t

t

r 2 r r

(10)

q c q

=

t t c

(11)

c

=

t

1

1 P q

1 + p

P c

DP

2 c 2 c

+

r 2 r r

(12)

c = 0, q = 0,

0 < r < ap , t = 0

(13)

The symmetry condition at the center of the particles and continuity condition on the

external surface of the adsorbent bed are expressed as

c

= 0,

r

k f (C b C s ) = Dp

c

,

r

r = 0, t > 0

(14)

r = ap , t > 0

(15)

The adsorption isotherm was favorable and nonlinear, and it described by Langmuir

isotherm

q=

q m bc

1 + bc

(16)

differential equations (1 to 16) is solved numerically by a reduction to set of ordinary

differential equations using the Explicit Finite Difference technique. Finite difference

technique has successfully applied to solve such type of partial differential equations in

other studies by Babu and Chaurasia [12,13,14,15,16,17]. A mathematical algorithm to

solve these coupled equations is developed and implemented into a computer program

using MATLAB (v.6.1) software. The same parameters reported by Bautista et al. [9] are

used for simulation in present study, which are given in Table 1.

3. Results and Discussion

The model used, as described above, determines the outlet adsorbate concentration at

different times based on different operating conditions. In the present model, linear

velocity variation along the bed is considered and the obtained results are compared with

the previous model given by Bautista et al. [9]. Same parameters given by Bautista et al.

Parameter

Value

0.58

0.53

p,

1970

b,

900

l,

1000

5.9 x 10-10

45.4

0.84

2.5 x 10-11

1.5 x 10-6

d, Bed diameter, m

0.016

[9] are used and some parameters (see Table 1) are assumed which are not given in

literature. The present model results show an improvement over the previous model given

by Bautista et al. [9] with respect to better steepness of the breakthrough curve which is

being validated by earlier study [6,18]. The results show that the breakpoint is obtained

earlier (Figure 2). Initially the sharp front of the breakthrough curve is seen followed by

broadening of tail of the breakthrough curve as shown in Figure 2 [18]. These obtained

results are more justifiable with theoretical phenomena occurring in the adsorption

system. The fluid velocity along the bed is a decreasing function of bed length [18]. The

velocity continuously decreases inside the bed with respect to bed length. This

phenomenon is validated by the mass balance (Eq. 6) for velocity variation.

This

establishes the fact that the effect of velocity variation on breakthrough curve is

significant. This fact is also in agreement with the results reported in the literature [18].

Based on the successful implementation of velocity variation in the model, and

supporting evidence in the literature, the simulations are carried out using the present

model to carryout a systematic parametric study. The present model is studied by varying

the different important parameters such as flow rate, bed height, inlet adsorbate

concentration and particle diameter.

1.0

0.8

with velocity variation

Cb/Cbo

0.6

0.4

0.2

0.0

0

2000

4000

6000

8000

Time (sec)

Figure 2: Breakthrough curve with and without fluid velocity variation

for a velocity of V=0.0020 cm/sec

The results for different solution flow rates are plotted for a bed height of 0.163 m and an

inlet adsorbate concentration of 1 mg/ml in Figure 3. The flow rates considered are 0.25,

0.5 and 1.0 ml/min. Figure 3 reveals that as the flow rate increases from 0.25 to 1.0

ml/min, the breakthrough curve becomes steeper. The break point time decreases from

1600 to 750 sec without considering the velocity variation along the bed and 1150 to 500

sec with velocity variation. This is because of the residence time of the solute in the

column, which is not long enough for adsorption equilibrium to be reached at high flow

rate. So at high flow rate the adsorbate solution leaves the column before equilibrium

occurs. Furthermore, a fixed saturation capacity of bed based on the same driving force

gives rise to a shorter time for saturation at higher flow rate. As the flow rate is 0.25

ml/min, the break point time is 1600 sec without considering velocity variation and 1150

sec with velocity variation along the bed. The percentage change in break point time is

28%. For the flow rates 0.5 and 1.0 ml/min, the percentage change in breakpoint time

(that is a ratio of difference between breakpoint time without velocity variation and with

velocity variation to the maximum breakpoint time obtained) are 17% and 15%,

respectively. This shows as the flow rate increases the velocity variation effect on

breakthrough curve decreases.

1.0

0.8

Q = 0.25 ml/min

Q = 0.25 ml/min(*)

Q = 0.5 ml/min

Q = 0.5 ml/min(*)

Q = 1.0 ml/min

Q = 1.0 ml/min(*)

Cb/Cbo

0.6

0.4

0.2

0.0

0

2000

4000

6000

8000

Time (sec)

(*) indicates model results with velocity variation

The effect of bed height on the effluent adsorbate concentration is presented for flow rate

of 0.25 ml/min and inlet adsorbate concentration of 1 mg/ml in Figure 4. The bed heights

considered are 0.163 and 0.20 m. It is observed that as the bed height increases from

0.163 to 0.20 m, the break point time increases from 1600 to 3475 sec without

considering the velocity variation and 1150 to 2625 sec with velocity variation along the

bed. This shows that at smaller bed height the effluent adsorbate concentration ratio

increases more rapidly than for a higher bed height. Furthermore, the bed is saturated in

less time for smaller bed heights. Smaller bed height corresponds to less amount of

9

adsorbent. Consequently, a smaller capacity for the bed to adsorb adsorbate from solution

and a faster increase in rate of adsorbate adsorption is expected. For the bed height of

0.163 m, the break point time is 1600 sec without considering velocity variation and 1150

sec with velocity variation along the bed. The percentage change in break point time is

13%. The percentage change in breakpoint time is 24% for bed height of 0.20 m. This

shows as the bed height increases the velocity variation effect on breakthrough curve

increases.

1.0

0.8

L = 0.163 m

L = 0.163 m(*)

L = 0.20 m

L = 0.20 m(*)

Cb/Cbo

0.6

0.4

0.2

0.0

0

2000

4000

6000

8000

Time (sec)

Figure 4: Effect of bed height on breakthrough curve

(*) indicates model results with velocity variation

The two-inlet adsorbate concentrations considered are 0.5 and 1.5 mg/ml. During these

simulations other parameters such as bed height and flow rate are kept constant. It is

observed that as the inlet adsorbate concentration increases from 0.5 to 1.5 mg/ml, the

break point time decreases from 2525 to 2275 sec without considering the velocity

variation and 1875 to 1575 sec with velocity variation along the bed. For larger feed

concentration, steeper breakthrough curves are found, because of the lower mass-transfer

10

flux from the bulk solution to the particle surface due to the weaker driving force. In

addition, at high concentration, the isotherm gradient is lower, yielding a higher driving

force along the pores. Thus the equilibrium is attained faster for values of higher

adsorbate concentration. For the inlet adsorbate concentration of 0.5 mg/ml, the break

point time is 2525 sec without considering velocity variation and 1875 sec with velocity

variation along the bed. The percentage change in break point time is 26%. The

percentage change in breakpoint time is 28% for inlet adsorbate concentration of 1.5

mg/ml. This indicates that as the inlet adsorbate concentration increases, there is no

significant effect of the velocity variation on breakthrough curve.

1.0

0.8

Cbo = 0.5 mg/ml(*)

Cbo = 1.5 mg/ml

Cbo = 1.5 mg/ml(*)

Cb/Cbo

0.6

0.4

0.2

0.0

0

2000

4000

6000

8000

Time (sec)

Figure 5: Effect of inlet adsorbate concentration on breakthrough curve

(*) indicates model results with velocity variation

The effect of particle size on effluent concentration is shown in Figure 6. The particle

radii considered are 3.1 x 10-4, 4.1 x 10-4 and 6.1 x 10-4 m. During these simulations other

parameters such as flow rate, bed height, and inlet adsorbate concentration are kept

constant. Figure 6 reveals that as the particle radius increases from 3.1 x 10-4 to 6.1 x 10-4

11

m, the steepness of the breakthrough curve decreases. The break point time increases

from 1325 to 2050 sec without considering the velocity variation and 975 to 1450 sec

with velocity variation along the bed. Smaller particle size resins provide quicker kinetic

equilibrium and therefore better breakthrough capacity is obtained at higher linear

velocities. This allows faster cycle times with no reduction in the resin capacity. As the

diameter of the particle increases, the thickness of stagnant film around the particles

increases, and also the total length of the path inside the pores increases. Under these

conditions, the overall kinetics of the process is slow, because the time for a molecule of

adsorbate to reach the adsorption site is more, as the diffusional path along the pores is

large. As the particle radius is 3.1 x 10-4 m, the break point time is 1325 sec without

considering velocity variation and 975 sec with velocity variation along the bed. The

percentage change in break point time is 17%. For the particle radii 4.1 x 10-4 and 6.1 x

10-4 m, the percentage change in breakpoint time is 22% and 29%, respectively. This

shows as the particle radius increases the velocity variation effect on breakthrough curve

increases.

1.0

0.8

aP = 3.1 x 10-4 m

aP = 3.1 x 10-4 m(*)

aP = 4.1 x 10-4 m

aP = 4.1 x 10-4 m(*)

aP = 6.1 x 10-4 m

aP = 6.1 x 10-4 m(*)

Cb/Cbo

0.6

0.4

0.2

0.0

0

2000

4000

6000

Time (sec)

Figure 6: Effect of particle radius on breakthrough curve

(*) indicates model results with velocity variation

12

8000

4. Conclusions

A generalized model that incorporates external film mass transfer resistance and pore

diffusion resistance with velocity variation through column bed has been formulated and

solved numerically. Following conclusions are drawn from the above-discussed results:

1.

curve, wherein the break point is obtained earlier. Initially the sharp front of the

breakthrough curve is seen followed by broadening of tail of the breakthrough

curve.

2.

As the flow rate is increased, the breakthrough curve becomes steeper. The break

point time is obtained earlier and effluent adsorbate concentration ratio increases

more rapidly.

3.

For smaller bed height, the effluent adsorbate concentration ratio increases more

rapidly than for a higher bed height.

4.

For larger feed concentration, steeper breakthrough curves are obtained and break

point time is achieved sooner.

5.

With decrease in particle radius, the breakthrough curve becomes steeper and the

break point time decreases.

These results improve the understanding of adsorption phenomena with reference to pore

diffusion, and are very useful in the design of adsorption columns.

References

[1]

[2]

[3]

[4]

[5]

B.V. Babu, S. Gupta, Modeling and Simulation for Dynamics of Packed Bed

Adsorption, Proceedings of International Symposium & 57th Annual Session of

IIChE in association with AIChE (CHEMCON-2004), Mumbai, December 27-30,

2004.

D.M. Ruthven, and C.B. Ching, Counter-current and simulated counter-current

adsorption separation processes, Chemical Engineering Science, 44 (1989) 10111038.

G. Ganetsos, P.E. Barker, Preparative and Production Scale Chromatography,

Marcel Dekker, New York, 1993.

K. Kaczmarski, M. Mazzotti, G. Storti, M. Morbidelli, Modeling fixed-bed

adsorption columns through orthogonal collocations on moving finite elements,

Computers and Chemical Engineering, 21 (1997) 641-660.

B.V. Babu, V. Ramakrishna, Dominant Design Variables and Modeling

Parameters for Adsorption in Batch Studies, Proceedings of International

13

[6]

[7]

[8]

[9]

[10]

[11]

[12]

[13]

[14]

[15]

[16]

[17]

[18]

(CHEMCON-2004), Mumbai, December 27-30, 2004.

Z. Ma, R.D. Whitley, N.H.L. Wang, Pore and Surface Diffusion in

Multicomponent Adsorption and Liquid Chromatography Systems, AIChE

Journal, 42 (1996) 1244-1262.

T.W. Webi, R.K. Chakravort, Pore and Solid Diffusion Models for Fixed-Bed

Adsorbers, AIChE Journal, 20 (1974) 228-238.

E. Furuya, Y. Takeuchi, K.E. Noll, Intraparticle Diffusion of phenols within

Bidispersed Macroreticular Resin Particles, J. Chem. Eng. Japan, 22 (1989) 670L.F. Bautista, M. Martinez, J. Aracil, Adsorption of -Amylase in a Fixed Bed:

Operating Efficiency and Kinetic Modeling, AIChE Journal, 49 (2003) 2631-2641.

S. Ghorai, K.K. Pant, Investigations on the column performance of fluoride

adsorption by activated alumina in a fixed-bed, Chemical Engineering Journal, 98

(2004) 165-173.

J.L. Sotelo, M.A. Uguina, J.A. Delgado, L.I. Celemin, Adsorption of methyl ethyl

ketone and trichloroethane from aqueous solutions onto activated carbon fixed-bed

adsorbers, Separation and Purification Technology, 37 (2004) 149-160.

B.V. Babu, A.S. Chaurasia, Modeling, Simulation, and Estimation of Optimum

Parameters in Pyrolysis of Biomass, Energy Conversion and Management, 44

(2003) 2135-2158.

B.V. Babu, A.S. Chaurasia, Modeling for Pyrolysis of Solid Particle: Kinetics and

Heat Transfer Effects, Energy Conversion and Management, 44 (2003) 2251-2275.

B.V. Babu, A.S. Chaurasia, Parametric Study of Thermal and Thermodynamic

Properties on Pyrolysis of Biomass in Thermally Thick Regime, Energy

Conversion and Management, 45 (2004) 53-72.

B.V. Babu, A.S. Chaurasia, Dominant Design Variables in Pyrolysis of Biomass

Particles of Different Geometries in Thermally Thick Regime, Chemical

Engineering Science, 59 (2004) 611-622.

B.V. Babu, A.S. Chaurasia, Pyrolysis of Biomass: Improved Models for

Simultaneous Kinetics & Transport of Heat, Mass, and Momentum, Energy

Conversion and Management, 45 (2004) 1297-1327.

B.V. Babu, A.S. Chaurasia, Heat Transfer and Kinetics in the Pyrolysis of

Shrinking Biomass Particle, Chemical Engineering Science, 59 (2004) 1999-2012.

D.M. Ruthven, Principles of Adsorption and Adsorption Processes, John Wiley &

Sons, New York, 1984.

14

Profiles of Authors:

Dr B V Babu is Professor & Head of Chemical Engineering Department apart from

being Assistant Dean of Engineering Services Division (ESD) at Birla Institute of

Technology and Science (BITS), Pilani. His biography is included in 2005 & 2006

editions of Marquis Whos Who in the World, and Thirty-Third Edition of the Dictionary

of International Biography in September 2006.

guided 2 PhD students, 25 ME Dissertation students and 24 Thesis students and around

160 Project students. He is currently guiding 7 PhD candidates, 3 Dissertation students

and 10 Project students. He currently has 3 research projects from UGC & DST.

His research interests include Evolutionary Computation (Population-based search

algorithms for optimization of highly complex and non-linear engineering problems),

Environmental Engineering, Biomass Gasification, Energy Integration, Artificial Neural

Networks, Nano Technology, and Modeling & Simulation.

He is the recipient of many National and International awards, and the Life member of

various professional bodies such as IIChE, ISTE, IE, IEA, SOM, Fellow of ICCE, and

Associate Member of ISSMO.

He has around 102 research publications (International & National Journals &

Conference Proceedings) to his credit. He completed three consultancy projects. He is a

Panel Expert for www.chemicalhouse.com. He has published three books and has written

several chapters in various books and lecture notes of different intensive courses.

He was the Invited Chief Guest and delivered the Keynote addresses at one international

conference and three national seminars. He organized many Seminars & Conferences,

and member of various academic and administrative committees at BITS-Pilani. He also

chaired 10 Technical Sessions at various International & National Conferences. He

delivered 23 invited lectures at various IITs and Univeristies.

He is Editorial Board Member of two International Journals Energy Education Science

& Technology and Research Journal of Chemistry and Environment. He is the referee

& expert reviewer of 15 International Journals, and on the Programme Committees as an

expert reviewer at 12 International Conferences. He reviewed three books of McGraw

Hill, Oxford University Press, and Tata McGraw Hill publishers. He is PhD Examiner

for one candidate and PhD Thesis Reviewer for 3 Candidates.

and currently pursuing his PhD under the supervision of Prof B V Babu. He has 3

publications to his credit. He is associate life member of IIChE.

15

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