Gas Absorption With RST Order Chemical Reaction in A Laminar Falling LM Over A Reacting Solid Wall PDF

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Applied Mathematical Modelling 32 (2008) 901–929

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Gas absorption with first order chemical reaction in a

laminar falling film over a reacting solid wall
M. Danish *, R.K. Sharma, S. Ali
Department of Chemical Engineering, Aligarh Muslim University, Aligarh, UP, India
Received 1 December 2005; received in revised form 1 November 2006; accepted 16 February 2007
Available online 12 March 2007
Abstract
In the present work, a general case of gas absorption with first order irreversible chemical reaction in a liquid film, for
laminar flow over a solid wall, has been analyzed theoretically. First order chemical reaction between the diffused solute
and the wall is also considered. Laplace transform followed by power series method has been applied to solve the govern-
ing equations. Thereafter, the obtained analytical solution of the developed general model has been successfully verified by
an explicit numerical scheme. The general model has also been reduced to six simplified cases, tackled by previous workers
and an excellent agreement in the solutions is observed. Moreover, the results are validated by the experimental data avail-
able in the literature. The obtained concentration profiles in both the phases have been used to find the absorption rates
and enhancement factor.
Further, the effect of various parameters on concentration profile of solute, enhancement factor and eigen-values have been
analyzed. Existence of positive eigen-values for the counter-current absorption is also described which was not pointed out by
any of the previous researchers. It is concluded that in a co-current system, for Hatta number greater than 7 approximately, the
variation in enhancement factor follows a linear trend on a log–log plot and that there is no effect of rate constants for higher
values of Hatta number. It is further shown that the reaction at solid wall has appreciable effect on the absorption rate.
2007 Published by Elsevier Inc.
Keywords: Absorption; Falling film; Chemical reaction; Mass transfer; Enhancement factor; Laplace transform
1. Introduction
Physical and chemical gas absorption is one of the most important separation processes and is widely
employed in chemical and allied industries either for separating undesirable components from a gas or for
the manufacturing purposes of some important chemicals. Generally, the former one is due to the stringent
environment norms, set nowadays and the latter one is the requirement of industry either for quality or design
purposes. Because of these vital reasons, a vast amount of theoretical as well as experimental research material
is available and still increasing.
*
Corresponding author. Tel.: +91 5712721152; fax: +91 5712700042.
E-mail address: mdanish77@rediffmail.com (M. Danish).
0307-904X/$ - see front matter 2007 Published by Elsevier Inc.

doi:10.1016/j.apm.2007.02.019
902 M. Danish et al. / Applied Mathematical Modelling 32 (2008) 901–929
Nomenclature
Ai series coefficients for the solution of dimensionless concentration in the liquid film
an nth coefficient of the series solution
B dimensionless gas phase or surface resistance parameter equivalent to Biot number for mass
transfer
Bi series coefficients for the solution of dimensionless concentration in the gas phase
Ca concentration of the solute A in the liquid phase, g/cm3
CA dimensionless concentration of the solute A in the liquid phase
CA Laplace transform of CA
c0 1st term in series solution of CA corresponding to k0 ¼ 0
C0 dimensionless solute concentration in the entering liquid
C a0 solute concentration at gas liquid interface, g/cm3
C A0 dimensionless solute concentration at gas–liquid interface
Cg concentration of the solute A in the gas phase, g/cm3
C g0 initial gas phase concentration of the solute A, g/cm3
CG dimensionless gas phase concentration of the solute A
CG Laplace transform of C G
DAB diffusion coefficient of solute A in the liquid phase, cm2/s
DAG diffusion coefficient of solute
A in the gas phase, cm2/s
E enhancement factor RR0
1
Fi series coefficients for the solution of absorption rate
f series function of g
kG mass transfer coefficient for infinitesimally small gas liquid interface, cm/s
k1 rate constant for 1st order chemical reaction in liquid film, 1/s
k2 rate constant for 1st order chemical reaction at solid wall, cm/s 2
d
K1 dimensionless rate constant for first order chemical reaction in the liquid film kD1AB
K2 dimensionless
rate constant for first order chemical reaction between solute and dissolving solid
wall Dk 2ABd
log logarithm of a quantity on base10
m the amount of gas absorbed qper unit area after a contact time s, g/m2
ffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
pffiffiffiffiffiffi p
M0 a form of Hatta number 4 K 1Z qffiffiffiffiffiffiffiffiffi
pffiffiffiffiffiffiffi p ffi
M 00 a form of Hatta number independent from rate constant 4 Z
R total mass rate of absorption, g/s
R01 total mass rate of absorption without reaction in an infinitely deep, stagnant liquid, g/s
s Laplace transform variable
Vg gas phase constant velocity, cm/s
Vy velocity in y-direction, cm/s ðV y ¼ 0Þ
Vz average linear velocity of the liquid film in the direction of flow, cm/s
Vz linear velocity of the falling film in the direction of flow, cm/s
V max maximum linear velocity of the liquid film in the direction of flow, cm/s
y coordinate along the thickness of the liquid film from interface, cm
Y dimensionless coordinate along the thickness of the liquid film from wall
z coordinate along the direction of flow of the liquid film, cm
Z dimensionless coordinate along direction of flow of the liquid film
Greek symbols
d thickness of the liquid film, cm
d1 width of the gas flow channel, cm
M. Danish et al. / Applied Mathematical Modelling 32 (2008) 901–929 903
g dimensionless distance along the thickness of the liquid film

ki ith eigen-value for the solution of dimensionless liquid phase concentration
q density of the flowing liquid, g/cm3
x ratio of liquid to gas volumetric flow rates
s contact time (z=V max Þ, s
/m absorption rate, g/cm2 s.
Subscripts
i; j index variables
n nth value of a parameter
The process of isothermal gas absorption with and without chemical reaction in the liquid film for laminar
flow over a solid surface has been analyzed by many researchers. Higbie in 1935 [1] carried out the analysis of
gas absorption process by assuming penetration theory model for short time of contact and Pigford in 1941 [2]
attempted the same by using parabolic velocity profile for long contact time. Later on, Pigford extended this
work for various other situations [3–8]. Nysing and Kramers [9] carried out an experimental study of CO2
absorption in solutions of Na2CO3/NaHCO3 and K2CO3/KHCO3 accompanied by 1st order chemical reac-
tion in a wetted wall column, to verify the penetration theory for short contact time. Olbrich and Wild [10]
and Walker and Davis [11] extended the work of physical gas absorption for several simple geometries.
Absorption with finite gas phase resistance was further demonstrated by Tamir and Taitel [12] and Gupta
et al. [13]. The same problem was studied by Tamir and Taitel [14], Stepanek and Achwal [15] and Best
and Horner [16], but with the addition of first order chemical reaction in the liquid film. Continuing with
the above problem, Datta and Rinker [17] provided solution of gas absorption for short time of contact, tak-
ing into account the finite gas phase resistance and axial decrease of the solute concentration in gas phase with
first order chemical reaction in the liquid film. Later, Riazi and Faghri [18] and Riazi [19] stretched the above
work for zero order chemical reaction in the liquid film. Elperin and Fominykh [20] in 2003, derived the coef-
ficients of mass transfer during chemical absorption from a single Taylor bubble in the approximation of the
thin concentration boundary layer in liquid phase and verified the results with those of Nysing and Kramer [9].
Recently, a comprehensive model of gas absorption with chemical reaction has been developed by Sharma [21]
in 2004 in which most of the above cases have been included.Sharma, Danish and Ali [22] in 2006, solved the
original penetration theory model of Higbie [1] by using Similarity transform, Laplace transform and Sine
transform methods. Various parameters considered by different authors for the isothermal gas absorption
problem along with chemical reaction are listed in Table 1.
The case of reaction at the solid wall has not been considered so far. In the present work, an attempt has
been made to obtain an analytical solution for a more general case of absorption with finite resistance and
axial decrease of the solute concentration in gas phase and irreversible first order chemical reaction in liquid
film in laminar flow over a reacting plane wall. A combined method of Laplace transform and power series has
been applied to arrive at the concentration profiles of both the phases, which are eventually used to evaluate
absorption rate and enhancement factor. Moreover, the effects of gas flow rate, gas phase resistance and reac-
tion rate constants on concentration profiles and enhancement factor have been shown and discussed in detail.
Subsequently, various simplified models, studied by different workers have been derived. To get more confi-
dence over the derived general analytical solution, a comparison with the results obtained by an explicit
numerical scheme has been carried out. By reducing the general analytical solution for a simplified case of
CO2 absorption in Na-buffer solution accompanied by 1st order chemical reaction, the expression for absorp-
tion rate has been derived. Thereafter, the absorption rate is compared successfully with the available exper-
imental data of Nysing and Kramer [9] and Elperin and Fominykh [20]. This substantiates the developed
model and its analytical solution.
The rest of the paper is organized as follows: In Section 2, the partial differential equations are formulated
for the general gas absorption model. Section 3 describes the solution for general case using Laplace transform
and power series methods; this section also illustrates the derivation of the expression for enhancement factor
Table 1
Various parameters considered by different workers
No. Authors Years d1 df K1 K2 B x n
1 Higbie 1935 X NA – – – – –
2 Pigford 1941 NA X – – – – –
3 Nysing and Kramers 1958 X NA X – – – 1
4 Olbrich and Wild 1969 NA X – – – –
5 Tamir and Taitel 1971 NA X – – X – –
6 Tamir and Taitel 1975 NA X X – X – 1
7 Stepnek and Achwal 1976 NA X X – X – 1
8 Best and Horner 1979 NA X X – – – 1
9 Riazi and Fagri 1985 NA X X – – – 0
10 Datta and Rinker 1984 X NA X – X X 1
11 Gupta et al. 1986 NA X – – X X 1
12 Elperin and Fominykh 2003 X NA X – – – 0, 1
13 Present analysis 2006 NA X X X X X 1
and reduction of the general model and its solution to various simplified cases. In the same section, a compar-
ison between the analytical and numerical solutions has been included and the results obtained from analytical
solution are verified with the available experimental data. Section 4 presents a detailed discussion on the
obtained results and is followed by Section 5, which concludes the whole study.
2. Physical model and model equations
A thin liquid film, in fully developed laminar flow, is falling down over a dissolving solid wall and is
exposed to a gas, which flows either co-currently or counter-currently with respect to the film; the schematic
view is shown in Fig. 1. Mass transfer of solute takes place from gas to liquid phase. Time of contact between
solute and liquid is long enough to presume a parabolic velocity profile. Steady state conditions are assumed to
prevail. A constant gas phase resistance is present and the concentration of solute in gas phase varies axially
due to the absorption by liquid. Irreversible first order chemical reaction takes place between the solute and
liquid. It is further assumed that the diffused solute in liquid phase also reacts with the wall with the same
order of reaction; physical properties of both the fluids remain constant.
The law of conservation of mass is applied on an infinitesimally small element in the liquid film as well as in
the gas phase, as shown in Fig. 1, and the governing relations [23,24] are obtained as below.
2.1. Steady state modeling equations for liquid phase
The steady state modeling equation for liquid phase is obtained by applying the species balance over an
infinitesimally small element in liquid phase as shown in Fig. 1. In doing so, it is assumed that there is no
velocity component in y-direction and the axial diffusive transport is negligible in comparison to convective
transport. The flow is fully developed and the density of the liquid and diffusivity of the solute are constant.
Incorporating these assumptions and putting the well-known parabolic velocity profile in the thus obtained
mass balance equation, we get the following linear partial differential equation along with the relevant bound-
ary conditions:

y 2 oC a o2 C a
V max 1 2 ¼ DAB 2 k 1 ðC a C 0 Þ: ð1Þ
d oz oy
B.C.1: C a ¼ C 0 at z ¼ 0.
B.C.2: DAB oCoy
a
¼ k G ðC g C a Þ at y ¼ 0.
oC a
B.C.3: DAB oy ¼ k 2 ðC a C 0 Þ at y ¼ d.
Gas Liquid
Cgo Co
y Y, η
z, Z
Vg = constant, Plug Flow Wall

Vz (y)
Cg (z) = constant Cg (z)

P1 P2
Ca (z,0)
P3
Ca (z,y)
dC g
Vg C g − DAG Reaction at
z dz z
P4 wall =
k2.(Ca - Co)
Δz kG (Cg − Ca )
dC g
Vg C g − DAG
z +Δz dz z +Δz Δy
δ1 Interface δ
At P1 : C g = C g At P
2
dCa
At P3 : kG (C g − Ca ) = − DAB
∂Ca
∂Ca Vz ( y)Ca z − DAB
∂y Vy Ca − DAB dz z
∂Ca
y ∂y y
At P4 : − DAB = k 2 (Ca − Co )
∂y k1(Ca −Co)
∂Ca
dC VyCa − DAB
Vz ( y)Ca z − DAB a
y +Δy ∂y y +Δy
dz z +Δz
Fig. 1. Schematic diagram of gas absorption process over a dissolving solid wall with axial variation of gas phase concentration.
2.2. Steady state modeling equations for gas phase
The species balance over an infinitesimally small element in gas phase, shown in Fig. 1, yields Eq. (2), with
the assumptions that gas flows with uniform velocity and the contribution of axial diffusion is insignificant in
comparison to convective transport. After some simple mathematical manipulations one easily arrives at the
following 1st order linear ordinary differential equation:
dC g kG
¼ ðC g C a Þ: ð2Þ
dz d1 V g
The associated B.C. is:
B.C.1: C g ¼ C g0 at z ¼ 0.
The preceding equations and the respective B.Cs are non-dimensionalized, using the following definitions
for dimensionless variables:
ðd yÞ Ca C0 C g C g0 DAB
g¼ ; CA ¼ ; CG ¼ ; Z¼ z;
d C g0 C 0 C g0 C 0 V max d2
2
kGd k2d k1d V max d
B¼ ; K2 ¼ ; K1 ¼ and x ¼ :
DAB DAB DAB V g d1
The governing equations thus take the following form:
For liquid phase:

oC A o2 C A
gð2 gÞ ¼ K 1CA: ð3Þ
oZ og2
B.C.1: C A ¼ 0 at Z ¼ 0 8g.
B.C.2: oC
og
A
¼ Bð1 þ C G C A Þ at g ¼ 1 8Z.
oC A
B.C.3: og ¼ K 2 C A at g ¼ 0 8Z.
For gas phase:

oC G
¼ xBðC G C A þ 1Þjg¼1 at g ¼ 1 8Z:
oZ
Using B.C.2 for liquid phase, the above equation can be rewritten as:

oC G oC A
¼ x at g ¼ 1 8Z: ð4Þ
oZ og g¼1
B.C.1: C G ¼ 0 at Z ¼ 0.
Eqs. (3) and (4) including all the B.Cs constitute the general model. The parameter x can be regarded as the
ratio of the maximum possible absorption capacity to the rate at which gas enters into the channel [13]. It may
be noted that the gas phase concentration C g0 , at the top of the column, is the inlet gas concentration for co-
current flow and the exit concentration when the gas flows counter-currently. The positive sign in Eq. (4) refers
to the counter-current flow, while the negative sign refers to the co-current flow. C 0 is the initial concentration
in the liquid film i.e. concentration of solute in the liquid film before absorption starts.
3. Solution by Laplace transform with power series method
After taking the Laplace transform of model Eqs. (3) and (4) along with their B.Cs, using the following
definition [25,26]
Z 1
CA ¼ C A esZ dZ ð5Þ
0
one obtains the equations, in transformed form as:

For liquid phase:
d2 C A
gð2 gÞsC A ¼ K 1CA: ð6Þ
dg2
dC A

B.C.2: dg
¼ B 1s þ C G C A at g ¼ 1 8Z.
dC A
B.C.3: dg
¼ K 2 C A at g ¼ 0 8Z.
For gas phase:

dC A
sC G ¼ x : ð7Þ
dg g¼1
3.1. Evaluation of liquid phase concentration profile
The transformed ordinary differential equation (6) is solved by using a power series solution of the form:
X1
CA ¼ an gn : ð8Þ
n¼0
Substituting the above in Eq. (6) leads to the following recurrence relation:
s K 1 an2
an ¼ ½2an3 an4 þ ; ð9Þ
nðn 1Þ nðn 1Þ

where, a1 ¼ K 2 a0 , a2 ¼ K21 a0 and a3 ¼ 3s þ K 16K 2 a0 .
Hence, one finds an independent series solution of C A as:

C A ¼ a0 ð1 þ K 2 :g þ K21 g2 þ 3s þ K 16K 2 g3 þ Þ or
ð10Þ
C A ¼ a0 f ; where; f is a function of s and g:
The coefficient a0 is obtained from B.C.2 as:

B sB of
a0 ¼ fþ
s Bx s Bx og g¼1
and the solution in transformed form becomes:
,

s Bx of
CA ¼ 1 sf þ f: ð11Þ
B og g¼1
After applying the residue theorem [26,27], the following expression for inverse Laplace transform of C A is
obtained:
X 1

s Bx of
CA ¼ lim ðs ki Þ þsf f esz ; ð12Þ
i¼0
s!ki B og g¼1
where, ki denote the eigen-values which are the zeros of the following relation:

s Bx of
þ s:f ¼ 0: ð13Þ
B og g¼1
Applying L’Hospital rule to evaluate the limit in Eq. (12), the required solution for concentration profile in the
liquid film is found to be:
X 1

ki Z 1 of s Bx o2 f of
CA ¼ Ai f e ; where; Ai ¼ 1 þf þ þs : ð14Þ
i¼0
B og B osog os g¼1
s¼ki
Fig. 2 demonstrates the liquid phase concentration profiles C A for x ¼ 1:0, K 1 ¼ 0:1, K 2 ¼ 0:1 and B ¼ 106 at
different Z.
3.2. Evaluation of gas phase concentration profile
To find the gas phase concentration profile, the above expression for liquid phase concentration i.e. Eq.
(14), is substituted in Eq. (4) to get
X 1
oC G of
¼ x Ai ek i Z ð15Þ
oZ i¼0
og g¼1
and is integrated. Alternatively, one can substitute Eq. (11) in Eq. (7) and obtain the gas phase concentration
by taking its inverse Laplace transform.
The subsequent steps are not as straight forward as were in the case of liquid phase and depend upon the
magnitude of first eigen-value. The two cases, covering all the intricacies that arise in such conditions, are
described below:
3.2.1. Case (a): k0 6¼ 0

These types of cases arise, when velocities of both phases have non-zero but finite values (i.e. x 6¼ 0) and
none of the two reaction rates are zero (K 1 6¼ 0; K 2 6¼ 0).
3.5
z=0.01 z=0.05 z=.1 z=.2 z=.3 z=.4 z=.5 z=.6 z=.7 z=1
6
B = 10 , ω = 1.0
DIMENSIONLESS LIQUID PHASE
3
K 1 = 0.1, K 2 = 0.1
CONCENTRATION, CA
2.5
1.5
0.5
0
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1
DISTANCE FROM SOLID WALL, η
Fig. 2. Development of concentration profile in the liquid film, for finite gas phase resistance and axial variation of gas phase
concentration for counter-current system over a dissolving wall under first order chemical reaction.
On integration with respect to Z, with limits from 0 to Z, Eq. (15) leads to:
" #
X1
Ai of X1
Ai of
ki Z
C G ¼ x e :
i¼0
k i og g¼1 i¼0
k i og g¼1
This may be rearranged as:

X 1
x Ai of
CG ¼ Bi ð1 eki :z Þ; where; Bi ¼ ; i ¼ 0; 1; 2 . . . ð16Þ
i¼0
ki og g¼1
Eq. (16) represents the concentration profile for solute in gas phase for those cases where magnitude of first
eigen-value is non-zero. Fig. 3 portrays the concentration profile of solute in gas phase for x ¼ 1:0,
K 1 ¼ 0:1; K 2 ¼ 0:1 and B ¼ 106 . Table 2 presents the eigen-values and series coefficients of the same, for dif-
ferent values of x with K 1 ¼ 0:1; K 2 ¼ 0:1 and B ¼ 106 .
3.2.2. Case (b): k0 ¼ 0

Following two sub-cases generate zero as their first eigen-value:
(i) All the absorption models with stationary liquid film and/or very high gas velocity (i.e. x ¼ 0), with/
without any of the two reactions and for any value of gas phase resistance.
(ii) All the absorption models with no reactions (K 1 ¼ K 2 ¼ 0) and with any values of x and gas phase
resistance.
Here, only the second sub-case is described and the same approach can be adopted for the first one.
3.2.2.1. Sub-case: k0 ¼ 0.
For such systems, the liquid phase concentration profile C A may be expressed as:
X1
C A ¼ c0 þ Ai f eki Z ; where; c0 ¼ A0 f eki Z js¼k0 ¼0 : ð17Þ
i¼1
h i
o2 f
Also, A0 is the series coefficient evaluated for the first eigen-value ðk0 ¼ 0Þ at g ¼ 1 or c0 ¼ 1= 1 x osog .
g¼1;s¼0
2.5
K1 = 0.1
K2 = 0.1
6
2
B = 10 ω = 1.0
DIMENSIONLESS GAS PHASE
CONCENTRATION, CG
1.5
0.5 ω = 0.4
0
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1
DIMENSIONLESS AXIAL DISTANCE, Z
Fig. 3. Gas phase concentration profile for counter-current flow.
Table 2
Eigen-values and series coefficients for counter-current gas absorption system at various range of axial variation parameter x, with
K 1 ¼ 0:1, K 2 ¼ 0:1 and B ¼ 106
n x ¼ 0:0 x ¼ 0:4 x ¼ 1:0
ki Ai Bi ki Ai Bi ¼ xF i ki Ai Bi ¼ xF i
0 0.0000 0.8679 – 0.0937 1.1048 1.3005 0.4090 1.6913 2.1365
1 5.6465 1.1944 0.0000 4.5732 1.4408 0.24415 2.8532 2.0393 0.9924
2 40.311 0.5297 0.0000 39.285 0.5414 0.0262 37.739 0.5558 0.0681
3 106.97 0.3528 0.0000 105.95 0.3557 0.0096 104.42 0.3590 0.0244
4 205.64 0.2687 0.0000 204.62 0.2698 0.0049 203.09 0.2711 0.0125
5 336.31 0.2189 0.0000 335.29 0.2195 0.0030 333.76 0.2201 0.0076
6 498.97 0.1857 0.0000 497.95 0.1860 0.0020 496.42 0.1864 0.0051
7 693.64 0.1619 0.0000 692.62 0.1621 0.0014 691.09 0.1623 0.0036
8 920.30 0.1439 0.0000 919.28 0.1440 0.0011 917.76 0.1442 0.0027
9 1178.9 0.1298 0.0000 1177.9 0.1299 0.0008 1176.4 0.1300 0.0021
10 1469.4 0.1178 0.0000 1468.3 0.1187 0.0006 1466.7 0.1187 0.0017
Consequently, the required liquid phase concentration profile is expressed as:

1 X 1
CA ¼ h i þ Ai f eki z ð18Þ
o2 f
1 x osog i¼1
g¼1;s¼0
and from Eq. (4), the gas phase concentration profile is obtained as:
X1
ki :z x Ai of
CG ¼ Bi ð1 e Þ; where; Bi ¼ ; i ¼ 1; 2; 3 . . . ð19Þ
i¼1
ki og g¼1
The above mentioned Eq. (19) represents the concentration profile of solute in gas phase for those cases where
magnitude of first eigen-value is zero and the gas possesses an axial variation in the solute concentration.
Fig. 4 shows the concentration profile of solute in gas phase for x ¼ 1:0, K 1 ¼ K 2 ¼ 0 and B ¼ 106 .
1.8
1.6
CONCENTRATION, CG
1.4
ω = 1.0
1.2
0.8
0.6
0.4
0.2
0
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1
Fig. 4. Development of gas phase concentration profile for counter-current flow for x ¼ 1:0, K 1 ¼ 0:0, K 2 ¼ 0:0 and B ¼ 106 at Z ¼ 1:0.
3.3. Enhancement factor
The influence of chemical reaction and finite film thickness on the absorption is best summarized by com-
paring the actual absorption rate R, with that of an infinitely deep stagnant liquid with no chemical reaction
R01 , as used in [16]. The ratio R=R01 is equal to the well-known enhancement factor E. The absorption rate
from penetration model, for physical absorption in an infinitely deep stagnant liquid exposed to a gas for a
time period z=V max , is given by:
rffiffiffiffiffiffi
0 4Z
R1 ¼ ðC g0 C 0 ÞdV max W : ð20Þ
p
In the present condition, the total amount of gas absorbed per unit elapsed time is evaluated from the diffusive
flux at interface and is given as:
Z z

oC a
R ¼ DAB W dz: ð21Þ
0 oY Y ¼d
Yet again, to determine the derivative term in the above expression, we consider two different cases depending
upon the magnitude of first eigen-value.
3.3.1. Case (a): k0 6¼ 0

As explained earlier, these types of cases arise when both the fluids have non-zero but finite velocities
(x 6¼ 0) and none of the reaction rates are zero (K 1 6¼ 0; K 2 6¼ 0). For such conditions, we directly use Eq.
(14) for liquid phase concentration profile and substitute it in Eq. (21) to get the following expression for
absorption rate:
R X 1
¼ F i ð1 eki Z Þ; ð22Þ
ðC a0 C 0 ÞdV max W i¼0

where, F i ¼ Akii of
og
¼ Bxi ; i ¼ 0; 1; 2 . . .
g¼1
A little use of mathematics leads to the following expression for enhancement factor E
P1
R F i ð1 eki Z Þ
E ¼ 0 ¼ i¼0 rffiffiffiffiffiffi : ð23Þ
R1 4Z
p
10000
1000
ω = 1.0
ω = 0.4
100
ENHANCEMENT FACTOR, E
10 ω = 0.0
1
0.01 0.1 1 10 100
ω = -0.4
0.1
ω = -1.0
0.01
ω = -2.0
0.001
√Μ''
p
Fig. 5. Log–log graph showing effect of x on variation of E with M 00 for cocurrent and counter-current flow systems at K 1 ¼ 0:1,
K 2 ¼ 0:1 and B ¼ 106 .
pffiffiffiffiffiffiffi
In Fig. 5, the enhancement factor E has been plotted on a log–log graph as a function of the modulus M 00
(a form of Hatta number independent of rate constant), for various values of x with K 1 ¼ K 2 ¼ 0:1 and
B ¼ 106 . The modulus is defined as:
rffiffiffiffiffiffiffiffiffiffiffi
ffi
pffiffiffiffiffiffiffi
00 p
M ¼ Z: ð24Þ
4
3.3.2. Case (b): k0 ¼ 0
As argued earlier, two situations yield zero as their first eigen-values i.e.
(i) x ¼ 0,
(ii) K 1 ¼ K 2 ¼ 0.
We now proceed to find the expression for enhancement factor E for the first case only, since for the second
situation, it does not have any meaning. By rearranging the liquid phase concentration profile, as given in Eq.
(17) and following the same procedure, as adopted in Section 3.2.2.1 the expression for c0 is found to be:
pffiffiffiffiffiffi
pffiffiffiffiffiffi K 2 sinh K 1 g
cosh K 1 g þ pffiffiffiffiffiffi
K1
c0 ¼ pffiffiffiffiffiffi pffiffiffiffiffiffi pffiffiffiffiffiffi :
K1 pffiffiffiffiffiffi K 2 cosh K 1 pffiffiffiffiffiffi K 2 sinh K 1
sinh K 1 þ þ cosh K 1 þ pffiffiffiffiffiffi
B B K1
Finally, one obtains the required concentration profile for liquid phase as:
pffiffiffiffiffiffi
pffiffiffiffiffiffi K 2 sinh K 1 g
cosh K 1 g þ pffiffiffiffiffiffi X
1
K1
C A ¼ pffiffiffiffiffiffi pffiffiffiffiffiffi pffiffiffiffiffiffi þ A f eki Z : ð25Þ
K1 pffiffiffiffiffiffi K 2 cosh K 1 pffiffiffiffiffiffi K 2 sinh K 1 i¼1 i
sinh K 1 þ þ cosh K 1 þ pffiffiffiffiffiffi
B B K1
With the substitution of C A from the above equation, we can evaluate the gas absorption rate as:
pffiffiffiffiffiffi pffiffiffiffiffiffi
R K 1 sinh K 1 þ K 2 cosh K 1
¼ Z pffiffiffiffi
K 1 pffiffiffiffiffiffi pffiffiffiffiffiffi pffiffiffiffiffiffi pffiffiffiffiffiffi pffiffiffiffiffiffi pffiffiffiffiffiffi
ðC a0 C 0 ÞdV max W ð K 1 sinh K 1 þ K 2 cosh K 1 Þ þ K 1 cosh K 1 þ K 2 sinh K 1
B
X 1
ki Z Ai of
þ F i ð1 e Þ where; F i ¼ ; i ¼ 1; 2; 3 . . . ð26Þ
i¼1
ki og g¼1
From Eqs. (20) and (26) we can find the enhancement factor E as:
8 9,
pffiffiffiffiffiffi pffiffiffiffiffiffi
R < ðK 1 sinh K 1 þ K 2 cosh K 1 Þ X
1
ki Z
= pffiffiffiffiffiffiffiffiffiffiffi
E ¼ 0 ¼ Z hpffiffiffiffi pffiffiffiffiffiffi p ffiffiffiffiffi
ffi p ffiffiffiffiffi
ffi iþ F i ð1 e Þ 4Z=p:
R1 : K1
ð K 1 sinh K 1 þ K 2 cosh K 1 Þ þ K 1 cosh K 1 þ K 2 sinh K 1 1
;
B
ð27Þ
3.3.2.1. Sub-case for x ¼ 0 with K 1 ¼ 0 and K 2 6¼ 0.

Here too, the first eigen-value comes out to be zero. The enhancement factor E given by Eq. (27) is no
longer valid because on substituting K 1 ¼ 0, it results in an indeterminate form. For such cases, one needs
to start again from Eqs. (6) and (7) keeping K 1 ¼ 0. Following the same steps, as adopted previously, c0 is
found to be:
1 þ gK 2
c0 ¼ :
1 þ K 2 þ KB2
Hence, the concentration profile C A , may be written as:
1 þ gK 2 X1
CA ¼ K2 þ Ai f eki Z : ð28Þ
1 þ K2 þ B i¼1
Now using this concentration profile, the enhancement factor E is expressed as:
K2 X1
K2 Z þ F i ð1 eki Z Þ
R 1 þ K2 þ B i¼1
E¼ 0 ¼ rffiffiffiffiffiffi : ð29Þ
R1 4Z
p
The enhancement factor E has been plotted on a log–log graph as a function of Hatta number in Fig. 10 for
x ¼ 0 and different values of K1 and K2.
3.4. Reduction of general model into simplified cases
To show the general nature of the developed model and its solution, we reduce it to some simple cases,
which were earlier studied by various researchers. Many more linear model equations can also be deduced.
The results obtained from the reduced models and their solutions match exceptionally well with those avail-
able in literature. Only the concentration profiles of both phases have been discussed; the enhancement factor
and other related quantities can be obtained in a similar way.
3.4.1. Reduced model 1 (x ¼ 0, K 1 ¼ K 2 ¼ 0 and B ¼ 1)
This is the simplest case of physical gas absorption which takes into account the parabolic velocity profile in
the liquid film without any gas phase resistance. The velocity of gas phase is considered to be very high. This
case was first considered by [2,4] and later on by [10]. The respective model equations for both phases along
with B.Cs are found by keeping x ¼ 0, K 1 ¼ K 2 ¼ 0 and B ¼ 1 in Eqs. (3) and (4) and are presented
below:
For liquid phase:

oC A o2 C A
gð2 gÞ ¼ : ð30Þ
oZ og2
B.C.1: C A ¼ 0 at Z ¼ 0 8g.
B.C.2: C A ¼ 1 at g ¼ 1 8Z.
B.C.3: oC
og
A
¼ 0 at g ¼ 0 8Z.
For gas phase:

oC G
¼ 0 at g ¼ 1 8Z: ð31Þ
oZ
B.C.1: C G ¼ 0 at Z ¼ 0.
The solution methodology for the above equations is as follows:
For liquid phase:

Taking Laplace transform of Eq. (30) and using B.C.1, one gets:
d2 C A
gð2 gÞsC A ¼ : ð32Þ
dg2
The other two boundary conditions now become:
B.C.2: C A ¼ 1s and B.C.3: dC
dg
A
¼ 0.
P1 n
Substituting, C A ¼ n¼0 an g in Eq. (32), and using B.C.3, the following recurrence relation is
obtained:
s s
an ¼ ð2an3 an4 Þ; where a1 ¼ 0; and a2 ¼ 0 and a3 ¼ a0 :
nðn 1Þ 3
Thus, the transformed concentration profile turns out to be:

s s s4
C A ¼ a0 1 þ g3 g4 þ g6 þ ¼ a0 f ðs; gÞ: ð33Þ
3 12 45
1 f ðs; gÞ
B.C.2 gives a0 ¼ and C A ¼ . After taking its inverse Laplace transform one finds:
sf jg¼1 sf jg¼1
X1
s ki
CA ¼ lim f ðs; gÞesZ ; where; ki are roots of sf jg¼1 ¼ 0:
s!ki sf j
0 g¼1
Using L’Hospital rule for evaluating the limits in the above equation, the following expression for C A is
obtained:
X
1
1 X
1
CA ¼ lim f ðs; gÞesZ ¼ Ai f ðki ; gÞeki Z ;
s!ki df
0 f þs 0
ds g¼1
1
where Ai ¼ lim or
s!ki df
f þs
ds g¼1
ð34Þ
X
1 X
1
C A ¼ A0 þ Ai f ðki ; gÞeki Z ¼ 1 þ Ai f ðki ; gÞeki Z ;
1 1
1
where; A0 ¼ lim ¼ 1:
s!k0 ¼0 df
f þs
ds g¼1
For gas phase:

Now, the gas phase Eq. (31) is integrated which gives the gas phase concentration C G ¼ 0 throu-
ghout.
3.4.2. Reduced model 2 (x ¼ 0, K 1 ¼ K 2 ¼ 0 and B 6¼ 1)

Tamir and Taitel [12] studied a similar case of physical gas absorption with x ¼ 0 along with finite gas
phase resistance, by considering parabolic liquid phase velocity profile. By putting the values of parameters
given above, the following desired model equations are obtained:
For liquid phase:

oC A o2 C A
oZ og2
B.C.1: C A ¼ 0 at Z ¼ 0 8g.
B.C.2: oC
og
A
¼ Bð1 C A Þ at g ¼ 1 8Z.
B.C.3: oC
og
A
¼ 0 at g ¼ 0 8Z.
For gas phase:

oC G
¼0 at g ¼ 1 8Z: ð36Þ
oZ
B.C.1: C G ¼ 0 at Z ¼ 0.
The above governing system of equations is solved by applying Laplace transform followed by
power series method as done previously and the obtained liquid phase concentration profile is given
below:
X 1 X
1
C A ¼ A0 þ Ai f ðki ; gÞeki Z ¼ 1 þ Ai f ðki ; gÞeki Z ; ð37Þ
1 1
where,
1
A0 ¼ lim 2

¼1
1 of 1 o f
s!k0 ¼0
B og
þf þs B osog
þ of
os
g¼1

1 of
and ki are the roots of s B og
þf ¼ 0.
g¼1
Proceeding in a similar manner like the previous case, for gas phase we have concentration C G ¼ 0
throughout.
3.4.3. Reduced model 3 (x ¼ 0, K 1 6¼ 0; K 2 ¼ 0 and B ¼ 1)

This case refers to the situation where gas absorption takes place with first order chemical reaction and
without gas phase resistance with no gas flow. Best and Horner [16] have described such a case. Appropriate
values of parameters give the following model equations.
For liquid phase:
oC A o2 C A
gð2 gÞ ¼ K 1CA: ð38Þ
oZ og2
B.C.1: C A ¼ 0 at Z ¼ 0 8g.
B.C.2: C A ¼ 1 at g ¼ 1 8Z.
B.C.3: oC
og
A
¼ 0 at g ¼ 0 8Z.
For gas phase:

oC G
¼0 at g ¼ 1 8Z: ð39Þ
oZ
B.C.1: C G ¼ 0 at Z ¼ 0.
Following the earlier solution methodology one finds the liquid phase concentration as:
X pffiffiffiffiffiffi
1
cosh K 1 g X 1
C A ¼ A0 þ Ai f ðki ; gÞeki Z ¼ pffiffiffiffiffiffi þ Ai f ðki ; gÞeki Z ; ð40Þ
1
cosh K 1 1
pffiffiffiffi
where, A0 ¼ lims!k0 ¼0 1
of ¼ cosh pKffiffiffiffi
1g
and ki are the roots of sf jg¼1 ¼ 0.
ð Þjg¼1 f þs os cosh K 1
Again for gas phase, we have concentration C G ¼ 0 throughout.
3.4.4. Reduced model 4 (x ¼ 0, K 1 6¼ 0; K 2 ¼ 0 and B 6¼ 1)

The process of gas absorption with first order chemical reaction and with finite gas phase resistance and no
gas flow was worked out by [14,15]. For this situation the general model Eqs. (3) and (4) reduce to:
For liquid phase:
oC A o2 C A
gð2 gÞ ¼ K 1CA : ð41Þ
oZ og2
B.C.1: C A ¼ 0 at Z ¼ 0 8g.
B.C.2: oC
og
A
¼ Bð1 C A Þ at g ¼ 1 8Z.
oC A
B.C.3: og ¼ 0 at g ¼ 0 8Z.
For gas phase:

oC G
¼ 0 at g ¼ 1 8Z: ð42Þ
oZ
B.C.1: C G ¼ 0 at Z ¼ 0.
For this case we get the following expression for liquid phase concentration:
X
1
1 X
1
C A ¼ A0 þ Ai f ðki ; gÞeki Z ¼ pffiffiffiffiffiffi pffiffiffiffi p ffiffiffiffiffi
ffi þ Ai f ðki ; gÞeki Z ; ð43Þ
1 cosh K 1 þ BK 1 sinh K 1 1
where,
1 1
A0 ¼ lim 2

¼ pffiffiffiffiffiffi pffiffiffiffi pffiffiffiffiffiffi
s!k0 ¼0 1 df
þf þs 1 o f
þ of
cosh K 1 þ BK 1 sinh K 1
B dg B osog os
g¼1

1 df
and ki are the roots of s B dg
þ f ¼ 0.
g¼1
Similarly, for gas phase we have concentration C G ¼ 0 throughout.
3.4.5. Reduced model 5 (x 6¼ 0, K 1 ¼ 0; K 2 ¼ 0 and B 6¼ 1)

Physical gas absorption with finite gas phase resistance and gas flow was theoretically analyzed by [13]. The
presence of non-zero x couples equations of both phases. The gas phase equation is solved after the liquid
phase concentration profile is found. For this case, we have a non-zero gas phase dimensionless concentration
unlike all the previous cases derived. The governing equations become:
For liquid phase:

oC A o2 C A
oZ og2
B.C.1: C A ¼ 0 at Z ¼ 0 8g.
B.C.2: oC
og
A
¼ Bð1 þ C G C A Þ at g ¼ 1 8Z.
oC A
B.C.3: og ¼ 0 at g ¼ 0 8Z.
For gas phase:

oC G oC A
¼ x at g ¼ 1 8Z: ð45Þ
oZ og g¼1
B.C.1: C G ¼ 0 at Z = 0.
Again, going through the same steps, we have the liquid phase concentration profile as given below:
X1
1 X
1
C A ¼ A0 þ Ai f ðki ; gÞeki Z ¼ þ Ai f ðki ; gÞeki Z ; ð46Þ
o f
2
1 1 x osog 1
g¼1

where, A0 ¼ lims!k0 ¼0 o2 f and ki are the roots of of
1
og
sxB
B
þ sf ¼ 0.
1xosog g¼1
g¼1
After putting this in Eq. (45), we get the gas phase concentration C G as:
! !
oC G oC A o X 1 X
1
of ðk ; gÞ
ki Z i ki Z
¼ x ¼ x A f ðk ; gÞe ¼ x A e :
og g¼1
i i i
oZ og 0
0
og
g¼1 g¼1
Integration of the above expression and using B.C.1 for gas phase gives:
!
X1
Ai of ðki ; gÞ X
1

C G ¼ x 1 eki Z ¼ Bi 1 eki Z ; ð47Þ
0
k i og g¼1 0

where, Bi ¼ x Akii of ðkogi ;gÞ .
g¼1
3.4.6. Reduced model 6 (x ¼ 0, K 1 ¼ 0; K 2 ¼ 0, B ¼ 1 and dy 1)

This is the simplest case first considered by [1], while founding the penetration theory for gas absorption for
short time of contact. Recently, Sharma et al. [22] have obtained the solution for this case by three different
techniques i.e. Laplace transform, Similarity transform and Sine transform. We describe below the solution by
Laplace transform only. The governing equations are as follows:
For liquid phase:

oC a o2 C a
V max ¼ DAB : ð48Þ
oz oy 2
B.C.1: C a ¼ C 0 at z ¼ 0.
B.C.2: C a ¼ C g0 at y ¼ 0.
B.C.3: C a ¼ C 0 at y ¼ d.
This system is made non-dimensionalized by using the same definitions except g ¼ dy (used for this case
only). Hence, the following parabolic partial differential equation is obtained:
oC A o2 C A
¼ : ð49Þ
oZ og2
B.C.1: C A ¼ 0 at Z ¼ 0.
B.C.2: C A ¼ 1 at g ¼ 0.
B.C.3: C A ¼ 0 at g ¼ 1.
Taking the Laplace transform with respect to Z on both sides of diffusion equation (49) and incorporating
the boundary condition at Z ¼ 0 gives:
d2 C A
sC A ¼ : ð50Þ
dg2
The solution of the ordinary differential Eq. (50) is given [5–7] as:
pffi pffi
C A ¼ Aeg s þ Beg s ; ð51Þ
where, C A is a function of s and g. The constants A and B are found with the help of the boundary conditions 2
and 3, and the solution in transformed form becomes:
pffi
eg s
CA ¼ : ð52Þ
s
The inverse transform of this expression is obtained by using Fourier–Mellin inversion theorem [26] as:
Z cþib
1
C A ðg; ZÞ ¼ lim C A esZ ds: ð53Þ
2pi b!1 cib
This is approximated by the contour integral [26,28] which is given by:
I
esZ C A ds: ð54Þ
Putting C A from Eq. (52) in Eq. (54) and after doing some mathematical manipulations, the following liquid
phase concentration profile of the absorbed solute, for short contact time, is obtained
g
C A ¼ erfc pffiffiffiffiffiffi : ð55Þ
4Z
3.5. Numerical solution of the general model
The developed analytical solution has been verified using a simple explicit numerical scheme for many sets
of parameter values. The scheme utilizes finite difference approach and the discretized model domain is dem-
onstrated in Fig. 13. The adopted finite difference method has been programmed in MATLAB 6 for ease and
the results are saved as an EXCEL data file. Only the liquid and gas phase concentration profiles are shown in
Figs. 14 and 15 respectively, for one set of parameter values pertaining to the general case. From the two plots,
it is clear that the results show a good agreement with the analytical solutions presented in Figs. 2 and 3.
3.5.1. Numerical scheme

The whole problem domain of interest was divided into two parts: one for the liquid film and the other for
gas phase, as depicted in Fig. 13. The liquid part was discretized along two directions; while gas phase was dis-
cretized along axial coordinate only. Subsequently, at their respective border points, B.Cs have been specified.
Discretization in liquid phases

The dimensionless liquid film thickness g and the dimensionless axial distance Z are divided into N and M
equal parts, respectively. The general model equation in liquid film at a point ði; j þ 1Þ is expressed as:

oC A o2 C A

gð2 gÞ ¼ K 1 A
C ; or
oZ i;jþ1 og2 i;jþ1
i;jþ1
ð56Þ
oC A o2 C A

gð2 gÞ K 1CA
oZ i;jþ1 og2 i;j
i;j
and the associated B.Cs are:

B:C:1 : C A ði; 0Þ ¼ 0; 8i 2 ½0; N ð57Þ

oC A
B:C:2 : ¼ Bð1 þ C G C A ÞjN ;jþ1 ; 8j 2 ½0; M ð58Þ
og N ;jþ1

oC A
B:C:3 : ¼ K 2 C A j0;jþ1 ; 8j 2 ½0; M: ð59Þ
og 0;jþ1
Discretization in gas phase

Only axial discretization is needed in gas phase and is given below:

oC G oC A
¼ x ; 8j 2 ½0; M: ð60Þ
oZ jþ1 og N ;jþ1
The B.C. for gas phase is introduced as:
B:C:1 C G ð0Þ ¼ 0: ð61Þ

Solution algorithm:
1. Concentrations C A and C G of liquid and gas phases at the starting of the boundary are specified using Eqs.
(57) and (61).
2. Using the discretized form of Eq. (56), the liquid phase concentrations C A ði; j þ 1Þ at the next axial position
are calculated for all i 2 ½1; N 1.
3. Thereafter, from Eq. (59), the liquid phase concentration at wall is obtained.
4. Next, C A ðN ; j þ 1Þ and C G ðj þ 1Þ are evaluated from Eqs. (58) and (60) simultaneously.
5. The procedure is repeated for the next axial step.
3.6. Verification of the mathematical model with the experimental results
Though the problem of gas absorption with and without chemical reaction has been tackled by many work-
ers and a vast amount of material, both theoretical and experimental, is available. Mostly, the experimental
studies have been carried out to find the related unknown parameters such as rate constant, diffusivity and
saturation concentration of solute in liquid etc. or the derived quantities like average or total absorption rate,
rather than to find the concentration profiles of both the phases. For the purpose of verification, the experi-
mental data are chosen from [9], in which an experimental study of CO2 absorption in the Na buffer solutions
of various strengths was carried out for short time of contact. The whole process of absorption was accom-
panied by 1st order homogeneous chemical reaction and the rate of absorption of CO2 was measured in a wet-
ted wall column.
The equations used in [9] for concentration profile, mass transfer rate per unit area and the total amount of
gas absorbed per unit area, in a certain time interval, have been reproduced below in terms of the symbols used
in the present paper:
0 sffiffiffiffiffiffiffiffiffiffi1 0 sffiffiffiffiffiffiffiffiffiffi1
rffiffiffiffiffiffiffiffi rffiffiffiffiffiffiffiffi
Ca 1 k1 B y k1z C 1 k1 B y k1z C
¼ exp y erfc@ qffiffiffiffiffiffiffi A þ exp y erfc@ qffiffiffiffiffiffiffi þ A: ð62Þ
C g0 2 DAB 2 zDAB V max 2 DAB 2 zDAB V max
V max V max
The rate of mass transfer through a unit area of the gas liquid interface is given [9] as:
0 sffiffiffiffiffiffiffiffiffiffi 1
k1 z
oC a pffiffiffiffiffiffiffiffiffiffiffiffiB k1z
e V max C
/m ¼ DAB ¼ C g0 DAB k 1 @erf þ qffiffiffiffiffiffiffiffiffiffiffiA: ð63Þ
oy y¼0 V max p Vkmax1z
z
The total amount of gas absorbed per unit area, after a contact time s ¼ V max is given [9] as:
20sffiffiffiffiffiffiffiffiffiffi 1 sffiffiffiffiffiffiffiffiffiffi 3
Z s rffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi k1 z
V max
z 6B k 1 z 1 C k1z e 7
mðsÞ ¼ /m dt ¼ C g0 DAB 4@ þ qffiffiffiffiffiffiffiAerf þ pffiffiffi 5: ð64Þ
0 V max V max 2 k1 z V max p
V max
In order to compare our results with the experimental data [9], the above quantities are now evaluated from
the present model equations for the case when x ¼ 0, K 1 6¼ 0; K 2 ¼ 0 and B ¼ 1.
The rate of mass transfer through a unit area of the gas liquid interface is given by:

oC a oC a DAB C g0 oC A
/m ¼ DAB ¼ D ¼ : ð65Þ
oy y¼0 oY Y ¼d og g¼1
AB
d
2
0 ðZDZ 0 Þ
The total amount of gas absorbed per unit area after a contact time s ¼ zDz
V max
¼d DAB
is given (Dz0 is the
height of end effects [9]) as:
Z s Z z Z Z
1 oC A
mðsÞ ¼ /m dt ¼ / dz ¼ C g0 d dZ; ð66Þ
0 V max 0 m 0 og g¼1
where

oC A pffiffiffiffiffiffi pffiffiffiffiffiffi X1
of
¼ K 1 tanh K 1 þ Ai eki Z ð67Þ
og g¼1 i¼1
og g¼1
or
!
pffiffiffiffiffiffi pffiffiffiffiffiffi X
1
ki Z Ai of
mðsÞ ¼ C g0 d Z K 1 tanh K 1 þ F i ð1 e Þ ; and Fi ¼
i¼1
ki og g¼1
!
DAB s pffiffiffiffiffiffi pffiffiffiffiffiffi X1 D s
ki AB
¼ C g0 d K 1 tanh K 1 þ F i ð1 e d Þ :
2
ð68Þ
d2 i¼1
The values of chosen parameters are same as those used for the runs 5 and 6 of [9] and are listed below:
Run No. 5 of [9]: C g0 ¼ 2:31 104 g cm3 ; k 1 ¼ 0:56 s1 ; d ¼ 0:04 cm;
DAB ¼ 1:17 105 cm2 s1 ; V max ¼ 32 cm s1 ; Dz ¼ 2 cm.
Table 3
Eigen-values and series coefficients for experimental data of gas absorption with first order chemical reaction, x ¼ 0, K 1 ¼ 76:5812 and
144.957265, K 2 ¼ 0 and B ¼ 1
No. of eigen-values For K 1 ¼ 76:5812 For K 1 ¼ 144:957265
ki Ai Fi ki Ai Fi
0 0.000000 0.0003165843 – 0.000000 0.0000118087 –
1 107.6611314 0.0099496611 0.00757368037899 185.8518694 0.0015920387 0.00369423528606
2 166.3823198 0.0348871199 0.00762832934056 257.1461211 0.0074742510 0.00419537415163
3 247.9379144 0.0656352839 0.00637605737965 350.5565811 0.0183812004 0.00391993865534
4 354.9497511 0.0911870510 0.00508712756082 468.4541818 0.0324252865 0.00341452963397
5 489.75184370 0.1068187151 0.00403212778099 612.5116393 0.0468084563 0.00289332452554
6 654.1933116 0.1134069768 0.00321390217994 784.0615829 0.0592897557 0.00243452255674
7 849.4538967 0.1139208620 0.00259132581195 984.2776336 0.0687116330 0.00197917740811
8 1076.1708969 0.1110551986 0.00198260994417 1214.1646337 0.0748928678 0.00262807504592
9 1334.5388988 0.1062974349 0.00842749504505 1474.1656341 0.0330288412 0.01797114826218
10 1625.5418988 0.0011747340 0.00518678921917 1726.177 1.358284e-05 0.00013246396498
Run No. 6 of [9]: C g0 ¼ 2:25 104 g cm3 ; k 1 ¼ 1:06 s1 ; d ¼ 0:04 cm;
DAB ¼ 1:17 105 cm2 s1 ; V max ¼ 32 cm s1 ; Dz ¼ 2 cm.
The obtained results have been shown in Fig. 16 and an excellent agreement is found between the analytical
solution and the experimental data. A detailed discussion of the results can be found in the next section. Eigen-
values and other coefficients for these runs have been shown in Table 3.
4. Results and discussion
The concentration profiles of solute, in both phases depend upon four parameters namely x, K1, K2 and B.
The liquid phase concentration shows variation in both y- and z-directions while, the gas phase concentration
varies with z only. The parameters also affect absorption rate in the liquid phase. An assessment of the plots of
various quantities for a range of parameter values reveals these variations.
4.1. Parameter x
Figs. 3 and 6 show that as gas phase velocity increases, both the liquid and gas phase concentrations
increase in counter-current systems. This is also true for co-current systems. When x is small, the axial var-
iation in gas phase concentration is negligible and the error introduced by assuming a constant axial concen-
tration is also small. However, as x increases, the variation in gas phase concentration becomes large.
x depends on the relative liquid to gas volumetric flow rates. For the gases of larger solubility, large axial
variation in the gas composition can be expected.
In the light of the above discussion, Figs. 3 and 15 may cause some confusion in the sense that the concen-
tration of solute in gas phase is large for lower gas velocity (i.e. x ¼ 1:0) as compared to the one for higher gas
velocity (i.e. x ¼ 0:4) for counter-current flow, for all values of Z. This is in sharp contrast with the above
discussion. This issue is resolved below.
A close look on Eq. (2) or (4) reveals that the slope oC oZ
G
decreases with increase in gas phase velocity. This
means that for higher gas phase velocities, the outlet and inlet concentrations are nearly same. Whereas, for
lower gas velocities the slope is positive which indicates that inlet concentration is greater than the outlet con-
centration C g0 . Since the outlet concentration C g0 has been used in all our calculations, and because the slope
3.5
ω = 0.0
3 ω = 0.4
ω = 1.0
DIMENSIONLES LIQUID PHASE
2.5
CONCENTRATION, CA
1.5
0.5
0
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1
DIMENSIONLESS DISTANCE FROM SOLID WALL, η
Fig. 6. Development of liquid phase concentration profile for counter-current flow, x varies from 0.0 to 1.0 for, K 1 ¼ 0:1, K 2 ¼ 0:1 and
B ¼ 106 at Z ¼ 1:0.
tends to zero for higher gas velocities, this C g0 will be available through out the axial direction for x ¼ 0.
However, for non-zero slopes, a concentration greater than C g0 , but lesser than inlet concentration is observed
for all axial positions and hence, a higher gas phase concentration at a particular Z is seen for lower gas veloc-
ities and vice-versa. To understand these arguments clearly, one can also study the plots by shifting the con-
centration profiles such that the inlet concentrations become same for all gas velocities, which accordingly
makes the outlet concentrations C g0 different.
Fig. 5 shows the variation of enhancement factor with Hatta number on a log–log plot for various values of
x. As is evident from the plot, the absorption rate for co-current system is much lower than that of constant gas
phase concentration. This is due to the gradual decline of gas phase concentration in a co-
current flow resulting in a finite amount of solute absorption. In counter-current or co-current systems, increase
in gas phase velocity leads to an increase in enhancement factor E. In co-current systems, it is also observed,
that enhancement factor E decreases linearly on a log–log plot for Hatta number greater than 7.
4.2. Parameter K1
As liquid film reaction rate constant K1 increases, the exit liquid phase concentration decreases which is
portrayed in Fig. 7. This is due to the enhanced rate of reaction which increases the absorption rate; it can
also be seen from the increasing slope of liquid phase concentration profiles at interface. Higher the absorption
rate, higher is the axial variation in gaspphase
ffiffiffiffiffiffiffi concentration as shown in Fig. 8.
Fig. 9 shows the variation of E with M 00 (Hatta number) and K1 for co-current as well as counter-current
systems. Initially, for any of the systems, the effect of K1 is negligible since the rate of reaction is small enough
(due to very low concentration in the liquid film) to impress any change in enhancement factor E. In co-cur-
rent systems, for Hatta number greater than 10, the absorption rate overcomes the reaction rate and satura-
tion starts. This behavior is shown by a single line with constant negative slope in spite of different values of
K1, while, in the case
ffi of counter-current system no such relation is found. The enhancement factor E increases
pffiffiffiffiffiffi
steadily with M 00 as the value of parameter K1 increases. The rate of absorption for counter-current flow is
higher than for co-current flow for fixed values of all process parameters. The reaction parameter K1, indicates
the ratio of the rate of reaction to the rate of diffusion in relation to the thickness of the film. Thus, a small
value of K1 may be due to a very slow reaction, a very thin film or a high rate of diffusion. The effect of film
thickness on the rate of absorption is seen only when K1 is less than 5. At higher values of K1, the rate of
K1 = 0.0
2
K1 = 0.1
K1 = 0.4
CONCENTRATION, CA
1.5 K1 = 2.0
0.5
0
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1
Fig. 7. Development of liquid phase concentration profile for counter-current flow over a dissolving solid wall, K1 varies from 0 to 2 for
x ¼ 0:4, K 2 ¼ 0:1 and B ¼ 106 at Z ¼ 1:0.
1.2
K1 = 0.0
1 K1 = 0.1
K1 = 0.4
CONCENTRATION, CG
0.8
K1 = 2.0
0.6
0.4
0.2
0
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1
Fig. 8. Gas phase concentration profile for counter-current flow over a dissolving solid wall, K1 varies from 0 to 2 for x ¼ 0:4, K 2 ¼ 0:1
and B ¼ 106 .
100
K1 =2.0
0.4 COUNTER-CURRENT
10
0.1
0.0
1
0.4 2.0
0.1
0.0
0.1 CO-CURRENT
0.01
0.01 0.1 1 10 100
√Μ''
p
Fig. 9. Log–log graph showing effect of K1 on variation of E with M 00 for co-current and for counter-current flows in gas phase at
K 2 ¼ 0:1 and B ¼ 106 .
reaction is sufficiently high to prevent the absorbed gas molecules from reaching the solid wall for a particular
Z.
4.3. Parameter K2
The effect of K2 on concentrations of both the phases and on enhancement factor E follows approximately
the same pattern as that of K1, while keeping other parameters constant. But these effects are slightly less due
100
10
0.1 &
0.0
K1 = 0.0 &
K1 = 0.2 &
K2 = 0.1
K2 = 0.0
1 0.1 &
0.1
0.1
0.1 1 10 100
√Μ''
p
Fig. 10. Log–log graph showing effect of K1 and K2 on variation of E with M 00 .
to the more pronounced effect of liquid phase reaction as compared to the reaction at the wall. With the help
of Fig. 10, the combined as well as independent effects of parameters K1 and K2 on the enhancement factor E
can be easily appreciated.
4.4. Parameter B
Figs. 11 and 12 show liquid and gas phase concentration profiles for a counter-current system at steady
state. It can easily be noticed that as the surface resistance increases i.e. parameter B decreases, the exit liquid
1.6
K1 = 0.1
K2 = 0.1
1.4
w = 0.4 at Z = 1.0
1.2
CONCENTRATION, CA
0.8
0.6
0.4 B = 106
at Z = 0.01
0.2
B = 10
0
0 0.2 0.4 0.6 0.8 1
DISTANCE FROM SOLID WALL, η
Fig. 11. Development of liquid phase concentration profile for counter-current flow, B varies from 10 to 106 for x ¼ 0:4 at Z ¼ 1:0 and
Z ¼ 0:01.
0.45
K 1 = 0.1
K 2 = 0.1
0.4
ω = 0.4 B = 106
0.35
CONCENTRATION CG
B = 10
0.3
0.25
0.2
0.15
0.1
0.05
0
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1
Fig. 12. Gas phase concentration profile for counter-current flow.
phase concentration decreases and a similar pattern is observed in the gas phase concentration at the interface.
It is also worth mentioning that in a counter-current system, the liquid phase concentration at interface may
be greater than the outlet gas phase concentration C g0 after some Z. This is because, the gas phase boundary
condition at Z ¼ 0, for the two systems i.e. co-current as well as counter-current, uses C g0 which is the inlet
concentration for co-current flow and the outlet concentration for counter-current flow. In case of co-current
flow, the inlet concentration C g0 is the highest concentration at interface among all axial positions whereas, for
counter-current flow it is the lowest. Therefore, in counter-current system the liquid film after some Z, encoun-
ters a gas phase concentration which is greater than C g0 . While, in co-current gas flow, the dimensionless liquid
phase concentration C A will be less than 1 for all values of Z.
4.5. Reduction of general model into simple cases
In Section 3.5, six simple cases have been successfully derived by reducing the general model for different
situations. All these cases were earlier researched by [1,2,4,10,12–16,22].
4.6. Numerical scheme
The numerical technique chosen is of explicit type, thus it is simple to implement. But, while discretizing the
problem, care should be taken in selecting a proper step size. At times, larger increments may destabilize the
method or may even give poor results. Though, smaller steps do give accurate results but the computational
time increases manifolds due to increase in the number of machine calculations.
For the selected parameters, we have taken N ¼ 20–50 and M ¼ 106 –105 . More powerful numerical
approaches will not only yield good results but also in a reasonable time. The employed scheme is pictorially
depicted in Fig. 13.
4.7. Validation by experimental data
The present general model and its solutions are compared with the available simplified experimental case of
gas absorption accompanied by 1st order chemical reaction in film only, with no gas phase resistance and no
Gas Liquid
Cgo Co
N, 0 N-1, 0 i+1, 0 i, 0 i-1, 0 3, 0 2, 0 1, 0 ,i

Z, j
N, 1 0, 1
N, 2 0, 2
N, 3 0, 3
Wall
N, 4 0, 4
N, 5 0, 5
N, 6 0, 6
N, j-1 0, j-1
N, j i+1, j i, j i-1, j
0, j
ΔZ
N, j+1 i, j+1
0, j+1
Δη
N, M-1
0, M-1
N, M
0, M
δ1 Interface δ
Fig. 13. Grid points in numerical scheme.
gas side flow. A close look on this model reveals that it can be considered as a practical example of reduced
model 3, described in Section 3. The amount of gas absorbed per unit area after a contact time s, calculated
presently and the one found by the other two groups [9,20], has been shown in Fig. 16 on a log–log scale. It is
easily understood that the outcome from our model and that of Nysing and Kramers [9] match outstandingly
and is even better than those discussed by Elperin and Fomynikh [20]. In initial stages or for short contact
time, our model deviates slightly from those of [9,20]. This is due to the limited terms considered in Eq.
(40), which makes the solution incompatible with B.C.1
pffiffiffiffiffiffi
cosh K 1 g X 1
C A jZ!0 ¼ 0 ¼ pffiffiffiffiffiffi þ Ai f ðki ; gÞ: ð69Þ
cosh K 1 1
Finite terms in the above equation do not satisfy it for small Z, while for larger Z, only few terms are sufficient.
That is why the present results deviate to a small extent only for initial values of Z and this point can also be
verified by varying the number of terms in Eq. (69).
4.8. Miscellaneous
Laplace transform technique is found to be superior to separation of variables method as it does not require
homogeneous boundary conditions and can easily be applied to systems of linear differential equations. Eigen-
values are found by the hybrid scheme of bisection and Newton–Raphson methods. Accuracy in eigen-values
3.5
Z=0.01 Z=0.05 Z=0.1 Z=0.2 0.3 Z=0.4 0.5 Z=0.6 0.7 Z=1.0
B = 10 , ω = 1.0
6
DIMENSIONLESS CONCENTRATION, CA
3
K1 = 0.1, K2 = 0.1
2.5
1.5
0.5
0
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1
Fig. 14. Liquid phase concentration profile evaluated from numerical scheme.
2.5
K1 = 0.1
K2 = 0.1
B = 106
2
ω = 1.0
CONCENTRATION, CG
1.5
0.5 ω = 0.4
0
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1
Fig. 15. Gas phase concentration profile evaluated from numerical scheme.
decreases with their numbers and therefore, only eleven eigen-values are presented. However, 11th eigen-value
was determined with some error. Higher eigen-values could not be found due to the divergence of the series in
Eq. (13). It is also observed that the 11th eigen-value cannot be found if we express Eq. (3) in terms of dimen-
sionless variable g ¼ dy (where, y coordinate starts from the interface). The nth eigen-value can be found from a
quadratic polynomial of n, which helped in predicting the initial guess for all the cases. This point was also
mentioned by [10]. It is also observed that the magnitude of eigen-values increases with an increase in any
of the rate constants while in case of increased surface resistance, it decreases. Further, the magnitudes of
eigen-values for co-current flow are greater than the corresponding eigen-values for counter-current flow
for the same absolute values of the parameters.
3.50
Run 5 Run 6
3.00 Ref. [20]

Ref. [20]
log (m(τ)/√τ) + 7.0

2.50 Ref. [9] &
Present work
2.00
Ref. [9] &
Present work
1.50
1.00
0.50
0.00
-1 -0.5 0 0.5 1 1.5 2 2.5 3
log τ
Fig. 16. Comparison with experimental data.
An important point regarding eigen-values is also discovered, that the first eigen-value becomes positive for
counter-current flow with axial variation in the gas phase concentration which was not mentioned by any of
the previous authors. The magnitude of this value increases with the increase in gas flow rate. Moreover, for
the two situations i.e. (i) x ¼ 0 and (ii) K 1 ¼ K 2 ¼ 0, we get zero as the first eigen-value. Table 4 shows the first
eigen-value for different values of parameters.
For special cases, our results show excellent agreement with those obtained by [1] for simple physical
absorption for small contact time; [4,10] for simple physical absorption for large time of contact; [9,16,20]
for gas absorption with 1st order chemical reaction; [12] for gas absorption with surface resistance; [14] for
gas absorption accompanying 1st order chemical reaction with finite gas phase resistance and [13] for gas
absorption with surface resistance and with gas side flow.
Table 4
First eigen-value for various sets of parameters values
S. no. x K1 K2 B k0
1 0.0 0.1 0.1 106 0.0000
2 0.4 0.1 0.1 106 0.0937
3 1.0 0.1 0.1 106 0.4090
4 0.0 0.0 0.0 106 0.0000
5 0.4 0.0 0.0 106 0.0000
6 1.0 0.0 0.0 106 0.0000
7 0.4 0.0 0.1 106 0.0483
8 0.4 2.0 0.1 106 0.5836
9 0.4 0.1 0.0 106 0.0517
10 0.4 0.1 2.0 106 0.3356
11 0.0 0.0 0.0 1 0.0000
12 0.0 0.0 0.0 104 0.0000
13 0.0 0.1 0.0 1 0.0000
14 0.0 0.1 0.0 104 0.0000
15 0.4 0.0 0.0 106 0.0000
16 0.4 0.0 0.0 10 0.0000
5. Conclusions
• A more general situation of gas absorption with finite gas phase resistance, axial variation in the gas phase
concentration and irreversible 1st order chemical reaction in the liquid film and at the wall is analyzed.
Eigen-values and series coefficients for various cases are also calculated and some of them are shown in
the Tables 2 and 3.
• Effects of various parameters on the liquid and gas phase concentrations as well as on the enhancement fac-
tor E are shown and it is found that a strong surface resistance leads to a negligible rate of gas absorption,
while a higher reaction rate increases the absorption rate for both the co-current and counter-current sys-
tems. Though, for counter-current system, the effect of K1 (or K2) on enhancement factor E may be observed
over the whole axial distance but for co-current system there is a limited region where this effect is visible,
beyond which K1 (or K2) does not have any effect and hence absorption rate for simple physical absorption
can be used. Changes due to reaction at wall follow a similar pattern as those exhibited by the reaction in
liquid film but these are less pronounced. For both the systems, the increase in gas phase velocity increases
the enhancement factor E. The total mass absorbed by a co-current system is constant and does not vary
with Z after attaining the steady state, while in case of counter-current system, it increases with thepaxial
ffiffiffiffiffiffiffi dis-
tance Z, which can be verified by evaluating the enhancement factor in terms of Hatta number M 00 .
• It is also concluded that the exit liquid phase concentration for B ¼ 1000 is nearly equal to the value for
B ¼ 1. It implies that for B ¼ 1000 and above, the gas film resistance is almost negligible. These results
are expected to be useful in measuring diffusivities, mass transfer coefficients, solubilities and reaction rate
constants for the experiments of gaseous mixtures. The present analysis is a step forward, as it is useful
when gas is not necessarily pure and it is applicable for the condition of low as well as high gas flow rates.
• The reaction parameter K1, indicates the ratio of the rate of reaction to the rate of diffusion in relation to
the thickness of the film. Thus, a small value of K1 could be due to a very slow reaction or a very thin film or
a high rate of diffusion. For K1 greater than 5, the film thickness does not have any effect on the rate of
absorption. The higher values of K1 prevent the penetration of the absorbed gas molecules towards the solid
wall. This is the reason that the results predicted from our analysis match very well with the experimentally
reported results of [9], where K 1
5 and the parabolic velocity profile was not taken into account and thus,
the film thickness did not come into picture.
• When x is small, the axial variation in the gas phase is negligible and hence the error introduced by assum-
ing a constant axial concentration is small. However, as x increases, the error becomes large.
• The present general model has been successfully reduced to some of the previously studied simple models.
Results obtained from an explicit numerical technique, programmed in MATLAB 6, have been presented
and compared with those of analytical solutions and an excellent agreement between the two has been
found.
• Absorption rates found from the analytical solution, for a simplified case, are verified with the experimental
data of [9]. The conformity between the two substantiates the present work.
Acknowledgements
The authors are gratefully indebted to Dr. Surendra Kumar, Professor, Department of Chemical Engineer-
ing, I.I.T. Roorkee, (Roorkee-247667, U.A., India.) for his invaluable guidance in the preparation of manu-
script. We are also thankful to Professor S. M. Yusuf, (Retd.), Department of Mechanical Engineering,
A.M.U., (Aligarh-202002, U.P., India.) for his helpful suggestions and to Ms. Arees Qamareen, Lecturer,
Department of Mechanical Engineering, A.M.U., (Aligarh-202002, U.P., India.) for her support in formatting
the document.
References
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(1935) 365–389.
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1247–1253.
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144–152.
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Applied Mathematical Modelling 32 (2008) 901–929

Gas absorption with ﬁrst order chemical reaction in a

0307-904X/$ - see front matter 2007 Published by Elsevier Inc.

g dimensionless distance along the thickness of the liquid ﬁlm

2. Physical model and model equations

2.1. Steady state modeling equations for liquid phase

Vg = constant, Plug Flow Wall

Cg (z) = constant Cg (z)

2.2. Steady state modeling equations for gas phase

The governing equations thus take the following form:

For liquid phase:

For gas phase:

3. Solution by Laplace transform with power series method

one obtains the equations, in transformed form as:

For gas phase:

3.1. Evaluation of liquid phase concentration proﬁle

3.2. Evaluation of gas phase concentration proﬁle

3.2.1. Case (a): k0 6¼ 0

This may be rearranged as:

3.2.2. Case (b): k0 ¼ 0

DIMENSIONLESS AXIAL DISTANCE, Z

Fig. 3. Gas phase concentration proﬁle for counter-current ﬂow.

Consequently, the required liquid phase concentration proﬁle is expressed as:

3.3. Enhancement factor

3.3.1. Case (a): k0 6¼ 0

3.3.2.1. Sub-case for x ¼ 0 with K 1 ¼ 0 and K 2 6¼ 0.

3.4. Reduction of general model into simpliﬁed cases

For liquid phase:

For gas phase:

The solution methodology for the above equations is as follows:

For liquid phase:

Thus, the transformed concentration proﬁle turns out to be:

For gas phase:

3.4.2. Reduced model 2 (x ¼ 0, K 1 ¼ K 2 ¼ 0 and B 6¼ 1)

For liquid phase:

For gas phase:

3.4.3. Reduced model 3 (x ¼ 0, K 1 6¼ 0; K 2 ¼ 0 and B ¼ 1)

For gas phase:

Again for gas phase, we have concentration C G ¼ 0 throughout.

3.4.4. Reduced model 4 (x ¼ 0, K 1 6¼ 0; K 2 ¼ 0 and B 6¼ 1)

For liquid phase:

For gas phase:

3.4.5. Reduced model 5 (x 6¼ 0, K 1 ¼ 0; K 2 ¼ 0 and B 6¼ 1)

For liquid phase:

For gas phase:

3.4.6. Reduced model 6 (x ¼ 0, K 1 ¼ 0; K 2 ¼ 0, B ¼ 1 and dy  1)

For liquid phase:

3.5. Numerical solution of the general model

3.5.1. Numerical scheme

Discretization in liquid phases

and the associated B.Cs are:

B:C:1 : C A ði; 0Þ ¼ 0; 8i 2 ½0; N  ð57Þ

Discretization in gas phase

The B.C. for gas phase is introduced as:

B:C:1 C G ð0Þ ¼ 0: ð61Þ

3.6. Veriﬁcation of the mathematical model with the experimental results

4. Results and discussion

DIMENSIONLESS DISTANCE FROM SOLID WALL, η

DISTANCE FROM SOLID WALL, η

Fig. 12. Gas phase concentration proﬁle for counter-current ﬂow.

4.5. Reduction of general model into simple cases

4.6. Numerical scheme

3.4.6. Reduced model 6 (x ¼ 0, K 1 ¼ 0; K 2 ¼ 0, B ¼ 1 and dy 1)

B:C:1 : C A ði; 0Þ ¼ 0; 8i 2 ½0; N ð57Þ