Numerical analysis of simultaneous

heat and mass transfer during

absorption of polluted gases by
cloud droplets

T. Elperin, A. Fominykh and B. Krasovitov

Department of Mechanical Engineering

The Pearlstone Center for Aeronautical Engineering
Studies
Ben-Gurion University of the Negev
P.O.B. 653, Beer Sheva 84105, ISRAEL

Outline of the presentation

Motivation and goals
Description of the model
Results and discussion
Conclusions

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Gas absorption by cloud droplets: Scientific background

Effect of vapor condensation at the surface of stagnant droplets on the

rate of mass transfer during gas absorption by growing droplets:
uniform temperature distribution in both phases was assumed (see
e.g., Karamchandani, P., Ray, A. K. and Das, N., 1984);
liquid-phase controlled mass transfer during absorption was
investigated when the system consisted of liquid droplet, its vapor
and solvable gas (see e.g., Ray A. K., Huckaby J. L. and Shah T.,
1987, 1989);
Gas absorption by falling droplets accompanied by subsequent
dissociation reaction (see e.g., Baboolal et al. (1981), Walcek and
Pruppacher (1984), Alexandrova et al., 2004);
Simultaneous heat and mass transfer during droplet evaporation or
growth:
model of physical absorption (Elperin et al., 2005);
model taking into account subsequent dissociation reaction (Elperin
et. al, 2007).
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Absorption equilibria
Air
SO2

is the species in dissolved state

Henrys Law:
Aqueous phase sulfur dioxide/water
chemical equilibria

Droplet
Gas-liquid
interface

pollutant molecule=
pollutant captured in solution=

Electro neutrality equation:

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Description of the model

Governing equations
1. gaseous phase r > R (t)
2
r2

r vr 0
t r

2
2
2 Y j

r
Y j
vr r Y j D j r
t
r
r
r

c pTe
t

vr r 2c pTe ke r 2 e
r
r
r

(1)

Dropl
et

(2)

Far
field

ds

(3)

m A

p p Rg Te Y j M j

m L

Gasliquid
interface

j 1

2. liquid phase 0 < r < R (t)

L
2 T L
2 T

r
L r
t
r
r
YA( L )

L
2
2

r
LYA L DL r
t
r
r

Gaseous
phase

(4)

j 1,..., K 1,
K
L S IV M S ( IV )
(5) j 1Y j 1; YA

In Eqs. (2)

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Description of the model

Stefan velocity and droplet vaporization rate
The continuity condition for the radial flux of the absorbate at the droplet
surface reads:
YA L
YA
j A r R YA vs D A
DL L
(6)
r r R
r r R

Other non-soluble components of the inert admixtures are not absorbed in the
liquid
(7)
J j 4R 2 j j 0,
j 1, j A
2
r vr 0
Taking into account Eq. (7) and using anelastic approximation
r
we can obtain the expression for Stefan velocity:

DL L YA L
vs
1 Y1 r

r R

D1 Y1
1 Y1 r r R

(8)

where subscript 1 denotes water vapor species

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Description of the model

Stefan velocity and droplet vaporization rate
The material balance at the gas-liquid interface yields:

d mL
4 R 2 s v R, t R
dt

(9)

Then assuming L we obtain the following expressions for the

rate of change of droplet's radius:
L

Y
D
L
A
R
1 Y1 r

r R

D 1 Y1
L 1 Y1 r r R

(10)

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Description of the model

Stefan velocity and droplet vaporization rate
DL L YA L
vs
1 Y1 r
L

Y
D
L
A
R
1 Y1 r

r R

r R

D1 Y1

1 Y1 r r R

D 1 Y1
L 1 Y1 r r R

vs
In the case when all of the inert
admixtures are not absorbed in
liquid the expressions for Stefan
velocity and rate of change of
droplet radius read

D1 Y1
1 Y1 r r R

D 1 Y1
L 1 Y1 r r R

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Description of the model

Initial and boundary conditions
The initial conditions for the system of equations (1)(5) read:
At t = 0, 0 r R0 :
At t = 0,

r R0 :

T L T0 L

L

Y AL YA,0

Y j Y j ,0 r

Te Te,0 r

(11)

At the droplet surface:

Dj

Y j
r

Y j vs
r R

Y
YA vs D A A
r

T
ke e
r

r R

r R

dR
T L
L Lv
kL
dt
r

YA L
DL L
r

r R

Te R T L

(12)
(13)
r R

YA L
La L DL
r

(14)
r R

(15)
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Description of the model

Initial and boundary conditions
The equilibrium between solvable gaseous and dissolved in liquid species
can be expressed using the Henry's law
(16)
C S IV H *
p
A

where

S ( IV) A

H S* ( IV)

K1

K1K 2

H SO2 1

H
H
In the center of the droplet symmetry conditions yields:
T L
r

0
r 0

YA L
r

(17)

(18)

r 0

At t 0 and r the soft boundary conditions at infinity are imposed

Y j
r

0
r

Te
r

(19)

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Method of numerical solution

Spatial coordinate transformation:
r
x 1
,
for 0 r R t ;
R t
1 r

w
1 , for r R t ;
R t
The gas-liquid interface is located at x w 0;
w 0, 1 x 0, 1 Coordinates x and w can be treated identically in
numerical calculations;
2

D
t
R
Time variable transformation:
L
0;

The system of nonlinear parabolic partial differential equations (1)(5) was

solved using the method of lines;
The mesh points are spaced adaptively using the following formula:

xi

i 1

i 1, , N 1
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Results and discussion

Average concentration of the

absorbed SO2 in the droplet:
relative absorbate concentration
is determined as follows:

Figure
Dependence
average aqueous
Figure
2. 1.
Dependence
ofof
dimensionless
average
sulfur dioxide
molar concentration
vs.various
time
aqueous
SO2 concentration
vs. time for
for various
of relative
humidity.
initial
sizes ofvalues
evaporating
droplet
R0.

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Results and discussion

Figure 5. Droplet surface temperature vs. time:
Figure
4. Effect
of Stefanthe
flow
and heat of
1 model
taking
into account
equilibrium
absorption
on droplet
surface
temperature
dissociation
reactions;
2 model
of physical
(Elperin et al. 2005).
absorption.

Figure 3. Droplet surface temperature vs. time

(T0 = 278 K, T = 293 K, RH = 70%).

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Results and discussion

Figure 7. Average concentration of aqueous
sulfur species and their sum vs. time ( RH =
101%).

pH is a measure of the acidity

or alkalinity of a solution.

Figure 6. Average concentration of aqueous

sulfur species and their sum vs. time ( RH =
70%).

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Results and discussion: the interrelation between

heat and mass transport
Absorption during
droplet evaporation

Diffusion of
absorbate

Thermal effect of
absorption

Reactions of
dissociation

Decreases Stefan
velocity
Decreases vapor flux
Increases droplet surface
temperature

Decreases effective
Henrys constant

Increases
vapor flux

Decreases absorbate
flux

Decreases droplet
surface temperature

Increases Stefan
velocity

Increases effective
Henrys constant
Increases absorbate
flux

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Conclusion
The obtained results show, that the heat and mass transfer rates in water
droplet-air-water vapor system at short times are considerably enhanced
under the effects of Stefan flow, heat of absorption and dissociation reactions
within the droplet.
It was shown that nonlinearity of the dependence of droplet surface
temperature vs. time stems from the interaction of different phenomena.
Numerical analysis showed that in the case of small concentrations of SO2 in
a gaseous phase the effects of Stefan flow and heat of absorption on the
droplet surface temperature can be neglected.
The developed model allows to calculate the value of pH vs. time for both
evaporating and growing droplets. The performed calculations showed that
the dependence of pH increase with the increasing relative humidity (RH).
The performed analysis of gas absorption by liquid droplets accompanied by
droplets evaporation and vapor condensation on the surface of liquid droplets
can be used in calculations of scavenging of hazardous gases in atmosphere
by rain, atmospheric cloud evolution.

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