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ANTHROPOGENIC
SOURCES
SO2, CO2, CO – fossil
fuels burning (crude oil and
coal), chemical industry;
NOx, CO2 – boilers,
furnaces, internal
combustion and diesel
engines;
HCl – burning of
municipal solid waste
(MSW) containing certain
types of plastics
Gas absorption in the presence of inert admixtures (see e.g., Plocker U.J.,
Schmidt-Traub H., 1972);
Diffusion of pollutant
molecules through
Vapor phase
Distance traveled by the polluted molecule
A g H 2O A H 2O
the gas
Gas-liquid interface
A H 2O is the species in
Dissolution into the
liquid at the interface
dissolved state
A H 2O H A p A
Diffusion of the
dissolved species
Solution from the interface
H A is the Henry’s Law
into the bulk of the
liquid constant
= pollutant molecule
= pollutant captured in solution
Aqueous phase sulfur dioxide/water chemical equilibria
KH
SO2 H 2O
K1
H HSO
3
H SO
2
3
K w H OH
HSO
K2
pSO2 SO2 H 2O
3
H HSO 2SO
3
2
3
where
S IV SO2 H 2O HSO3
SO32
is total dissolved sulfur in solution.
Gas absorption by stagnant droplet
Description of the model
Governing equations
1. gaseous phase r > R (t) Droplet
2
Far field
r2 r vr 0 (4) Gaseous phase
t r
Z m L
Y
r 2 Y j
t
r
vr r 2Y j D j r 2 j
r r
(5) ds
d
c pTe
r2
t
r
vr r 2c pTe ke r 2 e
r
T
r
(6)
m A q R
Gas-liquid
interface
Y
2. liquid phase 0 < r < R (t)
L j
2 T 2 T L
r L r (7) X
t r r
( L)
r 2 LYA L L DL r 2 A
t r
Y
r
(8) In Eqs. (5) j 1,..., K 1,
K
Y
j 1 j
1
anelastic approximation:
vr r 2 const (11)
p ~ v2
K Yj
p p Rg Te (12)
M
j 1 j
Stefan velocity and droplet vaporization rate
The continuity condition for the radial flux of the absorbate at the droplet
surface reads:
YA YA L
j A r R YA vs DA DL L (13)
r r R r r R
Other non-solvable components of the inert admixtures are not absorbed in the
liquid
J j 4R 2 j j 0, j 1, j A (14)
Taking into account this condition and using Eq. (10) we can obtain the
expression for Stefan velocity:
DL L YA L D1 Y1
vs (15)
1 Y1 r r R
1 Y1 r r R
DL L YA L D1 Y1
vs
1 Y1 r r R
1 Y1 r r R
L
D Y ρ D 1 Y1
R L A
1 Y1 r r R
ρ L 1 Y1 r r R
D1 Y1
vs
In the case when all of the inert
1 Y1 r r R
admixtures are not absorbed in
D1 Y1
liquid the expressions for Stefan R
velocity and rate of change of L 1 Y1 r r R
droplet radius read
Initial and boundary conditions
The initial conditions for the system of equations (1)–(5) read:
L
At t = 0, 0 r R0 : T L T0 L Y AL YA,0
(18)
At t = 0, r R0 : Y j Y j ,0 r Te Te,0 r
At the droplet surface the continuity conditions for the radial flux of non-
solvable gaseous species yield:
Y j
Dj Y j v s (19)
r r R
For the absorbate boundary condition reads:
YA YA L
YA v s D A DL L (20)
r r R r r R
T dR T L YA L
ke e L Lv kL La L DL (21)
r r R
dt r r R
r
r R
Initial and boundary conditions
The equilibrium between solvable gaseous and dissolved in liquid species
can be expressed using the Henry's law
CA H A pA (22)
YA L T L
0 0 (24)
r r r 0
r 0
At t 0 and r the ‘soft’ boundary conditions at infinity are imposed
Y j Te
0 0 (25)
r r
r r
Vapor concentration at the droplet surface and
Henry’s constant
The vapor concentration (1-st species) at the droplet surface is the function
of temperature Ts(t) and can be determined as follows:
1, s p1, s Ts M 1
Y1, s R, t Y1, s Ts (26)
pM
where p p
The functional dependence of the Henry's law constant vs. temperature reads:
H A T0 H 1 1
ln (27)
H A T RG T T0
6 1
2 2
1 exp 4 2 2
n Fo
n1 n Fig. 3. Comparison of the numerical results
with the experimental data (Taniguchi &
DLt Asano, 1992) and analytical solution.
Fo
Dd
Fig. 5. Dependence of average aqueous SO2
molar concentration vs. time
Cooperative
growing cumulus ~20 mm Convective
Precipitation
Experiment (CCOPE)
University of
Wyoming
fog 8mm – 0.5 mm E. Linacre and B.
Fig. 6. Vertical distribution of SO2.
Geerts (1999) Solid lines - results of calculations
with (1) an without (2) wet chemical
orographic up to 80 mm H. R. Pruppacher and reaction (Gravenhorst et al. 1978);
J. D. Klett (1997) experimental values (dashed lines) –
drizzle ~ 1.2 mm – (a) Georgii & Jost (1964); (b) Jost
(1974); (c) Gravenhorst (1975);
Rain drops 0.1 – 2.0 mm –
Georgii (1970); Gravenhorst (1975);
(f) Jaeschke et al., (1976)
Fig. 7. Dependence of dimensionless
average aqueous CO2 concentration vs.
time (RH = 0%).
Fig. 17. Dimensionless droplet radius vs. time Fig. 18. Dimensionless droplet radius vs. time
N2/CO2/H2O gaseous mixture YH2O = 0.011. N2/CO2/H2O gaseous mixture.
Conjugate Mass Transfer during Gas Absorption
by Falling Liquid Droplet with Internal Circulation
Developed model of solvable gas absorption from the mixture with inert gas by falling
droplet (Elperin & Fominykh, Atm. Evironment 2005) yields the following Volterra
integral equation of the second kind for the dimensionless mass fraction of an
absorbate in the bulk of a droplet:
3 sin q
X b ( ) 1
PeL
(1 H A D) 0
X b ( ) (q , )
d (28)
0 L
Heat and mass fluxes extracted/delivered from/to the droplet surface (B. Krasovitov
and E. R. Shchukin, 1991):
Ts
Pe
J T 4 R1 k e dTe (29)
4 T
Where n1
c1
n - dimensionless concentration;
Pe PeT Pe D - Peclet number.
UR UR
PeT Pe D
D1
Conclusions
In this study we developed a model that takes into account the
simultaneous effect of gas absorption and evaporation
(condensation) for a system consisting of liquid droplet - vapor of
liquid droplet - inert noncondensable and nonabsorbable gas-
noncondensable solvable gas.
Droplet evaporation rate, droplet temperature, interfacial
absorbate concentration and the rate of mass transfer during gas
absorption are highly interdependent.
Thermal effect of gas dissolution in a droplet and Stefan flow
increases droplet temperature and mass flux of a volatile species
from the droplet temperature at the initial stage of evaporation.
The obtained results show good agreement with the experimental
data .
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.