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Gas Absorption

Gas Absorption

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Published by Sagar Fuldeore
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Chemical Engineering Science 55 (2000) 2793
}
2812
Heterogeneous mass transfer models for gas absorption in multiphasesystems
D. W. F. Brilman
*
, M. J. V. Goldschmidt, G. F. Versteeg, W. P. M. van Swaaij
Uni
v
ersity of Twente, Department of Chemical Engineering, PO Box 217, 7500 AE Enschede, The Netherlands
Received 15 March 1998; accepted 23 August 1999
Abstract
Heterogeneous, instationary 2-D and 3-D mass transfer models were developed to study the e
ect of dispersed liquid-phasedroplets near the gas
}
liquid interface on the local gas absorption rate. It was found among other things that droplets (or particles)in
#
uence local mass transfer rates over an area exceeding largely the projection of the droplets on the gas
}
liquid interface. Fora speci
"
c application particle
}
particle interaction was studied and could be described by a single parameter, depending only on theminimum interparticle distance. For gas absorption
#
ux prediction an unit cell must be de
"
ned. The sensitivity of the absorption
#
uxto the de
"
nition of the unit cell was investigated. Finally, a complete strategy to arrive at gas absorption
#
ux prediction from singleparticle simulations has been proposed.
2000 Elsevier Science Ltd. All rights reserved.
 Keywords:
Mass transfer; Heterogeneous model; Enhancement; Multiphase
1. Introduction
In three-phase reactors, gas
}
liquid
}
solid or gas
}
liquid
}
liquid, frequently the absorption rate of a (spar-ingly) soluble gas-phase reactant to the reaction phase israte determining (see e.g. Beenackers & van Swaaij,1993).The gas
}
liquidmasstransferrate maybe enhancedsigni
"
cantly by the presence of a
"
nely dispersed, liquidor solid, phase present in the bulk liquid phase. This wasshown experimentally by among others Kars, Best andDrinkenburg (1979) and Alper and Deckwer (1981) forthe addition of 
"
ne solid particles to a gas
}
liquid system.The addition of 
"
ne particles caused an enhancement of the speci
"
c gas absorption rate (per unit of driving forceand interfacial area, based on the two-phase system),whereas larger particles showed almost no e
ect.The increase of the speci
"
c gas absorption rate, at unitdrivingforce andunit interfacialarea, due to the presenceof the dispersed phase can be characterized by an en-hancement factor,
E
. This enhancement factor is de
"
nedas the ratio of the absorption
#
ux in the presence of theparticles (which can be solid particles or liquid droplets)to the absorption
#
ux at the same hydrodynamic condi-tions and driving force for mass transfer without such
*
Corresponding author. Tel.: 0031-534894479; fax: 0031-534894774.
particles respectively. Using this de
"
nition, possible ef-fects of the presence of particles on the gas
}
liquid inter-facial area and on local hydrodynamics are taken intoaccount. For a complete and more detailed review thereader is referred to Beenackers and van Swaaij (1993).The enhancement of the speci
"
c absorption
#
ux due tothe presence of 
"
ne particles has been explained by theso-called
&
grazing
'
- or
&
shuttle
'
- mechanism, see Karset al. (1979) or Alper, Wichtendahl and Deckwer (1980).According to this shuttle-mechanism particles travel fre-quently between the stagnant mass transfer zone (accord-ing to the
"
lm theory) at the gas
}
liquid interface and theliquid bulk. Due to preferential absorption of the di
us-ing gas-phase component in the dispersed phase particlesthe concentration of this gas-phase reactant in the liquidphase near the interface will be reduced, leading to anincreased absorption rate. After a certain contact time,the particle is returned to the liquid bulk where the gas-phase component is desorbed owing to the local concen-tration di
erences and the particles are regenerated. Thisshuttle mechanism requires that the dispersed phase par-ticles are smaller than the stagnant mass transfer
"
lmthickness,
$
according to the
"
lm theory. For gas ab-sorption in aqueous media in an intensely agitated con-tactor, a typical value for
N
is approximately 10
}
20
m,whereas for a (laboratory) stirred cell apparatus thisvalue is typically about a few hundred microns.
0009-2509/00/$-see front matter
2000 Elsevier Science Ltd. All rights reserved.PII: S0 0 09 -2 5 0 9 (9 9 ) 0 0 4 91 - 1
 
Nomenclature
A
area, m
BCG Basic Composite Grid,
c
concentration, mol/m
D
di
usion coe
$
cient, m
/s
D
0
relative di
usion coe
$
cient
+
"
D
B
D
A
,
,dimensionless
d
characteristic particle diameter, m
d
N
particle diameter, m
d
B
drop diameter, m
E
enhancement factor, dimensionless
G
gas phase,
I
interaction parameter, dimensionless
J
mass transfer
#
ux, mol/m
s
k
*
liquid side mass transfer coe
$
cient, m/s
¸
distance to the gas
}
liquid interface, m
m
0
relative solubility or distribution coe
$
cient,dimensionless
N
number of particles, dimensionless
r
radial position, dimensionless
R
chemical reaction rate, mol/m
s
R
B
,
R
@
radius of droplet and bubble, respectively, mspc single particle cell
t
time, s
w
minimum (surface-to-surface)distance betweenparticles, m
x
position perpendicular to gas
}
liquidinterface, m
y
position along the gas
}
liquid interface, m
Greek letters
mass transfer zone near interface, m
N
penetration depth, m

fraction dispersed phase, dimensionless
Hatta number, dimensionless
gas
}
liquid contact time, s
Subscripts and superscripts
av average value
b
bubblebulk at bulk liquid phase conditionscon continuous phase
d
dropletdis dispersed phase
"
lm according to the
"
lm theorygas gas phasehet heterogeneous (model)hom homogeneous (model)max maximum
p
physical absorptionOwing to a particle size distribution also in applica-tions where the mean particle diameter is relatively large,a signi
"
cant enhancement of the gas absorption rate maybeobserved.This was con
"
rmedexperimentallyby Tingeand Drinkenburg (1995), who added very
"
ne particles toa slurry consisting already of larger ones and found thatthe enhancement of gas absorption to be similar to theenhancement of the gas absorption rate due to the addi-tion of only the same amount of 
"
ne particles to a clearliquid. Such size distributions will certainly occur in caseof gas absorption (or solids dissolution) in a liquid
}
liquiddispersion. Nishikawa et al. (1994) have shown forliquid
}
liquid systems that the e
ect of aeration isa broadening of the droplet size distribution, i.e. more
"
ne droplets. This implies that especially for gas
}
liquid
}
liquid systems enhancement of gas absorptioncan be expected when, of course, the solubility of thedi
using component in the dispersed liquid phase ex-ceeds the solubility in the continuous liquid phase.Experimentally, the gas absorption enhancement phe-nomenon in multiphase systems was frequently studiedand a summary of relevant studies is given in Table 1.Three types of (reaction) systems have been studied ex-perimentally; physical absorption experiments, systemswith a
"
rst-order reaction for the di
using component inthe continuous phase and one for a
"
rst-order reaction inthe dispersed phase. No experimental study concerningthe in
#
uence of an additional second liquid phase on theselectivity for multi-reaction systems has been found inliterature.All presented experiments show that mass transfer andchemical reaction in mass transfer limited gas
}
liquidsystems can be signi
"
cantly enhanced by the addition of a second dispersed liquid phase with a good solubility(
m
0
*
10) of the solute. Enhancement factors up to 26have been found experimentally, though usually the en-hancement factor
E
is within the range 1
}
5. Some typicalexperimentalresults ofthe enhancement factorvs. disper-sed liquid-phase hold up, as observed in G
}
L
}
L systems,are shown in Fig. 1. Note that these results are allobtained using labscale equipment.In order to elucidate and/or describe the enhancemente
ect many theoretical models were developed. Thesecan be categorized by using the model characterizations
&
stationary
'
or
&
instationary
'
models and
&
(pseudo-) ho-mogeneous
'
models or
&
heterogeneous
'
models. For theheterogeneous models a subdivision in one-dimensional,two-dimensional and three-dimensional models can bemade, see Table 2. In Table 3 the models presented inliterature are summarized in more detail.
2794
D. W. F. Brilman et al.
Chemical Engineering Science 55 (2000) 2793
}
2812
 
Table 1Overview of experimental work on gas absorption enhancement for G
}
L
}
L systems and for some other systemsAuthors System type System Apparatus Characteristics Geometric sizesMehra and Sharma(1985); Mehra, Panditand Sharma (1988-II)G
}
L
}
L Absorption of isobutylene, butene-1and propylene in emulsions of chlorobenzene in aqueous solutionsof sulphuric acidStirred cell
"
1
}
15
d
B
"
1
}
12
m

"
0.02
}
0.30
1
d
B
2
+
2
m
E
"
1.5
}
26
N
+
100
m
m
0
isobutene: 16171-Butene: 2014Propylene: 396Bruining, Joosten,Beenackers and Hofman(1986)G
}
L
}
L Oxygen absorption into emulsionsof hexadecane in sodium sulphateStirred cell
+
0.2
d
B
)
10
m

"
0.01
}
0.08
N
+
23.5
m
E
"
1
}
1.4
m
0
"
11.6Littel et al. (1994) G
}
L
}
L Physical absorption of CO
andpropylene into toluene/wateremulsionsStirred cell

"
0.01
}
0.39
d
B
)
3
mLaminar
"
lm
E
"
1
}
4.1
 


+
300
m
m
0
: CO
"
2.85
 


+
65
mPropylene
"
103Venugopal and Mehra(1994)G
}
L
}
L Absorption of CO
into emulsionsof aqueous sodium hydroxide in2-ethyl hexanolStirred cell
+
6.4
d
B
"
5
}
8
m

"
0.05
}
0.2
N
+
400
m
E
"
2.4
}
3.8
m
0
CO
"
1.9Van Ede et al. (1995) G
}
L
}
L Oxygen absorption into emulsionsof octene in sodium sulphateStirred cell
+
0.2
d
B
"
22
m

"
0.05
}
0.5
N
+
25
m
E
"
1.5
}
3.7
m
0
+
18Kars et al. (1979) G
}
L
}
S Absorption of propane in a slurryof active carbon in waterStirred cell
E
+
1.3
d
B
"
30
}
530
m

"
0.5
}
5 wt%
N
+
20
mAlper et al. (1980) G
}
L
}
S Absorption of CO
in an aqueouscarbonate-bicarbonate bu
er withcarbonic anhydrase supp. onoxirane-acrylic beadsStirred cell
+
0.32
d
B
"
1
}
20
m

"
0
}
0.5 wt%
N
+
37.5
m
E
"
1.2
}
3.5Pal, Sharma and Juvekar(1982)G
}
L
}
S Oxidation of aqueous sodiumsulphite in the presence of activatedcarbonStirred cell
+
2.7
d
B
"
1.7 and 4.3
m

"
0.01
}
2.0 wt%
N
+
56
m
E
"
1.4
}
1.9Mehra et al. (1988) S
}
L
}
L Alkaline hydrolysis of solid estersin emulsions of chlorobenzenein aqueous solution of potassiumhydroxideStirred cell
"
0.4
}
1.9
d

U
"!.
"
235
m

"
0.005
}
0.20
d
"!.
"
195
m
E
"
1.7
}
12
d
.
"
120
m
m
0
:
PB
"
5170
d
B
"
1
}
12
m2,4-DCPB
"
8890
1
d
B
2
+
3
}
4
mDCPB
"
7085
N
+
240
mTinge, Mencke andDrinkenburg (1987)G
}
L
}
S Absorption of a mixture of propaneand ethene in a slurry of activatedcarbon in waterStirred cell

"
0.01
d
B
"
40
}
63
m and
m
0

"
65 500
}
630
m
m
0

"
1500
N
(
100
mRols, Condoret, Fonadeand Goma (1990)G
}
L
}
L
}
S Oxygen absorption into emulsionsof 
n
-dodecane and per
#
uoro-carbonin water, in a culture of aerobacteraerogenesFermentationbroth

"
0.02
}
0.34
d
B

"
0.5
}
5
m
E
"
1.1
}
3.5
d
B

"
0.5
}
50
m
m
0
L
U
"
7.7
d
@
"
500
}
5000
m
m
0

"
17Junker et al. (1989-I) G
}
L
}
L
}
S Oxygen absorption inaqueous/per
#
uorocarbonfermentation systemsFermentationbroth

"
0.1
}
0.95
d
B
"
50
}
100
m
E
"
5
}
10
d
@
"
300
m
m
0

"
22
N
"
15
mVan der Meer, Beenackers,Burghard, Mulder andFok et al. (1992)G
}
L
}
L
}
S Oxygen absorption into emulsionsof 
n
-octane in water, in culture of pseud. olevoransFermentationbroth

"
0.05
}
0.11
d
B
"
0.5
m
E
"
1.1
}
1.6
N
"
5
m
The advantage of the homogeneous models is theirnumerical simplicity (for simple cases they can even besolved analytically) and short computation times. Forthese homogeneous models the following assumptionsare generally made.
E
the dispersed phase droplets are very small with re-spect to the mass transfer
"
lm thickness according tothe
"
lm theory,
E
the dispersed phase (a continuum) is homogeneouslydistributed throughout the continuous phase,
E
there is no direct gas-dispersed phase contact,
E
transport occurs only through the continuous phase,
E
mass transfer resistances within the dispersed phaseare neglected.Clearly, some of these assumptions are questionable. Theresults obtained with these models, however, do predict
 D. W. F. Brilman et al.
Chemical Engineering Science 55 (2000) 2793
}
2812
2795

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