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2nd International Conference on Population Balance Modelling

May 5-7, Valencia, Spain

Validation of bubble breakage, coalescence

and mass transfer models for gas-liquid
dispersion in agitated vessel
Marko Laakkonen1, Ville Alopaeus1,2, Juhani Aittamaa1

1 HelsinkiUniversity of Technology, Laboratory of Chemical Engineering

2 Neste Engineering, Porvoo, Finland
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Motivation

Gas-liquid reactors used widely in industry but

their design is problematic:
- Mass transfer limitations
- Inhomogeneous conditions in large reactors

Local conditions can be considered by combining

mass transfer models to a Computational Fluid
Dynamic (CFD) code
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Objective

RATE = FLUX × AREA

A model for mass Population balance model
transfer fluxes for bubbles
Validation against mass Validation against measured
transfer experiments local bubble size distributions

Tool for the calculation of

gas-liquid mass transfer rates
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Air – tap water in 194 dm3 vessel

Local bubble size distributions

Overall gas holdup

Power requirements of gassed

agitation

Absorption and
desorption of dissolved
oxygen
Gas sparger
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Local bubble size distributions

Capillary suction probe
R1

R2

R3 ~2000 bubbles per distribution

R4
Operating conditions
R5 Stirring 155 – 250 rpm
Gassing 0.018 – 0.093 vvm
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Comparison of techniques
Digital Imaging (DI)

C
B
Phase Doppler
Anemometry (PDA)

14 dm3 vessel
Capillary Suction Probe (CSP)
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Comparison of techniques
Number distribution Volume distribution
min. of DI
min. of CSP
max. of PDA
n(di) [-]

bubble size [mm] v(di) [-] bubble size [mm]

PDA 5 µm – 1.4 mm PDA
Imaging 0.2 mm – Imaging
Capillary 1.2 mm – 6 mm Capillary
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Multiblock model for stirred vessel

Considers local mass
transfer conditions

Simple enough for

the fitting of unknown
model parameters

Population balance
for bubbles

Multicomponent gas-liquid
mass transfer
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Relative velocity of bubbles (slip)

Affects local bubble size distributions and gas holdup è
Mass transfer area

Solved from force balance on bubble motion

Turbulence dampening correction of Bakker & Van den

Akker (1994) with a slight modification

µ = µC + C11 ?C ε 1/ 3
a 4/3

ADJUSTABLE PARAMETER
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Population balance for bubbles

dY/dt = Transportation in/out balance region +

Birth/death by breaking +
Birth/death by coalescing +
Growth/size reduction by mass transfer
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ADJUSTABLE PARAMETER

Case A Case B
Breakage rate (Alopaeus et al. 2002) Breakage rate (Luo & Svendsen, 1996)
 
g (a j ) = C1e1 / 3erfc C2 
s µC
+ C3 ε 
1/ 3
(1 + ξ )2 exp − C6σ χ ( f ) 
g (a j ) = C5 ⋅ (1 − α ) 2 
1 1
 
∫∫
2/3 5/3

?C e a j ?C ?D e1 / 3a 4j / 3  dξ df
a  ξ 11 / 3  ρ ε 2 / 3a 5 / 3ξ 11/ 3 
 j 0 ξ min  C j 
Breakage kernel
2 C4 Breakage kernel
3 3  ai2  ai3   ai3 
β (ai , a j ) =  9 + C4 + 9 ⋅ C4 + C4  3
 33 1 − 3 
2 C4
3 3  ai2  ai3   ai3 
2

β (ai , a j ) =  9 + C4 + 9 ⋅ C4 + C4  3
 33
 2 2  a j  a3j   a 
 j 
2 1 − 3 
 2 2  a j  a3j   a 
 j 

Coalescence rate Coalescence rate

(Coulaloglou & Tavlarides, 1977) (Coulaloglou & Tavlarides, 1977)

h(ai , a j )= C7 ⋅ e 1/ 3
(a + a ) (a
2 2/3
+a ) ?(a , a )
2 / 3 1/ 2
2
(
h(ai , a j )= C7 ⋅ e1 / 3 (ai + a j ) ai2 / 3 + a 2j / 3 ) ?(a , a )
1/ 2
i j
i j i j i j

Coalescence efficiency
Coalescence efficiency (Prince & Blanch, 1990)
(Coulaloglou & Tavlarides, 1977)
 rjk5 / 6 ρC1 / 2ε 1 / 3 
  λ (ai , a j ) = exp  − C9 
4
µ ρ ε  ai a j 
?(ai , a j ) = exp  − C8 C 2C   
σ 1/ 2 
σ a +a 
 i j 
  
 
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Fitting of bubble breakage and

coalescence models
70 bubble size categories needed to minimise
discretization error
Initial values of parameters by testing and from
literature

Insensitive and correlating parameters fixed on

reasonable values

All measured local BSDs from 14 and 194 dm3 vessels

included simultaneously to the fitting
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Volumetric BSDs in 194 dm3 vessel

Q=0.018 vvm Q=0.018 vvm
Q=0.041 vvm Q=0.041 vvm
v(di )

v(di )
N = 220 rpm N = 220 rpm
di di

Case A Case B
Markers (measured), Lines (simulated)
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Number BSDs in 14 dm3 vessel

n(di )

Case A
di
Case B
Digital Imaging

Stirring 340 rpm

Gassing 0.018 vvm
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Gas-liquid mass transfer fluxes

Two-film theory with simplified solution of Maxwell-
Stefan multicomponent diffusion

Validate the model by minimising the difference

between the simulated and measured concentrations
of oxygen vs. time

Mass transfer coefficients in liquid film (Kawase &

Moo-Young, 1990)

k L = C12 (ε v ) Sc −1 / 2
1/ 4

ADJUSTABLE PARAMETER
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Model vs. measured concentration of

dissolved oxygen in 194 dm3 vessel
Case A Case B

Markers (measured), Lines (validated model)

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0.28 (Prince & Blanch, 1990)

0.88 (Venneker et al. 2002)

0.02 (Bakker & Akker, 1994)

0.301 (Kawase & Moo-Young, 1990)

*not fitted at the final stage, # 95 % confidence limits

 N = 250 rpm, Q = 0.093 vvm 18(20)
Bubble surface Mass transfer rates
Gas holdup [vol-%] area [m2/m3] [10-4 mol/(sm3)]
0 0 0
1.00 1.05 1.00 19 18 15 (-3) (-2) (-2)
[6] [5] [4]

0 0 0 = water
1.09 1.14 1.05 23 20 16 (-4) (-3) (-2) = nitrogen
[9] [6] [4] = oxygen

0 0 0 0 0
1.11 0.91 0.87 25 15 13 (-5) (-2) (-1) (-5) (-5)
0.85 17 [11] [4] [3] [10] [10]
0.86 17
0 0
0(-16)[33]*/
1.22 1.30 1.06*/2.14 33 35 30*/60 (-10) (-13) -0(-33)[69]
[21] [27]
8.98 187 -101
0.85 18 0 0 0 0 -1551 (-64)
30 24 109 (-6) (-4) (-3) (-4) (-22)
1.36 1.28 0.78 7.47 15
[130]
[13] [7] [5] [8] [45]

0.93 0.71 20 20 0(-3)[7] 0(-2)[4]

Simulated (Case A) local mass transfer conditions in the 194 dm3 vessel
at the time 100 s from the moment, when pure nitrogen feed was switched to air
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Conclusions

Volumetric bubble size distributions can be

measured from air – water system with a
capillary probe

Multiblock stirred tank model is a useful tool

for the fitting of model parameters against
local experiments
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Conclusions

Good agreement between the validated

models and local bubble size / mass transfer
experiments at various agitation conditions

The validated models can be included to a

CFD program and used for the design and
scaleup of agitated gas-liquid reactors