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State Key laboratory of Chemical Engineering, Tsinghua University, Beijing 100084, China
State Key Laboratory of OrganicInorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China
CNPC Research Institute of Safety & Environment Technology, Beijing 102206, China
a r t i c l e
i n f o
Article history:
Received 9 April 2013
Received in revised form 8 August 2013
Accepted 12 December 2013
Available online 30 October 2014
Keywords:
Separation
Absorption
Mass transfer
Packed bed
Structured packing
Carbon dioxide
a b s t r a c t
This paper studies the mass transfer performance of structured packings in the absorption of CO2 from air with
aqueous NaOH solution. The Eight structured packings tested are sheet metal ones with corrugations of different
geometry parameters. Effective mass transfer area and overall gas phase mass transfer coefcient have been
measured in an absorption column of 200 mm diameter under the conditions of gas F-factor in 0.381.52 Pa0.5
and aqueous NaOH solution concentration of 0.100.15 kmolm3. The effects of gas/liquid phase ow rates
and packing geometry parameters are also investigated. The results show that the effective mass transfer area
changes not only with packing geometry parameters and liquid load, but also with gas F-factor. A new effective
mass transfer area correlation on the gas F-factor and the liquid load was proposed, which is found to t
experiment data very well.
2014 The Chemical Industry and Engineering Society of China, and Chemical Industry Press. All rights reserved.
1. Introduction
At present, global extreme weather occurs frequently. Various natural disasters threat gravely the human survival and development. All
these are related to the climate change which is caused by greenhouse
gas emission, especially CO2 emission [1]. Reducing CO2 and ghting
against climate change have already become global consensus.
There are three main ways to reduce CO2. The rst is the control
from the source. It can reduce CO2 and even achieve zero emission
when developing clean energy and renewable energy [2]. The second
is the control during the process. Improving the energy efciency can
reduce energy consumption and thus CO2 [3], which has great potential
in practical engineering applications. The third is the control at the end.
Currently CO2 capture and storage (CCS) is the most directive and most
effective way at the end of process [46].
CCS is of wide concern, but high cost and high energy consumption
are the main bottlenecks of CCS [7,8]. Researchers have done much
work, and most work is focused on solvents and process simulation
[914]. Some research works about packings used for CO2 absorption
has been done. Aroonwilas et al. [15] researched about different
http://dx.doi.org/10.1016/j.cjche.2014.10.003
1004-9541/ 2014 The Chemical Industry and Engineering Society of China, and Chemical Industry Press. All rights reserved.
43
2. Mathematical Model
According to two-lm theory, the interface mass transfer rate is
NA K G P yA ye :
lg
X
1
I c hi
Hw HA
13
hi h h hgas
14
2
2
5 2
lgH w 9:12295:9044 10
ye 0:
The value of h+, h and hgas were cited from Danckwerts [23].
The gas phase mass transfer coefcient (kG) for structured packing
could be calculated by the relation [25]:
G
yin
ln
:
PZ
yout
G dyA
:
PyA dZ
dnA
kG P A H A C AI S EkL C AI C AL S K G P A HA C AL S
dt
15
D
G uG dh 0:8 G 0:33
:
kG 0:0338 G
dh
G cos45
G DG
5
Ae
with
1
1
H
A:
K G kG EkL
T :
16
According to Eqs. (4) and (6), the effective mass transfer area (Ae)
can be calculated by
For a tower with height of 1.77 m which was much longer than that
of this study, it is believed that Eq. (4) (an integral formula) is suitable
for calculating KGAe in this study.
The mass transfer rate from the gas lm equals to that into the liquid
lm and it can be expressed as
T 7:8857 10
K G Ae
G
yin
ln
:
PZK G
KG
yout
17
q
1 H2a
Ha
kDA OH
:
kL
CO2 analyzer
Because the reaction between CO2 and NaOH is very fast, H2a 1.
Thus, the approximate equality holds:
p
kDA OH
:
E Ha
kL
Vavle
Packed
column
CO2 analyzer
Liquid flowmeter
Gas flowmeter
10
Vavle
The reaction rate constant (k) was calculated from the relations [24]:
Tank
2382
2
0:221Ic 0:0161Ic :
lgk 11:895
T
11
3
:
lgDA 8:1764
T
T2
12
Fan
Pump
Temperature Measurement
Fig. 1. Flow diagram of experiment.
44
Table 1
Parameters for the measurement
Parameter
Numerical value
0.1 MPa
301305 K
0.100.15 kmolm3
12.744.6 m3m2h1
0.381.52 Pa0.5
148273 m2m3
30, 37.5, 45
9 mm
75, 90, 105
Table 2
Contributions of anion, cation and gas to Henry's constant for CO2
h+/m3kmol1
h/m3kmol1
t/C
hgas/m3kmol1
Na+
OH
CO2
3
0.2
15
25
40
50
60
0.007
0.01
0.019
0.026
0.029
0.016
0.091
0.066
0.066
!x
Gw
Ap G
!x
22
45
Fig. 2. Geometry and arrangement of sheet corrugated structured packings. (a) 90 rotation; (b) 0 rotation.
300
240
=45e =90eh=9mm
250
220
Fs=0.48m h-1
=30e, =75e, h = 9mm
specific area
200
Ae
Ae
200
150
Fs=0.38Pa
0.5
Fs=0.76Pa
0.5
Fs=1.14Pa
100
50
10
0.5
15
20
25
30
35
40
45
180
160
o
0 rotation
o
90 rotation
140
10
15
25
30
35
40
Lw
Lw
Fig. 3. Ae for packings with = 45 and = 90 vs. liquid load for different gas F-factors
with a packing arrangement of 90 rotation.
20
46
300
Table 3
Effective mass transfer area correlations
=45e=90eh=9mm
Onda et al.
0.5
Fs=1.14Pa
250
!0:05
0:75
0:10
Ae
C
L
Ap L2
L2
1 exp41:45
2
Ap L
Ap
L
Ap L L
L g
!0:2 3
5
specific area
18
200
Ae
Ae
C
1 exp42:85
Ap
L
0:75
L
Ap L
0:20
Ap L
2L g
!0:05
L
Ap L L
!0:18 3
5
150
19
Experiment
This study
Modified Onda
Modified Henriques de Brito
100
50
Ae
uL 0:3
0:465 L
Ap
Ap L
10
20
20
25
30
Lw
35
40
45
15
21
Table 4
Modied effective mass transfer area correlations for different packings with a packing
arrangement of 90 rotation
specific area
=45e=90eh=9mm
200
Fs=0.38Pa0.5
Ae
150
100
No
/()
/()
h/mm
x1
x2
x3
1
2
3
4
5
6
7
8
30
30
37.5
37.5
37.5
45
45
45
75
90
75
90
105
75
90
105
9
9
9
9
9
9
9
9
0.1172
0.1167
0.08556
0.05905
0.06180
0.06160
0.04543
0.05289
0.2139
0.1492
0.1213
0.1225
0.1648
0.1706
0.1913
0.2471
0.2430
0.2748
0.3548
0.4453
0.3896
0.3850
0.4221
0.3430
3.8%
3.2%
6.9%
8.1%
7.9%
5.0%
1.3%
6.5%
Experiment
This study
Modified Onda
Modified Henriques de Brito
250
50
15
20
25
30
Lw
35
40
45
200
Ae
10
Lw=12.7
Lw=15.9
150
250
Fs=0.38 Pa
=45e=90eh=9mm
Fs=0.76Pa0.5
Lw=28.7
0.5
Lw=41.4
=75e
specific area
200
30
35
/()
40
45
Ae
100
Lw=44.6
150
Experiment
This study
Modified Onda
Modified Henriques de Brito
100
50
10
15
20
25
30
35
40
45
Lw
Fig. 6. Comparison of different correlations to experimental results at the gas F-factor of
0.76 Pa0.5 for packings with = 45 and = 90.
Fig. 8. Corrugated angle vs. Ae at gas F-factor of 0.38 Pa0.5 and = 75.
47
250
250
0.5
Fs=0.76 Pa
0.5
Fs=0.76 Pa
=45e
Ae
Ae
200
200
Lw=12.7
150
=45e =75e
=45e =105e
=30e =90e
=37.5e =90e
Lw=15.9
Lw=28.7
Lw=41.4
150
70
Lw=44.6
75
80
85
90
95
100
105
100
10
110
15
20
25
/()
=45e =90e
=30e =75e
=37.5e =75e
=37.5e =105e
30
Lw
35
40
45
Fig. 12. Comparison of Ae for different packings at the gas F-factor of 0.76 Pa0.5.
Fig. 9. Addendum angle vs. Ae at gas F-factor of 0.76 Pa0.5 and = 45.
300
300
0.5
Fs=1.14Pa
0.5
Fs=0.76 Pa
250
=37.5e
200
Ae
Ae
250
Lw=12.7
200
150
Lw=15.9
Lw=28.7
Lw=41.4
Lw=44.6
150
70
75
80
85
90
100
10
95
100
105
15
=45e =75e
=45e =90e
=45e =105e
=30e =75e
=30e =90e
=37.5e =75e
=37.5e =90e
=37.5e =105e
20
25
30
35
40
45
Lw
110
/(o)
Fig. 13. Comparison of Ae for different packings at the gas F-factor of 1.14 Pa0.5.
Fig. 10. Addendum angle vs. Ae at gas F-factor of 0.76 Pa0.5 and = 37.5.
0.0110
0.0105
200
Fs=0.38 Pa
0.5
Fs=0.76 Pa
0.0100
0.5
KGAe
0.0095
Ae
150
0.0090
0.0085
0.0080
50
10
=30e =75eh =9
0.0075
100
15
=45e =75e
=45e =90e
=45e =105e
=30e =75e
=30e =90e
=37.5e =75e
=37.5e =90e
=37.5e =105e
20
25
30
Lw
35
40
=37.5e =75eh =9
0.0070
0.0065
10
=45e =75eh =9
15
20
25
30
35
40
45
Lw
45
Fig. 14. Liquid load vs. KGAe for structured packings with different corrugated angles.
Fig. 11. Comparison of Ae for different packings at the gas F-factor of 0.38 Pa0.5.
apparent that KGAe increased with the increase of liquid and gas ow
rates. As the liquid and gas ow increased, more CO2 molecules were
allowed to travel to the reaction zone, which would result in the higher
mass transfer performance. Zeng et al. [28] observed that KGAe increased
with the increase of gas ow rate using CO2NH3H2O system.
Aroonwilas and Tontiwachwuthikul [22] also used CO2NaOH system
48
28
26
=45e =90eh=9 mm
24
KG/kG /%
22
Lw=15.9
20
18
16
14
12
10
0.4
0.6
0.8
1.0
1.2
1.4
1.6
Fs /Pa0.5
Fig. 15. Proportion which gas phase mass transfer resistance accounts for in total mass
transfer resistance vs. gas F-factor.
Nomenclature
Ae
effective mass transfer area, m2m3
Ap
specic area of packings, m2m3
CAL
concentration of A at gasliquid interface, kmolm3
CAI
concentration of A in the liquid subject
DA
diffusion coefcient of A in the liquid, m2s1
dh
hydraulic diameter of packing, m
E
chemical enhancement factor
Fs
gas F-factor, Pa0.5
G
total mole gas ow rate, kmolm2s1
Gw
gas mass ow rate, kgm2s1
HA
Henry's law constant for CO2 in aqueous electrolyte solution,
kPam3kmol1
Ha
Hatta number
Hw
Henry's law constant for CO2water, kPam3kmol1
h
corrugated peak height of sheet corrugated structured
packings, mm
hgas
contributions of gas to Henry's law constant
hi
contributions of i to Henry's law constant
h+
contributions of positive ion to Henry's law constant
h
contributions of negative ion to Henry's law constant
Ic
ionic strength, kmolm3
KG
overall gas phase mass transfer
coefcient, kmolm 2s 1kPa 1
kG
gas phase mass transfer coefcient, kmolm2s1kPa1
L
liquid mass ow rate, kgm2s1
Lw
spraying density, m3m2h1
NA
interface mass transfer rate of A, kmolm2s1
P
total system pressure, kPa
S
gasliquid contact area, m2
T
temperature, K
uL
ow rate of liquid, ms1
yA
mole ratio of CO2 in the gas phase
ye
mole fraction of component in the gas phase in equilibrium
with liquid subject concentration
yin
mole fraction of component in the gas phase entering
the column
yout
mole fraction of component in the gas phase leaving
the column
Z
height of packing layer, m
Subscripts
A
CO2
e
vapor liquid equilibrium
G
gas phase
i
composition of the uid
in
gas phase entering the column
L
liquid phase
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