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Article history: This paper studies the mass transfer performance of structured packings in the absorption of CO2 from air with
Received 9 April 2013 aqueous NaOH solution. The Eight structured packings tested are sheet metal ones with corrugations of different
Received in revised form 8 August 2013 geometry parameters. Effective mass transfer area and overall gas phase mass transfer coefficient have been
Accepted 12 December 2013
measured in an absorption column of 200 mm diameter under the conditions of gas F-factor in 0.38–1.52 Pa0.5
Available online xxxx
and aqueous NaOH solution concentration of 0.10–0.15 kmol·m−3. The effects of gas/liquid phase flow rates
Keywords:
and packing geometry parameters are also investigated. The results show that the effective mass transfer area
Separation changes not only with packing geometry parameters and liquid load, but also with gas F-factor. A new effective
Absorption mass transfer area correlation on the gas F-factor and the liquid load was proposed, which is found to fit
Mass transfer experiment data very well.
Packed bed © 2014 Chemical Industry and Engineering Society of China, and Chemical Industry Press. All rights reserved.
Structured packing
Carbon dioxide
1. Introduction commercial packings. Alix et al. [16] proposed a new structured packing
which generated a low pressure drop and a very high interfacial area.
At present, global extreme weather occurs frequently. Various natu- Mass transfer performance of packings was often evaluated by using
ral disasters threat gravely the human survival and development. All the systems including air–H2O–CO2 [17], air–H2O–O2 [18] and air–H2O–
these are related to the climate change which is caused by greenhouse NH3 [19], where only mass transfer process proceeds and no reaction
gas emission, especially CO2 emission [1]. Reducing CO2 and fighting occurs. In 2000, the model for predicting structured packing mass trans-
against climate change have already become global consensus. fer performance in CO2 chemical absorption was proposed [14]. Later,
There are three main ways to reduce CO2. The first is the control the effects of operating parameters on CO2 absorption in columns with
from the source. It can reduce CO2 and even achieve zero emission structured packings were obtained by using CO2–MEA system [15],
when developing clean energy and renewable energy [2]. The second and the effective mass transfer area of random packings (Raschig
is the control during the process. Improving the energy efficiency can super-rings) was studied with CO2–NaOH system [20].
reduce energy consumption and thus CO2 [3], which has great potential In comparison with random packings, structured packings are
in practical engineering applications. The third is the control at the end. made of thin corrugated metal sheets arranged side by side with
Currently CO2 capture and storage (CCS) is the most directive and most an opposing channel orientation [14], which offer excellent mass
effective way at the end of process [4–6]. transfer performance with a lower pressure drop [21]. Their specific
CCS is of wide concern, but high cost and high energy consumption area is up to 250–750 m2/m3 with a void fraction of 90%. There are
are the main bottlenecks of CCS [7,8]. Researchers have done much many kinds of commercial structured packings such as Gempak,
work, and most work is focused on solvents and process simulation Mellapak and Optifow.
[9–14]. Some research works about packings used for CO2 absorption The main objective of this study is to shed light on selection
has been done. Aroonwilas et al. [15] researched about different or development of a new structured packing used for CO2 chemical
absorption with a high efficiency. In this study, the effective mass
transfer area and overall gas phase mass transfer coefficient of
sheet metal structured packings with corrugations of different pack-
☆ Supported by the National Natural Science Foundation of China (51134017) and
PetroChina (2011E-24-09).
ing geometry parameters were measured. All of the data were ana-
⁎ Corresponding author. lyzed with respect to designing high efficient packing suitable for
E-mail address: cj-dce@tsinghua.edu.cn (J. Chen). CO2 chemical absorption.
http://dx.doi.org/10.1016/j.cjche.2014.10.003
1004-9541/© 2014 Chemical Industry and Engineering Society of China, and Chemical Industry Press. All rights reserved.
Please cite this article as: W. Yang, et al., X. Yu, Mass Transfer Performance of Structured Packings in a CO2 Absorption Tower, Chin. J. Chem. Eng.
(2014), http://dx.doi.org/10.1016/j.cjche.2014.10.003
2 W. Yang et al. / Chinese Journal of Chemical Engineering xxx (2014) xxx–xxx
2. Mathematical Model Henry's constant (HA) for CO2 in aqueous electrolyte solution could
be determined by [23]:
According to two-film theory, the interface mass transfer rate is
1 X
NA ¼ K G P ðyA −ye Þ: ð1Þ lg ¼− I c hi ð13Þ
Hw HA
The material conservation equation for the absorbed amount can be
written as
hi ¼ hþ þ h− þ hgas ð14Þ
−Gdy ¼ K G Ae P ðyA −ye ÞdZ: ð2Þ
−2 −5 2
Because of low CO2 concentration in the air, and OH− in the liquid lgH w ¼ 9:1229−5:9044 10 T þ 7:8857 10 T : ð15Þ
phase in large excess, there is no free CO2 in liquid, i.e.,
ye ¼ 0: ð3Þ The value of h+, h− and hgas were cited from Danckwerts [23] (See
Table 1).
Substituting Eq. (3) into Eq. (2) followed by integration results in The gas phase mass transfer coefficient (kG) for structured packing
could be calculated by the relation [25]:
G yin
K G Ae ¼ ln : ð4Þ D ρG uG dh 0:8 μ G 0:33
PZ yout kG ¼ 0:0338 G : ð16Þ
∘
dh μ G cos45 ρG DG
Though some authors (for example [22]) calculated KGAe by
According to Eqs. (4) and (6), the effective mass transfer area (Ae)
G dyA can be calculated by
K G Ae ¼ : ð5Þ
PyA dZ
K G Ae G yin
Ae ¼ ¼ ln : ð17Þ
For a tower with height of 1.77 m which was much longer than that KG PZK G yout
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 film equals to that into the liquid 3. Experimental Facility and Methods
film and it can be expressed as
The experimental facility and process are shown in Fig. 1. The
dn column was about 1.2 m tall with an inside diameter of 200 mm, in
− A ¼ kG ðP A −H A C AI ÞS ¼ EkL ðC AI −C AL ÞS ¼ K G ðP A −HA C AL ÞS ð6Þ
dt which the height of packed section is 0.8 m. Sheet corrugated structured
packing was packed in the column to promote contact between the gas
with and liquid phases. Air entered at the bottom of the column and flowed
upward, while NaOH solution was pumped to the top of the column
1 1 H
¼ þ A: ð7Þ and flowed downward. After absorption, NaOH solution returned to
K G kG EkL
the tank for cycling while the air exhausted from the top.
pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
ffi
kDA ½OH−
Ha ¼ : ð9Þ
kL
Packed
CO2 analyzer
column
Because the reaction between CO2 and NaOH is very fast, H2a ≫ 1.
Thus, the approximate equality holds: Liquid flowmeter
pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
ffi Gas flowmeter
kDA ½OH−
E ¼ Ha ¼ : ð10Þ
kL
Vavle
The reaction rate constant (k) was calculated from the relations [24]:
Tank
2382 2
lgk ¼ 11:895− þ 0:221Ic −0:0161Ic : ð11Þ
T
Fan
Pump
Because the concentration of NaOH is small (0.10–0.15 kmol·m−3) Temperature Measurement
and the viscosity of the solution is close to that of water, the effect of
solution viscosity on the diffusion coefficient for CO2 in the solution Fig. 1. Flow diagram of experiment.
(DA) can be ignored. So DA was calculated from the relation [23]:
During steady operation, the concentrations of CO2 in the gas entering
712:5 2:591 105 and leaving the column were measured respectively using an infrared gas
lgDA ¼ −8:1764 þ − : ð12Þ
T T2 analyzer with the precision of ±2 ml·m−3, while the concentration of
Please cite this article as: W. Yang, et al., X. Yu, Mass Transfer Performance of Structured Packings in a CO2 Absorption Tower, Chin. J. Chem. Eng.
(2014), http://dx.doi.org/10.1016/j.cjche.2014.10.003
W. Yang et al. / Chinese Journal of Chemical Engineering xxx (2014) xxx–xxx 3
NaOH solution was measured by double-tracer technique. From these 90° rotation arrangement allowed the liquid to spread not only from
measurements, the values of Ae and KGAe can be obtained. With the oper- side to side but also from front to back in the column. So the wetted
ation conditions changed, the mass transfer performance of different area increased.
packings can be studied. Table 2 lists the conditions for the measurement.
(See Table 2.) 4.2. Correlations for Ae
In order to study the effect of corrugated angle (α) on the mass
Correlations for Ae by Onda et al. [27] and Henriques de Brito et al. [25]
listed in Table 3 were tested to calculate Ae in this experiment. For com-
Table 1
Contributions of anion, cation and gas to Henry's constant for CO2
parison the parameters in the two correlations were regressed according
to the results for the packing with α = 45°, β = 90°, h = 9 mm of this
h+/(m3·kmol−1) h−/(m3·kmol−1) t/(°C) hgas/(m3·kmol−1) study. The calculated value and experimental value under different gas
+ −
Na 0.091 OH 0.066 0.2 −0.007 F-factors were shown in Figs. 5–7 respectively. It showed that although
CO32− 0.066 15 −0.01 the trends were the same, results calculated by Onda et al. and Henriques
25 −0.019
de Brito et al. could not predict Ae correctly with different gas flow rates.
40 −0.026
50 −0.029 The average relative error of new correlated Onda et al. correlation (19)
60 −0.016 was 18.0% while for the new correlated Henriques de Brito et al. correla-
tion (21) was 18.2%.
Onda et al. [27] considered that Ae did not change with gas flow rate.
Henriques de Brito et al. [25] discovered that Ae remained unaffected by
Table 2 Fs for packings with less specific area. So in their correlations, there was
Parameters for the measurement not a gas flow rate. However, it was found in this study that Ae improved
Parameter Numerical value with the increase of gas flow rate. In this paper, the correlation by
Pressure for both top and bottom of the tower 0.1 MPa
Henriques de Brito et al. [25] was modified so that the effect of gas
Temperature 301–305 K flow rate could be considered. The new correlation was in the following
Concentration for NaOH solution 0.10–0.15 kmol·m−3 form:
Spraying density 12.7–44.6 m3·m−2·h−1
pffiffiffi
Gas F-factor ( F s ¼ uG ρ) 0.38–1.52 Pa0.5 !x !x
Specific area for sheet corrugated structured packings 148–273 m2·m−3 Ae ρ u 2
Gw 3
¼ x1 L L : ð22Þ
Corrugated angle of packing sheet α (Fig. 2) 30°, 37.5°, 45° Ap Ap μ L Ap μ G
Corrugated peak height h (Fig. 2) 9 mm
Addendum angle β (Fig. 2) 75°, 90°, 105°
According to experimental results, the modification was conducted by
multiple linear regressions to identify new coefficients x1, x2 and x3. The
transfer, packings with α of 30°, 37.5° and 45° were used in this study correlations for the packings with different geometry parameters were
at the condition of small liquid/gas flow ratios usually used in the pro- shown in Table 4. The comparison of experimental Ae and calculated Ae
cess of CO2 absorption. by Eqs. (19), (21) and (22) were shown in Figs. 5–7.
For the packing with α = 45°, β = 90°, h = 9 mm in Figs. 5–7, the
4. Results and Discussion modified correlation Eq. (22) obtains the average relative error for Ae
as 1.3%, compared with 18.0% of Eq. (19) and 18.2% of Eq. (21). So the
4.1. Measurement of Ae modified correlations with the consideration of effects of gas flow
rates showed better agreement.
Under the condition of normal pressure and temperature, the gas
flow rate was maintained and the liquid flow rate was altered. By mea- 4.3. The effect of geometry parameters on Ae
suring the CO2 concentration in the gas entering and leaving the column
and NaOH concentration of the solvent, the effective mass transfer area There are three main geometry parameters of sheet corrugated
could be measured and calculated. Then, with the liquid flow rate main- structured packings. They are corrugated angle (α), corrugated peak
tained, the gas flow rate was changed. So the effective mass transfer height (h) and addendum angle (β) respectively. This paper tried to
area under different gas and liquid flow rates could be measured and change one parameter while fixing the other two parameters. Packings
calculated. with different geometry parameters were tested so that the effect of α
Fig. 3 showed that Ae was affected positively by gas and liquid flow and β on Ae could be studied.
rates. Wilson [26] also discovered the same results. Alix et al. [16] dis- When β of 75° was fixed, an example for the results of α variation was
covered that Ae of a new structured packing 4D-50% also increased shown in Fig. 8. At the Fs of 0.38 Pa0.5 when Lw was below 41.4 m3/m2·h
with the increase of gas and liquid flow rates, because an increase in packing with α of 45° exhibited the biggest Ae, while Lw was above
wetted packing surface facilitated the mass transfer. It is worth noting 41.4 m3/m2·h packing with α of 30° performed best. At the Fs of
that when the flow rate of gas and liquid increased to a certain value, 0.76 Pa0.5 or 1.14 Pa0.5, when Lw was below 15.9 m3/m2·h packing with
Ae would exceed the specific area of packing material. This is consistent α of 37.5° exhibited the biggest Ae, while Lw was above 15.9 m3/m2·h
with the fact that Ae was larger than the specific area of packings at a packing with α of 30° performed best.
sufficiently high liquid flow rate [20]. At the high flow rate, the instabil- Two examples for the results of β variation were shown in Figs. 9 and
ities in the liquid flow (like ripples or waves, detachment and fragmen- 10. At α of 45°, packing with β of 75° performed best except when Fs =
tation of the film into copious liquid showers) led to this phenomenon. 0.76 Pa0.5 and Lw = 44.6 m3/m2·h. However at α of 37.5°, when Fs =
The pattern of packing arrangement impacts the performance of 0.76 Pa0.5 or 1.14 Pa0.5, packing with β of 90° performed best. In brief
mass transfer. At the condition of the same gas and liquid flow rate, Ae the effect of α and β was also affected by gas/liquid flow rates. Under
was obtained with two arrangement ways of successive packings as most gas/liquid flow rates in this study, α = 30° and β = 75° were
illustrated in Fig. 2. From Fig. 4 Ae of packings with a 90° rotation was the best parameters. Aroonwilas et al. [15] also observed that corrugated
over 30% bigger than that with a 0° rotation. The result was similar to angles had important impact on mass transfer performance.
that in [15]. Aroonwilas et al. discovered that packings with a 90° rota- Packings with different geometry parameters exhibited different
tion provided a great and comparable efficiency. It was possible that a effective mass transfer area. In this study, eight different packings were
Please cite this article as: W. Yang, et al., X. Yu, Mass Transfer Performance of Structured Packings in a CO2 Absorption Tower, Chin. J. Chem. Eng.
(2014), http://dx.doi.org/10.1016/j.cjche.2014.10.003
4 W. Yang et al. / Chinese Journal of Chemical Engineering xxx (2014) xxx–xxx
Fig. 2. Geometry and arrangement of sheet corrugated structured packings. (a) 90° rotation; (b) 0° rotation.
300
240 3
Fs=0.48m /h
¢=45e,£=90e,h=9mm
250 α =30e, β =75e, h = 9mm
220
specific area
200 200
Ae
Ae
180
150
0.5
Fs=0.38Pa 160
100 0.5 o
Fs=0.76Pa 0 rotation
o
0.5 140 90 rotation
Fs=1.14Pa
50 10 15 20 25 30 35 40
10 15 20 25 30 35 40 45
Lw Lw
Please cite this article as: W. Yang, et al., X. Yu, Mass Transfer Performance of Structured Packings in a CO2 Absorption Tower, Chin. J. Chem. Eng.
(2014), http://dx.doi.org/10.1016/j.cjche.2014.10.003
W. Yang et al. / Chinese Journal of Chemical Engineering xxx (2014) xxx–xxx 5
Table 3 300
Effective mass transfer area correlations
¢=45e,£=90e,h=9mm
Onda et al. 0.5
250 Fs=1.14Pa
2 !−0:05 !0:2 3
0:75 0:10 specific area
Ae σC L Ap L2 L2
¼ 1− exp4−1:45 2
5
Ap σL Ap μ L ρL g Ap ρL σ L
200
Ae
Recorrelated for the present packing with α = 45°, β = 90°, h = 9 mm:
150
!0:191
Ae ρ u
¼ 0:414 L L
Ap Ap μ L
Table 4
Modified effective mass transfer area correlations for different packings with a packing
arrangement of 90° rotation
specific area No α β h x1 x2 x3 ε
¢=45e,£=90e,h=9mm 1 30 75 9 0.1172 0.2139 0.2430 3.8%
200
Fs=0.38Pa0.5 2 30 90 9 0.1167 0.1492 0.2748 3.2%
3 37.5 75 9 0.08556 0.1213 0.3548 6.9%
4 37.5 90 9 0.05905 0.1225 0.4453 8.1%
5 37.5 105 9 0.06180 0.1648 0.3896 7.9%
150 6 45 75 9 0.06160 0.1706 0.3850 5.0%
7 45 90 9 0.04543 0.1913 0.4221 1.3%
Ae
100 Experiment
This study
Modified Onda 250
Modified Henriques de Brito
50
10 15 20 25 30 35 40 45
Lw
200
Lw=12.7
150 Lw=15.9
200 100
30 35 40 45
¢
Ae
150 Fig. 8. Corrugated angle vs. Ae at gas F-factor of 0.38 Pa0.5 and β = 75°.
Experiment
This study
Modified Onda
100 Modified Henriques de Brito
Please cite this article as: W. Yang, et al., X. Yu, Mass Transfer Performance of Structured Packings in a CO2 Absorption Tower, Chin. J. Chem. Eng.
(2014), http://dx.doi.org/10.1016/j.cjche.2014.10.003
6 W. Yang et al. / Chinese Journal of Chemical Engineering xxx (2014) xxx–xxx
250 250
0.5 0.5
Fs=0.76 Pa Fs=0.76 Pa
¢=45e
200
Ae
Ae
200
Lw=12.7 150
α =45eβ =75e α =45e β =90e
Lw=15.9
α =45eβ =105e α =30eβ =75e
Lw=28.7 α =30eβ =90e α =37.5eβ =75e
Lw=41.4 α =37.5e β =90e α =37.5e β =105e
Lw=44.6 100
150 10 15 20 25 30 35 40 45
70 75 80 85 90 95 100 105 110
Lw
£
Fig. 9. Addendum angle vs. Ae at gas F-factor of 0.76 Pa0.5 and α = 45°. Fig. 12. Comparison of Ae for different packings at the gas F-factor of 0.76 Pa0.5.
300
300 0.5
Fs=1.14Pa
0.5
Fs=0.76 Pa
250
¢=37.5e
250
Ae
200
Ae
Lw=12.7
α =45e β =75e α =45eβ =90e
200 Lw=15.9 150
α =45e β =105e α =30e β =75e
Lw=28.7 α =30e β =90e α =37.5e β =75e
Lw=41.4 α =37.5e β =90e α =37.5e β =105e
Lw=44.6 100
10 15 20 25 30 35 40 45
150
70 75 80 85 90 95 100 105 110 Lw
£
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 α = 37.5°.
0.0110
0.0105
200 0.5
Fs=0.76 Pa
Fs=0.38 Pa
0.5
0.0100
0.0095
0.0090
KGAe
150
0.0085
Ae
0.0080
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 flow mass transfer performance. Zeng et al. [28] observed that KGAe increased
rates. As the liquid and gas flow increased, more CO2 molecules were with the increase of gas flow rate using CO2–NH3·H2O system.
allowed to travel to the reaction zone, which would result in the higher Aroonwilas and Tontiwachwuthikul [22] also used CO2–NaOH system
Please cite this article as: W. Yang, et al., X. Yu, Mass Transfer Performance of Structured Packings in a CO2 Absorption Tower, Chin. J. Chem. Eng.
(2014), http://dx.doi.org/10.1016/j.cjche.2014.10.003
W. Yang et al. / Chinese Journal of Chemical Engineering xxx (2014) xxx–xxx 7
28
will be used to evaluate the performance of mass transfer with different
26 packings.
24 α =45e,β =90e,h=9 mm
Nomenclature
22
Lw=15.9 Ae effective mass transfer area, m2·m−3
KG/kG (%)
Please cite this article as: W. Yang, et al., X. Yu, Mass Transfer Performance of Structured Packings in a CO2 Absorption Tower, Chin. J. Chem. Eng.
(2014), http://dx.doi.org/10.1016/j.cjche.2014.10.003
8 W. Yang et al. / Chinese Journal of Chemical Engineering xxx (2014) xxx–xxx
Please cite this article as: W. Yang, et al., X. Yu, Mass Transfer Performance of Structured Packings in a CO2 Absorption Tower, Chin. J. Chem. Eng.
(2014), http://dx.doi.org/10.1016/j.cjche.2014.10.003
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