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ScienceDirect
Energy Procedia 114 (2017) 1665 – 1670

13th International Conference on Greenhouse Gas Control Technologies, GHGT-13, 14-18

November 2016, Lausanne, Switzerland

Overall Mass Transfer Coefficient of CO2 Absorption in a

Diameter-varying Spray Tower
Xiaomei Wua,b, Min Hea,b, Yunsong Yua, Zhen Qina,b, Zaoxiao Zhanga,b,*
a
School of Chemical Engineering and Technology, Xi’an Jiaotong University, No.28 Xianning West Road, Xi’an 710049, P.R. China
b
State Key Laboratory of Multiphase Flow in Power Engineering, Xi’an Jiaotong University, No.28 Xianning West Road, Xi’an 710049, P.R.
China

Abstract

The application of spray towers for CO2 capture is a development trend in recent years. However, most of the previous jobs were
conducted in a cylindrical tower by using a single spray nozzle, whose configuration and performance is not good enough for
industrial application. To solve this problem, the present work proposed a diameter-varying spray tower and a new spray mode of
dual-nozzle opposed impinging spray to enhance the absorption performance of CO2 spray absorption process. Experiments were
conducted to investigate the effects of varies operating parameters on the overall mass transfer coefficient in various operating
conditions. Experimental results showed that liquid to gas ratio and mole ratio of MEA to CO2 are key factors which affect the
performance of CO2 absorption process and the maximum overall mass transfer coefficient for the diameter-varying dual-nozzle
opposed impinging spray tower is 0.4773 kmol·m-3·h-1·kPa-1.
© 2017
© 2017TheTheAuthors.
Authors. Published
Published by by Elsevier
Elsevier Ltd.Ltd.
This is an open access article under the CC BY-NC-ND license
Peer-review under responsibility of the organizing committee of GHGT-13.
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
Peer-review under responsibility of the organizing committee of GHGT-13.
Keywords: CO2 capture; diameter-varying spray tower; overall mass transfer coefficient; absorption performance

1. Main text

Carbon capture and storage from large point emission sources is promising to mitigate the climate [1,2]. Among
all the techniques, chemical absorption with amine based solvents is recognized as the most promising option for
separating CO2 from fossil-fuel flue gas [3]. The main obstacle for the application of conventional amine scrubbing

* Corresponding author. Tel.: +86-29-82660689; fax: +86-29-82660689.

E-mail address: zhangzx@xjtu.edu.cn

1876-6102 © 2017 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
Peer-review under responsibility of the organizing committee of GHGT-13.
doi:10.1016/j.egypro.2017.03.1295
1666 Xiaomei Wu et al. / Energy Procedia 114 (2017) 1665 – 1670

Nomenclature
ae effective contacting area, m2·m-3 CG gas concentration, vol %
-3
CL amine concentration, kmol·m d diameter, m
-2 -1
GI inert gas flow rate, kmol·m ·h KGae overall mass transfer coefficient, kmol·m-3·h-1·kPa-1
P pressure, MPa qG molar gas flow rate, kmol·m-3·h-1
S cross-sectional area, m2 T temperature,ć
*
yCO2 ,G mole fraction in gas phase yCO 2
equilibrium mole ratio in gas phase

YCO2 ,G mole ratio in gas phase Z tower height, m

¬ proportionality coefficient

technology is its high energy consumption in regeneration process, leading to the extremely high operating cost for
industrial application [4,5].
In order to reduce the cost, apart from choosing good absorbent, it is very important to select effective reactor and
proper operating conditions [6]. This paper focuses on the enhancement of CO2 absorption process by using an
improved diameter-varying spray tower. As mentioned in literature, CO 2 absorption in spray tower mainly occurs in
the nozzle exit, hence increasing the space of nozzle exit is a feasible way to enhance the absorption performance
[7,8]. The reaction sections of the proposed spray tower are composed of two parts: the cylindrical section and the
conical section. The existence of the conical section would lead to an increase of the effective contacting area and
gas-liquid contacting time, which will enhance the CO2 absorption performance. A new spray mode of dual-nozzle
opposed impinging spray was also proposed to enhance the absorption performance. When droplets from two
opposite spray nozzles impinge and exchange momentum in the centre of the tower, the droplets breakup into
smaller size which would cause a rapid increase of interfacial area between the gas and liquid phases, leading to
better heat and mass transfer performance. The performance of the proposed diameter-varying dual-nozzle opposed
impinging spray tower was evaluated experimentally under various operating conditions to reveal the effects of
process parameters on the overall mass transfer coefficient.

2. Experimental Method

2.1. System description

The flow chart of CO2 spray absorption process is shown in Fig. 1. The diameter-varying spray tower is uniquely
fabricated with two spray nozzles locating on the opposite side and at the upper part. Fig. 1 only shows one side of
the gas and liquid inlets for clear process description. During the experiment, aqueous MEA solution is pumped
through the spray nozzles to form droplets, then contact with the gas mixture entered from the bottom of the tower.
The CO2 concentration in the gas mixture is continuously measured at both gas inlets and gas outlets, using an
infrared gas analyzer. The range of the analyzer is 0-20.0% of CO2 by volume with the accuracy of 0.1% of the full-
scale reading. Experiments are repeated to validate the reproducibility of the results. The geometry of the diameter-
varying spray tower and the operating parameters in experiments are listed in Table 1.
 Xiaomei Wu et al. / Energy Procedia 114 (2017) 1665 – 1670 1667

*DVIORZ 3UHVVXUH
PHWHU JDXJH
3

'U\LQJ
&RPSXWHU
WRZHU
1 &2


&2
DQDO\]HU
6SUD\ 3

3UHVVXUH
WRZHU
JDXJH
*DVIORZ
PHWHU )HHG
3
3XPS UHFHLYHU
3UHVVXUH
JDXJH /LTXLG
*DVPL[LQJ IORZPHWHU
WDQN

/LTXLG
UHFHLYHU

Fig. 1. Schematic of experimental setup of CO2 spray absorption by MEA solution

Table 1. Geometry and operating parameters of the diameter-varying dual-nozzle opposed impinging spray tower.

Parameter Value
Geometry
Tower diameter (mm) 120-200
Tower height (mm) 500
Orifice diameter (mm) 0.5
Operating conditions
MEA flow rate, QL (L ·h-1) 60, 80, 100, 120
MEA concentration, CL (wt %) 10, 20, 30, 40
Gas flow rate, QG (m3·h-1) 1, 2, 3, 5
CO2 concentration, CG (vol %) 8, 12, 16, 18
Temperature, T (ć) 20
Pressure, P (MPa) 0.1

2.2. Mass transfer method

x The overall mass transfer coefficient

x The overall mass transfer coefficient is a lumped parameter that represents the absorption performance per unit
volume of reactor. It is a combination of thermodynamics, kinetics, and hydrodynamics of CO 2 absorption
system. Thus, it is really necessary to introduce the overall mass transfer coefficient to qualify the mass transfer
performance of the proposed spray tower. The material balance of the spray tower can be expressed as
x K G ae P( yCO ,G  yCO )dZ GI dYCO ,G
*

2 2 2
(1)

x where G is the inert gas flow rate, P( yCO  yCO ) is the mass transfer driving force of gas phase, Z is the
*
I 2
,G 2

height of the tower, YCO 2

,G
is the mole ratio of CO2 in gas phase.
x According to equation (1), the overall mass transfer coefficient can be expressed as
§ GI · § dYCO ,G ·
x K G ae ¨ ¸¨ ¸ (2)
2

© P( yCO ,G  yCO ) ¹ © dZ ¹
*

2 2

x As it is a diameter-varying spray tower, the equivalent cross-sectional area can be calculated by integrating
cylindrical section and conical section, which is expressed as
O1S d12 O2S d22
x S O1S1  O2 S2  (3)
4 4
1668 Xiaomei Wu et al. / Energy Procedia 114 (2017) 1665 – 1670

x where ¬ 1, ¬ 2 are proportionality coefficient, d1 is the diameter of cylindrical absorption section, d2 is the
equivalent diameter of the conical absorption section.

3. Results and Discussion

3.1. Effect of liquid flow rate

As can be seen from Fig. 2, the overall mass transfer coefficient increases with liquid flow rate in varies CO2
inlet concentrations. In a fixed 12 vol% CO2 inlet concentration, the overall mass transfer coefficient increases from
0.2837 to 0.3833 kmol·m-3·h-1·kPa-1 as the liquid flow rate increases from 60 L·h-1 to 120 L·h-1. This is because with
the increase of liquid flow rate, the droplets flow rate increases and the boundary layer of liquid phase decreases. So
the resistance for gas diffusion to the liquid phase decreased and the mass transfer performance is enhanced. As a
result, the overall mass transfer coefficient increases with the liquid flow rate. However, the increasing tendency
dropped rapidly at the higher range of liquid flow rate, this is because the reduction in droplet size by the increasing
liquid flow rate becomes insignificant and the increase of effective interfacial area is limited. Hence, the mass
transfer performance can not be enhanced furthermore at higher liquid flow rate.

3.2. Effect of MEA concentration

Fig. 3 shows the overall mass transfer coefficient increases from 0.2943 to 0.4044 kmol·m-3·h-1·kPa-1 as the MEA
concentration increases from 10 wt% to 40 wt% in a fixed 12 vol% CO2 inlet concentration. This tendency holds
true for other CO2 inlet concentrations. This is attributed to the fact that the increase of the MEA concentration
yields more active MEA molecules available to diffuse toward the gas-liquid surface and then react with CO2
molecules, which enlarge the reaction enhancement factor and lead to a better mass transfer performance.
Nevertheless, from the point of industrial application, the viscosity of solution increases significantly and severe
corrosion would occur in the equipment at higher MEA concentration. These side effects would block the
improvement of CO2 absorption performance and increase the maintenance cost. Hence, the overall mass transfer
coefficient and cost should be balanced when increasing the concentration of MEA.

3.3. Effect of gas flow rate

Fig. 4 shows that the overall mass transfer coefficient increases from 0.1432 to 0.4773 kmol·m-3·h-1·kPa-1 as the
gas flow rate increases from 1.0 m3·h-1 to 5.0 m3·h-1 in a fixed 12 vol% CO2 inlet concentration. This tendency also
holds true for other CO2 inlet concentrations. According to the gas-liquid mass transfer theory, the mass transfer
coefficient increases with the increase of gas flow rate. This is because as the total gas flow rate increased, the
amount of CO2 molecules available to diffuse toward the gas-liquid surface and then contact and react with MEA
molecules increased, which will lead to an increase of the overall mass transfer coefficient.

3.4. Effect of CO2 concentration

The experimental results in Fig. 5 show that the overall mass transfer coefficient decreases from 0.3326 to 0.2146
kmol·m-3·h-1·kPa-1 as the CO2 concentration increases from 8 vol% to 18 vol% in a fixed 80 L·h-1 liquid flow rate.
This tendency also holds true for other liquid flow rate. In general, according to the two-film theory, the gas phase
driving force and gas phase mass transfer coefficient increase with the increase of CO 2 concentration, which will
enhance the absorption process. Whereas, the mole ratio of MEA to CO 2 decreases with the increasing CO2 inlet
concentration, which means more CO2 molecules react with limited active MEA molecules and this will cause the
 yCO ) increased with the
*
reduction of absorption performance. Moreover, the gas phase driving force P( yCO 2
,G 2

increase of CO2 concentration, which will also lead to the decrease of the overall mass transfer coefficient.

3.5. The gas phase mass transfer coefficient and effective contacting area
 Xiaomei Wu et al. / Energy Procedia 114 (2017) 1665 – 1670 1669

The parameters discussed above can be summarized as the effect of liquid to gas ratio and mole ratio of MEA to
CO2. As can be seen from Fig. 6, the overall mass transfer coefficient increases obviously with the increase of liquid
to gas ratio and mole ratio of MEA to CO 2. The overall mass transfer coefficient increases from 0.1668 to 0.4519
kmol·m-3·h-1·kPa-1 as the liquid to gas ratio increases from 0.0136 to 0.0335. This is because with the increase of
liquid to gas ratio, the liquid flow rate increases and the boundary layer of liquid phase become thinner, which
decreased the mass transfer resistance and accelerate the reaction process. Furthermore, the increasing of liquid to
gas ratio leads to an increasing of liquid to gas contacting area and this will also enhance the absorption performance.
However, under the larger values of liquid to gas ratio, the growth of the overall mass transfer coefficient changes
slower. Fig. 7 provides that in a fixed liquid to gas ratio of 0.0267, the overall mass transfer coefficient increases
from 0.2784 to 0.3709 kmol·m-3·h-1·kPa-1 as the mole ratio of MEA to CO2 increases from 6.39 mole/mole to 25.5
mole/mole. The reason is that at the same liquid to gas ratio, the increase of MEA to CO 2 mole ratio allows more
active MEA molecules to contact and react with CO 2 molecules, leading to the increase of overall mass transfer
coefficient. It can be concluded that liquid to gas ratio and mole ratio of MEA to CO 2 are two key factors which
affect the performance of CO2 absorption process.
0.400 0.42 0.50
CO2 concentration CO2 concentration CO2 concentration
0.375 0.40 0.45
12% 12% 12%
16% 0.38 16% 16%
-1

-1

-1
0.350 18% 18% 0.40 18%
KGae/kmol·m ·h ·kPa

KGae/kmol·m ·h ·kPa

KGae/kmol·m ·h ·kPa
0.36
0.325 0.34 0.35
-1

-1

-1
0.300 0.32 0.30
-3

-3

-3
0.275 0.30 0.25
0.28
0.250 0.20
0.26
0.225 0.24 0.15

0.200 0.22 0.10

3.5 4.0 4.5 5.0 5.5 6.0 6.5 7.0 7.5 8.0 8.5 5 10 15 20 25 30 35 40 45 50 100 150 200 250 300 350
3 -2 -1 3 -2 -1
Liquid flow rate/m · m · h MEA concentration/wt% Gas flow rate/m · m · h

Fig. 2. Effect of liquid flow rate on the overall Fig. 3. Effect of MEA concentration on the Fig. 4. Effect of total gas flow rate on the
mass transfer coefficient. overall mass transfer coefficient. overall mass transfer coefficient.
(CL=30 wt%, QG=3 m3·h-1, T=20 ć) (QL=80 L·h-1, QG=3 m3·h-1, T=20 ć) (QL =80 L·h-1, CL =30 wt%, T=20 ć)

0.50 0.50 0.38

MEA flow rate
3 -2
4.1 m ·m ·h
-1 0.45
0.45 3 -2 -1
0.36
5.4 m ·m ·h
-1

-1

0.40
KGae (kmol/m *h*kPa)
KGae/kmol·m ·h ·kPa

KGae/kmol·m ·h ·kPa

3 -2 -1
6.8 m ·m ·h
0.40 0.34
0.35
-1

-1
3

0.35 0.30 0.32

-3

-3

0.25
0.30 0.30
0.20
0.25 0.28
0.15

0.20 0.10 0.26

6 8 10 12 14 16 18 20 0.012 0.016 0.020 0.024 0.028 0.032 0.036 4 6 8 10 12 14 16 18 20 22 24 26
3 -1 3
CO2 concentration/vol% Liquid to gas ratio/m · h /m · h n(MEA)/n(CO2)

Fig. 5. Effect of CO2 concentration on the Fig. 6. Effect of liquid to gas ratio on the Fig. 7. Effect of mole ratio of MEA to CO2
overall mass transfer coefficient. overall mass transfer coefficient. on the overall mass transfer coefficient.
3 -1
(CL=30 wt%, QG=3 m ·h , T=20 ć) (CL=30 wt%, T=20 ć, CG=8 vol%) (CL=30 wt%, T=20 ć, CG=8 vol%,
QL/QG =0.0267)

4. Conclusions

Experimental studies on the overall mass transfer coefficient of the proposed diameter-varying dual-nozzle
opposed impinging spray tower were carried out. Experimental results show that the liquid to gas ratio and mole
ratio of MEA to CO2 play an important role in the CO2 spray absorption process. The overall mass transfer
coefficient is a function of the main operating variables, it increases with the liquid flow rate, MEA concentration
and total gas flow rate, but decreases with CO2 concentration. Under the experimental conditions, the maximum
overall mass transfer coefficient for the diameter-varying dual-nozzle opposed impinging spray tower is 0.4773
kmol·m-3·h-1·kPa-1.
1670 Xiaomei Wu et al. / Energy Procedia 114 (2017) 1665 – 1670

Acknowledgements

Financial support of the National Natural Science Foundation of China (No. 51276141) is gratefully
acknowledged. This work is also supported by the Natural Science Basic Research Plan in Shaanxi Province of
China (No. 2015JQ5192) and “Fundamental Research Funds for the Central Universities”.

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