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GHGT-9

Mass-transfer efficiency of a spray column for CO2 capture by

MEA
Jeffery Kuntz, Adisorn Aroonwilas *
Faculty of Engineering, University of Regina, Regina, Saskatchewan, Canada S4S 0A2

Elsevier use only: Received date here; revised date here; accepted date here

Abstract

A parametric study of carbon dioxide (CO2) absorption performance into an aqueous solution of monoethanolamine (MEA) in
the spray column was carried out experimentally over wide ranges of process conditions. The performance of the spray was
interpreted in terms of the overall mass transfer coefficient (KGae) and was found to vary with process parameters, including gas
flow rate, liquid flow rate, CO2 partial pressure, MEA concentration, CO2 loading, and size of spray nozzle. The performance of
the spray column was compared to that of a packed column and showed a promise for CO2 capture application.

2008Elsevier
c 2009 Elsevier Lt Open access under CC
Ltd. vedBY-NC-ND license.

Keywords: CO2 capture; CO2 absorption; spray column; mass transfer coefficient; mass transfer area; alkanolamine

1. Introduction

Gas absorption into an aqueous alkanolamine solution is the most well-established of the technologies available
for carbon dioxide (CO2) capture [1]. However, its cost is still prohibitively high for the environmental application.
The reduction of cost can be attained through the use of proper gas-liquid contactors. For a number of years, the CO2
absorption using packed and tray columns has produced a large amount of published data with many types of
solvents and column internals being tested [2-9]. whereas the CO2 absorption using spray column has been studied
by few and to date there has been little data published in the area of CO2 capture [10]. Specifically in case of the
CO2 absorption using alkanoalmine such as monoethanolamine (MEA), there has been no data on spray absorber
published. This work therefore examined the feasibility of using spray column for CO2 capture using MEA. The
performance of spray column was evaluated experimentally under various conditions to reveal effects of process
parameters, including CO2 partial pressure in gas phase, gas flow rate, liquid flow rate, concentration of MEA, CO2

* Corresponding author. Tel: 1-306-337-2469. Fax: 1-306-585-4855.

E-mail address: aroonwia@uregina.ca.

doi:10.1016/j.egypro.2009.01.029
 206 J. Kuntz,
Kuntz A. Aroonwilas
and Aroonwilas / Energy
/ Energy Procedia
Procedia 00 1(2008)
(2009)000000
205209

loading of absorption solution, and size of spray nozzle. A set of absorption experiments using a packed column
was also conducted to determine the performance of conventional column for comparison purposes.

2. Absorption Experiments

The gas absorption setup used in this work is shown in Figure 1. The experiments were conducted in two separate
columns, i.e. spray and packed column. The spray column was constructed of acrylic plastic that was 0.55 m high
and had an inside diameter (ID) of 0.10 m. The spray column was operated with one of three 316 stainless steel
nozzles manufactured by BETE Industrial Spray Nozzles (models P-20, P-28, and P-40). The packed column was
also constructed of acrylic plastic with an ID of 0.10 m but had a height of 0.80 m. The packed column was fitted
with Mellapak 500Y structured packing provided by Sulzer Brothers Limited, Winterhur, Switzerland. The packing
was installed with each layer rotated by 90 with respect to the previous one. The CO2 concentrations were
measured using an infrared gas analyzer (Model 302WP, Nova Analytical Systems Inc.). The reading range of the
analyzer was 0.0 to 20.0 % of CO2 by volume with the accuracy of 2% of the full-scale reading.
O ff g a s
Packed
c o lu m n
Feed
r e s e r v o ir

S p ra y
c o lu m n

G a s f lo w
m e te rs

CO2
a n a ly z e r
A ir CO 2 L iq u id
r e c e iv e r

Figure 1 Schematic diagram of CO2 absorption apparatus

The experiments began by introducing a mixture of air and CO2 at a desired flow rate and CO2 concentration to
the bottom of the column. The gas mixture once in the column passed through a dispersion outlet to disperse
uniformly across the column. At the same time, the prepared liquid solution was pumped to the top of the column
where it entered the column through either a spray nozzle (for the spray column) or the liquid distributor (for the
packed column). This brought the gas and liquid into contact counter-currently, and the CO2 in the gas phase was
absorbed. The gas then carried out through the top of the column while the CO2 rich solution was collected out of
the bottom of the column in the liquid receiver. Once the system reached steady state, the CO2 concentration of the
exit gas was measured and a liquid sample was collected out of the bottom of the column. The liquid sample was
analyzed for CO2 loading and total concentration of MEA. Details of experimental setup and procedure can be found
in Kuntz (2006) [11].

3. Results and Discussion

More than 400 runs were carried for both spray and packed columns over ranges of conditions as listed in Table
1. The mass transfer performance was determined in terms of the volumetric overall mass transfer coefficient (KGae)
by using the following equation: [6]
GI dYCO ,G
K G ae
 
2
(1)
P y  y * dZ
CO2 ,G CO2
where GI is inert gas flow rate in kmol/m2-hr, P is total pressure on the system in kPa, Z is column height in m.,
*
y CO2 ,G and yCO 2
are mole fraction of CO2 in gas stream and equilibrium mole fraction of CO2, and YCO2 ,G is mole
ratio of CO2 in gas stream. Parametric results are given in Figure 2.
 J.Kuntz
Kuntz,and
A. Aroonwilas
Aroonwilas//Energy
EnergyProcedia
Procedia100
(2009) 205209
(2008) 000000 207

Table 1 Test conditions of spray and packed columns

Parameter Condition
Absorption solvent Monoethanolamine (MEA)
Gas Phase
Gas flow rate Up to 764 m3/m2-h
Feed CO2 partial pressure 5, 10, 15 kPa
Liquid Phase
Liquid flow rate Up to 10.3 m3/m2-h
MEA concentration 3, 5, 7 kmol/m3
CO2 loading 0, 0.15, 0.25, 0.35, 0.45 mol/mol
Temperature 25C

0.8
CO2 loading
0.7 0.0 m ole/mole 0.45

KGae (kmol/m *h*kPa)

0.15 mole/mole
KGae (kmol/m *h*kPa)

0.6 0.25 mole/mole

0.45 mole/mole
0.5

3
0.35
3

0.4

0.3
MEA Concentration
0.25
0.2 3 kmol/m3
5 kmol/m3
0.1 7 kmol/m3

0 0.15
0 5 10 15 20 0 200 400 600 800
3
CO2 partial pressure (kPa) Gas flow rate (m /m 2-h)

(a) (d)
2.50 7
Nozzle s ize
6 P-20
2.00
KGa e (kmol/m 3*h*kPa)

KGae (kmol/m *h*kPa)

P-28
5
Liquid flow rate P-40
1.50 1.91 m3/m2-h 4
3

4.59 m3/m2-h
3
1.00
2
0.50
1

0.00 0
0 0.1 0.2 0.3 0.4 0.5
0 200 400 600 800 1000
3 2
Gas flow rate (m /m -h) CO 2 loading (mole CO2 /mole MEA)
(b) (e)
2.40 6.40
CO2 Loading CO2 Loading
0 mole/mole 5.60 P-28 0 mole/mole
2.00 0.15 mole/mole P-28 0.15 mole/mole
P-28 0.25 mole/mole
0.25 mole/mole 4.80
KGa e (kmol/m3*h*kPa)
KGa e (kmol/m 3*h*kPa)

P-28 0.35 mole/mole

1.60 0.35 mole/mole P-28 0.45 mole/mole
4.00 P-40 0 mole/mole
0.45 mole/mole
P-40 0.15 mole/mole
1.20 3.20 P-40 0.25 mole/mole
P-40 0.35 mole/mole
2.40 P-40 0.45 mole/mole
0.80
1.60

0.40 0.80

0.00
0.00
1.9 3.9 5.9 7.9 9.9
1.9 2.4 2.9 3.4 3.9 4.4 4.9
Liquid flow rate (m 3/m 2-h)
Liquid flow rate (m 3/m 2-h)

(c) (f)

Figure 2 Effects of parameters on spray performance (a) Effect of CO2 partial pressure on KGae. (Nozzle = P-20, Liquid flow rate = 1.53 m3/m2-h,
Gas flow rate = 382 764 m3/m2-h), (b) Effect of gas flow rate on KGae at different liquid flow rates (Nozzle = P-28, PCO2=15 kPa,
[MEA] =5M), (c) Effect of liquid flow rate on KGae P-28 nozzle (PCO2=15 kPa, [MEA] =5M, Gas flow rate=382 m3/m2-h), (d) Effect of
the concentration of the MEA on KGae at CO2 loadings of 0.25 mole/mole (Nozzle=P-20, PCO2=15 kPa), (e) Effect of CO2 loading on
KGae for different nozzles (for P-20 nozzle, [MEA] =3M, Gas flow =76 m3/m2-h, Liquid flow = 1.53 m3/m2-h; for P-28 nozzle, [MEA]
=5M, Gas flow =382 m3/m2-h, Liquid flow = 4.59 m3/m2-h; and for P-40 nozzle, [MEA] =5M, Gas flow =382 m3/m2-h, Liquid flow
=10.32 m3/m2-h), and (f) Effect of the nozzle size on KGae (Gas flow rate=382 m3/m2-h, PCO2=15kPa, [MEA] =5 kmol/m3)
 208 J. Kuntz,
Kuntz A. Aroonwilas
and Aroonwilas / Energy
/ Energy Procedia
Procedia 00 1(2008)
(2009)000000
205209

Effect of CO2 partial pressure. KGae decreases with CO2 partial pressure. By considering mass flux of CO2
absorption (NCO2), an increase in CO2 partial pressure leads to an increasing amount of CO2 transferred into liquid
phase. However, the increasing mass flux occurs in a lower extent compared to the change in partial pressure,
causing KGae to reduce as partial pressure increases. Note that the effect of CO2 partial pressure becomes less at the
CO2 loading of more than 0.25 mole/mole and the partial pressure of more than 10 kPa. This may be caused by the
restricted diffusion and amount of reactive MEA in the liquid phase. The mass transfer may be mainly controlled by
CO2 reaction in the liquid, thus resulting in only a small change in the amount of CO2 absorbed as the partial
pressure increases.

Effect of gas flow rate. KGae increases with gas flow rate to a certain point and then remains constant. This
suggests the gas-phase controlled mass transfer takes place at low gas flow rates (below 300 m3/m2-h) and the
liquid-phase controlled mass transfer takes over at high gas flow rate. In general, as the gas flow increases the
amount of CO2 molecules available for the absorption increases. This would lead to a higher mass transfer flux.
However, the overall rate of gas absorption is not only dependent upon the gas flow rate, but also the liquid flow rate
and availability of reactive MEA in the liquid which as seen in this case controls the rate of mass transfer after the
gas flow rate reaches the point of 300 m3/m2-h.

Effect of liquid flow rate. KGae increases with liquid flow rate. This is because increasing the liquid flow
increases effective interfacial area (ae), between liquid and gas. Note that KGae increases more rapidly at low flow
rates compared to at high flow rates. The rapid increase was caused by 1) a reduction in size of spray droplets from
larger diameter to smaller diameter, thus resulting in an increase in droplet surface area per unit volume of dispersed
liquid and 2) an increase in number of droplets produced by the nozzle and also the surface area available for mass
transfer. At the high liquid flow rate, the reduction in droplet size by the increasing liquid flow is insignificant,
leaving the increasing number of spray droplets to be the primary factor that defined the lower increase in mass
transfer performance.

Effect of MEA concentration. KGae increases with MEA concentration (up to 7 kmol/m3). This is due to the fact
that the increasing MEA concentration yields a higher amount of the active MEA available to diffuse towards the
gas-liquid interface and react with CO2. This finding differs from the behavior observed in the packed column in that
the KGae of packed column decreases by 5% for every molarity of MEA increasing beyond 3 kmol/m3.[9] Such
decrease in KGae is caused by an increase in solution viscosity. This shows that the solution viscosity is more
influential on the effective area in the spray column than in the packed column.

Effect of CO2 loading. KGae decreases with CO2 loading. This is due to the fact that as the CO2 loading increases
the amount of active MEA decreases, causing the KGae to decrease.

Effect of nozzle size. Three nozzles with different orifice sizes were tested, i.e. P-20, P-28, and P-40. It was
found that KGae of a larger nozzle is lower that of a smaller nozzle at the low end of liquid flow rate. This is because
the spray of the lager nozzle is not fully developed, resulting in a lower effective area (ae). As the liquid flow rate
increases, the spray is more fully developed with the smaller liquid droplets that offer higher ae, causing the KGae to
increase accordingly.

Performance comparison (spray versus packed column). The comparison was made for the spray column
fitted with P-40 nozzle and the packed column fitted with Mellapak 500Y. It was found in Figure 3 that the spray
column provides a much higher KGae. This is because the spray nozzle offers a much higher gas-liquid interfacial
area than the packing does.
 J.Kuntz
Kuntz,and
A. Aroonwilas
Aroonwilas//Energy
EnergyProcedia
Procedia100
(2009) 205209
(2008) 000000 209

5.00
CO2 Loading
0.15 mole/mole

4.00 0.45 mole/mole

KGae (kmol/m3*h*kPa)
Packed 0.15 mole/mole

Packed 0.45 mole/mole

3.00

2.00

1.00

0.00
4.5 5.5 6.5 7.5 8.5 9.5
Liquid flow rate (m 3/m 2-h)

Figure 3 Mass transfer performance comparison between packed and spray columns

4. Conclusions

The CO2 absorption performance of the spray column is affected by process parameters. KGae decreases with CO2
partial pressure and CO2 loading, but increases with liquid flow rate and MEA concentration. KGae increases with
gas flow rate and then remains constant when the gas flow rate exceeds 300 m3/m2-h. Different nozzle sizes offer
different ranges of KGae due to the difference in hydrodynamic capacity of each spray nozzle. The spray column
offers a superior CO2 absorption performance to the packed column due to a greater interfacial area provided.

Acknowledgment

Authors gratefully acknowledge the financial support received from the Natural Sciences and Engineering
Research Council of Canada (NSERC) and the structured packing donated by the Sulzer Chemtech, Winterthur,
Switzerland.

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