Energy

Energy Procedia 4 (2011) 512–518 Procedia

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Energy Procedia 00 (2010) 000–000
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GHGT-10

Comparison of removal efficiencies of carbon dioxide between

aqueous ammonia and NaOH solution in a fine spray column
Guo Yincheng *, Niu Zhenqi, Lin Wenyi
1

Department of Engineering Mechanics, School of Aerospace

Tsinghua University, Beijing 100084, China
Elsevier use only: Received date here; revised date here; accepted date here

Abstract

Experimental studies on carbon dioxide capture in a spray column were carried out. Fine spray of aqueous ammonia and NaOH
solution were used as CO2 absorbent. Effects of different operating and design parameters, including concentration of aqueous
ammonia solution and NaOH solution, absorbent solution volume flow rate and total gas flow rate on CO2 removal efficiency
were investigated. Experimental results showed that the higher concentration of aqueous ammonia solution and NaOH solution,
the larger volume flow rate of absorbent solution and the lower flow rate of total gas mixture of nitrogen and CO2 were beneficial
to promote CO2 removal efficiency. In order to have high removal efficiency of CO2, the mole ratios of absorbents to CO2 should
be larger than certain values for aqueous ammonia solution and NaOH solution, respectively.
⃝
©c 2010
2011 Elsevier
PublishedLtd.
by Elsevier Ltd.
All rights reserved
Open access under CC BY-NC-ND license.

Keywords: Carbon dioxide; spray; absorption; aqueous ammonia; NaOH

1. Introduction

Removal of carbon dioxide from flue gases is a key measure to reduce CO 2 emission. In the coming few decades,
it has huge potential for the contribution to carbon emission reduction by carbon capture and storage [1]. Several
technologies of CO2 sequestration include absorption methods, adsorption methods, cryogenic methods, membrane
separation and biological fixation. The absorption process is one of the most common industrial technologies today.
Recent economic studies indicated that the absorption process will also remain competitive in the future [2], but the
cost to capture CO2 from flue gas of power plants using current technologies is very high. It is estimated that the
energy penalty from using the well-known monoethanolamine (MEA) process for CO 2 capture from coal-fired
power plants is about 15% to 35% [3].
Absorbent is important for the absorption method. In recent years, some researchers found that aqueous ammonia
seems to be an alternative and promising absorbent for removing CO2 from flue gas. Yeh and Bai [4] carried out
experimental investigations of the ammonia and MEA capturing CO2 in a bubble reactor. Their tests showed that the
NH3 absorbent was superior to MEA absorbent in its capacity to absorb and remove CO2 from flue gas systems. The

* Corresponding author. Tel.: +86-10-62772112-802; fax: +86-10-62781824.

E-mail address: guoyc@tsinghua.edu.cn.

doi:10.1016/j.egypro.2011.01.082
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CO2 removal efficiency for NH3 absorbent could be as high as 99% under proper operating conditions. And the CO2
absorption capacity by NH3 scrubbing could be over 1.0 kg CO2 kg NH3. On the other hand, the maximum CO2
removal efficiency and absorption capacity using MEA absorbent are 94% and 0.4 kg CO 2 kg MEA, respectively.
Yeh et al. [5] performed CO2 absorption and regeneration with aqueous ammonia in a semi-continuous flow reactor.
It was found that the regeneration energy saving for the aqua ammonia process was approximately 62% compared
with the MEA process. Diao et al. [6] designed a sieve-plate tower system and performed experiments in an open
continuous flow reactor. They studied the mechanism and kinetics of the reaction between CO2 and NH3 absorbent.
Their experiment results showed that the reaction temperature played a key role in the CO2 removal. The CO2
removal efficiency reached the highest at 33C. The overall CO2 removal efficiency could be above 95%. Li et al. [7]
studied the possibility of using ammonia carbonation directly in the gas phase and conducted experiments in a glass
tube reactor at ambient pressure and temperature. Their experimental results showed that the NH3 concentration
played an important role in CO2 removal. The solid ammonia carbonation products could be formed quickly in the
gas-phase reaction among NH3, CO2, and water vapor. So, it is possible to achieve efficient removal of CO 2 by
formation of NH4HCO3 and NH2CO2NH4 through ammonia carbonation in the gas phase. Yeh and Pennline [8]
provided a new method for multi-component removal in flue gas by aqua ammonia. The above studies showed that
the CO2 removal efficiency reached up to 50% in the CO2 and NH3 gas phase reaction, 95% in the wet scrubbing
reactor, and 99% in the bubbling reactor.
NaOH solution is another alternative absorbent for CO2 removal. Chen et al. [9] employed a laboratory-scale spray
dryer system to investigate the removal efficiency of CO2, using different absorbents NaOH, diethanolamine,
triethanolamine, mixed with commercial Ca(OH) 2 slurry. Their experiment results showed that the best removal
efficiency of CO2 by a spray dryer was 48% as the absorbent was 10%NaOH+5%Ca(OH) 2 and the operating
temperature was 150C. Different from conventional CO2 capture for large point sources, Storaloff et al. [10] studied
the feasibility of a NaOH spray-based contactor for capturing carbon dioxide directly from ambient air. When
considering absorbent recovery and CO2 sequestration, the cost of CO2 capture using NaOH solution ranges from 53
to 127 $/ton-CO2 under alternate operating parameters, the low end of the cost range is reached by a spray with 50
m mean drop diameter. Their research suggested that a structure area of about 760 by 760 m would be required to
capture 1 Mt/yr of CO2 under the base-case contactor running at the cost-optimal flow rate. Mahmoudkhani and
Keith [11] described a novel technique for recovering sodium hydroxide from an aqueous alkaline solution of sodium
carbonate for capturing CO2 from ambient air. The proposed energy efficient process potentially requires about half
of the energy requirement for the conventional causticization process using lime.
In this paper, the experiments for studying the removal of CO2 by aqueous ammonia solution and NaOH solution
fine spray were carried out in a laboratory-scale reactor. The effects of several operating parameters such as
absorbent concentration, absorbent solution volume flow rate, the total gas flow rate and inlet concentration of
carbon dioxide on the CO2 removal efficiency were studied.

2. Experimental setup

The absorption reactor was made of stainless steel with 120 mm inner diameter and 1300 mm height. The
artificial flue gases were obtained from the mixture of pure CO2 gas and N2 gas from cylinders. The influent mixture
gas and the aqueous ammonia solution or NaOH solution were heated to the desired operating temperature by
electric heaters before being fed into the reactor. Thermocouples were placed at each inlet of the flue gas and the
aqueous ammonia solution or NaOH solution, and the temperatures were continuously monitored. Two atomizers
were placed at the upper part of the reactor and the Sauter mean diameters (SMD) of the absorbent spray were 30 to
40 m when the pressure of the pump was 0.69 to 1.11 MPa. In order to make CO2 and absorbent contact and react
thoroughly, the flue gases were fed into the reactor from the bottom of the reactor, thus the fine spray of the
absorbent solution and flue gas stream were in a counter flow pattern.
An infrared CO2 analyzer was used to measure the concentration of CO2 in exhaust gas. The sampling process
was well arranged. At first, the sampling gas was induced into the small gas dryer filled with desiccant CaCl2, where
most of water vapor and NH3 were absorbed. Then, the sampling gas flowed into the washing bottle loading vitriol,
where the left NH3 was absorbed. After that, the sampling gas was fed into the gas dryer filled with desiccant CaSO4,
where the left water vapor was absorbed. Finally, the sampling gas was fed into the CO2 analyzer.
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3. Reaction mechanism

3.1. Reaction mechanism of the absorption of CO2 into aqueous ammonia solution

The possible reactions among NH3, CO2, and H2O were reviewed by Bai and Yeh [12]. There are two mechanisms
for the formation of ammonium bicarbonate from NH 3, CO2, and H2O [7]. One mechanism is taken place in aqueous
ammonia solution, ammonium carbonate is formed as an intermediate by the reaction of NH 3 and CO2 in aqueous
ammonia solution. The ammonium carbonate is further transformed into ammonium bicarbonate by the reaction
with CO2 and H2O. The reaction sequence is as follows:
2NH4OH (l )  CO2 ( g)  ( NH4 )2 CO3 (s)  H2O(l ) (R.1)
( NH4 )2 CO3 (s)  CO2 ( g)  H2O(l )  2NH4 HCO3 (s) (R.2)
Another mechanism is taken place in the gas phase, NH 3 gas exists in the gas phase due to evaporation of
aqueous ammonia solution, and ammonium carbonate is first formed by the reaction of NH3 with CO2 in the gas
phase, which is further hydrolyzed into ammonium bicarbonate. The reaction sequence is as follows:
CO2 ( g )  2NH3 ( g )  NH2COONH4 (s) (R.3)
NH2COONH4 (s)  CO2 ( g )  2H2O(l / g )  2NH4 HCO3 (s) (R.4)

3.2. Reaction mechanism of the absorption of CO2 into sodium hydroxide solution

The absorption of CO2 into sodium hydroxide solutions has been widely studied. The reaction equations of CO2
with sodium hydroxide solution can be written as the following scheme [13-15]:
CO2  H 2O  HCO3  H  (R.5)
CO2  OH   HCO3 (R.6)
  
HCO  OH  CO  H 2 O
3 3 (R.7)
[14]
Reaction (R.5) has a negligible effect on the rate of CO2 absorption in alkaline solution with PH>10 . Reaction
(R.6) is followed by an instantaneous reaction (R.7). The overall reaction between CO 2 and NaOH solution can be
expressed as:
CO2  2OH   CO3  H 2O (R.8)
[14]
Reaction (R.8) is second-order and may be considered to be irreversible .

4. Results and discussion

Effects of different operating and design parameters on CO 2 removal efficiency were investigated. Detailed
parameters in experiments of absorption using aqueous ammonia solution and NaOH solution are given in Table 1
and Table 2, respectively.

4.1. Effect of concentration of absorbent solution

Figure 1 shows the CO2 removal efficiency profile under different concentrations of absorbent solution. In these
cases, the flow rate of aqueous ammonia solution and NaOH solution had the same value of 180 mL/min, the total
gas flow rate was 7.6 L/min, the concentration of CO2 at the inlet was 15% (v/v), and the initial temperature of the
column was 28C. It can be found that the concentration of absorbent solution plays an important role on the CO 2
removal efficiency. With the values of absorbent concentration increasing, the CO2 removal efficiency increased to
a high level. The increasing concentration yields a higher amount of the active ammonia and NaOH available to
diffuse toward the gas-liquid interface and react with CO2. This results in an enhancement of the absorption rate,
which leads to a higher CO2 removal efficiency. For aqueous ammonia solution, the maximum value of 98.4% of
CO2 removal efficiency was achieved when the concentration of aqueous ammonia solution was 8% (w/w). When
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the concentration of aqueous ammonia solution and NaOH solution were higher than 8%, the CO2 removal
efficiency increased slightly. In general, the CO2 removal efficiency by aqueous ammonia solution is larger than that
by NaOH solution when the concentration of absorbent solution changing from 2%(w/w) to 10%(w/w).

Table 1 Experimental parameters of aqueous ammonia solution

Ammonia Flow rate of aqueous Total gas flow rate CO2 inlet
Initial temperature, C
concentration %, w/w ammonia solution, mL/min L/min concentration %, v/v
2~10 180 7.6 28 15

5 120~200 13.0 28 15

8 160 7.6~24.7 28 15

5 180 7.6 28~38 15

5 180 7.6 28 7~15

Table 2 Experimental parameters of NaOH solution

Concentration of NaOH Flow rate of NaOH Total gas flow rate CO2 inlet
Initial temperature, C
solution %, w/w solution, mL/min L/min concentration %, v/v
2~10 180 7.6 28 15

5 120~200 7.6 28 15

5 180 7.6~24.7 28 15

5 180 7.6 28~54 15

5 180 7.6 32 7~15

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Figure1 Effect of absorbent concentration Figure 2 Effect of absorbent solution volume flow rate
on CO2 removal efficiency on CO2 removal efficiency

4.2. Effect of the absorbent solution volume flow rate

The influence of absorbent solution volume flow rate on the CO2 removal efficiency was investigated. Figure 2
gives the CO2 removal efficiency profile at different absorbent solution volume flow rates. In these cases, the
concentration of absorbent solution was 5% (w/w), the concentration of CO2 at the inlet was 15% (v/v), the initial
temperature of the column was 28C, and the total gas flow rate were 13.0 L/min and 7.6 L/min for the experiments
using aqueous ammonia solution and NaOH solution, respectively. When aqueous ammonia solution volume flow
rate increased from 120 to 200 mL/min, the CO2 removal efficiency increased from 76.4% to 85.4%. Previous
studies on CO2 absorption in a spray tower [16] revealed that the overall mass transfer coefficient increased with
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increasing absorbent solution flow rate. More absorbent would be spread in the spray column with the absorbent
solution flow rate increasing, and this gave rise to an increase in the interfacial area per unit volume. Then, the
enhanced absorption rate resulted in an increase of CO2 removal efficiency. For the process of absorption using
NaOH solution, the CO2 removal efficiencies are larger than that by aqueous ammonia solution due to the small
flow rate of the total gas in experiments of NaOH solution.

4.3. Effect of the total gas flow rate

Figure 3 shows the CO2 removal efficiency profile when total gas flow rate of CO 2 and N2 increased from 7.6 to
24.7 L/min. In these cases, the concentration of aqueous ammonia solution was 8% (w/w), the concentration of
NaOH solution was 5% (w/w), the concentration of CO2 at the inlet was 15% (v/v), the initial temperature of the
column was 28C, and the volume flow rates of aqueous ammonia solution and NaOH solution were 160 mL/min
and 180 mL/min, respectively. Experimental results showed that the total gas flow rate has a remarkable effect on
the CO2 removal efficiency. When using aqueous ammonia solution, it was found that the CO2 removal efficiency
declined from 96% to 78.7% when the total gas flow rate increased from 7.6 to 24.7 L/min. It is known that the mole
ratio of ammonia to CO2 is reduced with the total gas flow rate increasing. A lot of CO2 remained in the outlet
mixed gases, which resulted in the CO2 removal efficiency decreased.

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Figure 3 Effect of total gas volume flow rate Figure 4 Effect of CO2 inlet concentration
on CO2 removal efficiency on CO2 removal efficiency

For the absorption process of NaOH solution, the CO2 removal efficiency declined from 90.2% to 41% when
total gas flow rate of CO2 and N2 increased from 7.6 to 24.7 L/min. The main reason for low CO2 removal efficiency
at high total gas flow rate is that the reaction between CO 2 and NaOH solution is insufficient. Besides, with the total
gas flow rate increasing, the velocity of the mixture of carbon dioxide and nitrogen increased. Thus, the contract
time between CO2 and absorbent solution spray was reduced which gave rise to low CO2 removal efficiency.

4.4. Effect of the inlet concentration of carbon dioxide

The influence of CO2 inlet concentration on the CO2 removal efficiency was also investigated. Figure 4 shows the
CO2 removal efficiency when the inlet concentration of CO2 changed from 7% (v/v) to 15% (v/v). In these cases, the
concentration of absorbent solution was 5%, the flow rate of absorbent solution was 180 mL/min, the total gas flow
rate was 7.6 L/min, and the initial temperatures of the column were 28C and 32C for the experiments using
aqueous ammonia solution and NaOH solution, respectively. Experimental results showed that the CO2 removal
efficiency is larger than 90% at different CO 2 inlet concentrations. It is known that the gas phase driving force and
the gas phase mass transfer coefficient will increase with the increasing CO2 partial pressure, which is beneficial to
enhance absorption rate. So, an increase in the CO2 inlet concentration allows more CO2 molecules to travel from
gas bulk to the gas-liquid interface, which results in higher removal efficiency. However, with the CO2 inlet
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concentration increasing, the mole ratios of absorbent (NH3 and NaOH) to carbon dioxide decreased, which gave
rise to the reduction of removal efficiency. Accordingly, The CO2 removal efficiency declined a little with the inlet
concentrations of CO2 increasing.

4.5. Effect of the initial temperature in the column

Figure 5 shows the CO2 removal efficiency profile under different initial temperatures in the spray column. In
these cases, the flow rates of aqueous ammonia solution and NaOH solution were 180 mL/min, the total gas flow
rate was 7.6 L/min, the concentration of CO2 at the inlet was 15% (v/v), and the concentration of absorbent solution
was 5% (w/w). In the experiments of absorption using aqueous ammonia, the initial temperatures of the column
were 28C, 32C, 35C, and 38C. Experimental results showed that the CO2 removal efficiency increased from
91.8% to 96.4% when the initial temperature in the column increased from 28C to 38C. When the temperature was
higher than 60°C, it was found that ammonium bicarbonate and ammonium carbonate decomposed [17]. At lower
temperatures, the forward reactions of (R.1), (R.2), or (R.4) took place mainly. With temperature increasing,
diffusion rate and reaction rate increase. Besides, more NH3 exists in the gas phase by volatilization of aqueous
ammonia with temperature increasing. The solid ammonia carbonation products could be formed quickly in the gas-
phase reaction among NH3, CO2, and water vapor [7]. In the experiments of absorption using NaOH solution, the
initial temperatures of the column ranged from 28C to 54C. It can be found that an increase in temperature results
in higher absorption performance, which is primarily caused by the increasing absorption rate.

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Figure 5 Effect of initial temperature in the column Figure 6 Effect of mole ratio of absorbent to carbon
on CO2 removal efficiency dioxide on CO2 removal efficiency

4.6. Effect of the mole ratio of absorbent to carbon dioxide

According to the experimental parameters given in Table 1 and Table 2, mole ratios of absorbents (NH3 and
NaOH) to CO2 were calculated. Figure 6 shows the effect of mole ratio of absorbent to carbon dioxide on CO2
removal efficiency. In general, with the mole ratio of absorbent to CO2 increasing, the CO2 removal efficiency
increases. Furthermore, when the mole ratios of absorbents to CO2 have nearly the same values at different
conditions, the CO2 removal efficiencies also have a nearly same value.
In experiments of absorption using NaOH solution, it seems that there exists a critical value of the mole ratio of
NaOH to CO2. When the mole of NaOH to CO2 has a value of 4.43, a value of 90.2% of the CO2 removal efficiency
is achieved. When the mole ratio of NaOH to CO2 is larger than 4.43, the difference between CO 2 removal
efficiencies at different experimental conditions is small. Thus, if the target value of CO2 removal efficiency is given
as 90%, the mole ratio of NaOH to CO2 is suggested to have the value of 4.43 in the spay column in order to save
the reaction material of NaOH and energy for recovering sodium hydroxide.
The same trend can also be observed in experiments of absorption using aqueous ammonia solution, when the
mole ratio of ammonia to CO2 has a value of 9.68, the value of the CO2 removal efficiency is 91.8%. When the mole
ratio of ammonia to CO2 is larger than 9.68, the increasing trend of CO2 removal efficiency increased slightly. Thus,
 518 Y.G.
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in order to save energy for recovering aqueous ammonia, when the target value of CO2 removal efficiency is given
as 90%, the mole ratio of ammonia to CO2 is suggested to have the value of 9.68 in the spay column.

5. Conclusions

The removal efficiencies for CO2 absorption into aqueous ammonia solution and NaOH solution were
investigated in a spray column. The Sauter mean diameters (SMD) of the absorbent spray were 30 to 40 m.
Experimental results showed that the concentration of absorbent solution plays an important role on the CO 2
removal efficiency. With the values of absorbent concentration increasing, the CO2 removal efficiency increased to
a high level.
Experimental results also showed that the mole ratio of absorbent (NH3 and NaOH) to CO2 is a key parameter for
CO2 absorption. When the target value of CO2 removal efficiency is assumed as 90%, in order to save the reaction
material of absorbent and energy for recovering absorbent, the suitable values of the mole ratios of absorbents to
CO2 were 4.43 and 9.68 for NaOH solution and aqueous ammonia solution in the spray column, respectively.

Acknowledgment

This research was supported by Beijing Municipal Commission for Science & Technology under Grant
No.Z08040902950803.

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