Applied Energy 225 (2018) 367–379

Contents lists available at ScienceDirect

Applied Energy
journal homepage: www.elsevier.com/locate/apenergy

Experimental and numerical study on CO2 absorption mass transfer T

enhancement for a diameter-varying spray tower
⁎ ⁎
Xiao M. Wua,b, Zhen Qina,b, Yun S. Yua, , Zao X. Zhanga,b,
a
School of Chemical Engineering and Technology, Xi’an Jiaotong University, No. 28 Xianning West Road, Xi’an 710049, PR China
b
State Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, No.28 Xianning West Road, Xi'an 710049, PR China

H I GH L IG H T S G R A P H I C A L A B S T R A C T

• Orthogonal tests were used to evaluate

importance of operating parameters in
CO2 capture.
• Two different spray methods were
discussed for performance compar-
ison.
• luation
Optimal conditions for different eva-
indices were obtained by
range analysis.
• major
MEA and CO concentrations were
2
factors affecting absorption
performance.
• CFD simulation was performed to il-
lustrate the enhancement of gas-liquid
flow field.

A R T I C LE I N FO A B S T R A C T

Keywords: In this research article, orthogonal experiments were performed in a proposed diameter-varying spray tower
Carbon capture system to evaluate the importance of operating parameters and analyse the relationship between factors and the
Orthogonal experiments mass transfer evaluation indices (the CO2 removal rate and overall absorption rate). Two different spray methods
Diameter-varying spray tower such as dual-nozzle opposed impinging and spray in the middle method were discussed for performance com-
Absorption performance
parison. Optimal operating conditions for different evaluation indices were obtained by using range analysis.
After analysis it was found that the absorption performance was mainly affected by two parameters, mono-
ethanolamine concentration and CO2 concentration. The effects of different operating parameters on the CO2
removal rate and overall absorption rate were also discussed by using trend analysis. Furthermore, gas phase
mass transfer coefficient and effective contacting area were determined by experimental data. A comparison
with reported conventional reactor systems demonstrated a great application potential for proposed spray tower
in CO2 capture. Finally, simulation results were illustrated which shows that the gas phase and liquid phase
distributions for the dual-nozzle opposed impinging spray method enhance CO2 absorption performance.

1. Introduction
Carbon dioxide (CO2) emission from fossil fuel combustion makes a
major contribution to the global warming and greenhouse gas effect
[1–4]. Global warming leads to negative impacts like increasing global
average temperature, elevating sea level, coastal region erosion, en-
dangerment of arctic species, and increasing mortality associated with
extreme weathers [5,6]. These side effects are proven to be catastrophic
for both natural ecosystem and human civilization. Hence, CO2 reduc-
tion become a vital international scientific and environmental issue

⁎
Corresponding author.
E-mail addresses: cloud.pine02@mail.xjtu.edu.cn (Y.S. Yu), zhangzx@xjtu.edu.cn (Z.X. Zhang).

https://doi.org/10.1016/j.apenergy.2018.04.053
Received 26 December 2017; Received in revised form 11 April 2018; Accepted 25 April 2018
0306-2619/ © 2018 Elsevier Ltd. All rights reserved.
X.M. Wu et al.
Nomenclature
ae effective contacting area, m2 qm−3
C molar concentration, kmol m−3
CG CO2 concentration, vol%
CL MEA concentration, wt%
D diffusion coefficient, m2 s−1
d diameter, m
H Henry’s coefficient, kPa m3 kmol−1
KG overall mass transfer coefficient of gas phase, kmol m−2
h−1
KGae volumetric overall mass transfer coefficient, kmol m−3
h−1 kPa−1
kG gas phase mass transfer coefficient, kmol m−2 h−1
kL liquid phase mass transfer coefficient, kmol m−2 h−1
[7,8].
Carbon capture and storage (CCS) technology has been recognized
as a promising method to significantly reduce CO2 emissions from
large-point sources such as power plants and heavy manufacturing in-
dustries [9,10]. Compared with other CCS methods, post-combustion
carbon capture is a better route in near and middle term on account of
its economic and feasible retrofit for existing plants without radical
changes [11–14]. Meanwhile, chemical absorption with mono-
ethanolamine (MEA) absorbent is the most well-established technology
for post-combustion carbon capture [15,16].
The packed tower, one of the conventional gas-liquid reactor for
CO2 chemical absorption process, was commonly used absorber on both
lab and industrial scale systems [17–19]. According to number of
meaningful conclusions, it was concluded that this technology was not
yet fully developed for large-scale industrial applications and may not
be economically competitive because of its high capital and operating
costs [20–22]. There are some drawbacks for packed tower like high
gas-phase pressure drop, liquid channeling and flooding and deposition
onto packing material [23]. Therefore, it is necessary to develop effi-
cient gas-liquid reactors for CO2 capture process to enhance the se-
paration performance.
In the past decades, spray tower has been mainly used for sulfur
dioxide removal. Theoretical and experimental studies were conducted
to investigate the promising features like simple construction, lower
pressure drop, large handling capacity, low investment and main-
tenance cost [24–26]. Despite being widely used in the desulfurization
process, the application of spray tower for CO2 scrubbing process is a
relatively recent development trend. Some research has been published
on spray absorption of CO2 by NaOH and ammonia. However, less at-
tention is paid on the utilization of spray tower in CO2 scrubbing pro-
cess with aqueous amine solvents so far. Kuntz and Aroonwilas [27,28]
compared the mass transfer performance of spray tower with packed
tower from lab-scale CO2 absorption with MEA solvent. The spray tower
was declared as a very promising reactor for CO2 capture due to its
higher overall mass transfer coefficient. Niu et al. [29] conducted ex-
periments by using spray tower to study CO2 absorption with MEA
solution and investigated effects of different operating parameters.
Experimental results showed that the mass transfer performance of
scrubbing process was improved by ejecting absorbent through the
nozzle. It was also found that the spray tower achieved more than 95%
CO2 removal rate. Seyboth et al. [30] proposed a bench-scale two-way
experimental approach to investigate the absorption of CO2 by single
spray droplet and demonstrate the applicability of spray scrubbing
process. The results showed that effective contacting area is crucial for
CO2 absorption. Tamhankar et al. [31,32] provided the experimental
data on droplet size distribution for amine sprays and quantified the
available surface area from droplet size measurements for the first time.
Koller et al. [33] investigated a larger pilot spray scrubber plant having
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Applied Energy 225 (2018) 367–379
k1 reaction rate constant, s -1
P pressure, kPa
QG gas flow rate, m3 h−1
QL gas flow rate, L h−1
qG molar gas flow rate, kmol m−3 h−1
S cross-sectional area, m2
T temperature, °C
Vr reactor volume, m3
Y1, Y2 inlet and outlet mole ratio in gas phase
y1, y2 inlet and outlet mole fraction in gas phase
β enhancement factor of chemical reaction
η CO2 removal rate
λ1, λ2 proportionality coefficient
Φ overall absorption rate, kmol m−3 h−1
gas flow rate up to 160 m3/h. They found that the measured absorption
performance achieved by using single nozzle was not sufficient. It was
proposed that spray tower design was improved in future by using
multi-nozzles. The available literature review has revealed the feasi-
bility of spray tower used in CO2 capture process with amine-based
solvents because the existence of spray nozzle significantly increases
interfacial surface area between absorbent and flue gas [34].
The mass transfer performance of traditional spray tower, however,
is not high enough for industrial application. Most of the previous ex-
periments were conducted in a cylindrical tower by using a single spray
nozzle. The configuration of this cylindrical tower was different from
that used in actual industry makes the results of these studies far away
from application. Keeping in view the above discussion, the current
study has been carried out for the enhancement of CO2 absorption
process by using an improved diameter-varying spray tower. As pre-
viously studied, CO2 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 [30,33]. The reaction sections of
the proposed diameter-varying spray tower comprising of major two
parts namely: the cylindrical section and the conical section. The ex-
istence of the conical section would increase the effective contacting
area and gas-liquid contacting time, which will improve the absorption
performance. Some interesting results have been obtained by using the
proposed diameter-varying spray tower in our published work [35,36].
The effects of operating parameters such as MEA concentration, li-
quid flow rate, CO2 concentration and gas flow rate on the CO2 capture
performance has been discussed by the single variable experimental
method in many researches, but few focused on the degree of sig-
nificance of the factors on absorption performance [27,37–39]. Liao
et al. using orthogonal tests to study the mass transfer performance (in
terms of volumetric overall mass transfer coefficient) of blended DEEA-
MEA solution for capturing CO2 in a lab-scale packed reactor and ob-
tained the influence degree order of different operating parameters
[40]. It verified the possibility of orthogonal experimental method
using in CO2 absorption system. However, little attention has been paid
to the spray tower. In this research, orthogonal experiments were
conducted to evaluate the importance of factors (operating parameters)
and analyse the relationship between factors and the mass transfer
evaluation indices (the CO2 removal rate and overall absorption rate)
for the proposed diameter-varying spray tower. Range analysis has been
carried out to obtain the optimal conditions for different performance
evaluation indices and indicate the significance of the factors on CO2
absorption performance. The relationship between the mean values of
each factor and the evaluation indices was obtained by trend analysis.
Two different spray methods were discussed in this work. One is the
dual-nozzle opposed impinging spray method proposed by our research
group, the other is mostly literature discussed spray in the middle
method. Orthogonal test were also performed in order to compare the
X.M. Wu et al. Applied Energy 225 (2018) 367–379

performance of the two different spay methods under the same oper- Table 1
ating conductions. Moreover, the gas phase mass transfer coefficient Geometry parameters of the spray tower.
(kG) and the effective contacting area (ae) were calculated by experi- Parameters Value
mental data. Correspondingly, an attempt has been made to compare
the performance of the proposed system with those available in lit- d1, d2, d3 /mm 200, 120, 160
h1, h2, h3, h4 /mm 50, 200, 300, 235
erature in terms of the interfacial area and gas phase mass transfer
Liquid inlets S2, S3/S1
coefficient. Finally, simulation work was performed to illustrate the gas Liquid outlet S6
and liquid flow field inside the proposed spray tower. Gas inlets S4, S5
Gas outlet S1/S2, S3
Spray nozzles S1, S2, S3
2. Experimental details and analytical methods Orifice diameter/mm 0.5
Spray angle/deg 60
2.1. Experimental description

The proposed diameter-varying spray absorption system is illu-
strated in Fig. 1(a). Fig. 1(b) shows the diameter-varying spray tower in
detailed. The diameter-varying spray tower was fabricated with three
spray nozzles (S1, S2 and S3). Two different spray methods are pre-
sented in this research article, one is dual-nozzle opposed impinging
spray method (S2 and S3 are used as liquid inlets), the other is spray in
the middle method (S1 is used as liquid inlet). For clear process de-
scription, one side of the gas/liquid inlets and one spray method are
show in Fig. 1(a). During the absorption process, flue gas enters the
absorber from the bottom gas inlets (S4 and S5) and then interacts with
aqueous sprayed MEA lean solution entered from the upper part of
tower (S2, S3/S1) for absorption. After the absorption of CO2 by MEA
lean solvent, the produced CO2 rich solvent leaves the absorber at the
bottom and the top vent gas is dried by a drying tower packed with
anhydrous silica gel. An infrared gas analyzer (model IRME-S, Xi'an
Weichuang Instrument Inc.) was used to record the inlet and outlet
concentration of CO2. The reading range of the analyzer is 0–20.0% of
CO2 by volume with the accuracy of 0.1% of the full-scale reading. MEA
solution was pumped to the spray nozzles by using a plunger metering
pump (0.8–1.0 MPa), and the flow rate is measured with a calibrated
rotameter. CO2 and N2 were mixed to simulate the flue gas before en-
tering absorber. The gas mixture was fed into a gas mixing tank to
ensure a uniform distribution of species in the gas. The flow rate of gas
mixture was controlled by a mass flow controller. Experiments were not
terminated until the outlet CO2 concentration reached a steady state.
Experiments are repeated three times to validate the reproducibility of
the results. The standard deviations for the original data (concentration
of CO2 in the outlet of the spray tower) were less than 2.0% and the
largest deviation for the evaluation index (the overall absorption rate)
was 2.4%, which verify the repeatability of the experiments. The geo-
metry parameters of the proposed diameter-varying spray tower are
listed in Table 1.
2.2. Orthogonal experimental design
Orthogonal experimental design method was selected to analyse the
influence degree of MEA concentration (factor A), liquid flow rate
(factor B), CO2 concentration (factor C) and total gas flow rate (factor
D) on CO2 absorption performance. The absorption performance is
evaluated on the basis of the CO2 removal rate (η) and the overall ab-
sorption rate (Φ). The effect of these variables on the absorption per-
formance of CO2 were identified as previously discussed [27,41]. The
orthogonal design table L16 (45), is an orthogonal array of five factors
and each factor has four levels as listed in Table 2. It was assumed that
any two factors did not interact with each other. Sixteen trials were
randomized to avoid any personal or subjective bias. Range analysis
was carried out to reflect the optimal operating conditions and their
magnitudes. Optimal conditions were obtained by the orthogonal ex-
periments and the subsequent data analysis.
2.3. Range analysis
Two crucial parameters in the range analysis are Kji and Rj. Kji is
defined as the sum of evaluation indices of all levels (i = 1, 2, 3, 4) in

Gas flow Pressure

meter gauge

Drying
Computer
tower
N2 CO2
CO2
analyzer
Spray
Pressure
tower
gauge
Gas flow
meter
Feed
Pump receiver
Pressure
gauge
Liquid
Gas mixing flow meter
tank

Liquid
receiver

(a)
Fig. 1. Schematic of experimental setup of CO2 absorption by aqueous MEA in the diameter-varying spray tower (a), the detailed geometry of proposed spray tower
(b).

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X.M. Wu et al. Applied Energy 225 (2018) 367–379

Table 2 diameter-varying spray tower.

Orthogonal experimental design factors and levels for the proposed diameter-
varying spray tower. 3.2.1. CO2 removal rate
Exp. number Codified factors Numerical values The CO2 removal rate characterizes the overall results of CO2 ab-
sorption process and it is simply determined by the amounts of CO2
A B C D A/wt% B/L h−1 C/vol% D/m3 h−1 entering and leaving the spray tower, which is determined by the fol-
1 1 1 1 1 10 40 10.6 1.5
lowing equation
2 1 2 2 2 10 45 14.2 2.5 Y1−Y2
3 1 3 3 3 10 30 18.6 2.0 η= × 100%
4 1 4 4 4 10 35 6.8 3.0
Y1 (12)
5 2 1 2 3 20 40 14.2 3.0
where the mole ratio Y of CO2 to N2 is calculated by using following
6 2 2 1 4 20 45 10.6 2.0
7 2 3 4 1 20 30 6.8 2.5
equation
8 2 4 3 2 20 35 18.6 1.5 y
9 3 1 3 4 30 40 18.6 2.5 Y=
1−y (13)
10 3 2 4 3 30 45 6.8 1.5
11 3 3 1 2 30 30 10.6 3.0 Finally, the CO2 removal rate is obtained by combining Eqs. (12) and
12 3 4 2 1 30 35 14.2 2.0
(13), which was calculated by the following equation
13 4 1 4 2 35 40 6.8 2.0
14 4 2 3 1 35 45 18.6 3.0 y1−y2
15 4 3 2 4 35 30 14.2 1.5 η= × 100%
y1 (1−y2 ) (14)
16 4 4 1 3 35 35 10.6 2.5

3.2.2. Overall absorption rate

each factor (j = A, B, C, D) and kji (the mean value of Kji) is calculated The overall absorption rate is an important parameter to evaluate
to determine the optimal level and the optimal combination of factors. the performance of a reactor. According to literature [21], the overall
The largest kji suggests the optimal level of each factor. Rj is calculated absorption rate was calculated by the following equation
by the range between the maximum and minimum value of kji and it is
used to evaluate the importance of factors. A larger value of Rj means qG (Y1−Y2)
Φ=
the more importance of the corresponding factor. Consider factor A and Vr (15)
the evaluation index η, the calculation process is shown as following. As the diameter of the spray tower is varied along the tower height, the
KA1 = η1 + η2 + η3 + η4 (1) equivalent cross-sectional area is calculated by integrating the cylind-
rical section and conical section, which can be expressed as
KA2 = η5 + η6 + η7 + η8 (2)
λ1 πd12 λ2 πd 22
KA3 = η9 + η10 + η11 + η12 (3) S = λ1 S1 + λ2 S2 = +
4 4 (16)
KA4 = η13 + η14 + η15 + η16 (4) where λ1, λ2 are proportionality coefficient; d1 is the diameter of cy-
lindrical absorption section; d2 is the equivalent diameter of the conical
KA1 K K K
KA1 = ; kA2 = A2 ; A1 ; k 44 = A4 ; absorption section.
4 4 4 4 (5)

Rj = max(kAi )−min(kAi ) (6) 3.2.3. Gas phase mass transfer

where kAi is the k value of i level for the factor A and ηi is the value of
calculated CO2 removal rate for the experimental number i. Other k
values of the other three factors and overall absorption rate Φ can be
obtained by similar steps.
3. Reaction mechanism and mass transfer model
Effective contacting area calculation provides a convenient method
to assess the efficiency of reactor. Furthermore, the effective contacting
area is required to compare the proposed spray tower with the tradi-
tional packed reactor and single-nozzle spray tower in Section 4.
According to the two-film theory, the total resistance of absorption
process consists of gas phase resistance and liquid phase resistance,
which can be presented as [42,43]

3.1. Absorption reaction mechanism 1 1 H

= +
KG kG βkL0 (17)
As the primary amine, MEA directly reacts with CO2 and produces The right-hand side terms of the equation represent the gas and liquid
stable carbonates. The reactions of CO2 with MEA are described as film resistance, respectively.
follows: The unit volume absorption rate Φ was written as
H2 O↔ H3 O+ + OH− (7) Φ = K G ae (PA−PA∗ ) (18)
CO2 + 2H2 O↔ H3 O+ + HCO−3 (8) Following Eq. (19) was obtained from Eqs. (17) and (18) as
HCO−3 + H2 O↔ CO32 − + H3 O+ (9) PA 1 1 1H
= +
Φ ae k G β kL (19)
MEAH+ + H2 O↔ MEA + H3 O+ (10)
Edward’s analogy research proved that the absorption of CO2 using
MEACOO− + H2 O↔ MEA + HCO−3 (11) MEA solution is a rapid pseudo-first-order reversible reaction process
[44]. Thus, the enhancement factor β is calculated as
3.2. Mass transfer model k1 DCO2 C
β=
kL (20)
The CO2 removal rate, overall absorption rate, gas phase mass
transfer coefficient and effective contacting area were selected as the where k1 is the reaction rate constant of CO2 absorption in MEA solu-
indices to evaluate the absorption performance of the proposed tion; DCO2 is the diffusion coefficient of CO2 in aqueous MEA solution; C

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is MEA concentration at gas-liquid interface which is approximately 4. Results and discussions

equal to that of liquid bulk.
Since the solubility and the diffusivity of CO2 in amine solutions is 4.1. Range analysis
difficult to be measured directly. Therefore N2O analogy is frequently
used to estimate the properties of CO2 in amine solutions by using the Orthogonal tests for dual-nozzle opposed impinging spray method
following relations [45]: (results shown in Table 3) and spray in the middle method (results
shown in Table 4) are presented in this section. The amounts of CO2
0
HCO2 = HN2O (HCO2
/ HN02O) (21) entering and leaving the diameter-varying spray tower were used to
determine the CO2 absorption performance evaluation indices (in terms
0
DCO2 = DN2O (DCO / DN02O) (22) of the CO2 removal rate and the overall absorption rate). According to
2
the orthogonal table, sixteen tests were carried out for each spray
where HN2O is the solubility of N2O in amine solution and DN2O is the method. The calculated CO2 removal rate, overall absorption rate and
diffusivity of N2O in amine solution. the range analysis results of two different spray method are shown in
The correlation of solubility and diffusivity of N2O and CO2 in water Tables 3 and 4. These results were considered as the base for sub-
are given as [46,47] sequent range analysis. As already been discussed, for each factor, a
higher mean value (kji) indicates that the level has a larger effect on the
HN02O = 8.5470 × 106exp(−2284/ T ) (23) evaluation index. Therefore, the best level for each factor can be de-
termined by the highest mean value of the experimental condition (kji).
0
HCO = 2.8249 × 106exp(−2044/ T ) (24) Range value (Rj) indicates the significance of the factor’s effect and a
2
larger Rj means the factor has bigger impact on evaluation index.
As shown in Table 3, the range of the CO2 removal rate and the
DN02O = 5.07 × 10−6exp(−2371/ T ) (25) overall absorption rate for dual-nozzle opposed impinging spray
method varies from 76.2% to 99.0% and 0.599 to 2.924 kmol m−3 h−1
0
DCO2
= 2.35 × 10−6exp(−2119/ T ) (26) respectively. The highest CO2 removal rate was obtained at 35 wt%
MEA concentration, 40 L h−1 liquid flow rate, 6.8 vol% CO2 con-
According to the above-mentioned equations, it is concluded that centration and 1.5 m3 h−1 gas flow rate. However, the highest overall
absorption rate was obtained at 35 wt% MEA concentration, 40 L h−1
1 P 1 HCO2 1 1
= A = + liquid flow rate, 18.6 vol% CO2 concentration and 3 m3 h−1 gas flow
K G ae Φ ae k1 DCO2 C ae k G (27) rate. This indicates that the highest CO2 removal rate and the highest
PA HCO2 1
overall absorption rate cannot be obtained simultaneously at the same
The figure of versus is plotted to determine the slope of , condition, so we have to balance their effects in choosing optimal op-
Φ k1 DCO2 C ae
1 1 erating parameters. Comparing the range values of different factors, the
the intercept of ae kG
. Finally, the ae and kG is calculated by math in-
verse. factor’s level of significance for the CO2 removal rate is as MEA

Table 3
Range analysis results of the CO2 removal rate and the overall absorption rate for dual-nozzle opposed impinging spray method.
Exp. number Factor A Factor B Factor C Factor D CO2 removal rate (η)/% Overall absorption rate(Φ)/kmol m−3 h−1

1 1 1 1 1 85.0 0.805
2 1 2 2 2 76.2 1.560
3 1 3 3 3 76.8 1.722
4 1 4 4 4 78.1 0.975
5 2 1 2 3 83.0 2.072
6 2 2 1 4 85.9 1.101
7 2 3 4 1 87.7 0.865
8 2 4 3 2 86.2 1.392
9 3 1 3 4 84.0 2.254
10 3 2 4 3 99.0 0.599
11 3 3 1 2 84.3 1.576
12 3 4 2 1 90.0 1.559
13 4 1 4 2 94.8 0.776
14 4 2 3 1 88.9 2.924
15 4 3 2 4 88.1 1.107
16 4 4 1 3 89.0 1.365

CO2 removal rate (η)/% Overall absorption rate(Φ)/kmol m−3 h−1

A B C D A B C D

K1 316.1 346.8 344.2 351.6 5.062 5.907 4.848 6.153

K2 342.8 350 337.3 341.5 5.431 6.184 6.298 5.305
K3 357.3 336.9 335 347.8 5.988 5.271 8.292 5.758
K4 360.8 343.3 359.6 336.1 6.173 5.291 3.215 5.437
k1 79.0 86.7 86.0 87.9 1.265 1.477 1.212 1.538
k2 85.7 87.5 84.3 85.4 1.358 1.546 1.575 1.326
k3 89.3 84.2 83.8 87.0 1.497 1.318 2.073 1.440
k4 90.2 85.8 89.9 84.0 1.543 1.323 0.804 1.359
Rj 11.2 3.3 6.1 3.9 0.278 0.228 1.269 0.212

Influence degree A > C>D > B C > A>B > D

Best level 35 wt% 45 L h−1 6.8 vol% 1.5 m3 h−1 35 wt% 45 L h−1 18.6 vol% 3 m3 h−1
Best group A(35 wt%)-B(45 L h−1)-C(8 vol%)-D(1.5 m3 h−1) A(35 wt%)-B(45 L h−1)-C(18.6 vol%)-D(3 m3 h−1)

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Table 4
Range analysis results of the CO2 removal rate and the overall absorption rate for spray in the middle method.
Exp. number Factor A Factor B Factor C Factor D CO2 removal rate (η)/% Overall absorption rate(Φ)/kmol m−3 h−1

1 1 1 1 1 83.9 0.769
2 1 2 2 2 77.5 1.614
3 1 3 3 3 74.7 1.676
4 1 4 4 4 77.3 0.945
5 2 1 2 3 82 2.047
6 2 2 1 4 84.7 1.086
7 2 3 4 1 87 0.853
8 2 4 3 2 85.5 1.414
9 3 1 3 4 83.4 2.238
10 3 2 4 3 95.4 0.577
11 3 3 1 2 82.5 1.553
12 3 4 2 1 89.6 1.515
13 4 1 4 2 93.6 0.759
14 4 2 3 1 88.3 2.901
15 4 3 2 4 88.6 1.118
16 4 4 1 3 88.5 1.358

CO2 removal rate (η)/% Overall absorption rate(Φ)/kmol m−3 h−1

A B C D A B C D

K1 313.4 342.9 339.6 348.8 5.005 5.813 4.767 6.038

K2 339.2 345.9 337.7 339.1 5.400 6.191 6.294 5.340
K3 350.9 332.8 331.9 340.6 5.882 5.200 8.229 5.659
K4 359 340.9 353.3 334 6.137 5.232 3.135 5.387
k1 78.4 85.7 84.9 87.2 1.251 1.453 1.192 1.510
k2 84.8 86.5 84.4 84.8 1.350 1.548 1.573 1.335
k3 87.7 83.2 83.0 85.2 1.471 1.300 2.057 1.415
k4 89.8 85.2 88.3 83.5 1.534 1.308 0.784 1.347
Rj 11.4 3.3 5.3 3.7 0.283 0.248 1.273 0.175

Influence degree A > C>D > B C > A>B > D

Best level 35 wt% 45 L h−1 6.8 vol% 1.5 m3 h−1 35 wt% 45 L h−1 18.6 vol% 3 m3 h−1
Best group A(35 wt%)-B(45 L h−1)-C(8 vol%)-D (1.5 m3 h−1) A(35 wt%)-B(45 L h−1)-C(18.6 vol%)-D(3 m3 h−1)

Fig. 2. Effect of MEA concentration on the CO2 removal rate (a) and the overall absorption rate (b) in two different spray methods.

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concentration > CO2 concentration > gas flow rate > liquid flow rate.
However, for the overall absorption rate, the factor’s level of sig-
nificance sequence is CO2 concentration > MEA concentration > liquid
flow rate > gas flow rate. The results indicate that MEA concentration
is the key parameter which affect the CO2 removal rate. And a slight
variation in CO2 concentration may significantly change the overall
absorption rate. Other factors are not as important as MEA concentra-
tion and CO2 concentration. Therefore, it was concluded that higher
CO2 removal rate and overall absorption rate can be obtained by ad-
justing the operating values of MEA concentration and CO2 con-
centration rather than liquid flow rate and gas flow rate.
Table 4 shows that the range of CO2 removal rate and overall ab-
sorption rate varies from 74.7% to 95.4% and 0.577 to 2.901 kmol m−3
h−1 respectively for the typical spray in the middle method. The values
of CO2 removal rate and overall absorption rate for spray in the middle
method are smaller than that of dual-nozzle opposed impinging spray
method, which indicates that the dual-nozzle opposed impinging spray
method has better absorption performance. The highest CO2 removal
rate and the highest overall absorption rate were obtained in the same
conditions as that of using the dual-nozzle opposed impinging spray
method. The factor’s level of significance for the CO2 removal rate and
the overall absorption rate are also the same. This proves the results of
orthogonal experiments once again.
4.2. Trend analysis
Figs. 2–5 show the relationship between the mean values of each
factor and the evaluation indices, as well as the performance compar-
ison of the two different spray methods. These results show similar
trends as the results obtained by single variable experiment. It was
observed that these graphs can only used to describe the trends of each
factor rather than predicting other values.
4.2.1. Effect of MEA concentration
From Fig. 2, it can be seen that the MEA concentration clearly in-
fluenced the CO2 absorption performance positively. Both the CO2
Fig. 3. Effect of liquid flow rate on the CO2 removal rate (a) and the overall absorption rate (b) in two different spray methods.
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Applied Energy 225 (2018) 367–379
removal rate and the overall absorption rate increased noticeably with
the increase of aqueous MEA concentration. Based on thermodynamic
principles, the reaction potential moves toward positive direction with
the increasing concentration of absorbents. The reason is that the mole
ratio of MEA to CO2 increases with the increasing MEA concentration.
Under this condition, more active MEA molecules tend to diffuse to-
ward the gas-liquid surface and then react with CO2 molecules, which
will enlarge the reaction enhancement factor β and lead to a higher
absorption rate. Hence, both the CO2 removal rate and the overall ab-
sorption rate are increased accordingly. However, the viscosity of so-
lution increases at higher MEA concentration which significantly cause
severe corrosion problems in the equipment that limits its industrial
application. These side effects would block the improvement of ab-
sorption performance and increase the capital cost for the maintenance.
Hence, the absorption performance and operating cost should be ba-
lanced when increasing the concentration of MEA.
In detail, Fig. 2(a) and (b) show the effects of MEA concentration on
the CO2 removal rate and the overall absorption rate in the two dif-
ferent spray methods respectively. It is concluded that compared with
spray in the middle method, the dual-nozzle opposed impinging spray
method shows better absorption performance (higher CO2 removal rate
and overall absorption rate). This phenomenon can be attributed to the
fact that for the dual-nozzle opposed impinging spray method, droplets
from two opposite spray nozzles (S2 and S3) impinge and exchange
momentum in the center of the tower, and droplets break into smaller
size ones, which would cause a rapid increase of interfacial area leading
to better mass transfer performance.
4.2.2. Effect of liquid flow rate
The effect of the liquid flow rate on the CO2 removal rate and the
overall absorption rate is shown in Fig. 3. With the increase of liquid
flow rate, both the CO2 removal rate and the overall absorption rate are
increased. It is because as the liquid flow rate increases, the spray
nozzles split the solution into large number of minute droplets and then
spread absorbent in the diameter-varying space. In this sense, the larger
effective interfacial area between the liquid phase and gas phase offers
X.M. Wu et al. Applied Energy 225 (2018) 367–379

Fig. 4. Effect of CO2 concentration on the CO2 removal rate (a) and the overall absorption rate (b) in two different spray methods.

Fig. 5. Effect of gas flow rate the CO2 removal rate (a) and the overall absorption rate (b) in two different spray methods.

a great opportunity for absorption, leading to a better mass transfer
performance between MEA and CO2 molecules. Besides, with the in-
crease of liquid flow rate, the droplets flow rate increases and the
boundary layer of liquid phase decreases, which implied that the re-
sistance for gas diffusion to the liquid phase decreases. Consequently,
both the CO2 removal rate and the overall absorption rate increase with
liquid flow rate. However, it is clearly seen that the increasing tendency
dropped gradually at the higher range of liquid flow rate. This is be-
cause the increase of effective interfacial area is limited due to the
droplets size decrease, leading to a lower increasing tendency. Hence,
the mass transfer performance will not be enhanced further at a higher
liquid flow rate. Previous studies on the CO2 absorption in packed re-
actor also revealed the same trend [48,49].
In detail, Fig. 3(a) and (b) show the effects of liquid flow rate on the

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CO2 removal rate and the overall absorption rate in two different spray
methods respectively. It can be concluded that the dual-nozzle opposed
impinging spray method is more efficient as compared to spray in the
middle method. It was also observed that the CO2 removal rate is less
affected by the liquid flow rate as compare to the effect of MEA con-
centration. However, for the overall absorption rate, the effect of liquid
flow rate is more significant than that of MEA concentration, because of
the larger difference in the overall absorption rate with the changing
liquid flow rate. This phenomenon agrees well with the results of range
analysis as shown in Table 4. It can be concluded that the overall ab-
sorption rate is dominated by the gas mass transfer coefficient as the
liquid flow rate below 35 L h−1. This is the reason why the overall
absorption rate almost keeps stable as the liquid flow rate increases
from 30 L h−1 to 35 L h−1.
4.2.3. Effect of CO2 concentration
Experimental results in Fig. 4 show that the increase of CO2 con-
centration decrease the CO2 removal rate but increase the overall ab-
sorption 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 CO2 concentration, thus giving rise to the increase
of overall absorption rate. Whereas, the mole ratio of MEA to CO2 de-
creases with the increasing CO2 concentration, which means more CO2
molecules will react with limited active MEA molecules. Thus, the CO2
removal rate decreases with the increasing of CO2 concentration. This
demonstrates that the effect of CO2 concentration on the CO2 removal
rate and the overall absorption rate shows opposite effects. Therefore, it
is necessary to maintain the CO2 concentration at a suitable value for a
proper CO2 removal rate and overall absorption rate.
In detail, Fig. 4(a) and (b) show the effects of CO2 concentration on
the CO2 removal rate and the overall absorption rate in the two dif-
ferent spray methods respectively. Fig. 4(a) shows that the dual-nozzle
opposed impinging spray method obviously shows higher CO2 removal
rate at smaller CO2 concentration range. However, in the larger CO2
concentration range, gap is gradually narrowing. This may because
with the increase of CO2 concentration, the effect of more CO2 mole-
cules reaction with limited active MEA molecules dominate the ab-
sorption process, which leads to the reduction in the CO2 removal rate
equivalently both for the dual-nozzle opposed impinging spray method
and spray in the middle method. Fig. 4(b) shows that with the increase
of CO2 concentration, the overall absorption rate changing trend for the
dual-nozzle opposed impinging spray method and spray in the middle
method are almost the same. Under these experimental conditions, the
optimal CO2 concentration for the CO2 removal rate and the overall
absorption rate were found to be 6.8 vol% and 18.6 vol% respectively.
overall absorption rate as compare to the effect of MEA concentration
and CO2 concentration. This also agrees well with the results of range
analysis as shown in Table 4.
From the full trend analysis view, it can be concluded that the
proposed dual-nozzle opposed impinging spray method is a better
technical route for CO2 absorption process compared with traditional
spray in the middle method.
4.3. Results of gas phase mass transfer coefficient and effective contacting
area
Effective contacting area is a frequently-used indicator to assess the
efficiency of a gas-liquid reactor. However, it is difficult to acquire the
theoretical model of effective contacting area and gas phase mass
transfer coefficient, since the fluid flow, mass transfer and reaction
process are very complex in the diameter-varying spray tower. Hence,
semi-empirical correlations coupled with experimental data analysis
were adopted here to calculate the gas phase mass transfer coefficient
and effective contacting area. For the experiments, the total gas flow
rate and the liquid flow rate were set as 3 m3 h−1 and 80 L h−1 re-
spectively. The temperature was record as 20 °C. The CO2 concentra-
tions at the outlet of the tower were obtained after CO2 absorption
using MEA concentrations of 10 wt%, 20 wt%, 30 wt%, 40 wt% re-
spectively. According to Eq. (27), MEA concentrations reflect the cor-
responding HCO2/ (k1 DCO2 C )0.5 and PA /Φ . Linear correlation is accurately
achieved through plotting PA /Φ versus HCO2/ (k1 DCO2 C )0.5 under dif-
ferent CO2 concentrations (correlation coefficients are over 0.98) as
shown in Fig. 6. According to the data in Fig. 6, ae and kG are calculated
and provided in Table 5. As seen in Table 5, the values of ae and kG are
in the range of 168.4–199.6 m2 m−3 and 0.0021–0.0056 kmol m−2 h−1
respectively. When CO2 concentration at 8 vol%, the calculated ae is
168.3 m2 m−3, which is smaller than that in other CO2 concentrations.
It is due to the fact that the liquid flow rate for 8 vol% CO2 con-
centration is in the range of 40–100 L h−1 other than 60–120 L h−1 for
other CO2 concentrations.
Table 6 shows the comparison of the CO2 absorption performance
between the calculated results of the proposed diameter-varying spray
tower and the traditional packed tower system and the single-nozzle
spray tower system. The effective contacting area of the diameter-
varying spray tower is almost double than that of single-nozzle spray
tower and slightly larger than that of packed tower. It implied that the
proposed spray tower could effectively increase the gas-liquid con-
tacting area. Moreover, the gas phase mass transfer coefficient of pro-
posed system is distinctly larger than that of traditional packed tower
system and single-nozzle spray tower system, which also demonstrate

4.2.4. Effect of gas flow rate

Fig. 5 shows that with the increase of gas flow rate, the overall
absorption rate increased while the CO2 removal rate decreased. The
trend coincides with the gas-liquid mass transfer theory stating that the
mass transfer coefficient increases with the increase of gas flow rate.
Furthermore, the high partial pressure of CO2 guaranteed by replen-
ishment of CO2 in the gas-liquid interface contributes to the increase of
the overall absorption rate. However, the liquid to gas ratio decreases
with the increasing gas flow rate, which demonstrates that the excess
flue gas contacted with limited absorbent leading to a decrease of the
CO2 removal rate. Therefore, in order to keep both the CO2 removal
rate and the overall absorption rate at a higher value, it is essential to
maintain gas flow rate at a suitable value.
In detail, Fig. 5(a) and (b) show the effects of gas flow rate on the
CO2 removal rate and the overall absorption rate in the two different
spray methods respectively. It is apparently found that the dual-nozzle
opposed impinging spray method presents higher values of CO2 re-
moval rate and overall absorption rate compared with spray in the
middle method. From the value difference point of view, the effect of Fig. 6. Relationship between PA /Φ and HCO2/ (k1 DCO2 C )0.5 for the diameter-
gas flow rate is significantly less on the CO2 removal rate and the varying spray tower.

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Table 5
Calculated gas phase mass transfer coefficient and effective contacting area.
CO2 concentration kG/kmol m−2 h−1 ae/m2 m−3
8 vol% 0.0056 168.3
12 vol% 0.0031 198.4
16 vol% 0.0029 189.4
18 vol% 0.0021 199.6
the better absorption performance. The interesting results show that the
mass transfer performance of the diameter-varying spray tower is better
than that of traditional packed tower and single-nozzle spray tower,
which demonstrate a great application potential of using the proposed
spray tower in CO2 capture.
4.4. Numerical results of the proposed spray tower
To further discuss the performance of the proposed diameter-
varying spray tower in two different spray methods (dual-nozzle op-
posed impinging spray method and spray in the middle method).
ANSYS Fluent17.2 software was used to simulate gas-liquid two-phase
flow inside the proposed diameter-varying spray tower. The practical
equipment structure and operating conditions of the experiments were
simulated. The aim of this study is to investigate the flow field dis-
tribution of continuous gas phase and dispersed liquid phase. According
to the mesh independence confirmation, 690,000 grids have been put in
use in this work. The continuous gas phase has been described in an
Euler framework and the dispersed liquid phase has been characterized
by a Lagrange approach [52]. In order to analyse the flow field inside
the absorber, some assumptions were made as below:
(a) Only N2 and CO2 in gas phase and the gas phase itself was con-
sidered as incompressible Newtonian fluid.
(b) Liquid inlets were considered as solid-cone spray nozzles and dro-
plets were assumed to be spherical having same diameter.
(c) The dispersed liquid phase occupies a low volume fraction.
(d) The liquid pond was simplified into solid wall, neglecting the im-
pact of the liquid level fluctuation on the flue gas.
(e) The impact of spray pipes and other components in tower on the
flow field was neglected.
(f) The mass transfer and reactions between the flue gas and droplets
were neglected.
4.4.1. Continuous gas phase flow field distribution
Fig. 7 shows the velocity flow field of the diameter-varying spray
tower in two spray methods (dual-nozzle opposed impinging spray
method in Fig. 7(a) and spray in the middle method in Fig. 7(b)).
Fig. 7(a) and (b) indicates that initially flue gas velocity decreased
greatly in the tower due to strong collision and its own volume en-
largement in both spray methods. The flow field of the dual-nozzle
opposed impinging spray method has more vortex than that of spray in
the middle method. Because of the effect of droplets distribution on gas
flow, the dual-nozzle opposed impinging spray forms more vortex. The
vortex make strong turbulent flow, leading to higher degree of disorder
and longer gas-liquid contacting time, which intensifies gas-liquid mass
transfer process. Hence, the spay tower with dual-nozzle opposed im-
pinging spray method shows better CO2 absorption performance than
spray in the middle method. This phenomenon explains the experi-
mental results well. However, for gas phase flow field, vortex may cause
pressure drop and energy loss. Thus, the positive effect of vortex on gas-
liquid absorption process and negative effect on the gas phase flow field
should be balanced by the proper operating conditions.
4.4.2. Dispersed liquid phase concentration distribution
Fig. 8 shows that the droplets distribution for both spray in the
middle method and dual-nozzle opposed impinging spray method looks
uniform. However, particle residence time in Fig. 9 shows that droplets
in the dual-nozzle opposed impinging spray tower stay longer than
droplets in the spray in the middle tower. Longer residence time in-
creases gas-liquid contacting time and improves the absorption per-
formance. Therefore, dual-nozzle opposed impinging spray method
shows more reasonable droplets concentration field distribution com-
pared with spray in the middle method.
5. Conclusions
Orthogonal experiments were conducted here to evaluate the im-
portance of factors (operating parameters) and analyse the relationship
between factors and the mass transfer evaluation indices (the CO2 re-
moval rate and overall absorption rate) in a proposed diameter-varying
spray tower system. Two different spray methods were considered for a
performance comparison. One is the dual-nozzle opposed impinging
spray method proposed by our research group, the other is mostly lit-
erature discussed spray in the middle method.
Range analysis obtained optimal operating conditions for different
indices and indicated that monoethanolamine concentration and CO2
concentration were two major factors affecting the absorption perfor-
mance. This may provide a guidance for industries, to reach better CO2
absorption performance, it is better to mainly focus on adjusting the
operating values of monoethanolamine concentration and CO2 con-
centration rather than liquid flow rate and gas flow rate. For a specific
industry, the CO2 concentration in flue gas did not change a lot. Then
it’s easy to adjust monoethanolamine concentration in a specific CO2
concentration to reach an optimal performance. Trend analysis showed
that both the CO2 removal rate and the overall absorption rate in-
creased as liquid flow rate and MEA concentration increasing. With the
increase of gas flow rate and CO2 concentration, the CO2 removal rate
decreased while the overall absorption rate increased. The performance
comparison of two different spray methods show that the proposed
dual-nozzle opposed impinging spray method is a better choice for CO2

Table 6
Mass transfer performance comparison.
Reactor type ae/m2 m−3 kG/kmol m−2 h−1 Reactor size Experimental conditions Ref.

Packed tower 115.5–135.9 0.00065–0.0076 Packing height: Temperature: 20 °C; Pressure: 0.1 MPa; Absorbent: 2–8% mole/L ammonia; CO2 [50]
400 mm concentration: 15 vol%; Gas flow rate: 0.96–1.68 m3 h−1; Liquid flow rate: 0.27 L
Tower diameter: min−1
100 mm
Single-nozzle spray 81.87–99.25 0.0018–0.0022 Tower height: 350 Temperature: 20 °C; Absorbent: 1–7% mole/L ammonia; CO2 concentration: [51]
tower mm 10–20 vol%; Gas flow rate: 0.2–0.4 m3 h−1; Liquid flow rate: 0.15–0.3 L min−1
Tower diameter:
55 mm
Diameter-varying 168.3–199.6 0.0021–0.0056 Tower height: 600 Temperature: 20 °C; Absorbent: 10–40 wt% MEA; CO2 concentration: 8–18 vol%; This
spray tower mm Gas flow rate: 1–5 m3 h−1; Liquid flow rate: 40–120 L min−1 work
Tower diameter:
120 mm

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Fig. 7. Velocity flow field of dual-nozzle opposed impinging spray method (a) and spray in the middle method (b).

Fig. 8. Droplets concentration distribution of dual-nozzle opposed impinging spray method (a) and spray in the middle method (b).

absorption compared with traditional spray in the middle method. After
further bench-scale and industrial-scale tests, it may be a promising
choice for large-scale industrial application. Furthermore, the gas phase
mass transfer coefficient and effective contacting area were determined
by experimental data. Compared with the conventional packed reactor
system and single-nozzle spray absorption system, the greater gas phase
mass transfer coefficient and effective contacting area indicated that the
proposed diameter-varying spray tower is a promising technical route
for CO2 amine absorption system. Finally, simulation results illustrated
that the gas phase and liquid phase distribution for the dual-nozzle
opposed impinging spray method enhanced absorption performance.
Acknowledgements
Financial supports of the National Natural Science Foundation of
China (Nos. 21736008 and 51506165) is gratefully acknowledged. This

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Fig. 9. Droplets residence time distribution of dual-nozzle opposed impinging spray method (a) and spray in the middle method (b).

work is also supported by the Natural Science Basic Research Plan in [15] Yu YS, Li Y, Lu HF, Yan LW, Zhang ZX, Wang GX, et al. Multi-field synergy study of
Shaanxi Province of China (No. 2015JQ5192) and “Fundamental CO2 capture process by chemical absorption. Chem Eng Sci 2010;65:3279–92.
[16] Zhao B, Su Y, Tao W, Li L, Peng Y. Post-combustion CO2 capture by aqueous am-
Research Funds for the Central Universities”. monia: a state-of-the-art review. Int J Greenh Gas Con 2012;9:355–71.
[17] Yeh JT, Pennline HW, Resnik KP. Study of CO2 absorption and desorption in a
Appendix A. Supplementary material packed column. Energ Fuel 2001;15:274–8.
[18] Bishnoi S, Rochelle GT. Absorption of carbon dioxide into aqueous piperazine: re-
action kinetics, mass transfer and solubility. Chem Eng Sci 2000;55:5531–43.
Supplementary data associated with this article can be found, in the [19] Yeh JT, Pennline HW, Resnik KP. Study of CO2 absorption and desorption in a
online version, at http://dx.doi.org/10.1016/j.apenergy.2018.04.053. packed column. Abstr Pap Am Chem S. 2000;220:U391-U.
[20] Tan LS, Shariff AM, Lau KK, Bustam MA. Factors affecting CO2 absorption efficiency
in packed column: a review. J Ind Eng Chem 2012;18:1874–83.
References [21] Zeng Q, Guo Y, Niu Z, Lin W. The absorption rate of CO2 by aqueous ammonia in a
packed column. Fuel Process Technol 2013;108:76–81.
[22] Wang C, Perry M, Rochelle GT, Seibert AF. Packing characterization: Mass Transfer
[1] Rochelle GT. Amine scrubbing for CO2 capture. Science 2009;325:1652–4.
Properties. 6th Trondheim Conference on CO2 Capture, Transport and Storage.
[2] Florides GA, Christodoulides P. Global warming and carbon dioxide through sci-
2012;23:23–32.
ences. Environ Int 2009;35:390–401.
[23] Lim Y, Choi M, Han K, Yi M, Lee J. Performance characteristics of CO2 capture using
[3] Tan Y, Nookuea W, Li H, Thorin E, Yan J. Property impacts on Carbon Capture and
aqueous ammonia in a single-nozzle spray tower. Ind Eng Chem Res
Storage (CCS) processes: a review. Energ Convers Manage 2016;118:204–22.
2013;52:15131–7.
[4] Oh S-Y, Binns M, Cho H, Kim J-K. Energy minimization of MEA-based CO2 capture
[24] Codolo MC, Bizzo WA. Experimental study of the SO2 removal efficiency and vo-
process. Appl Energ 2016;169:353–62.
lumetric mass transfer coefficients in a pilot-scale multi-nozzle spray tower. Int J
[5] Walther G-R, Post E, Convey P, Menzel A, Parmesan C, Beebee TJ, et al. Ecological
Heat Mass Tran. 2013;66:80–9.
responses to recent climate change. Nature 2002;416:389–95.
[25] Bandyopadhyay A, Biswas MN. Critical flow atomizer in SO2 spray scrubbing. Chem
[6] Wu X, Yu Y, Qin Z, Zhang Z. The advances of post-combustion CO2 capture with
Eng J 2008;139:29–41.
chemical solvents: review and guidelines. Energy Procedia 2014;63:1339–46.
[26] Zhu J, Ye Sc, Bai J, Wu Zy, Liu Zh, Yang Yf. A concise algorithm for calculating
[7] Zhao B, Su Y, Tao W. Mass transfer performance of CO2 capture in rotating packed
absorption height in spray tower for wet limestone–gypsum flue gas desulfurization.
bed: dimensionless modeling and intelligent prediction. Appl Energ
Fuel Process Technol 2015;129:15–23.
2014;136:132–42.
[27] Kuntz J, Aroonwilas A. Performance of spray column for CO2 capture application.
[8] Wu XM, Yu YS, Zhang CY, Wang GX, Feng B. Identifying the CO2 capture perfor-
Ind Eng Chem Res 2008;47:145–53.
mance of CaCl2-supported amine adsorbent by the improved field synergy theory.
[28] Kuntz J, Aroonwilas A. Mass-transfer efficiency of a spray column for CO2 capture
Ind Eng Chem Res 2014;53:10225–37.
by MEA. Energy Procedia 2009;1:205–9.
[9] Leung DYC, Caramanna G, Maroto-Valer MM. An overview of current status of
[29] Niu ZQ, Guo YC, Lin WY. Carbon dioxide removal efficiencies by fine sprays of
carbon dioxide capture and storage technologies. Renew Sust Energ Rev
MEA, NaOH and aqueous ammonia solution. J Tsing Hua Univ. 2010;07:1130–4.
2014;39:426–43.
[30] Seyboth O, Zimmermann S, Heidel B, Scheffknecht G. Development of a spray
[10] Karimi F, Khalilpour R. Evolution of carbon capture and storage research: trends of
scrubbing process for post combustion CO2 capture with amine based solvents.
international collaborations and knowledge maps. Int J Greenh Gas Con
Energy Procedia 2014;63:1667–77.
2015;37:362–76.
[31] Tamhankar Y, King B, Whiteley R, Resetarits M, Cai T, Aichele C. Aqueous amine
[11] Wang M, Joel AS, Ramshaw C, Eimer D, Musa NM. Process intensification for post-
spray absorption and droplet distribution data for CO2 capture applications. Energy
combustion CO2 capture with chemical absorption: a critical review. Appl Energ
Procedia 2014;63:293–300.
2015;158:275–91.
[32] Tamhankar Y, King B, Whiteley J, McCarley K, Cai T, Resetarits M, et al. Interfacial
[12] Li BY, Duan YH, Luebke D, Morreale B. Advances in CO2 capture technology: a
area measurements and surface area quantification for spray absorption. Sep Purif
patent review. Appl Energ 2013;102:1439–47.
Technol 2015;156:311–20.
[13] Wang M, Lawal A, Stephenson P, Sidders J, Ramshaw C. Post-combustion CO2
[33] Koller M, Wappel D, Trofaier N, Gronald G. Test results of CO2 spray scrubbing with
capture with chemical absorption: a state-of-the-art review. Chem Eng Res Des
monoethanolamine. Energy Procedia 2011;4:1777–82.
2011;89:1609–24.
[34] Javed KH, Mahmud T, Purba E. The CO2 capture performance of a high-intensity
[14] McGurk SJ, Martín CF, Brandani S, Sweatman MB, Fan X. Microwave swing re-
vortex spray scrubber. Chem Eng J 2010;162:448–56.
generation of aqueous monoethanolamine for post-combustion CO2 capture. Appl
[35] Wu X, Yu Y, Qin Z, Zhang Z. Performance of CO2 absorption in a diameter-varying
Energ 2017;192:126–33.
spray tower. Chinese J Chem Eng. 2017;25:1109–14.

378
X.M. Wu et al.
[36] Wu X, He M, Yu Y, Qin Z, Zhang Z. Overall mass transfer coefficient of CO2 ab-
sorption in a diameter-varying spray tower. Energy Procedia 2017;114:1665–70.
[37] Zhao B, Liu F, Cui Z. Enhancing the energetic efficiency of MDEA/PZ-based CO2
capture technology for a 650 MW power plant: process improvement. Appl Energ
2017;185:362–75.
[38] Chu F, Liu Y, Yang L. Ammonia escape mass transfer and heat transfer character-
istics of CO2 absorption in packed absorbing column. Appl Energ
2017;205:1596–604.
[39] Abanades S, André L. Design and demonstration of a high temperature solar-heated
rotary tube reactor for continuous particles calcination. Appl Energ
2018;212:1310–20.
[40] Liao H, Gao H, Xu B, Liang Z. Mass transfer performance studies of aqueous blended
DEEA-MEA solution using orthogonal array design in a packed column. Sep Purif
Technol 2017;183:117–26.
[41] Liu Y, Fan W, Wang K, Wang J. Studies of CO2 absorption/regeneration perfor-
mances of novel aqueous monothanlamine (MEA)-based solutions. J Clean Prod
2016;112:4012–21.
[42] Luo X, Hartono A, Hussain S. Mass transfer and kinetics of carbon dioxide ab-
sorption into loaded aqueous monoethanolamine solutions. Chem Eng Sci
2015;123:57–69.
[43] Ma S, Chen G, Zhu S. Mass transfer of ammonia escape and CO2 absorption in CO2
379
Applied Energy 225 (2018) 367–379
capture using ammonia solution in bubbling reactor. Appl Energ 2016;162:354–62.
[44] Ma S, Zang B, Song H, Chen G, Yang J. Research on mass transfer of CO2 absorption
using ammonia solution in spray tower. Int J Heat Mass Trans 2013;67:696–703.
[45] Liao CH, Li MH. Kinetics of absorption of carbon dioxide into aqueous solutions of
monoethanolamine plus N-methyldiethanolamine. Chem Eng Sci 2002;57:4569–82.
[46] Tsai TC, Ko JJ, Wang HM, Lin CY, Li MH. Solubility of nitrous oxide in alkanola-
mine aqueous solutions. J Chem Eng Data 2000;45:341–7.
[47] Ko JJ, Tsai TC, Lin CY, Wang HM, Li MH. Diffusivity of nitrous oxide in aqueous
alkanolamine solutions. J Chem Eng Data 2001;46:160–5.
[48] Aroonwilas A, Tontiwachwuthikul P, Chakma A. Effects of operating and design
parameters on CO2 absorption in columns with structured packings. Sep Purif
Technol 2001;24:403–11.
[49] Tan C-S, Chen J-E. Absorption of carbon dioxide with piperazine and its mixtures in
a rotating packed bed. Sep Purif Technol 2006;49:174–80.
[50] Zeng Q, Guo YC, Niu ZQ. Mass transfer performance of CO2 absorption into aqueous
ammonia in a packed column. CIESCJ 2011;62:146–50.
[51] Taniguchi I, Takamura Y, Asano K. Experimental study of gas absorption with a
spray column. J Chem Eng Jpn 1997;30:427–33.
[52] Hu Y, Tan CK, Broughton J, Roach PA. Development of a first-principles hybrid
model for large-scale reheating furnaces. Appl Energ 2016;173:555–66.