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Article history:
Received 22 March 2013
Received in revised form 7 August 2013
Accepted 12 August 2013
Available online 18 September 2013
Keywords:
CO2 absorption
Packed column
Structured packing
Mass transfer coefcient
Cyclic capacity
a b s t r a c t
The mass transfer performance of the absorption of CO2 in aqueous blended MDEA-MEA solutions was
evaluated experimentally in a lab-scale absorber packed with high efciency DX structured packing over
MDEA-MEA concentrations of 27/3, 25/5, and 23/7%wt under atmospheric pressure using a premixed
feed gas containing 15% CO2 balanced with N2 . The absorption performance was presented in terms
of overall mass transfer coefcient (KG av ) and CO2 concentration prole. The results showed that the
mass transfer performance increased as ratio of MEA in the blended solution, temperature, and liquid
ow rate increased but decreased as CO2 loading increased. In addition, it was found that the cyclic
capacity and relative solvent regeneration ability decreased as the ratio of MEA in the blended solution
increased. Based on mass transfer performance, cyclic capacity, and relative solvent regeneration ability,
23/7%wt MDEA-MEA was found to be the most effective blend ratio among the three ratios investigated
in the present work. Also, the correlation for predicting KG av for CO2 absorption into aqueous blended
MDEA-MEA was successfully developed with an AAD of 21.8%.
2013 Elsevier Ltd. All rights reserved.
1. Introduction
One of the options for reducing carbon dioxide (CO2 ) emissions is absorption of CO2 from gas streams using reactive amine
solvents, which has recently been considered as one of the
most mature and reliable CO2 reduction technologies (Kohl and
Nielsen, 1997; Rao and Rubin, 2002; Liang et al., 2011). The
use of an effective solvent is considered to be one of the key
parameters of this technology. Charkravarty et al. (1985) rstly
introduced blended solvent systems by mixing primary (or secondary) amines with tertiary amines in order to capitalize on
the advantages of each amine and counter the disadvantages
of one amine with another amine. Presently, several blended
conventional amines have been introduced for absorbing CO2
such as blended monoethanolamine (MEA)-methyldiethanolamine
(MDEA), diethanolamine (DEA)-MEA, triethanolamine (TEA)-MEA,
MEA-2-amino-2-methyl-1-propanol (AMP), AMP-MDEA, AMPpiperazine (PZ), and MDEA-PZ (Horng and Li, 2002; Mandal et al.,
2003; Aroonwilas and Veawab, 2004; Ramachandran et al., 2006;
Setameteekul et al., 2008; Huang et al., 2011; Samanta and
Nomenclature
AAD
AMP
Cs
CO2
DEA
GI
kL
KG
KG av
L1
MDEA
MEA
N2
P
PZ
T
TEA
xCO2
yA
yA,G
YA,G
Z
Greek letters
KG av =
GI
P(yA,G yA )
dYA,G
dZ
(1)
3. Experimental
3.1. Chemicals
MDEA and MEA were purchased from Fisher Scientic, Canada,
with purities of 99%. The premixed 15% CO2 (balanced with N2 )
was supplied by Praxair Inc., Canada. All materials in this study were
used as received without further purication. Aqueous solutions of
blended MDEA-MEA of desired concentrations were prepared by a
known amount of deionized water and predetermined amounts of
MDEA and MEA.
3.2. CO2 absorption in packed column
The mass transfer in a packed column occurs when CO2 in the gas
phase transfers across the gasliquid interface into the liquid phase.
In the present work, the mass transfer performance was evaluated
in terms of the overall volumetric mass transfer coefcient KG av and
the CO2 concentration prole along the height of the column. The
KG av can be calculated using Eq. (1), in which several parameters
can be obtained from the experiment. Generally, the experiments
were done at atmospheric pressure P. The inert gas ow rate GI can
be determined from the gas ow rate measurement using electronics Aalborg GFM-17 mass ow meter (ranging from 5 to 50 L/min
with a 0.15%/ C accuracy). The mole fraction of CO2 in the gas
phase yA,G can be determined from an infrared CO2 gas analyzer
(model 301D, Nova Analytical System Inc., Hamilton, ON, Canada),
which is capable of measuring CO2 concentration up to 20% with
0.5% accuracy. The measurement of CO2 concentration was done
along the height of the column through the sampling ports, which
are connected to the CO2 gas analyzer. The mole fraction of CO2 at
interface (yA ) can be calculated using the Henrys law relationship.
The Henrys law constant of blended MDEA-MEA can be calculated
by the correlation established by Wang et al. (1992). The mole ratios
of CO2 in the gas phase (YA,G ) at various heights of the column can be
obtained from the CO2 analyze, and the, plotted against the height
of the column to get dYA,G /dZ.
The glass laboratory absorption column (diameter of
27.5 102 m and height of 2.15 m) was packed with 37 elements of stainless steel Sulzer DX structured packing (with
900 m2 /m3 packing surface area). The schematic diagram of the
experimental setup of CO2 absorption in the packed column is
presented in Fig. 1. The operational procedure of the absorption
column can be found in our previous works (Fu et al., 2012; Naami
et al., 2012). In order to validate the absorption column used in the
present work, 2 M MEA solution was tested and compared with
the results from deMontigny (2004). It was found that the results
obtained in the present work are in good agreement with those
obtained in deMontigny (2004) as shown in Fig. 2.
4. Results and discussion
The mass transfer performance of CO2 absorption into aqueous
solutions of blended MDEA-MEA was experimentally determined
in the laboratory-scale absorption column packed with DX structured packing and reported in terms of KG av and CO2 concentration
prole along the height of the column. The values of KG av are proportional to the mass transfer performance in that the higher the
KG av , the higher mass transfer performance. For the CO2 concentration prole, a lower CO2 concentration prole indicates a larger
amount of CO2 that has been removed from the gas stream resulting
in higher mass transfer performance.
The experiments were done at various MDEA-MEA concentrations of 27/3, 25/5, and 23/7%wt (which are equivalent
to MDEA-MEA molar ratios of 2.3/0.5, 2.1/0.8, and 1.95/1.16,
Fig. 1. Schematic diagram of the experimental setup of CO2 absorption in packed column.
absorbed CO2 removed CO2
100% (2)
absorbed CO
Fig. 2. Validation of packed column using 2.0 M MEA at temperature of 294 K, CO2
loading at absorber top of 0.2 mol CO2 /mol amine, liquid ow rate of 5 m3 /m2 , inert
gas ow rate of 17.85 kmol/m2 h, and YCO2 of 0.09.
Fig. 3. Effect of MDEA-MEA blended ratio on CO2 concentration prole at temperature of 294 K, CO2 loading at absorber top of 0.25 mol CO2 /mol amine, liquid ow
rate of 5 m3 /m2 , and inert gas ow rate of 15.99 kmol/m2 h.
Fig. 7. Effect of CO2 loading at absorber top on CO2 concentration prole of 23/7%wt
MDEA-MEA at temperature of 294 K, liquid ow rate of 5 m3 /m2 , and inert gas ow
rate of 18.65 kmol/m2 h.
Fig. 12. Experimental set up for determining relative solvent regeneration ability.
10
Fig. 13. Relative solvent regeneration ability of 5 M MEA, 2 M MDEA, and 2.3/0.5 M
(27/3%wt) MDEA-MEA.
the blended solutions, the higher the amounts of the more reactive
MEA molecules that can absorb CO2 ; thus, a higher mass transfer
performance was observed. By comparing the three MDEA-MEA
blend ratios (27/3, 25/5, and 23/7%wt MDEA-MEA), it was observed
that the 23/7%wt MDEA-MEA provided the best mass transfer performance among the three as shown in Figs. 3, 4, 6, 8 and 10.
However, in order to effectively use blended MDEA-MEA, not only
mass transfer performance, but also the cyclic capacity and relative
regeneration ability should be taken into consideration.
In summary, by increasing the ratio of MEA in the blended solution, the mass transfer performance would be increased but the
cyclic capacity and the relative solvent regeneration ability would
be decreased. As shown in Figs. 3, 4, 6, 8 and 10, it can be observed
that the mass transfer of 23/7%wt MDEA-MEA is much higher than
those of 25/5 and 27/3%wt MDEA-MEA, respectively. On the other
hand, the cyclic capacities of the three blend ratios are considerably close to each other as presented in Fig. 11. Therefore, it can be
reported that the effect of ratio of MEA in the blended MDEA-MEA
solutions on mass transfer performance is more signicant than
that on cyclic capacity. As a result, based on above discussion, it
is reasonable to conclude that the 23/7%wt MDEA-MEA provides
the best CO2 absorption performance among the three blending ratios over the operating conditions conducted in the present
work.
4.7. Empirical predictive correlation for KG av of blended
MDEA-MEA
Liang et al. (2011) mentioned that in order to effectively
design an absorption column, the KG av is required. However, it
is an expensive and time consuming process to experimentally
determine the KG av in a packed column. Thus, the predictive correlation for KG av is then found to be important since it can be
used to determine the KG av from operating conditions without
experimental work. Dey and Aroonwilas (2009) proposed a predictive correlation for blended AMP-MEA. The model was tested
with the experimental mass transfer data of blended AMP-MEA
in a laboratory-scale absorption column packed with DX structural packing. They concluded that the predictive results were
found to be in good agreement with the experimental results.
For the MDEA-MEA system, the predictive correlation can be seen
in Eq. (3).
KG av = K eA(MDEA/MEA) eB eCxCO2 L1D eECs eF/T
(3)
11
Table 1
Summary of parameters for predictive equation presented in Eq. (3).
Concentration of
blended
MDEA-MEA (% wt)
Condential level
AAD
27/3
25/5
23/7
0.97
0.97
0.99
0.0032
0
0.04
4
1.1
3.65
10.325
14.3
11.4
0.8531
0.559
0.91
0.1438
0.3665
0.2
595.211
511.5
443
0.9254
1
1
20.9%
21.7%
22.8%
References
Fig. 14. Parity chart compares predicted and experimental values of KG av for CO2
absorption into blended MDEA-MEA solutions.
5. Conclusions
The mass transfer performance of CO2 absorption into aqueous
solutions of blended MDEA-MEA was experimentally determined
(in terms of KG av and CO2 concentration prole) in a laboratoryscale absorption column packed with DX structured packing. The
experiments were conducted at various operating conditions of
MDEA-MEA blending ratios (27/3, 25/5, and 23/7%wt), temperatures (298, 303, and 318 K), CO2 loadings at the absorber top
(0.05, 0.17, and 0.25 mol CO2 /mol amine), and liquid ow rates
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increases within the range of conditions using in the present work.
On the other hand, the cyclic capacity and the relative solvent
regeneration ability decrease as the ratio of MEA in the blended
solution increases. However, after taking into consideration all
three parameters (i.e., mass transfer performance, cyclic capacity, and relative solvent regeneration ability), it can be concluded
that 23/7%wt MDEA-MEA provides the best CO2 absorption performance among the three blend ratios over the operating conditions
conducted in the present work.
Acknowledgments
The rst author (A. Naami) would like to acknowledge and
appreciate the scholarship support from the Libyan Higher Educational studies through the cultural section of the Libyan Embassy
in Ottawa, Canada. The nancial support from the National Natural
Science Foundation of China (NSFC No. 21276068, 21250110514,
and 21376067), Ministry of Science and Technology of the Peoples of Republic of China (MOST No. 2012BAC26B01), Ministry
of Education of the Peoples of Republic of China-Supported Program for Innovative Research Team in University (No. IRT1238),
Shaanxi Yanchang Petroleum (Group) Co., LTD, Chinas State
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