Chemical Engineering Science 229 (2021) 116041

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Chemical Engineering Science

journal homepage: www.elsevier.com/locate/ces

Experimental investigation of hydrodynamic parameters and bubble

characteristics in CO2 absorption column using pure ionic liquid and
binary mixtures: Effect of porous sparger and operating conditions
Masroor Abro a, Liang Yu b, Guangren Yu a,⇑, Xiaochun Chen a,⇑, Abdul Basit Qazi a
a
Beijing Key Laboratory of Membrane Science & Technology, College of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, PR China
b
Department of Biological Systems Engineering, Washington State University, Pullman, WA 99164, USA

h i g h l i g h t s

Bubble size and hydrodynamic parameters were compared for pure ionic liquid and binary mixtures.

Effect of sparger pore size and operating conditions was studied in gas-pure ionic liquid system.

Empirical correlations were proposed to predict the bubble size gas holdup in pure ionic liquid.

Correlations can be used for different bubble column sizes.

a r t i c l e i n f o a b s t r a c t

Article history: For first time, bubble size distribution, bubble shape, bubble orientation, mean bubble size (d32), gas
Received 11 April 2020 holdup (eg) and interfacial area in pure IL [BMIM][BF4] were compared with those in its binary mixtures
Received in revised form 10 July 2020 with MEA and MeOH. Experiments were performed in small-scale cylindrical bubble column with a por-
Accepted 10 August 2020
ous sparger using a high-speed image capture system. Further, to investigate effects of sparger pore size,
Available online 13 August 2020
column diameter, temperature and gas flow rate, experiments were performed employing gas-pure IL
system. Compared with pure IL, d32 in binary mixtures was smaller, which decreased with increasing
Keywords:
MEA or MeOH concentration, whereas, gas holdup and interfacial area were increased. MeOH exhibited
Ionic Liquid
Binary mixtures
profound effect as compared to MEA. In gas-pure IL, sparger pore size and temperature significantly influ-
CO2 capture system enced on aforementioned parameters. Correlations were proposed for predicting d32 and eg in pure IL for
Bubble column two different column sizes demonstrating their applicability in higher column dimensions and scaling-
Bubble size up.
Hydrodynamics Ó 2020 Elsevier Ltd. All rights reserved.

1. Introduction
Greenhouse gases have resulted in the severe consequences on
our society such as rapidly increasing global warming. Among all
the greenhouse gases, Carbon dioxide is responsible for contribut-
ing more than 60% global warming (Tagiuri et al., 2014). Therefore,
CO2 capture has received huge attention with the regard of green-
house gas control (Zeng et al., 2017). Till now, several CO2 capture
techniques have been developed such as membrane separation (Yu
et al., 2019), adsorption (Cho et al., 2019) and absorption (Wang
et al., 2010). Aqueous amine based chemical absorption processes
have been extensively used in industries due to higher CO2 absorp-
⇑ Corresponding authors. Tel./Fax: +86-10-6443-4892.
E-mail addresses: gryu@mail.buct.edu.cn (G. Yu), chenxc@mail.buct.edu.cn
(X. Chen).
tion rate under the conditions of low gas partial pressure (Sun
et al., 2017). However, these processes have a few disadvantages,
i.e., loss of volatile amines and uptake of water into gas streams
which overall increases the regeneration cost, energy and con-
sumption and corrosion as well (Li et al., 2008). The physical sol-
vents such as methanol and ethanol are also used for CO2
capture in industries due to advantages over others such as low
viscosity, low surface tension and easy availability and good CO2
capture performance (Chen et al., 2013). Even though, methanol
(MeOH) is a non-corrosive solvent, its high volatility results into
the huge solvent loss making the separation process uneconomical
(Lei et al., 2013). Thus, the suitable absorption processes could be
desirably adopted.
Presently, the environmentally benign ionic liquids (ILs) have
been paid huge attention by virtue of their great versatility and
tunability and they are considered as promising candidates for

https://doi.org/10.1016/j.ces.2020.116041
0009-2509/Ó 2020 Elsevier Ltd. All rights reserved.
2 M. Abro et al. / Chemical Engineering Science 229 (2021) 116041
CO2 capture. Their advantageous characteristics include negligible
vapor pressure which prevents the contamination of gas stream
and solvent loss, wide liquidus range, and high thermal and chem-
ical stability (Zeng et al., 2017). More importantly, the CO2 absorp-
tion in common ILs is physical in nature which makes the
desorption of CO2 and regeneration of ILs relatively economical
and energy-efficient (Zhang et al., 2012). However, the conven-
tional ILs have few inherent demerits of high viscosity, cost and
small CO2 solubility under ambient pressure which can be using
task specific ILs (TSILs) being capable of CO2 chemisorption. CO2
mass transfer performance is mainly limited by their viscosity.
The operating temperature and pressure can reasonably improve
the CO2 performance Basically, the TSILs are synthesized by intro-
ducing suitable moieties such as amines into conventional ILs
which reasonably increase CO2 capture performance. CO2 capture
performance of TSILs is as good as to those by aqueous amines.
Nevertheless, complexity in their synthesis process and high vis-
cosity still lead to high synthesis cost and slow CO2 transfer rate,
which are challenges with their practical applications (Aghaie
et al., 2018).
Therefore, binary mixture of conventional ILs with other sol-
vents such as aqueous amine, pure amine and methanol could be
a suitable choice to achieve the desirable CO2 capture and avoid
the aforementioned drawbacks by retaining the desirable proper-
ties of ILs (i.e., affinity for CO2 capture). Yang et al. (2014) reported
that mixed IL- aqueous monoethanol amine (MEA) solution (30 wt
% MEA + 40 wt% [BMIM][BF4] + 30 wt% H2O) improved CO2 absorp-
tion as compared to 30 wt% MEA aqueous solution. Taib and
Murugesan (2012) used hybrid solvent by mixing bis(2-
hydroxyethylammonium acetate [bheaa] and 1-butyl-3-
methylimidazolium tetrafluoroborate [BMIM][BF4] with aqueous
amine solutions. These studies suggested that CO2 absorption per-
formance of such mixtures was comparable to those of aqueous
amines. However, uptake of water in the gas stream was still a
problem causing the corrosion of equipment, which can be over-
come by preparing the binary mixture of pure amine and IL. Yu
et al. (2016) used four binary mixtures MEA-[BMIM][PF6], MEA-
[BMIM][BF4], MEA-[EMIM][BF4] and MEA-[EMIM][PF6]. They found
that binary mixtures significantly increased the CO2 absorption
compared with those by pure ILs. Moreover, combination of ami-
nes and ILs also reduces the loss of amine solvent and the cost of
solvent regeneration. Similarly, binary mixtures of ILs with famous
physical absorbent i.e., MeOH, are preferable candidate over either
a pure IL or MeOH for CO2 capture. Since, it integrates the advan-
tages of both the methanol which lowers the viscosity, surface ten-
sion and stimulates the CO2 absorption, and IL which offers the
non-volatility, ultimately decreases the methanol loss. Dai et al.
(2015) proposed the use of [OMIM][Tf2N]-MeOH mixture for CO2
capture. They found that the loss of methanol in the absorption
column was greatly decreased as a result of using their mixture
as an absorbent. Taheri et al. (2018) measured the CO2 solubility
in pure [AMIM][Tf2N], pure methanol and their binary mixture.
The addition of IL into MeOH increased the CO2 solubility and
decreased the loss of methanol into the gas stream. These studies
reveal that a binary mixture of IL with amine and methanol can
desirably enhance CO2 capture. CO2 absorption in pure ILs at ele-
vated temperature could be a way to limit the hindering effect of
ILs’ viscosity on CO2 mass transfer. Zhang et al. (2014) reported a
positive effect of temperature on CO2 diffusivity and mass transfer
coefficient in ILs, which is favorable for increasing mass transfer
performance. Bao et al. (2015) numerically investigated that rate
of CO2 mass transfer in IL was affected by operating temperature
and pressure. Most of ILs have advantages of high thermal stability,
therefore, they can be easily exposed under conditions of elevated
temperature. Selection of proper operating conditions and use of
ILs mixed solvents could open the door for their industrialization.
In order to propose the ILs and its aforementioned binary mixtures
for the industrial CO2 capture processes, it is strongly recom-
mended to develop a better insight into their hydrodynamic
behavior in multiphase contacting devices.
Bubble column is one of the simplest and advantageous multi-
phase contacting devices to be used in industries for physical and
chemical processes. Study on gas–liquid dynamics in bubble col-
umn provides useful guideline in designing and scaling-up the
industrial reactors since it governs overall operation. In gas–liquid
mass transfer process, one of the key parameter is the interfacial
area which is significantly affected by the gas holdup and bubble
size which strongly depend on the operating conditions, liquid
properties and gas sparger configuration (Camarasa et al., 1999;
Gemello et al., 2018). Previously, several studies on the bubble
behavior and hydrodynamic characteristics of different liquids
have been reported, such as water (Akita and Yoshida, 1974;
Besagni et al., 2018; Chen et al., 2004; Gemello et al., 2018), piper-
azine solution (Pashaei et al., 2017) methanol, isopropanol, toluene
and acetone (Pohorecki et al., 2005a). A few studies have been
reported on hydrodynamic behavior and CO2-IL system such as
gas bubbling through IL (Kaji et al., 2009), rise and deformation
of a single bubble through ILs (Dong et al., 2010), bubble behavior
in ILs with different water content (Zhang et al., 2014). Wang et al.
(2010) used coupled CFD-PBM model to investigate the mass
transfer properties of CO2 absorption in IL employing a new drag
correlation. Ali et al. (2019) used improved volume of fluid (VOF)
model coupled with FW-H acoustic model to understand the bub-
ble formation in IL through an orifice. Ali et al. (2018) used CFD
model to understand the hydrodynamic characteristics of both
the amine and IL in flat bubble column. Zhang et al. (2012) con-
ducted a series of experiments in bubble column consisting of IL-
CO2/N2 and studied the bubble size distribution (BSD), gas holdup
and interfacial area. They proposed a new correlation for predicting
the Sauter mean diameter (d32) in ILs. Similar with other examples
of CO2
Developing an industrial CO2 capture process using ILs and their
mixed solvents, the gas–liquid hydrodynamics in bubble columns
could be the subject to the research. In designing of the bubble col-
umn reactors, several factors such as, gas holdup, mean bubble
size, interfacial area, BSD have great significance. BSD is important
to describe the extent of coalescence and breakage of bubbles in
bubble columns, as well as to define the flow regime. It is mainly
controlled by gas sparger configurations, operating conditions
and dimensions of bubble column. Porous/fine spargers usually
produce small bubbles stabilizing the uniform flow regime,
whereas, the coarse spargers produce large bubbles, and existing
regime will be heterogenous flow regime (Besagni et al., 2017c).
For developing CO2 capture bubble columns employing ILs and
their mixed solvents, lack of knowledge regarding these parame-
ters is still a bottleneck. In addition, the shape of bubbles is also
a crucial parameters in terms of characterizing the multiphase flow
behavior of different systems (Ziegenhein and Lucas, 2017). To the
best of our knowledge, these all parameters have been never
reported together in the past literature for pure ILs and specially
for their mixed solvents. Moreover, the effect of gas sparger partic-
ularly a porous sparger on the bubble size and gas holdup in the
gas-IL system could be a new contribution. Since, the gas sparger
is a highly influential factor on the bubble size and overall dynamic
characteristics of a gas–liquid bubble column (Anastasiou et al.,
2013). Different sparger types such as perforated, membrane and
porous have been used in a bubble column. Porous spargers are
advantageous over others, since, they inject numerous smaller
bubbles and offer a higher interfacial area (Kazakis et al., 2008).
Therefore, in this study, a small-scale cylindrical bubble column
equipped with a porous sparger was taken, which was filled with
quiescent liquid. For the liquid phase, pure IL i.e., [BMIM][BF4],
 M. Abro et al. / Chemical Engineering Science 229 (2021) 116041
and its four binary mixtures were chosen. MEA and MeOH were
used as additives in the binary mixtures at different concentra-
tions. [BMIM][BF4] has been widely reported in applications of
CO2 capture, its basic advantages include, physical absorption
Gas phase was a mixture of N2 (90 vol%) and CO2 (10 vol%). A series
of experiments was conducted using a high-speed image capture
system under different operating conditions. First, bubble size dis-
tribution, aspect ratio E distribution, bubble orientation distribu-
tion, mean bubble size (d32), gas holdup and interfacial area in
pure IL i.e., [BMIM][BF4] were compared with those in its binary
mixtures. Further, to develop the insight into the role of design
and operating factors, such as sparger pore size, column diameter,
temperature and gas flow rate, the experiments were performed
employing a gas-pure IL system. The present study has also con-
tributed to propose empirical correlations for prediction of sauter
mean diameter d32 and overall gas holdup in pure gas-pure IL sys-
tem. This study was aimed at investigating the hydrodynamic
parameters and aforementioned bubble characteristics without
encompassing the CO2 mass transfer into liquid phase, which could
be a subject to future study. The well known design and scale-up
criteria of bubble column are: DC  0.15 m and column height to
diameter ratio >5 (Kantarci et al., 2005; Wilkinson et al., 1992).
The frequent studies have been conducted on hydrodynamics of
low viscous liquids in bubble columns following the above criteria
(Besagni and Inzoli, 2016a,b; Besagni et al., 2017b; Guédon et al.,
2017). However, these studies are not limited to low viscous liq-
uids only, there is a few studies who reported high viscous liquids
(Cho et al., 2002; Kang et al., 1999), slurries (Krishna et al., 2001) in
large scale bubble column meeting the above scale-up criteria.
These studies can be mimicked for high viscous ILs to investigate
the fluid dynamic behavior in such large bubble columns which
is still an obstruction for their industrialization. However, consid-
ering the high cost of ILs, small size bubble column was selected
in this study. Hydrodynamic study in small bubble columns has
been reported in several past literatures (Götz et al., 2016). There
are several examples in past those have used the bubble columns
with diameter <0.15 m and investigated the hydrodynamic mass
transfer and heat transfer properties (Deckwer et al., 1980; Kaji
et al., 2009; Krishna et al., 1994). Likewise, the major focus of this
work to perform parametric investigations of basic hydrodynamic
parameters and bubble characteristics in pure IL and its binary
mixtures. Even though the bubble column scale-up criteria was
not followed in present setup, the basic phenomena covered in this
work and results will provide useful guidelines and general trends
for future study of CO2 absorption systems in industrial bubble col-
umn reactors and validation of the different CFD models to get a
deep insight into multiphase dynamic characteristics.
2. Experiments
2.1. Materials
[BMIM][BF4] was synthesized by adopting previously reported
method (Dharaskar et al., 2016). To achieve the high degree of ionic
liquid purity, it was dried under vacuum at 80 °C for ~ 24 h and
finally filtered under vacuum to remove the traces of impurities
such as, dichloromethane before its final use. [BMIM][BF4] has
been widely reported in CO2 capture processes. In this work, it
was selected because, imidazolium based ILs offer remarkable
CO2 solubility and selectivity in real applications when the gas
stream comprises of multiple components (Camper et al., 2008;
Khan et al., 2016). Another advantage of imidazolium based ILs is
their high thermal stability (Cao and Mu, 2014), enabling the CO2
capture under elevated temperatures also. [BF4] was chosen as
anion specie because, compared with non-fluorinated ILs, fluori-
3
nated ILs offer higher CO2 affinity (Ramdin et al., 2012). Neverthe-
less, studies are not limited to imidazolium based ILs and till now,
a broad variety of ILs have been tested for the CO2 absorption
capacity, such as Trialkyl imidazolium, sulfonium, pyridinium,
and pyrrolidinium cations based ILs containing di (Farahipour
et al., 2016), which were found to be promising physical absorption
solvents. Maiti (2009) investigated that guanidinium cation based
ILs were found to be more efficient for CO2 capture than imida-
zolium based ILs containing same anion. Here, we restrict our dis-
cussion regarding the selection of ILs because this study is mainly
focused upon the investigation of hydrodynamic parameters and
bubble characteristics in pure IL and binary mixtures. It is also rec-
ommended to perform same experimental investigations for differ-
ent variety of potential ILs in future study.
Monoethanol amine (MEA) was purchased from Tianjin Fuchen
Chemical Reagents Co. Ltd. company with the purity of 99%-100%,
and methanol (MeOH 99.5% pure) was purchased from Beijing
Chemical Works. Two pairs of the binary mixtures; one composed
of IL and MEA and other composed of IL and MeOH, were synthe-
sized and in each, their different concentrations were used without
any treatment. The viscosity (ml) of pure IL and binary mixtures was
measured using a digital viscometer (BROOKFIELD DV-II + Pro), for
the density (ql ) measurement, a standard pycnometer was used.
The composition and physical properties of all liquid systems are
summarized in Table 1.
2.2. Experimental setup
The schematic representation of the current experimental setup
is depicted in Fig. 1. The experiments were performed in a small-
scale cylindrical bubble column equipped with a porous gas spar-
ger, whose dimensions were; inner diameter (DC) of 2 cm and
height (H) of 30 cm. The bubble column was surrounded by
another cylindrical column and their annular gap was filled with
water to achieve the desirable temperature of ionic liquid and bin-
ary mixtures, as well as to minimize the optical distortion in image
capturing and improve the flow visualization. The column was
filled with liquid to initial height of 10 cm and gas was introduced
homogeneously at the bottom through a porous plate sparger. The
gas phase was a mixture of N2 (90 vol%) and CO2 (10 vol%) in all
experiments, whereas, the different liquids varying in viscosity,
density and surface tension (as enlisted in Table 1), were used as
the liquid phase. In this work, two spargers namely Sp-A and Sp-
B with different pore sizes i.e., 4–9 mm and ~ 16 mm respectively
were used. The sparger was connected to a gas cylinder through
a pressure control valve and a calibrated volumetric flowmeter (ro-
tameter) in order to control and measure the gas flow rate (Qg). The
selected range of gas flow rate was 30 cm3/min to 250 cm3/min
corresponding to superficial gas velocity of 0.0016 m/s 0.013 m/s
under which the bubble column is operated within uniform or
pseudo-uniform regime. In addition, porous plate spargers generate
smaller bubbles usually, which develop uniform/pseudo-uniform
flow regime even to a certain range of high gas flow rates as com-
pared to other gas spargers, it is their key advantage. All the exper-
iments were performed under the atmospheric pressure, however,
the liquid phase temperature was varied in the range of 300 K-
333 K. A water bath was used to adjust the temperature of the sur-
rounding water and ultimately the temperature of liquid inside the
bubble column which was measured by a lab-thermometer. The
gas temperature was not a concern in this setup due to its minimal
effect on properties of gas in this range. Moreover, gas flow rate
conditions were taken in low range leading an insignificant effect
of gas temperature on overall temperature of system which was
guaranteed by measuring the system temperature continuously
at different intervals. At a given temperature, experiments were
4 M. Abro et al. / Chemical Engineering Science 229 (2021) 116041

Table 1
Liquids used in experiments and their properties against temperature.

Liquid T(K) [BMIM][BF4](Vol. %) MEA(Vol. %) MeOH(Vol. %) ml(Pa.s) ql (Kg/m3) r(N/m)

Pure IL 300 100 0 0 0.082 1195.2 0.04384
313 0.0559 1189.13 0.0435
333 0.0274 1176.16 0.043
IL/MEA-1 300 90 10 0 0.06592 1177.56 0.0442
IL/MEA-2 300 80 20 0 0.05703 1169.13 0.0446
IL/MeOH-1 300 66.66 0 33.33 0.01548 1045.65 0.0313
IL/MeOH-2 300 50 0 50 0.006685 979.18 0.0283

Fig. 1. Schematic representation of experimental setup.

performed under different gas flow rates, by adjusting the gas vol- image processing using Image Pro Plus is an advantageous tech-
umetric flow meter. Every time, careful measures were taken to nique which directly converts the number of pixels into length unit
well clean the bubble column in order to avoid presence of any to measure the size of required object, however it is reasonably a
contamination resulting into poisoning of images quality. time taking procedure. For a single experiment, three images
recorded at different times were randomly selected from a total
number of 2000 and an adequate number of bubbles (~200) per
2.3. Image capture and analysis system
image were measured for average bubble size. In this way three
different readings of d32 per single experiment were obtained
A high-speed image capture system comprising of a high-speed
and error of bubble size measurement was analyzed in terms of
camera (Mikrotron CAMMC1362) and a frame-grabber (OR-Y4C0-
relative standard deviation (Supplementary information S1). The
XMX00 model) was employed. This system was easily integrated
lens of camera was focused on the inner column to capture the
into a standard personal computer, and images were recorded on
middle vertical plane. Due to overall small diameter of column,
its storage disk. The specific regions of the bubble column were
the entire middle plane of inner column was captured. It is men-
provided with a glass sheet as background, behind which, a lamp
tioned in previous section, that surrounding water improved the
was illuminated allowing the uniform distribution of light. After
flow visualization, still the optical distortion was present due to
injecting gas, a time interval of almost 3 mins (which was found
round shape of column. This optical distortion was corrected by
to be sufficient time for such a small system) was set to achieve
adopting the procedure of (Legendre and Zevenhoven, 2019), in
a fully developed flow behavior and BSD inside the column for each
which a square grid pattern was used to determine distortion, later
experimental run. The images were recorded for every 10 sec peri-
the grid point were used to perform linear piecewise transforma-
odically at an interval gape of 30 sec, and total sampling time was
tion of captured images for correction of curvature effect (supple-
200 sec. A metering tape was pasted on the column and a known
mentary information Fig. S2). A maximum error of 8.33% was found
distance in the given field was measured for the calibration of
between distorted image and distortion corrected image in all
the image capture system. The present high-speed image capture
measurements. To further obtain accuracy in image analysis, the
system was found efficient at measuring the minimum bubble size
bubbles in wall adjacent layer were not sampled.
of ~0.1 mm. The images were captured at the rate of 500 fps with
The obtained images gave 2D representation of bubbles com-
resolution of 1280  1024 and the size of bubbles was obtained
prising of different shapes such as ellipsoidal and spherical. There-
using Image Pro Plus software which helps at differentiating easily
fore, the bubble size was defined by spherical equivalent diameter
the interfaces of bubbles Zhang et al. (2012), therefore, size of
(db Þ which requires the knowledge about the length of major and
small as well as large bubbles can be measured effectively. Digital
 M. Abro et al. / Chemical Engineering Science 229 (2021) 116041 5

minor axis of bubbles. Using Image Pro Plus, these distances were
measured and equivalent diameter was obtained by Eq. (1).
qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
3 max 2 min
db ¼ db db ð1Þ
max min
where db and db are the length of major and minor axis of bub-
bles respectively as shown in Fig. 2. The mean bubble size is repre-
sented by the Sauter mean diameter d32 , which was calculated as,
PN 3
di
d32 ¼ Pi¼1
N 2
ð2Þ
i¼1 di

The bubble size was measured in the axial region between 6 cm

and 9 cm above the gas sparger.

3. Results and discussion

3.1. Distribution of bubble size, aspect ratio and bubble orientation

This section presents the quantitative analysis of distribution of

bubble size (BSD), bubble shape (aspect ratio (E)) and bubble orien-
tation (h). These mainly depend upon liquid properties, sparger
pore size and operating parameters. Here, one-time-one-factor
(OTOF) approach was used to investigate the significance of each
parameter. Spatial evolution of BSD was not considered, it was
computed in a fixed region over an area of 2 cm  3 cm against
the selected parameters. Assessment of bubble size distribution
(BSD) in a gas–liquid system clearly demonstrates the extent to
which the bubbles undergo breakage or coalescence phenomenon
in the bubble column. It is worth noting that under the given oper-
ating conditions, all bubbles were found to be either spherical or
ellipsoidal. Therefore, it was quite reasonable to create their syn-
thetic images and use them to determine the bubble aspect ratio
E [-] (Eq. (3)) and bubble orientation [h] as shown in Fig. 2. Based
on the results of BSD obtained, it was concluded that that under
most of the conditions the bubble column was operated in pseudo-
uniform flow regime.
min
db
E¼ max ð3Þ
db

3.1.1. Measurement in pure IL and binsary mixtures
The BSD was estimated in terms of relative bubble number fre-
quency and compared for different liquid systems at the gas flow
rate (Qg) of 30 cm3/min, 300 K and column diameter (DC) of
2 cm, as shown in Fig. 3(a). It can be seen that a wider BSD was
obtained for pure IL, which was narrowed by adding MEA or
MeOH. At low concentration of MEA, BSD was slightly varied, how-
ever, addition of further MEA reasonably shifted BSD towards the
smaller bubbles. As compared to MEA, MeOH significantly nar-
rowed the BSD, and it existed within the range of sub-millimeter
bubbles offering low coalescence. Poly-dispersed distribution of
Fig. 3. Comparison of (a) BSD, (b) E [-] distribution and (c) bubble orientation
distribution in different liquid systems.
bubble size in pure IL, IL/MEA-1 and IL/MEA-2 indicates that flow
regime existed in pseudo-uniform regime, however, in IL/MeOH-1
and IL/MeOH-2 uniform flow regime was observed. Bubble aspect
ratio E distribution in pure IL and binary mixtures is presented in
Fig. 3(b) for gas flow rate Qg of 30 cm3/min, operating temperature
of 300 K. For our understanding, we consider the bubbles with E of
0.4–0.69 as highly deformed, E of 0.7–0.89 as moderately deformed

Fig. 2. Image processing for determination of bubble aspect ratio (E) and orientation (h).
6 M. Abro et al. / Chemical Engineering Science 229 (2021) 116041

and 0.9 to 1 as spherical. Fig. 3(b) suggests that in pure IL, the
extent of bubble deformation was highest and relative frequency
of highly deformed, moderately deformed and spherical bubbles
was 0.495, 0.45, and 0.055 respectively. In binary mixtures, the dis-
tribution was shifted to bubbles with high E such that a glaring
decrease in fraction of highly deformed bubbles (IL/MEA-1;
0.105, IL/MEA-2; 0.075, IL/MeOH-1; 0.107 and IL/MeOH-2; 0.125)
and increase in fraction of spherical bubbles (IL/MEA-1; 0.34, IL/
MEA-2; 0.2, IL/MeOH-1; 0.39 and IL/MeOH-2; 0.395) was obtained.
This effect can be explained as, compared with large bubbles, the
small bubbles undergo low shape deformation as BSD is already
explained in Fig. 3(a). Fig. 3(c) depicts the bubble orientation (h)
distribution in pure IL and binary mixtures at the same operating
conditions as mentioned above. The relative frequency of bubbles
with 0° was obtained in order; IL/MeOH-1 & IL/MeOH-2 > IL/ME
A-1 > IL/MEA-2 & Pure IL. This trend coincides with quantification
of spherical bubbles distribution presented in Fig. 3(b). Overall, the
bubbles with orientation angle below or above 0° (10° to 5° and
5° to 10°) was obtained order: IL/MeOH-1 & IL/MeOH-2 < IL/MEA-
1 < IL/MEA-2 & Pure IL. The obtained results demonstrate that vari-
ation in physical properties of liquid phase specially the viscosity
and surface tension exerted a conspicuous effect on BSD, E and h
distribution under the given operating condition.

3.1.2. Effect of gas flow rate

Fig. 4(a) shows the variation in BSD with respect to operating
gas flow rate in pure IL, which demonstrates that for any given flow
rate, the system was characterized with poly-dispersed BSD.
Therefore, the uniform flow regime (as defined earlier) can be clas-
sified as pseudo-uniform regime. In the range of low flow rate i.e.,
up to 50 cm3/min, BSD was negligibly varied. Beyond this, an obvi-
ous effect of gas flow rate was found, such that, BSD was shifted
towards large bubbles gradually as the gas flow rate was increased.
It indicated that under the high gas flow rate conditions, the phe-
nomenon of coalescence was improved due to increases in number
of gas bubbles and probability of inter-bubble collisions enhancing
coalescence. The results were consistent to general trends reported
in past literature. As depicted in Fig. 4 (b), for all gas flow rates,
bubbles with E of 0.6–0.69 and 0.7–0.79 had maximum relative
frequency. Generally speaking, with increasing gas flow rate, the
relative frequency of highly deformed was increased slightly up
to 50 cm3/min and then decreased reasonably. Increasing relative
frequency of moderately deformed bubbles was noticed with Fig. 4. Effect of gas flow rate on (a) BSD, (b) E [-] distribution and (c) bubble
increasing gas flow rate. With exception of 50 cm3/min, the relative orientation distribution.
frequency of spherical bubbles was approximately same for all gas
flow rate. These results can be qualitatively visualized in
Figs. 9 (a-e). Bubble orientation distribution at different gas flow
rates is compared in pure IL as shown in Fig. 4 (c). In range of small sparger pore size (Sp-A), the BSD existed relatively in narrow
30 cm3/min to 80 cm3/min, h distribution was almost same; bub- range with 0.95 fraction covered by submillimeter bubbles (deq-
bles with 0° had relative frequency of 0.47, bubbles with 10° to  0.9 mm) which controlled the overall bubble size. For Sp-B, the
5° and 5° to 10° had relative frequency from 0.24 to 0.28 and BSD was significantly shifted towards large bubbles. Considering
0.25 to 0.31 respectively. At higher gas flow rates (130 cm3/min the Sp-A, BSD was bimodal with first peak found at 0.2 mm and
and 250 cm3/min), slight decrease in the number of bubbles with other found at 0.5 mm. Similarly, sparger pore size significantly
0° was obtained, while, number of bubbles with 5° and 5° was influenced bubble E, such that, extent of bubble shape deformation
remarkably decreased. At 130 cm3/min, there was a significant was substantially decreased in case of Sp-A (Fig. 5(b)). E distribu-
increase in number of bubbles with 10° and 10° and minute tion was greatly shifted to moderately deformed and spherical
increase in bubbles having orientation angle of 20°. At bubbles in case of using Sp-A. The fraction of highly deformed bub-
250 cm3/min, bubbles with orientation 20° to 15° and 15° to bles (E = 0.4–0.69) produced by Sp-A was 0.21 which was far less
20° had relative frequency of 0.14 and 0.1 respectively. The results than that of Sp-B (0.495). This could be explained as, Sp-A was
indicate that bubbles at high gas flow rate have more tendency to characterized by producing more small bubbles which were rela-
rise in zig-zag manner. tively stable to resist deformation in their shape. Fig. 5(c) presents
the distribution of bubbles orientation for sparger pore size. There
3.1.3. Effect of sparger pore size was a considerable increase in fraction of bubbles with orientation
The BSD, E distribution, bubble orientation distribution against 0° for Sp-A due to increased number of spherical bubbles (Fig. 5(b))
the sparger pore size presented in Fig. 5(a-c), at Qg 30 cm3/min and as well as overall decrease in bubble size (Fig. 5(c)). Since, smaller
300 K reveal a significant effect of sparger size. As expected, for the bubbles are less likely to spin and follow a zig-zag rising path.
 M. Abro et al. / Chemical Engineering Science 229 (2021) 116041 7

Fig. 5. Effect of sparger pore size on (a) BSD, (b) E [-] distribution and (c) bubble orientation distribution.

3.1.4. Effect of temperature
Fig. 6(a) shows the histogram profiles of BSD in pure IL at dif-
ferent operating temperatures (300 K-333 K) in bubble column
equipped with sparger Sp-B. It illustrates that frequency of small
bubbles was directly linked to the temperature, such as at higher
temperature 333 K, a greater number of small bubbles were pro-
duced and bubble size was distributed in narrowest range. At low
temperature, relative frequency of large bubbles was increased
and range of BSD was widened. Such a trend of BSD is consistent
to previous findings of Zhang et al. (2012). Fig. 6(a) clearly sug-
gests that, at any given temperature, the bubble size was dis-
tributed in poly-dispersed manner, hence, it can be stated that
in all these conditions, system operated in pseudo-uniform
regime. As shown in Fig. 6(b), the fraction of moderately
deformed and spherical bubbles was increased with increase in
temperature which is credited to increased number of smaller
bubbles. Usually, the large bubbles are capable of stretching more
along their major axis causing shape deformation. Therefore,
greater number of highly deformed bubbles was appeared at
300 K. Distribution of bubble orientation is compared at different
8 M. Abro et al. / Chemical Engineering Science 229 (2021) 116041

Fig. 6. Effect of temperature on (a) BSD, (b) E [-] distribution and (c) bubble orientation distribution.

temperatures in Fig. 6 (c). It is clear from the results, that number
of bubbles having 0° was increased gradually with temperature,
as it was obtained as 0.47 at 300 K, 0.56 at 313 K and 0.61 at
333 K respectively. However, there was an increase in fraction
of bubbles with h = -10° and 10°, which could be due to frequent
spinning motion of slightly large and ellipsoidal bubbles by the
effect of decrease in liquid viscosity.
3.1.5. Effect of column H/DC ratio (A.R)
Figs. 7(a-c) present the profiles of BSD, E distribution and bub-
ble orientation distribution for different columns with dimeter DC
(2 and 2.5 cm) and static liquid (HS) of 10 cm. The results reveal
that DC had an insignificant effect resulting into a minute variation
in these parameters. This is explained as, column diameters were
very close to each other, also the same sparger (Sp-B) was used.
 M. Abro et al. / Chemical Engineering Science 229 (2021) 116041 9

Fig. 7. Effect of column’s H/DC ratio on (a) BSD, (b) E [-] distribution and (c) bubble orientation distribution.

3.2. Bubble size
3.2.1. Measurement of d32 in pure IL and binary mixtures
The sauter mean diameter d32 in pure IL was compared with
those of its binary mixtures together with highlighting the signifi-
cance of additive’s concentration in binary mixtures. The experi-
ments were performed at different flow rates and constant
temperature of 300 K, in bubble column (DC = 2 cm) consisting
of gas sparger Sp-B. As shown in Fig. 8, adding certain quantities
of MEA and MeOH to pure IL, noticeably varied d32 under a given
Qg and it was obtained in order of; pure IL > IL/MEA-1 > IL/MEA-
2 > IL/MeOH-1 > IL/MeOH-2. Compared with MEA, considerably
lower d32 was obtained in MeOH containing binary mixtures. The
results suggest that liquid properties had important role as it given
in Table 1, addition of either MEA or MeOH to pure [BMIM][BF4]
lowered the liquid viscosity. The decrease in viscosity as a result
of MeOH addition was relatively more sizeable. Whereas, the sur-
face tension of liquid was increased slightly by increasing MEA
concentration and decreased significantly by increasing MeOH
concentration. Therefore, it can be concluded that decrease in vis-
cosity as well as surface tension of a liquid decreases the bubble
size at a given flow rate of gas. This statement is supported by find-
10 M. Abro et al. / Chemical Engineering Science 229 (2021) 116041
Fig. 8. Effect of liquid properties on d32.
ings from the past literature (Chaumat et al., 2007; Zhang et al.,
2012). Difference between surface tension of pure IL and IL/MEA
binary mixtures is negligible, thus, variation in d32 is credited to
viscosity only. However, for mixtures IL/MeOH, both viscosity
and surface tension exhibited their governing effect to control
the bubble coalescence phenomena, ultimately diminished the
overall d32. Gemello et al. (2018) reported that presence of ethanol
in water results in modified mobility of bubble surface suppressing
the overall coalescence phenomena, this reason can be considered
for present results also. It is worth noting that effect of MeOH con-
centration was less than that of MEA in their respective binary
mixtures, indicating that addition a certain quantity of MeOH to
pure IL could achieve a stable flow uniform regime.
3.2.2. Effect of gas flow rate on local bubble size
The bubble size was locally measured in pure IL [BMIM][BF4] at
different Qg in the selected range at constant temperature of 300 K
using Sp-B. For each case, images represent the axial position
between 6 cm and 9 cm height above gas sparger, as shown in
Fig. 9. It can be observed that bubble size showed its strong depen-
dence on the Qg. The increasing Qg resulted in an increased ten-
dency of smaller bubbles to coalesce and form larger bubbles.
Therefore, the maximum bubble size in Fig. 9(a) was 1.75 mm,
while in Fig. 9(e), it was 2.8 mm. Gas flow rate was highly influen-
tial towards the number density of bubbles, thus, under high flow
rates, bubbles collision frequency was increased enhancing the
coalescence phenomenon. Regardless of different number density
and size bubbles at different Qg, bubbles were uniformly dispersed
over the cross-section of column, which is attributed to porous gas
sparger. Generally, the relation between bubble size and gas flow
rate is consistent with results of Zhang et al. (2012).
3.2.3. Effect of sparger pore size on d32
Configurations of gas sparger is one of the key parameters, with
a predominant role on hydrodynamics and bubbles characteristics
of bubble column. Spargers used in this work had different pore
sizes, values of d32 for both spargers are illustrated in Fig. 10 The
obtained results demonstrate that pore size of sparger had great
impact of bubble size. In case of Sp-A, d32 was noticeably smaller
under all operating conditions. For Sp-A, d32 was negligibly varied
in low range of flow rate, however, at high flow rates, visible
changes in d32 were found. Nevertheless, the gas was injected into
the column homogeneously through both spargers, the difference
in size of bubble could be attributed to the initial bubble size gen-
erated at sparger. Sp-A produced notably smaller bubbles which
were more stable and thus reluctant to adequate coalescence.
3.2.4. Effect of temperature on d32
Liquid properties such as viscosity and surface tension strongly
depend upon the temperature. Fig. 11 shows the d32 measured in
pure IL at 300 K, 313 K and 333 K for both spargers in bubble col-
umn (DC = 2 cm). For two spargers, bubble size was decreased with
increasing temperature, at ambient temperature (~300 K), the vis-
cosity of pure IL is usually high which favors the formation of large
bubbles at sparger. Large rising bubbles undergo frequent coales-
cence resulting into higher d32. As given in Table 1, the viscosity
and surface tension of pure IL were decreased as temperature
was increased. Decrease in surface tension was negligible, there-
fore, formation of smaller bubbles at high temperature could be
attributed to the viscosity only. The results suggest that combined
effect of sparger pore size and temperature was sufficient to
decrease d32 remarkably. The relationship between bubble size
and temperature is similar to that reported by Zhang et al. (2012)
3.2.5. Effect of column H/DC ratio (A.R) on d32
To investigate the effect of H/DC ratio of column on bubble size,
two columns with DC (2 cm and 2.5 cm) and HS of 10 cm were used.
Although, the selected values of DC were in a narrow range to high-
light its importance, the consideration was given based on the
overall small size of column. Experiments were performed using
pure IL at 300 K, whereas, Qg was varied in selected range. For
given gas flow rate, effect of DC on d32 was almost negligible
(Fig. 12). Invariance of d32 against DC could be due to, same sparger
pore size and selection of DC in narrow range. The results obtained
indicated that overall bubble size was profoundly controlled by its
initial value produced at sparger. A comprehensive study about the
effect of broad ranged value of column diameter on the bubble size
can be subject to the future research for present systems.
3.3. Comparison of experimental bubble aspect ratio E [-] with
correlations from past literature
Previously, several studies have been performed on the investi-
gation of shapes of bubbles/drops in quiescent liquid. There exists
a sufficient number of correlations to predict the E in terms of
dimensionless parameters. Well known correlations based on
 !

Eötvös number Eo ¼ g ðql 2qg Þdb were proposed by (Wellek et al.,
2
r
1966) (Eq. (4)), (Sugihara et al., 2007) (Eq. (5)), (Okawa et al.,
2003) (Eq. (6)) and (Besagni and Inzoli, 2016a) (Eq. (7))
1
E¼ ð4Þ
ð1 þ 0:163Eo0:757 Þ
1
E¼ ð5Þ
ð1 þ 6:5Eo1:925 Þ
1
E¼ ð6Þ
ð1 þ 1:97Eo1:3 Þ
1
E¼ ð7Þ
ð1 þ 0:553Eo0:266 Þ
Besagni and Deen (2020) stated that none of above-mentioned
correlations have predicative ability over complete range of Mor-
ton number (Mo), since the bubble shape depends upon all the
forces acting upon it, whereas, these correlations consider the
 M. Abro et al. / Chemical Engineering Science 229 (2021) 116041
Fig. 9. Bubble size at different Qg and 300 K (a) 30 cm3/min, (b) 50 cm3/min, (c) 80 cm3/min, (d) 130 cm3/min and (e) 250 cm3/min.
Fig. 10. Effect of sparger pore size on d32.
effect of surface and buoyant forces only. Besagni and Deen (2020)
proposed a correlation (Eq. (8)) that considers the viscous and iner-
tial forces in addition.
1 predict the theoretical E in a remarkable agreement with experi-
E¼
ð1 þ 0:45EoReÞ0:08
Myint et al. (2007) proposed a correlation (Eq. (9)) to predict the
shape of droplets based on the Tadaki number (Ta).
11
E ¼ 1  0:0487Ta  0:0289Ta2 ð9Þ
Moore (1965) proposed the E correlation based on the Weber
number (We) (Eq. (10)), which is ratio of dynamic pressure pro-
moting the deformation to the surface tension pressure resisting
the deformation. This correlation is suitable for the bubbles under-
going small deformation in their shape
1
E¼ ð10Þ
ð1 þ 0:141WeÞ
In this section, presently obtained experimental results of bub-
ble shapes are compared against the aforesaid correlations. Gener-
ally, the porous plate spargers are characterized with formation of
small bubbles. Moreover, the conditions of gas flow rate were
taken in low range, thus, their combined effect produced overall
small bubbles with low Eo. The experimentally measured bubble
aspect ratio compared with literature correlations existed within
range of 0.7 to 1 for Eo  1.6 and Mo of 8.82e-7 to 0.0044. Inter-
estingly, at a given Eo, EoRe, Ta and We, bubbles of different shapes
were found therefore, none of the correlations was proved to fit
with experimental measurements well (Fig. 13). However, all the
correlations gave reasonable prediction for the bubbles with small
deformation except of Eq. (5) and Eq. (6) which significantly under-
estimated the E at the moderate to high Eo in given range. There-
fore, it is strongly recommended to derive a correlation that can
ð8Þ mental measurements in future study. It can also be noted from
Fig. 13, with increasing Eo, EoRe, Ta and We, number of spherical
bubbles (E = 0.9 to 1) was decreased together with increasing num-
ber of deformed bubbles (E 0.7).
12 M. Abro et al. / Chemical Engineering Science 229 (2021) 116041
Fig. 11. Effect of temperature on d32.
Fig. 12. Effect of column’s H/DC ratio on d32.
Clift et al. (1978) proposed a graphical correlation known as
Grace diagram to investigate the bubble shapes as function of Eo,
Mo and Reynold number (Re). According to this correlation, at a
given Mo the bubble shape changes from spherical to ellipsoidal
and finally to cap bubbles with increasing Eo. This correlation also
helps to determine the Re and ultimately the bubble rise velocity.
However, Grace diagram may not compute the actual bubble rise
velocity as it was formulated for single bubbles instead of bubble
plumes (Besagni et al., 2018). In this work, bubble shapes were
investigated in liquids with different Mo (8.82e-7 to 0.0044), and
the sampled bubbles were characterized with spherical and ellip-
soidal shapes. The data regarding the shapes of bubbles in pure
IL (at 300 K (Log10 M = -2.35), 313 K (Log10 M = -3) and 333 K
(Log10 M = -4.228)), IL/MEA-1 (at 300 K (Log10 M = -2.74)), IL/
MEA-2 (at 300 K (Log10 M = -3)), IL/MeOH-1 (at 300 K (Log10
M = -4.76)) and IL/MEA-1 (at 300 K (Log10 M = -6.05)) is plotted
in Fig. 14. For present study, bubbles with E  0.9 were regarded
as spherical bubbles, whereas, the reamining bubbles were
regarded as ellipsoidal. Under the given conditions of Eo and Mo,
the all the bubbles were supposed to exist within spherical bubble
regime, however, certain number of bubbles with E < 0.9 was also
found. Overall, the experimental results reasonably agreed with
diagram prediction, apart from some deformed bubbles. There
existed a number of very small bubbles characterized with sub-
stantially low Eo which was beyond the range of diagram at given
Mo, therefore, those bubbles were not covered by Grace diagram
(indicated by dotted lines extended out of diagram). This could
be due to generation of very small bubbles with low Eo as a result
of combined effect of gas sparger and gas flow rate conditions for a
given Mo considered in this work.
3.4. Gas holdup and interfacial area
Gas holdup (eg Þ is key hydrodynamic factor which has impor-
tant effect on the overall performance bubble column (Besagni
et al., 2017a). It was measured through the method of volume
expansion, by recording volumes of both the static liquid and aer-
ated liquid (before and after gas injection respectively) photo-
graphically. Eq. (11) was employed to compute the gas holdup
VD  VS
eg ¼ ð11Þ
VD
where V S and V D are volumes of static liquid and aerated liquid
respectively. Presently, a uniform cross-sectional column was used,
therefore, Eq. (11) was simplified as given below.
HD  HS
eg ¼ ð12Þ
HD
where HS and HD stand for the height of static and aerated liquids
respectively.
Like gas holdup, gas–liquid interfacial area (aÞ is also a signifi-
cant parameter in absorption systems. Higher rates of mass trans-
fer can be achieved by increasing the gas–liquid interfacial area
(Mouza et al., 2005). It was predicted from the given gas holdup
and bubble size data using Eq. (13).
eg ð1  eg Þ
a¼6 ð13Þ
d32
Gas holdup and gas–liquid interfacial area are mainly influ-
enced by operating conditions, physical properties of liquid, spar-
ger configurations and dimensions of column, their role is
explained as,
 M. Abro et al. / Chemical Engineering Science 229 (2021) 116041 13

Fig. 13. Comparison between experimentally measured E [-] and correlations based on different dimensionless numbers for different Mo numbers.
14 M. Abro et al. / Chemical Engineering Science 229 (2021) 116041
Fig. 13 (continued)
3.4.1. Measurement of gas holdup and interfacial area in pure IL and
binary mixtures
The properties of a liquid are important in terms of bubbles size,
as well as their distribution and ultimately on the gas holdup
(Kantarci et al., 2005). Presently used pure IL and its binary mix-
tures differ significantly in terms of their physical properties
(Table 1). Therefore, results of overall gas holdup in pure IL were
compared with those in its binary mixtures in bubble column
(DC = 2.5 cm) under different gas flow rates and 300 K, as shown
Fig. 15(a). With the exception of IL/MEA-1 at Qg of 30 cm3/min,
the gas holdups were higher in all binary mixtures as compared
to pure IL. Compared with addition of MEA (which reduced the liq-
uid viscosity only), the effect of adding MeOH (significantly
reduced the liquid viscosity and surface tension) was more pro-
nounced, which increased the gas holdup by > twofold of that in
pure IL. These results were expectedly obtained based on the gen-
eral relation between liquid viscosity and gas holdup. The effect of
MeOH concentration on the gas holdup was relatively higher in the
range of low Qg, and it seemed to decrease at high Qg. As depicted
in Fig. 15(b), that addition of MEA and MeOH to pure IL enhanced
the gas–liquid interfacial area. The interfacial area was obtained in
similar trends as the gas holdup was obtained. Moreover, in all the
cases, the interfacial was increased with increasing Qg, except of
the case with IL/MeOH-2, by increasing gas flow rate from
50 cm3/min to 80 cm3/min, there was a negligible decrease in
interfacial area. It can be demonstrated as, both the gas holdup
and d32 increase with increasing gas flow rate. Hence, increase in
interfacial increases with increasing gas flow rate reveals a domi-
nant effect of gas flow rate on holdup and vice versa. Therefore,
for IL/MeOH-2 at 80 cm3/min, the gas flow rate showed slightly
prevailing impact on d32, a result the interfacial area was negligibly
declined.
3.4.2. Effect of sparger pore size on gas holdup and interfacial area
Variation in gas holdup with respect to sparger pore size is pre-
sented in the Fig. 16(a). Since the Sp-A is characterized of generat-
ing relatively smaller bubbles which comprise a dense phase. The
rising velocity of bubbles is directly proportional their size, the
small bubbles rise slowly compared with large bubbles. Therefore,
gas holdup for Sp-A was higher than that of Sp-B. Similar phenom-
ena was pointed out by Bhole et al. (2006) also. Fig. 16(a) also
shows that effect of sparger was more pronounced at gas flow
rate < 100 cm3/min. The gas holdup for Sp-A was almost double
to that with Sp-B at Qg of 30 cm3/min. Fig. 16(b) highlights the
importance of sparger pore size in terms of gas–liquid interfacial
area. Obviously, the Sp-A resulted in greater gas–liquid interfacial
area than Sp-B by exhibiting small bubble size and high gas holdup
comparatively.
3.4.3. Effect of temperature on gas holdup and interfacial area
Figs. 17 (a & b) present the gas holdup data for pure IL versus
gas flow rate at different operating temperatures for Sp-A and
Sp-B respectively. For the viscous liquids like ILs, the temperature
has a positive influence on gas holdup. Figs. 17 (a-b) suggest that
gas holdup underwent a noticeable increase when the temperature
was increased. At low temperature, more coalescence produced
large bubbles, with increasing temperature, low liquid viscosity
decreased promoted formation of small bubbles, as a result gas
 M. Abro et al. / Chemical Engineering Science 229 (2021) 116041 15

holdup was higher. Considering the Sp-A, at 333 K, gas holdup
reached almost a constant value at higher gas flow rates. However,
a combined effect of Sp-A sparger and temperature remarkably
varied gas holdup. It has been also observed that effect of
temperature exhibited the significant increase in interfacial area
(Figs. 17(c-d)). For Sp-B, a monotonic behavior of interfacial area
was found under all temperature conditions. On the other hand,
for Sp-A, at higher temperature the interfacial area was initially
increased with gas flow rate up to 80 cm3/min, above this, it was
decreased suggesting that gas flow rate influenced more pro-
foundly on the d32. Issaoui and Ben Mansour (2019) also observed
that increase in temperature results into the increased gas holdup
in oil/water emulsion with increasing temperature. Variation in
gas holdup and interfacial area at different temperature was also
reported in CO2–[BMIM][BF4] system by Zhang et al. (2012).
3.4.4. Effect of DC ratio on gas holdup and interfacial area
Fig. 18 compares the values of gas holdup and interfacial area
obtained experimentally in bubble columns with DC of 2 cm and
2.5 cm. For the measurement of gas holdup, instead of static liquid
height (HS ), the volume of static liquid (V S ) was considered as an
initial reading, since cross-sectional area of both columns was dif-
ferent. Hence, in both columns, equal volume of liquid was poured
and readings of gas holdup were recorded. It has been observed
that, in small DC column, the gas holdup was markedly higher than
that in large DC column over the entire range of gas flow rate. As
depicted in Fig. 18(b), the interfacial area in small DC column
was much higher than that in large DC column. It is discussed in
above section that DC had negligible effect on d32, therefore, varia-
tion in interfacial area by in different DC was majorly associated
with change in gas holdup.

Fig. 14. Experimental data of bubble shape plotted on Grace diagram at different Log M.
16 M. Abro et al. / Chemical Engineering Science 229 (2021) 116041
Fig. 14 (continued)
Under all conditions, the gas holdup in pure IL as well binary
mixtures was increased with increasing gas flow rate. This is cred-
ited to fact, that existing flow regime in bubble column is uniform
or pseudo-uniform because, the selected gas flow rate conditions
were in low range. Same phenomenon was discussed by Zhang
et al. (2012)
3.5. Correlations of sauter mean diameter (d32) and gas holdup (eg Þ,
and bubble column scaling-up approach
Prediction of d32 for multiphase systems in bubble columns is of
great importance, therefore, it would be useful to propose an
empirical correlation to predict d32. According to Pohorecki et al.
(2005b), d32 is mainly influenced by gas flow rate and liquid prop-
erties (density, viscosity and surface tension). Moreover, the size of
sparger and column dimensions have great significance in terms of
bubble size. Similarly, gas holdup is key parameter which charac-
terizes the transport properties of a reactor and plays a vital role
in design and scale-up of bubble columns. For ILs based multiphase
systems, a reliable correlation to predict the overall gas holdup is
not available particularly when a porous sparger is used in the
bubble column. However, it will make a good contribution in
designing the reactors employing ILs for practical applications of
gas separation processes. Gas holdup mainly depends upon the
gas flow rate, liquid properties, column dimensions and operating
conditions. Therefore, an empirical correlation proposed by Akita
and Yoshida (1973) was taken into account as basis which was fur-
ther presented with modification. According to this correlation, gas
 M. Abro et al. / Chemical Engineering Science 229 (2021) 116041 17

Fig. 15. Effect of liquid properties on (a) gas holdup and (b) interfacial area.

Fig. 16. Effect of sparger on (a) gas holdup and (b) interfacial area.

holdup in pure IL is directly proportional to gas flow rate and inver- 5) In both studies, different gas phases were used.
sely proportional to liquid density and viscosity. The correlations of
d32 and eg are given as Eq. (14) and Eq. (15) respectively. The key Predicted values of d32 and eg were obtained in well
advantages of proposed correlations are; agreement with those obtained from both experimental studies
(Figs. 19(a-b)).
1) These are proposed based on the present experimental mea-
!a  b  c !d  e
surements of d32 and eg as well the data was taken from past ql r3 q l H Ug do
literature of (Zhang et al., 2012) (Copy rights are received d32 ¼ do pffiffiffiffiffiffiffiffi
ffi ð14Þ
qg g ll 4 DC gDC DC
from Journal).
2) The correlations predict the said parameters for different
where g is acceleration due to gravity (m2/s).
bubble column dimensions, i.e., DC = 0.02 m to 0.025 m,
The constants of Eq. (14) and Eq. (15) (a, b, c, d, e,f) were calcu-
H = 0.1 m/ column aspect ratio = 5 (this study) to
lated through the least square method and their values are given in
DC = 0.052, H = 0.75 m/ Column aspect ratio 14.4 (Zhang
Table 2.
et al., 2012).
3) All the measurements (this work and (Zhang et al., 2012)) !a !b !c  d  e  f
used for correlations were taken at operating temperature gDC 2 ql gDC 3 Ug qg HS do
eg ¼ pffiffiffiffiffiffiffiffiffi ð15Þ
of 288 K to 333 K. r tl 2 gDC ql DC DC
4) In both studies entirely different gas spargers were used,
such as presntly used spargers were porous plate with very The proposed correlations predict d32 and gas holdup as func-
fine pore size, whereas, Zhang et al. (2012) used a sparger tions of dimensionless groups and their applicability over two dif-
consisting of four-orifices each having opening size of ferent reactor sizes indicate their significance to be desirably used
0.27 mm. for higher column dimensions and bubble column scaling-up.
18 M. Abro et al. / Chemical Engineering Science 229 (2021) 116041

Fig. 17. Effect of temperature on (a), (b) gas holdup and (c), (d) interfacial area.

Fig. 18. Effect of column’s H/DC ratio on (a) gas holdup and (b) interfacial area.
 M. Abro et al. / Chemical Engineering Science 229 (2021) 116041
Fig. 19. Comparison of experimental and predicted values (a) d32 and (b) gas holdup of present work and Zhang et al, (2012) (with copy rights from Journal).
Table 2
Correlation parameters.
a b
Eq. (14) 0.07271 0.04322
Eq. (15) 1.16708 0.31166
4. Conclusions
In this work, it was for the first time that distribution of bubble
size (BSD), bubble aspect ratio (E) and bubble orientation (h), mean
bubble size (d32), gas holdup (eg) and interfacial area in pure IL i.e.,
[BMIM][BF4] were compared with those in its binary mixtures with
monoethanol amine (MEA vol. % of 10 and 20) and methanol
(MeOH vol. % of 33.33 and 66.66). The experiments were per-
formed in a small-scale cylindrical bubble column consisting of a
porous sparger using high-speed image capture system. Further,
to develop the insight into the role of design and operating factors,
such as sparger pore size, column diameter (DC), temperature and
gas flow rate, experiments were performed employing the gas-
pure IL system. The bubble size was measured in the axial region
from 6 cm to 9 cm above the gas sparger. The results revealed that,
compared with pure IL, smaller bubble size was obtained in binary
mixtures. With increasing the concentration of MEA or MeOH, d32
was decreased, and both the gas holdup and interfacial area were
increased, also the BSD was narrowed with increase in fraction of
smaller bubbles. The effect of adding MeOH was relatively more
profound than that of MEA. In pure IL, a notable decrease in d32
and narrow range of BSD were obtained by decreasing the sparger
pore size, which increased the overall gas holdup and interfacial
area, the similar effect was exhibited by increasing temperature.
Distribution of E and h were also reasonably affected by these
parameters. Effect of DC was negligible on d32, BSD, E and h distri-
bution, however, in small diameter column, gas holdup and inter-
facial area were relatively higher. Under all conditions, the gas
holdup in pure IL as well binary mixtures was increased with
increasing gas flow rate. This is credited to fact, that existing flow
regime in bubble column is uniform or pseudo-uniform because,
the selected gas flow rate conditions were in low range. In most
of the cases (except of IL/MeOH-1 and IL/MeOH-2), BSD was
poly-dispersed, thus existing flow regime was defined as pseudo-
uniform flow regime. Present findings reveal that liquid properties
have significant effect on selected hydrodynamic parameters and
bubble characteristics. Our results were consistent with general-
19
c d e f
0.16528 0.27752 0.71397 –
0.31959 1.04812 1.49479 0.86208
ization; in low viscous liquids, a large number of smaller bubbles
are formed existing in a stable uniform flow regime which enhance
the overall gas holdup and interfacial area. Whereas, the highly vis-
cous liquid give rise to formation of large bubbles which decrease
the gas holdup and interfacial area. In this work, bubble column
was operated in pseudo-uniform regime at most of the conditions.
The additional contribution of the present study was to propose
empirical correlations to predict d32 and eg. The correlations were
obtained on the basis of experimental measurements for two dif-
ferernt bubble column sizes. Predicted values of d32 and eg were
in remarkable agreement with those measured experimentally.
Although, present work focused on use of small-scale bubble col-
umn, however, the results obtained would be useful to provide
key guidelines and general trends for the further study in more
realistic systems. Moreover, the proposed correlations predict d32
and eg as functions of dimensionless groups and their applicability
over two different column sizes indicate their significance to be
desirably used for different sizes of bubble columns and their
scale-up.
Future recommendations include,
In this study, [BMIM][BF4] was used as IL, however, future study
plan may include understanding of complicated multiphase flow
behavior in variety of other ILs (suitable candidates for CO2 absorp-
tion) and their mixed solvents. Also, the future study should be
dedicated to investigate the CO2 mass transfer performance in sev-
eral ILs and their mixed solvents.
It is also recommended to investigate the fluid dynamic behav-
ior and transport properties of gas-ILs/binary mixtures in large
scale bubble columns (meeting the well-known criteria of design
and scale-up), which is still an obstruction for their
industrialization.
CRediT authorship contribution statement
Masroor Abro: Experiments, Conceptualization, Writing - orig-
inal draft, Data compilation and processing. Liang Yu: Revising
20 M. Abro et al. / Chemical Engineering Science 229 (2021) 116041

original draft of manuscript. Guangren Yu: Idea, technical guid- Chen, W.-H., Chen, S.-M., Hung, C.-I., 2013. Carbon dioxide capture by single droplet
using Selexol, Rectisol and water as absorbents: a theoretical approach. Appl.
ance and revising manuscript. Xiaochun Chen: Review, edit, draft
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