Gas–liquid flow mass transfer in a T-shape microreactor stimulated with 1.7
MHz ultrasound waves

Mona Akbari, Masoud Rahimi, Mahboubeh Faryadi

PII: S1004-9541(16)30767-4
DOI: doi:10.1016/j.cjche.2017.03.010
Reference: CJCHE 773

To appear in:

Received date: 10 August 2016

Revised date: 3 March 2017
Accepted date: 4 March 2017

Please cite this article as: Mona Akbari, Masoud Rahimi, Mahboubeh Faryadi,
Gas–liquid flow mass transfer in a T-shape microreactor stimulated with 1.7 MHz ul-
trasound waves, (2017), doi:10.1016/j.cjche.2017.03.010

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 ACCEPTED MANUSCRIPT

Fluid Dynamics and Transport Phenomena

Gas-liquid flow mass transfer in a T-shape microreactor stimulated

with 1.7 MHz ultrasound waves

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Mona Akbari, Masoud Rahimi*, Mahboubeh Faryadi

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CFD research center, Chemical Engineering Department, Razi University, Kermanshah, Iran

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Corresponding author: Chemical Engineering Department, Razi University, Taghe Bostan,
Kermanshah, Iran,Tel:(+98)8314274530,Fax:(+98)8314274542,Email:m.rahimi@razi.ac.ir and
masoudrahimi@yahoo.com
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Gas-liquid flow mass transfer in a T-shape microreactor stimulated with 1.7

MHz ultrasound waves

Mona Akbari, Masoud Rahimi*, Mahboubeh Faryadi

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CFD research center, Chemical Engineering Department, Razi University, Kermanshah, Iran

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Abstract

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This paper describes the application of ultrasound waves on hydrodynamics and mass transfer
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characteristics in the gas-liquid flow in a T-shape microreactor with a diameter of 800 μm. A 1.7

MHz piezoelectric transducer (PZT) was employed to induce the vibration in this microreactor.
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Liquid side volumetric mass transfer coefficients were measured by physical and chemical
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methods of CO2absorption into water and NaOH solution. The approach of absorption of CO2

into a 1mol·L-1 NaOH solution was used for analysis of interfacial areas. With the help of a
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photography system, the fluid flow patterns inside the microreactor were analyzed. The effects of

superficial liquid velocity, initial concentration of NaOH, superficial CO2 gas velocity and length
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of microreactor on the mass transfer rate were investigated. The comparison between sonicated

and plain microreactors (microreactor with and without ultrasound) shows that the ultrasound

wave irradiation has a significant effect on kLa and interfacial area at various operational

conditions. For the microreactor length of 12 cm, ultrasound waves improved kLa and interfacial

area about 21% and 22%, respectively. From this study, it can be concluded that ultrasound wave

irradiation in microreactor has a great effect on the mass transfer rate. This study suggests a new

enhancement technique to establish high interfacial area and kLa in microreactors.

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Keywords: ultrasound waves; microreactor; gas-liquid flow; mass transfer; absorption

1. Introduction

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One of the most important operations in many industrial processes is gas-liquid contacting

processes such as gas absorption, which is especially used for environmental protection fields [1-

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9]. There are several conventional gas-liquid contactors used for these processes, including spray

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column, bubble column and packed tower. The main problems in these operations are limitations

on mass transfer, low efficiency and high operational costs. Therefore, finding a convenient

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method to enhance mass transfer and solving these problems is quite necessary [10-14]. In recent
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years, employing microreactors, as effective gas-liquid contactors, is the subject of many

research [1, 15-18]. Microreactors with micrometer dimensions and ultra-high surface to volume
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ratiocan increase heat and mass transfer significantly compared with conventional contactors and
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reactors [1, 15, 19-21]. In addition, gas–liquid phases mass transfer rates are greatly increased

due to very large gas–liquid interfacial areas up to 20000 m2·m-3 [22-24]. On the other hand, the
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miniaturization of chemical reactors has many other benefits including minimal environmental

hazards and increase safety due to the smaller volume besides reduction of process costs [25,
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26].

Some researchers focused on employing the microtechnology with greater potential performance

in many chemical processes such as gas-liquid reactions, liquid-liquid reactions and gas-liquid-

solid reactions [27-36]. However, for suitable designs of such microreactors, the key issues in

them related to the characteristics of hydrodynamic and reaction process. Up to now, several

research have been conducted for a better understanding of hydrodynamics, flow pattern regime,

heat and mass transfer rate for gas–liquid and liquid-liquid two-phase flows in microreactors. An

experimental investigation on characterization of gas-liquid-liquid in T-shape microreactors was

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undertaken by Rajesh et al. [37]. In particular, they studied the effects of distributors and

addition of surfactant to understand controlled generation of various flow regimes in

microchannels. In series of studies done by Yue et al.[38-40], gas–liquid flow and mass transfer

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characteristics in a rectangular microchannel for CO2absorption were investigated. Hessel et al.

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[41] studied the CO2 absorption into NaOH solution in microreactors and compared their

efficiency with a packed column. Their results showed that the micro-devices give a yield with a

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larger order of magnitude than the conventional packed beds.

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On the other hand, the application of ultrasound wave irradiation technique is a well-known

approach for improving a wide variety of processes. Ultrasonic wave propagation through a
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liquid causes cavitation bubbles, which produce shock wave and micro-jet during their collapse.

Moreover, ultrasound energy dissipation in the liquid leads to the formation of a rather intense
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macroscopic liquid flow called the acoustic streaming. Ultrasonic waves are divided into two

groups, high frequency and low frequency ultrasound. Waves with a frequency of 20 to 100 kHz
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are defined as low frequency ultrasound. These waves need high power to transmit through the
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environment. At low frequency ultrasound, strong acoustic energy can be generated to induce
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cavitation in liquids. This has considerable mechanical and chemical effects on various chemical

processes. Waves with frequencies in the range of 100 kHz-1MHz called high frequency

ultrasound. High frequency waves are used commonly in the medical industry and chemical

analysis. High frequency ultrasound has weaker mechanical and chemical effects compared with

low frequency one and consequently uses lower energy.

High frequency ultrasound, in the range of MHz, induces convective flows and micro-streams

(continuous flow of generated bubble induced by ultrasounic wave), simultaneously. Waves in

this range are capable to produce cavitation, which can improve micromixing. The implosive

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collapse of microbubbles, result in a variety of mechanical effects such as micro-streaming and

micro-jet that have ability to increase the mass transfer rate and causing turbulence-jet in a fluid.

Therefore, it is possible to reach a more efficient macro and micromixing by using ultrasound

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waves [42, 43].

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An interesting study was carried out by Chen et al.[44] on the effect of low frequency ultrasound

(20 kHz) on the mass transfer and fluid flow hydrodynamic. They found the overall mass-

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transfer coefficient was improved by 3–20 times under ultrasonication. Moreover, they

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demonstrated that ultrasound oscillation disturbs the bubble formation process and changes the

initial bubble length and pressure drop.

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Despite of interesting studies on low frequency ultrasound in the microchannel, high frequency

ultrasound do not investigate properly [44-47]. Both of low frequency and high frequency
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ultrasonic make bubbles in sonicated systems. Low frequency waves cause more strong bubble

implosions and thereby increase dominant physical effects and mixing performance. However,
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higher frequency waves create more smaller bubbles which leads to the generation of acoustic
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streams in the bulk of liquid with mixing effect [48]. In addition, these waves consume lower
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power in compared with low frequency ones.

In our previous work [49], micromixing efficiency of homogenous liquid flows were

investigated in different types of microchannels irradiated with high frequency ultrasound. The

results revealed that, the T-type microreactor in the presence of ultrasound wave irradiation

could establish higher micromixing efficiency in comparison with plain microreactor and

segregation index, improved up to 18%–36%. Based on this previous research, it can be said that

development of the combined microreactor with high frequency ultrasound waves of 1.7 MHz

can be effective for increasing micromixing and mass transfer rate between the liquid-liquid and

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gas-liquid interface. As already mentioned, many research on gas-liquid phases in plain

microreactors have been done. The effect of flow pattern and various geometries of

microchannel on the mass transfer rate of gas-liquid two phase flows were investigated.

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However, there are limited studies on application of ultrasound waves for improvement of mass

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transfer efficiency and its effect on created flow patterns in microreactors. Therefore, in the

present work, it has been tried to investigate the effect of high frequency ultrasound wave

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irradiation in the range of MHz on a micro-scale gas-liquid contactor. This work introduces a

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new technique for enhancing the mass transfer rate between gas-liquid phases in microreactors

by employing high frequency ultrasound. Hence, the microreactor was put in an ultrasonic
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container equipped with high frequency (1.7 MHz) piezoelectric transducer. Mass transfer

efficiency and mass transfer coefficient (kLa) of presenting microreactor in the presence and
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absence of ultrasound wave irradiation were evaluated using both chemical and physical CO2

absorption. In these experimental conditions, the influences of different parameters on two-phase

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flow pattern, pressure drop, mass transfer coefficient and interfacial area were investigated. In
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addition, a comparison study was carried out between the obtained results of both modes
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(sonicated and plain microreactor).

2. Apparatus and experimental procedures

Two T-shaped glass microreactors were used in the experiments. The external and internal

diameters of channels were 1mm, 800 μm, respectively. The main channel lengths were

considered60 and 120mm. Fig. 1 shows a schematic view of the experimental setup and the

snapshot of the container equipped with ultrasonic transducer. As shown in this figure, pure CO2

from a gas cylinder was driven into A channel via a pressure regulator and liquid solution was

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introduced to B channel from a liquid tank by a peristaltic pump (QisTM DSP100). A gas flow

controller was used to ensure a constant gas flow rate into the microreactor. The pressure drop

was measured using three pressure transducers (BD sensor, DMP 343, Germany) installed at the

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inlets and the end of the microreactor. The microreactor was immersed in a container, equipped

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with an ultrasound wave transducer, to evaluate the effect of ultrasound waves on the mixing and

mass transfer rate performance inside the microreactor. A high frequency piezoelectric

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transducer (1.7 MHz, model ANN-2517GRL, Annon piezo technology Co.Ltd, China) with a

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diameter of 1.5 cm was installed at the bottom of the container. In order to use the maximum

effect of ultrasound wave, the piezoelecteric transducer was placed under the contact point and
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mixing channel. In order to analyze gas-liquid flow pattern in the main channel and to evaluate

the effect of ultrasonic wave on it, gas-liquid flow regimes were recorded with the aid of an
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electronic microscope (640×480 pixels, magnification 10x-300x). The images were received by

computer and used for later analysis. After fluid contacting in the main channel, two-phase
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mixture flowed downward into a phase separator and unabsorbed CO2wasvented into the air.
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Water and NaOH solution was selected as the liquid solution to investigate the physical and
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chemical mass transfer coefficient. Warder Method, the standard technique of titration liquid

samples with HCl solution, was used to determine the amount of physically and chemically

absorbed CO2. Phenolphthalein and methyl orange were chosen as the indicators for the first and

second endpoints, respectively. At the first titration point, all the hydroxide and part of the

carbonate reacted:

OH   H 3O   2H 2O (1)

2
CO3  H 3O   HCO3  H 2O (2)

At the second titration point, the reaction was completed according to:

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HCO3  H 3O   CO2 ()  2H 2O (3)

Based on the two-titrant volumes, the carbonate concentration in the liquid sample collected in a

separator was calculated. All experiments were conducted at 25  2 C

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under atmospheric

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pressure.

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Fig. 1 Schematic diagram of the experimental setup and the snapshot of the container equipped
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with ultrasonic transducer: (1) CO2 cylinder, (2) Pressure Sensor, (3) Microreactor, (4)
Piezoelectric transducer, (5) gas flow meter, (6) Peristaltic pump, (7) phase separator, (8)
Electronic microscope, (9) PC computer.
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3. Result and discussion

Experiments were carried out in two approaches, with and without activation of the piezoelectric

transducer. The influence of both modes on the various operating conditions was studied.

3.1. Two-phase flow patterns

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In order to investigate two-phase flow pattern and the effect of ultrasound waves on it, water and

CO2 gas were selected. Moreover, in order to show clearer images of the flow pattern the water

colorized with pink color. A very little amount of pink ink was added to water to be sure that its

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effect on the water properties is negligible. By examination different gas and liquid flow rates,

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typical flow patterns, generally reported in the existing literature, such as bubbly flow, slug flow,

slug-annular flow, annular flow and churn flow were identified. Fig. 2 shows some

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representative images at five types of flow pattern captured at the middle section of the

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microreactor for both modes.
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Without US With US
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(a)Bubbly flow (UL= 1 m·s-1, UG= 0.11 m·s-1)

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(b)Slug flow (UL= 0.166 m·s-1, UG= 0.75 m·s-1)

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(c)Slug-annular flow (UL= 0.33 m·s-1, UG= 12 m·s-1)

(d)Churn flow (UL= 1 m·s-1, UG= 10 m·s-1)

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(e)Annular flow (UL= 0.166 m·s-1, UG= 15 m·s-1)

Fig. 2 Representative photographs of CO2-water flow pattern in the microchannel.

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Turning to Fig.2, distinct and small bubbles with diameters smaller than the channel size that

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dispersed in the continuous liquid phase characterize the bubbly flow (Fig. 2 (a)). In this flow

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pattern, due to surface tension force, the bubble almost seems spherical. By increasing the bubble

diameter, the effect of surface tension decreases and the bubbles lose their spherical shapes. Slug

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flow is determined by elongated Taylor bubble with axial larger than the channel diameter (Fig.
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2 (b)). As illustrated in this figure, the gas slugs were separated by the liquid segments in axial

direction. With increasing UG and decreasing UL, gas slugs became longer while shorter liquid
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slugs was established. With further increasing of gas flow, Taylor elongated bubbles eventually
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join and develop ring flow or slug-annular flow (Fig. 2(c)). This flow pattern is formed by long
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gas segments that are distinguished by small liquid waves that are made due to the interfacial
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instability waves arising from the viscous shear stress. In the higher liquid flow rate, churn flow

occurs, in which the bubbles are unstable at their trailing ends. Finally, in the higher UG, gas
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stream continuously flows in the center of channel and liquid flows as a thin layer on the wall

(Fig. 2 (d)), named annular flow pattern. On the other hand, the ultrasonic wave can cause

changes in the two-phase flow pattern that are also depicted in Fig. 2. Based on this figure, it can

be concluded there is a regular stream in the plain microreactor while the stream behavior is

more irregular in the sonicated layout. Presence of ultrasonic wave in the contact point makes

irregular contact of two phases and changes the shape, the bubbles size and length of liquid and

gas slugs. This can be explained by the fact that the performance of sonicated microreactor on

flow pattern can be due to stronger induced micro-streams and micro-jets by the collapse of

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microbubbles, generated by ultrasound wave propagation [50-52]. Thereby, sonication increases

the local turbulences inside the fluid. According to this figure, the effect of ultrasound wave is

more significant at lower superficial liquid and gas velocity such as bubbly and slug flow

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patterns. This might indicate that at a lower overall velocity, the ultrasound wave has a more

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significant effect on micromixing with increasing local turbulence intensity. However the effect

of ultrasound irradiation in the other flow patterns is lower than bubbly and slug flow. However,

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it still causes irregularities in the flow patterns.

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Fig. 3 reveals the developed flow pattern map for CO2-water flow. The flow transition lines

predicted by Triplett et al. [53] for a 1.097 mm diameter circular microchannel are used for
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comparison with the obtained experimental data in this work. As shown in this figure, the

production lines are generally in good agreement with the experimental observations overall flow
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transitions. In addition, the results indicate that depending on the amount of UL and UG, various

flow patterns are generated. At relatively low UL, the slug flow, which includes the most data in
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the map, dominates at the low-to-moderate UG. With increasing UG, slug bubbles are leading to
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be unstable slug and in the higher UG transition occurs from slug to slug-annular. In the higher
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UL bubble and churn flow is formed at low UG and moderate to high UL, respectively. Finally,

flow pattern forms annular flow at higher UG. Moreover, by comparison of two modes, with and

without activation piezoelectric transducer in microreactor, one can find that the ultrasound wave

has not a significant effect on changing of the flow pattern and transition lines. As far as high

frequency ultrasound has low power, it needs to enough residence time to influence on flow

regime. At higher flow rates residence time decreased. On the other hand, ultrasonic waves make

local turbulence and irregularities in the microchannel. At higher flow rate of liquid and gas

flow, turbulence increased in the microchannel and effect of ultrasound decreased compared with

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the effect of flow rate. This method is more effective to increase the local turbulence, internal

circulation and to change the size and shape of gas bubble and liquid slug.

On the other hand, with a comparison between high frequency waves in this paper and low

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frequency ultrasound waves achieved by Chen et al. [44], it can be concluded that the effect of

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low frequency ultrasonic is obvious by bubble oscillations. High frequency ultrasonic makes

very small bubbles that make oscillation in the gas–liquid interface, so it cannot be obvious in

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Fig. 2. On the other hand, piezoelectric transducer was placed below the inlet junction of

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microreactor, therefore the effect of high frequency ultrasonic was determined by the size of

slugs, bubbles and the distance between them.

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(a)Without ultrasound

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(b) With ultrasound

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Fig. 3 Comparison between the observed flow pattern data for CO2-water flow in the
microchannel with the transitional lines of Triplett et al. [29].

3.2. Pressure drop

Pressure drop, due to the direct relationship with energy consumption, is known as one of the

most important parameters in the study of the microreactors. In order to unsure pressure results,

pressure drop was measured three times for each UG and UL. It was shown that the uncertainty of

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pressure is more in higher flow rates. The maximum uncertainty of pressure drop yields a

measurement error of 5%.

Fig. 4 illustrates the measured two-phase pressure drop results as a function of UL and UG for

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CO2-water flow in the microreactor in the presence and without ultrasound wave irradiation for

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12 cm microreactor length. Turning to this figure, the maximum difference between

experimental data was selected for error bars. Therefore, difference equal to 5% is a maximum

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possible error and experimental data are reliable. However, a few data points of pressure drop in

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Fig. 4 differ significantly beyond the experimental error bars, also beyond the 5% level of

measurement error. It seems that some unknown factor causes the abnormal measurements. From
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this figure, one can be clearly seen that pressure drop increases linearly with increase in UG at the

same UL. The slopes of these lines obviously increased with increase of UL varying from 0.07 to
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1 m·s-1. Furthermore, change in UL has a greater impact on pressure drop than UG. The
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experimental results indicate that sonication has caused a very low difference in pressure drop
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across the microreactor.

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16000

14000

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12000

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10000
ΔP (Pa)

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8000

6000

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4000 MA
2000
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0
0 2 4 6 8 10 12 14 16
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UG (m/s)
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UL=0.07 m/s, without US UL=0.07 m/s, with US

UL=0.17 m/s, without US UL=0.17 m/s, with US
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UL=0.33 m/s, without US UL= 0.33 m/s, with US

UL= 0.5 m/s, without US UL= 0.5 m/s, with US
UL= 1 m/s, without US UL= 1 m/s, with US
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Fig. 4 Measured two-phase pressure drop data as a function of UL and UG for CO2-water flow in
12 cm microreactor length for both modes.

In order to define how much ultrasonic power was dissipated in the microreactor, the

calorimetric study was performed. Actual energy dissipated (Pdiss.) was calculated as follow [54,

55]:

Pdiss.  mC p dT dt
(4)

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Where, m and Cp denote mass and specific heat capacity of water. t denotes time and dT/dt time

is the rate of water temperature increase. The transducer consumes the electrical power around

9.5W. Based on our previous study[49], the amount of actual energy dissipated (Pdiss.) in the bulk

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of liquid (in the container) and in the microreactor were obtained 8.526 (W) and 4.45×10 -4 (W),

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respectively. Therefore, ultrasound waves seem to be less effective on pressure drop in a broad

domain of gas/liquid flow rates and flow pattern. However, ultrasound waves have a significant

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effect on the mass transfer efficiency that its more explanation will be presented in the

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consequent sections.
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3.3. Mass transfer characteristics

3.3.1. Physical absorption

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Experiments for physical absorption were carried out to examine the mass transfer of the pure

CO2 into deionized water in the studied microreactor. Since the main part of mass transfer
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resistance is related to the liquid phase, the mass transfer resistance in the gas phase was
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considered negligible. Therefore, liquid side volumetric mass transfer coefficient kLa was
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obtained based on the following mass balance:

 QL dCCO2  k L a(C *  C )dV (5)

And thereby, kLa could be derived as follows:

QL C *  Cin
kLa  ln( * ) (6)
V C  Cout

Where Cin and Cout are molar concentrations of dissolved CO2 in the inlet and outlet of the

microreactor, respectively. Moreover, V is the volume of the main channel and QL is the liquid

flow rate. In some studies, the output was connected to a separator by a tube. So, another

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microchannel without the length of out channel was used and results were referred to second

microchannel. In this study, the second microchannel was not needed and output directly entered

to the separator. As the rate of CO2 absorption is quite high, the equilibrium at the interface can

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be described by Henry’s law [56]:

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*
CCO2 ,int erface
 HPCO2 (7)

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Where H and PCO2 are the equilibrium solubility of CO2 in the liquid phase and the partial

pressure of CO2 in the gas phase, respectively. The gas solubility into an electrolyte solution is

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influenced by various parameters as follows:

H
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log( )   (hi  hG )Ci (8)
H water i

Where Ci is ion concentration and hi is a parameter related to each ion in the solution. Moreover,
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hG denotes the absorbed gas in the liquid phase. The values of hi and hG were presented by
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Schumpe [57].
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Since the two-phase mixture in the main channel directly entered to the separator, the end effect
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was considered negligible. Fig. 5 describes the measured kLa in the microreactor as a function of
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UL and UG with and without ultrasound wave irradiation. The observed flow patterns in the

considered range are slug and slug-annular flow patterns. The presented results for two different

lengths of microreactor in Fig. 5(a) and 5(b) indicate that kLa value increases significantly with

increasing in UL and UG. However, both superficial liquid and gas velocity increase the value of

kLa, but the effect of these parameters on the absorbed concentration of CO2 is different. By

increasing the value of UL at a fixed UG, the residence time and contact time between two phases

decrease. Increase in kLa is mainly attributed to the fact that the increase of UL can increase the

local turbulence and subsequently cause thinner thickness of the liquid boundary layer, which

results in reduction of mass transfer resistance between gas-liquid phases. This can cause an
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increase in the liquid side mass transfer coefficient. On the other hand, it can also see that with

increase in UG at a fixed value of UL, kLa was increased. This can be due to enhancement of gas

holdup and turbulence of the microreactor, which increases contact between two phases and

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thereby, the rate of mass transfer. From the obtained results, it seems that UG changes have a

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significant effect on kLa value compared with changes in UL. For example, with increase in the

UG from 0.17 to 0.33 m·s-1 in the fixed value of 0.17 m·s-1 for UL, kLa increases about three

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times. On the other hand, with change in UL from 0.17 to 0.33 m·s-1 in UG of 0.17 m·s-1 caused

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an increase of almost 1.5 times in liquid side mass transfer coefficient.

As depicted in Fig. 5, with increase in the length of microreactor from 6 to 12 cm at a fixed UG

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and UL, the kLa decreased. However, with an increase in microreactor length, contact time of two

phase increases, while the value of kLa has decreased. By taking more distance from the
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confluence zone, the concentration of CO2 solved in the liquid phase increases. So the decline of

difference between C and C* decreases mass transfer rate and kLa and consequently average kLa.
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According to the results it can be concluded that ultrasound wave propagation in the
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microreactor has a significant effect on the kLa values. The obtained kLa in the layout with this
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approach for microreactor with UL=0.17 m·s-1 was increased up to 34% and 28% for length of 6

and 12 cm, respectively. The collapse of microbubbles, generated by the high frequency wave

propagation, leads to induce strong micro streams and more local turbulence in the microreactor.

In addition, ultrasound wave assists to better internal circulation within slugs[50]. In addition,

ultrasound wave may disrupt the interface and guide jets of one phase into the other.

These phenomena can effectively increase the solution mixing and more contact of between

CO2gas and water. These can increase the mass transfer coefficient and improvement of

absorption of CO2 in water.

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8

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kLa (1/s)

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4 MA UL=0.17 m/s, without US

UL=0.17 m/s, with US

2 UL=0.33 m/s, without US

UL=0.33 m/s, with US

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0
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0 0.5 1 1.5 2 2.5 3 3.5

UG (m/s)
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(a) L= 6 cm
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8

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6

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kLa (1/s)

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4

UL=0.17 m/s, without US

3 MA UL=0.17 m/s, with US
2
UL=0.33 m/s, without US
1
UL=0.33 m/s, with US
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0
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0 0.5 1 1.5 2 2.5 3 3.5

UG (m/s)
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(b) L= 12 cm
Fig. 5 Effect of superficial gas and liquid velocities on liquid side volumetric mass transfer
coefficient in the microreactor.
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3.3.2. Chemical absorption

3.3.2.1. Mass transfer coefficient determination

In this paper, NaOH solution was chosen to study the mass transfer coefficient by chemical

absorption. Therefore, in order to find the k*La, mass transfer parameters should be examined in

the microreactors. The global reaction happens in the microreactor is[58]:

CO2  CO32  H 2O  2HCO3 (9)

Based on the achieved results by Robert and Danckwerts [59], the apparent first-order rate

constant for this reaction,k1,app, is 0.86 s-1. According to absorption values presented in Fig. 5, it
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can be expected the following inequality should be fulfilled for CO2 absorption into buffer

solution and physical absorption under the same ranges of UL and UG:

k L a(1   )k1,app (10)

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It indicates that the present microchannel reaction rate is much smaller than mass transfer rate of

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CO2 into solution, so absorption process in buffer solution can be assumed as physical one.

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Therefore, k*La can be derived as kLa.

Fig. 6demonstrates the chemical volumetric mass transfer coefficient in liquid phase as a

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function of UG and UL at a constant initial concentration of NaOH solution. The results are

presented for both modes, sonicated and plain microreactor, in different lengths of microreactor.
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Changes in chemical k*La at various UL, UG and ultrasound wave irradiation are similar to
D

physical kLa changes that mentioned above. In addition, the results for this method indicated that
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sonication through the microreactor has a significant impact on the k*La in comparison with the

plain microreactor at various examined operational conditions. The collapse of cavitation

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microbubbles at the interface of two phases makes more irregularity as well as more efficient

mixing, which causes higher mass transfer rate. Therefore, ultrasound can promote chemical
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reaction by its mechanical effect. The measured k*La with this approach for the microreactor

length of 6 and12 cm in UL value of 0.17 m·s-1 was increased up to 31% and 24%, respectively.

However, with a comparison between kLa and k*La values, shown in Fig.s5 and 6, it can

obviously see that the obtained mass transfer coefficient by chemical absorption has lower value

than that of physical one. This can be due to the fact that the diffusivity of CO2 in water is more

than electrolyte solutions, such as NaOH solution[60].

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10

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8

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6

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k*La (1/s)

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4
UL=0.17 m/s, with US

UL=0.17 m/s, without US

MA
2
UL=0.33 m/s, without US

UL=0.33 m/s, with US

D

0
TE

0 0.5 1 1.5 2 2.5 3 3.5

UG (m/s)
P

(a) L= 6 cm
CE
AC

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5

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4
k*La (1/s)

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3

NU
UL=0.17 m/s, without US
2
MA UL=0.17 m/s,with US

UL=0.33 m/s, without US

1
UL=0.33 m/s, with US
D

0
0 0.5 1 1.5 2 2.5 3 3.5
TE

UG (m/s)

(b) L= 12 cm
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Fig. 6 Effect of superficial gas and liquid velocities on liquid side volumetric mass transfer
(CNaOH= 0.5 mol·L-1).
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In Fig. 7 the values of the k*La at various UG for two initial NaOH concentrations are shown. The

influence of NaOH concentration on k*La is illustrated in this figure. As depicted in this figure,

for both modes, increase in concentration of NaOH caused a decrease in k*La value. This can be

because of lower diffusion coefficient in electrolyte solution with higher concentration[60].The

amount of absorbed CO2 increased with increase in solution concentration, but it decreased in

comparison with the initial solution concentration. Therefore, according to the Eq. (5), the ratio

of concentration differences is reduced during the microreactor and lead to a reduction in k*La.

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Moreover, increase in superficial gas velocity caused an increase in gas holdup and flow

turbulence intensity. In addition, the gas–liquid mass-transfer resistance decreases with

increasing of UG value, resulting in increase of CO2 mass transfer and CO2 concentration in the

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liquid phase. On the other hand, the k*La value of sonicated microreactor is greater than that of

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the plain microreactor at various conditions. The enhancement of mixing and local turbulence by

ultrasound waves increases the CO2 solubility and decrease the gas-liquid mass transfer

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resistance. Therefore, higher k*La was achieved in the sonicated microreactor.

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5 MA
0.5 M NaOH, without US
4.5
0.5 M NaOH, with US
4 1 M NaOH, without US
D

1 M NaOH, with US
3.5
TE

3
k*La (1/s)

2.5
CE

2
AC

1.5

0.5

0
0.17 0.33 1 3.32
UG (m/s)

Fig. 7.The values of the k*La at various superficial gas velocities for two initial NaOH
concentrations.

For better express the effect of ultrasound wave on improving mass transfer coefficient in the

microreactor, the relative mass transfer coefficient enhancement (E) is defined as follows:

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(k:L aus  kL a plain)

E  100 (11)
kL a plain

Where (k L a)US is the value of mass transfer coefficient in the sonicated microreactor and

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(k L a) plain is that of the plain one. This dimensionless parameter has been used in order to clarify

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the contribution of the ultrasound effect on kLa at various operating conditions. Chemical method

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was considered for measuring of k*La value. Fig. 8illustrates the values of E for various UL and

UG at a fixed length of microreactor. The results indicate that with an increase in UL in various

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UG, the relative mass transfer coefficient enhancement decreases almost significantly. As shown
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in this figure, with reduction in UL, the effect of ultrasound irradiation on obtaining value of E is

increased and the ultrasound wave at lower UL has a more significant effect on obtaining k*La by
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chemical method. The reason can be explained by the fact that at higher velocity, the role of
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macromixing and convective flow circulation is more significant than extra mixing and local

turbulence induced by ultrasound waves. In addition, the weakening effect of ultrasound under
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higher flow rates can also be attributed to the shorter irradiation time.
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40

35 UL= 0.17 m/s

UL= 0.33 m/s

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30

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25

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E (%)

20

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15
MA
10
D

5
TE

0
0.17 0.33 1 3.32
P

UG (m/s)
CE

Fig. 8.Effect of superficial gas and liquid velocities on the relative mass transfer coefficient
enhancement (L= 12cm, CNaOH= 0.5mol·L-1)
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The effect of ultrasound wave on value of E in various lengths of microreactor and UG was also

investigated. The obtained results for different UG and microreactor length in a constant UL are

listed in Table 1.The tabulated values show that with increasing in the microreactor length, the

contact time increases while the driving force (concentration difference) decrease along the

microreactor length. It is evident that with increasing in the microreactor length, the relative

mass transfer coefficient enhancement decreased. This may be explained by a fact that with an

increase in UG at a fixed microreactor length, the local turbulence and concentration of CO2 in

the two-phase interface enhanced, while the effect of ultrasound waves reduces. This leads to the

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reduction of the E value. In addition, the ultrasound wave effect is more significant at lower

velocities. This might indicate that at lower velocities the ultrasound waves, which caused extra

local turbulence during the microreactor, have a more significant effect on increasing of mass

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transfer coefficient. Consequently, the E value increases at lower velocity and shorter

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microreactor length.

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Table 1.Effect of superficial gas velocities and length of main channel on E.

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-1 -1 E/%
UL /m·s UG /m·s
L= 12 cm L= 6 cm
0.17 24. 5 35.79
MA
0.33 18.18 27.75
0.17
1 13.24 16.87
3.32 6.76 9.36
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3.3.2.2. Interfacial area determination

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There are two methods to measure the interfacial area in a microreactor:

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1. Danckwerts method

2. Calculation directly from the recorded image.

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In the sonicated microreactor, ultrasound wave makes fluctuations in the shape and the size of

slugs and increases the internal circulation in the slugs. Hence, the interfacial area cannot be

calculated precisely from recorded image and Danckwerts method is more suitable.

The chemical method developed by Danckwerts [58] was used to measure the two-phase

interfacial area in the microreactor. This method is based on the absorption of CO2 into a 1mol·s-
1
NaOH solution. The reaction considered between CO2 and NaOH solution can be expressed as

follow:

CO2  OH   HCO3 , (12)

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HCO3  OH   CO32  H 2O. (13)

The rate of reaction (13) is significantly higher than that of reaction (12) because of ionic

transfer. Therefore, the reaction (12) that of second order is rate controlling. A general

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correlation of this reaction, k OH  , was given by Pohorecki and Moniuk [61]:

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R  kOH  COH  CCO2 (14)

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2382
log10 (kOH  )  11.916   (0.221 I )  (0.016  I 2 ) (15)
T

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I  0.5 Ci zi
2
(16)
i MA
Reaction (13) can be considered as a fast pseudo-first-order reaction under the following

conditions:
D

DCO2 k OH  COH 
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Ha Number  2
 3 (17)
k * L ,CO2
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DCO2 kOH  COH  DCO2 COH  DOH 

 
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*2 * (18)
k L DOH  2C DCO2
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In these conditions, the gas side mass transfer resistance is negligible and the concentration of

OH- is the same in the liquid side.

Sharma and Danckwerts [62] proposed a specific rate of absorption per unit area for a second-

order reaction satisfying the above conditions as:

2
R  C * DCO2 kOH  COH   k *L (19)

Since the value of k*L2 is very small compared the first term, so this term has been removed from

the Eq. 20:

R  C * DCO2 kOH  COH  (20)

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Hence, the interfacial area can be obtained from the following equation [38, 63]:

QL ( COH  ,inlet  COH  ,outlet )

a (21)
C *Vmc DCO2 kOH 

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The diffusivities of CO2 and of NaOH in the liquid phase are calculated using Eqs. (22) and (23)

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as follows [56]:

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DCO2( L )  1.97  10 9 (1  0.129COH   0.261CCO2 ) (22)
3

DNaOH ( L )  1.7 D1.35 (23)

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Inequalities (17) and (18) in various operational conditions are listed in Table 2. As shown in this
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table, both of inequalities are true for all conditions, so consideration of fast pseudo-first-order

reaction for reaction (8) is correct.

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Table 2.Calculated inequalities (17) and (18) in different conditions.

DCO2 kOH  COH  DCO2 COH  DOH 
CNaoh UL UG Ha number  
P

*2 DOH  2C * DCO2
k L
-
0.5 mol·L
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1 0.17 0.17 35.85 35.85<<1156.546 Satisfied

0.17 0.33 29.02 29.02<<490.5403 Satisfied
0.17 1 18.57 18.57<<290.6719 Satisfied
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0.17 3.31 10.27 10.27<<193.6023 Satisfied

1 mol·L-1 0.17 0.17 54.8 54.8<<2793.9 Satisfied
0.17 0.33 44.37 44.37<<1185.45 Satisfied
0.17 1 28.40 28.40<<702.7531 Satisfied
0.17 3.31 15.72 15.72<<468.3231 Satisfied

Fig. 9 reveals the obtained interfacial area in layouts with and without ultrasound wave

irradiation at different value of UG. Since literatures indicated that the value of UL has not

significant effect [23, 34 and 47], UL=0.07 m·s-1 was selected for evaluation of interfacial area

values. As illustrated in this figure, with increasing UG value, the interfacial area in both modes

increases. In addition, the results demonstrate that the ultrasound wave increases the gas-liquid
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interfacial area about 30% at various UG. Moreover, the effect of sonication is more significant at

lower UG, which can be due to irregularities made by ultrasonic on the flow pattern.

6000

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5000

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SC
4000
a (m2/m3)

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3000

MA
2000

without US
1000
D

with US
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0
0 0.5 1 1.5 2 2.5 3 3.5
P

UG (m/s)
Fig. 9 Effect of superficial gas and liquid velocities on interfacial area in the microreactor for
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both modes. (L= 12 Cm, CNaOH= 1mol·L-1).

In order to ensure about calculated interfacial data, in Table 3the data in this work are compared
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with two other studies. As shown in this table, interfacial area in three systems is in the same

range and difference between them is due to channel diameter, length of main channel, the shape

of cross-section, superficial gas/liquid velocity and other operational parameters.

Table 3.The comparison between the interfacial areas in different microreactors.

Microreactor diameter Interfacial area (m2·m-3)

Yue et al. [38] 0.667 mm 3000-9000
Su et al. [29] 1 mm 4000-10000
This work 0.8 mm 2000-6000

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To further investigate of interfacial area, the ratio of the measured interfacial area to the

geometrical wall surface (RA) was calculated. Table 4 demonstrates this parameter at UL=0.07

m·s-1. As depicted in this table, RAwithUS becomes more than 1 at the maximum velocity of the

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gas. However, the layout without ultrasound irradiation could not reach to this value in the whole

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range of examined gas velocities.

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Table 4.Calculated RA at various gas velocities.
UG RAWithout US RAWith US
5 0.395221
MA 0.623371
10 0.470626 0.670251
30 0.714074 0.817522
100 0.961692 1.049512
D
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4. Conclusions

In this study, a novel method presented based on application of ultrasound wave for improving
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the mass transfer rate in a glass microreactor with a diameter of 800μm. For this purpose,

absorption of CO2in water and NaOH solution (0.5 and 1 mol·L-1) was investigated. Experiments
AC

for both modes were carried out, without and with activation of 1.7 MHz ultrasound piezoelectric

transducer. In the experiments, the superficial velocities were chosen in the range of 0.17-15 m·s-

1
for gas flow and 0.07- 1 m·s-1 for liquid flow. Water and CO2were entered to the microreactor

and various two-phase flow patterns were observed using an electronic microscope.

Experimental data showed a good agreement with the transition lines suggested by Triplett et al.

[42]. By investigating the effect of sonication, it was found that ultrasound wave did not change

the flow patterns, but it disturbs the bubble formation process, changes the liquid slug lengths

and size of bubbles in bubble and slug flow regimes. However, it has not any significant effect

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on other flow regimes. Pressure drops were measured in both cases, with and without ultrasound

wave. Results revealed that the pressure drop increased linearly with an increase in the amount of

UG at the same UL and its changes are more dependent on UL than UG. In addition, it was found

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that sonication changes the pressure drop slightly, almost less than 10%, which can be neglected.

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In addition, the effect of ultrasound wave on gas–liquid flow and mass transfer characteristics

was evaluated. For investigation of the effect of ultrasound wave irradiation on mass transfer

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rate, liquid side volumetric mass transfer coefficients for physical and chemical absorption

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process were calculated. The results revealed that with increasing UG and UL, kLa increased

significantly.
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Besides, with enhancing in the microreactor length, driving force of mass transfer decreased and

thereby kLa declined. The mass transfer coefficient for microreactor with the length of 6 cm is
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more about 30% compared with other microreactor. On the other hand, the value of kLa in

physical absorption was higher than that of chemical absorption. Based on these results, for
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microreactor with the length of 12 cm, mass transfer coefficients in physical absorption are
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higher about 10% and 100% compared with mass transfer coefficients in chemical ones in NaOH
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concentrations equal to 0.5 mol·L-1 and 1 mol·L-1, respectively. This was explained by lower

diffusion coefficient in the electrolyte solution compared with pure water. The results indicated

that for both modes increase in concentration of NaOH cause a decrease in k*La value.

In another part of this study, gas-liquid interfacial area was measured by the Danckwerts pseudo-

first order reaction method for both layouts, the sonicated and plain microreactor. The results

showed that the interfacial area in both modes increased with an increase in the UG value. In

addition, the results revealed that the ultrasound wave could increase the interfacial area up to

30%. For better understanding of the ultrasound irradiation effect on mass transfer, a dimension-

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less parameter, relative mass transfer coefficient enhancement (E), was presented. It has been

illustrated that the sonication enhances the mass transfer coefficient up to 34%. The results

showed that the high frequency ultrasound can generate acoustic streams, which have ability to

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increase mixing and local turbulence inside the microreactor.

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Nomenclature

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a Interfacial area, m2/m3
MA
C Concentration, mol/m3
C* Physical solubility of CO2 in the liquid, mol/m3
Cin Concentrations of dissolved CO2 in the inlet liquid phase, mol/m3
D

Cout Concentrations of dissolved CO2 in the outlet liquid phase, mol/m3

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Cp Specific heat capacity, J/(Kg.°C)

DCO2 Diffusivity of CO2 in the liquid, m2/s
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E Relative mass transfer coefficient enhancement, dimensionless

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H Equilibrium solubility of CO2 in the liquid phase, Pa/(mol/m3)

hG Absorbed gas in the liquid phase
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hi Parameter related to each ion in the solution

Ha Hatta number, dimensionless
I Ionic strength, mol/m3
kLa Liquid side volumetric mass transfer coefficient, s−1
k*La Liquid side volumetric mass transfer coefficient obtaining by
chemical absorption, s−1
kOH- Rate constant for reaction between carbon dioxide and hydroxyl
ion, m3/(mol s)
L Main microchannel length, m
m Mass, Kg
ΔP Two phase pressure drop, Pa

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PCO2 Partial pressure of CO2 in the gas phase, Pa

Pdiss. Energy dissipated, W
QL Liquid phase volumetric flow rate, m3/s
R Reaction rate, mol/(m3.s)

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T Temperature, K
t time

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UG Superficial velocity of gas, m/s

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UL Superficial velocity of liquid, m/s
V Volume, m3

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z Valence of ion I, dimensionless

Subscripts
MA
in microchannel inlet
out microchannel outlet
D

mc main channel
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G gas
L liquid
P
CE
AC

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Table captions:

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Table 1.Effect of superficial gas velocities and length of main channel on E.

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Table 2.Calculated inequalities (17) and (18) in different conditions.

Table 3.The comparison between the interfacial areas in different microreactors.

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Table 4.Calculated RA at various gas velocities.
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Figure captions:
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Fig. 1 Schematic diagram of the experimental setup and the snapshot of the container equipped
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with ultrasonic transducer: (1) CO2 cylinder, (2) Pressure Sensor, (3) Microreactor, (4)
Piezoelectric transducer, (5) gas flow meter, (6) Peristaltic pump, (7) phase separator, (8)
Electronic microscope, (9) PC computer.
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Fig. 2. Representative photographs of CO2-water flow pattern in the microchannel.

Fig. 3.Comparison between the observed flow pattern data for CO2-water flow in the
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microchannel with the transitional lines of Triplett et al. [29].

Fig. 4.Measured two-phase pressure drop data as a function of UL and UG for CO2-water flow in
12 cm microreactor length for both modes.

Fig. 5 Effect of superficial gas and liquid velocities on liquid side volumetric mass transfer
coefficient in the microreactor

Fig. 6 Effect of superficial gas and liquid velocities on liquid side volumetric mass transfer
(CNaOH= 0.5 M).
Fig. 7.The values of the k*La at various superficial gas velocity for two initial NaOH
concentrations.

Fig. 8.Effect of superficial gas and liquid velocities on the relative mass transfer coefficient
enhancement. (L= 12cm, CNaOH= 0.5 M)

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Fig. 9.Effect of superficial gas and liquid velocities on interfacial area in microreactor measured
by chemical absorption method for both modes.(L= 12 Cm, CNaOH= 1M)

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Without US With US

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(a) Bubbly flow (UL= 1 m/s, UG= 0.11 m/s)

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(b) Slug flow (UL= 0.166 m/s, UG= 0.75 m/s)

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(c) Slug-annular flow (UL= 0.33 m/s, UG= 12 m/s)
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(d) Churn flow (UL= 1 m/s, UG= 10 m/s)

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(e) Annular flow (UL= 0.166 m/s, UG= 15 m/s)

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CO2-water flow pattern in the studied microchannel

Graphical abstract

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