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Article history: The gas-liquid two-phase flow and mass transfer with fast chemical reaction in a microchannel were investigated
Received 9 June 2017 experimentally. Result showed that the bubble volume decreased exponentially with its movement along the channel in a
Accepted 12 June 2017 quickly reactable absorbent. The volumetric mass transfer coefficient k La increased with gas flow rate, while it was insensitive
to liquid flow rate under experimental condi-tions, although the mass transfer coefficient k L increased with liquid flow rate. In
slug-bubbly flow regime, the kL decreased when increasing gas flow rate, but inverse tendency was found for slug flow pat-
Keywords:
Microchannel tern. Both kL and kLa increased with the increase of absorbent concentration. A new correlation for pre-dicting the volumetric
Mass transfer mass transfer coefficients kLa was proposed by taking the enhancement factor E of chemical reaction into account.
Gas-liquid two-phase flow
Chemical absorption
2017 Elsevier Ltd. All rights reserved.
1. Introduction Yue et al. [3] investigated the absorption of oxygen in the deion-ized
water, but the experimental volumetric mass transfer coeffi-cients were less
In recent years, microfluidic technology has been widely applied in many evidently than the prediction values of Bercic and Pintar [1] and van Baten et
industrial fields such as chemical, material, biol-chemical, pharmaceutical and al. [2]. Yue et al. [3] argued that the mass transfer between the liquid film and
food engineering, etc., due to its excellent mass and heat transfer liquid slug was mostly stemmed from the diffusion without the convective
performances. The systematical investigation on the mass transfer mechanism mixing, thereby the mixture between the liquid film and liquid slug was
inside microchannel is of critical importance for the design and optimization incomplete due to the short diffusive time for the short liquid slug. Moreover,
of the microreactor. the dissolution rate of CO2 bubble into water also was experimentally
investigated [4,5].
Bercic et al. [1] investigated the absorption of methane into water in
capillaries under Taylar flow regime. They found that the volumetric mass The analysis on the mechanism of mass transfer between gas and liquid
transfer coefficient relies mainly on the length and velocity of liquid slug, and phases under the Taylor flow has been implemented through a bubble and
the contribution of mass transfer in the liquid film is inapparent. following liquid slug [6,7]. Kreutzer et al.
[6] thought that the mass transfer could be divided into three dif-ferent steps:
van Baten et al. [2] suggested that the mass transfer coefficient was a sum (1) From the bubble directly to the liquid film, (2) from the bubble to the
of two contributions: bubble caps and liquid film sur-rounding the bubble. A vortex region in the liquid slug, (3) from
criterion of Fo number (Fo = D/(t filmd2film), D is the diffusivity of liquid the vortex region to the liquid film.
phase, tfilm the contact time of liquid film with Taylor gas bubble, and dfilm Sobieszuk et al. [8] investigated the mass transfer of CO2/N2 absorption
the thickness of film sur-rounding buble.) was proposed to judge the into KHCO3/K2CO3 solution and determined the mass transfer coefficients
contribution of the mass transfer. If Fo < 0.1, both the bubble caps and the for bubble caps (kL,cap) and liquid film (kL,film), respectively. They found
film region were important; if Fo > 1, the contribution of the bubble caps was
that the values of kL,cap and kL,film were mutually approximate. Yao et al. [9]
dominant due to the saturation of liquid film region.
investigated the flow and mass transfer of CO2-water system under elevated
pressures in a microchannel. On the basis of the dissolution rate of gas
bubbles, the mass transfer coefficients were calculated using a unit cell
⇑ Corresponding author. model. The difference of dissolution rates in the main channel at
E-mail address: ygma@tju.edu.cn (Y. Ma).
http://dx.doi.org/10.1016/j.ijheatmasstransfer.2017.06.054 0017-
9310/ 2017 Elsevier Ltd. All rights reserved.
84 C. Zhu et al. / International Journal of Heat and Mass Transfer 114 (2017) 83–89
different flow rates was very little for a short contact distance. In addition, Aladdin, China) solution were feeded into the gas and liquid inlets of the
many reseachers [10–12] have found that the mass trans-fer during the microchannel, respectively. After the flow stabilized about 5 min for a new
formation stage of bubbles is relatively large in the total mass transfer experimental condition, the formation and move-ment of the bubble in
process. microchannel were recorded by a high-speed digital camera (MotionPro Y5,
Mikaelian et al. [13,14] studied the gas-liquid mass transfer of spherical IDT, USA) at 2000 frames per second. The pressure of gas phase at inlet was
measured by a piezometer (ST3000, Honeywell, USA. The precision is
bubbles in square and circular microchannels through CFD analysis, and
found the recirculation between two successive bubbles. Furthermore, they 0.02%), and the pressure at outlet is atmospheric pressure. CO2 was used as
proposed a model for describing the dissolution of a chain of spherical pure the dispersed phase and a series of NaOH aqueous solutions with 0.3wt%
gas bubbles into a non-volatile liquid. Jia and Zhang [15] numeically sodium dodecyl sulfate were used as the continuous phase. The density q,
investigated the mass transfer of Taylor flow in a microfluidic T-junction viscosity lL and surface tension r of solution were measured respectively
using three-dimensional Volume of Fluid, and found the vortices in both the using densimeter (DMA4500, Anton Paar, Austria), automatic ubbelohde
concentration and velocity fields in the liquid slug. In addition, the simulation viscometer (iVisc, LAUDA, Germany) and ten-siometer (OCA15ECm Data
results showed that the mass transfer through the thin liquid film around the Physics Instruments GmbH, Germany) at 293.15 K, and the data were given
in Table 1. The experiments were carried out at 293.15 ± 1 K and atmosphere
Taylor bubble was dominant during the dissolution, and the dominance
gradually disappeared with the increase of the liquid film thickness, the pressure, the ranges of QG and QL are separately (10–320) mL h 1 and (20–
maximum of mass transfer rate appeared at the top end of the caps in the cap 80) mL h 1 for mass transfer, and QL with (10–80) mL h 1 for flow pattern.
region.
When the bubbles in the channel are less than the channel width, the
regime is named as bubbly flow, and the bubble could be regarded as a
2. Experiment sphere. When the bubbles in the channel are lar-ger than the channel width,
the regime is slug flow, and the slug bubble includes two semispheroid ends
As shown in Fig. 1, a square cross-section microchannel with depth 400 and a body. In our exper-imental, the capillary number Ca = lLu/r, (u is
lm, width 400 lm and length 40 mm was adopted in the experiment. The superficial velocity of gas-liquid flow, u = (QG + QL)/w2, w is the width of
channel was fabricated in a polymethyl methacrylate (PMMA) plate, and then
channel) is less than 0.003, thus we assume that the cross section of slug bub-
sealed with another PMMA plate by screws. The gas flow rate QG and liquid ble body is approximately flat on the side regions and constant curve with
flow rate QL were controlled respectively by pumps (PHD 2000, Harvard radius r in the corners in square microchannel [21], and its area was 90% of
Apparatus, America. The accuracy is ±0.35%.). cross section of microchannel [22]. The vol-ume VB and surface area AB of a
slug bubble could be separately cal-culated by:
The CO2 (the mass fraction purity 99%, Tianjin Liufang Gas Station,
China) and NaOH (the mass fraction purity is 99.4%,
Table 1 Because the specific area a = A/Vt, Eq. (7) could be written as:
Physical properties of NaOH solutions.
dng
q/ lL/ r/ 104 He/
3
(g cm ) (mN m ) 1 3
(mol m Pa ) 1a dt ¼ VtkLaðCe CÞ ð8Þ
(mPa s)
0.2 mol L 1
1.00688 1.068 33.36 4.16 where Vt is the volume of microchannel, kLa is the overall liquid vol-umetric
0.4 mol L 1 1.01551 1.113 32.18 4.45 mass transfer coefficient for the whole microchannel. In the experiment, the
0.8 mol L 1 1.03213 1.209 30.72 5.07 absorbent was sufficient, and the values of Hatta
pffiffiffiffiffiffiffiffiffiffiffi
a Henry coefficient He was calculated according to Ref. [19].
number Ha (Ha ¼ k2cD=kc , k2 is the reaction rate constant, D the diffusivity
of CO2 in liquid, kc is the liquid-side mass transfer coef-ficient of CO2 in
solvent without chemical absorption.) are larger than 3 for the reaction of
3.2. Mass transfer coefficient CO2 and NaOH solution used in this work. Thus the reaction could be
considered to be a fast irreversible reac-tion, and thus the concentration of
For gas-liquid interphase mass transfer of the absorption pro-cess of pure carbon dioxide in the liquid was ignorable, that is C = 0 [11].
gas, the gas-film resistance is negligible according to two-film theory of
Whitman et al. [23] hence the mass transfer efficiency of carbon dioxide into dng
sodium hydroxide aqueous solu-tion depends only on the liquid film [24]. The
dt ¼ VtkLaCe ð9Þ
mass transfer flux N could be written as:
Integrating Eq. (9):
where A is the interfacial area between the gas-liquid two-phase for the whole
microchannel, and it could be considered as a constant for a given
experimental condition, m is the number of bubble in the microchannel, n g is
molar quantity of carbon dioxide absorbed into the liquid, t is time.
Fig. 2. Flow patterns of gas-liquid two-phase flow accompanying with mass transfer (c is initial concentration of NaOH in solution.).
86 C. Zhu et al. / International Journal of Heat and Mass Transfer 114 (2017) 83–89
pinVgeft
Dnin ¼ RT ð12Þ
poutVoutft
Dnout ¼ RT ð13Þ
Then the overall molar quantity of carbon dioxide absorbed into liquid
within t is:
n ðpinVge poutVoutÞft 14
D g¼ RT ð Þ Fig. 5. Effect of operating conditions on kL (concentration of NaOH c = 0.8 mol L 1). The
dashed line is the transition between bubbly regime and slug-bubbly regime; the solid line is the
where pin and pout are the pressure in the inlet and outlet of the microchannel,
transition between slug-bubbly regime and slug regime. The insets depict bubbles in the inlet
respectively. Vout is the volume of the bubble in the outlet of the and outlet of microchannel, respectively.
microchannel. f is the formation frequency of the bub-ble. Vge is the
theoretical formation volume of the bubble without absorption at the same
condition, and it can be calculated by: rising liquid flow rate, it is much different from the results in the literature.
QG Tan et al. [25] observed that kLa increased evidently with the increase of the
Vge ¼ f ð15Þ gas and liquid flow rate. Yue et al. [3] also found that kLa increased with the
Taking the Eq. (14) into the Eq. (10): increase of the liquid slug length. How-ever, Li et al. [26] found that, with the
increase of the liquid flow rate, kLa decreased for small gas flow rate, but
ka ðpinVge poutVoutÞf 16 increase when the gas flow rate reached a critical flow rate. The discrepancy
between literature and present experiment could be attributed to the differ-
L ¼ VtCeRT ð Þ
ence of materials and operating conditions. In principle, there exist two
Then kL could be calculated by:
inverse effects of the liquid flow rate on the mass transfer: (1) The increase of
k ðpinVge poutVoutÞf 17 liquid flow rate could lead to long liquid slug and contact time between liquid
slug and liquid film, also it could pro-mote the convection mass transfer in
L¼ ACeRT ð Þ liquid slug, these would increase the volume mass transfer coefficient; (2)
The errors of kLa and kL were estimated as 5%. The kLa and kL for The increase of liquid flow rate would lead to a decrease in specific interfacial
bubbly flow, slug-bubbly flow and slug flow were obtained from images area. Therefore the volume mass transfer coefficient decreases. As a result, a
recorded by high-speed digital camera in the ranges of QG (10–320) mL h 1 completive result of above the two kinds of influences would lead to different
and QL (20–80) mL h 1. The values of k La, kL and a were listed in Table S1 effects of liquid flow rate on the volume mass transfer coefficient.
in Supplementary Material.
With rising gas flow rate, the bubble volume would increase, while the
ratio of the interfacial area of bubble caps to the total interfacial area between
bubble and liquid in the microchannel would decline. Meanwhile, the
residence time of the bubble on the liquid film would be certainly
prolongated. These would pro-mote the saturation of liquid film. Therefore,
the total mass trans-fer coefficient decreases. In addition, the increase in gas
flow rate also would lead to a faster movement of bubble and liquid slug,
which could accelerate the recirculation in liquid to intensify the mass transfer
[27]. Therefore, with the increase of gas flow rate, the mass transfer
coefficient gradually decreases under the slug-bubbly regime, but increases
under the slug regime. Tan et al.
Fig. 4. Effect of gas and liquid flow rates on the volumetric mass transfer coefficient
(concentration of NaOH c = 0.8 mol L 1).
C. Zhu et al. / International Journal of Heat and Mass Transfer 114 (2017) 83–89 87
[25] also observed the decrease of kL with the increase of the gas flow rate.
Dc
E ¼ 1 þ DNaOHCe ð19Þ
Supplementary data associated with this article can be found, in the online
version, at http://dx.doi.org/10.1016/j.ijheatmasstrans-fer.2017.06.054.
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