Chemical Engineering Science 60 (2005) 1465 1475 www.elsevier.

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Effect of liquid properties on the performance of bubble column reactors with ne pore spargers
A.A. Mouza, G.K. Dalakoglou, S.V. Paras
Department of Chemical Engineering, Aristotle University of Thessaloniki Univ.Box 455, GR 54124 Thessaloniki, Greece Received 4 November 2003; received in revised form 20 September 2004; accepted 7 October 2004

Abstract This work is a study of the effect of liquid properties on the performance of bubble column reactors with ne pore spargers. Various liquids covering a range of surface tension and viscosity values are employed, while the gas phase is atmospheric air. A fast video technique is used for visual observations and, combined with image processing, is used for gas holdup and bubble size measurements. New data on average gas holdup values, bubble size distributions and Sauter diameters are presented and are consistent with existing physical models on coalescence/breakage. A correlation based on dimensionless groups for the prediction of gas holdup in the homogeneous regime is proposed and found to be in good agreement with available data. 2004 Elsevier Ltd. All rights reserved.
Keywords: Bubble column; Porous sparger; Gas holdup; Bubble size; Coalescence; Liquid properties; Flow regimes

1. Introduction Bubble columns are widely used in industrial gasliquid operations (e.g. gas/liquid reactions, agitation by gas injection, fermentations, etc.) in chemical and biochemical process industries, due to their simple construction, low operating cost and high-energy efciency. In all these processes gas holdup and bubble size are important design parameters, since they dene the gasliquid interfacial area available for mass transfer. In turn, bubble size distribution and gas holdup in gasliquid dispersions depend largely on column geometry, operating conditions, physico-chemical properties of the two phases and type of gas sparger (Camarasa et al., 1999). The design of bubble columns has primarily been carried out by means of empirical or semi-empirical correlations based mainly on experimental data. Since the multiphase ow is in general complex in structure, the design and scale up of such type of equipment is still a difcult task and subject to errors (Deckwer and Schumpe, 1993).
Corresponding author. Tel.: +30 23 10 996174; fax: +30 23 10 996209.

E-mail address: paras@cheng.auth.gr (S.V. Paras). 0009-2509/$ - see front matter 2004 Elsevier Ltd. All rights reserved. doi:10.1016/j.ces.2004.10.013

Despite the extensive and long lasting study of bubble column performance many basic questions about the effect of important operational parameters remain unanswered. For example, although bubble column characteristics have been studied extensively in the past few decades, there is still considerable uncertainty concerning the prevailing mechanisms of bubble formation, as well as the most appropriate correlations for practical applications. Break-up and coalescence of uid objects play a crucial role in a broad spectrum of multiphase ow processes, such as the evolution of the bubble size distribution in stirred tanks and bubble columns (Delhaye and McLaughlin, 2003). Shah et al. (1982) and Parasu Veera and Joshi (1999) have reviewed and summarized the work done in this area. It is generally accepted that, depending on the gas ow rate, two main ow regimes can be readily observed in bubble columns, i.e., the homogeneous bubbly ow regime encountered at low gas velocities and characterized by a narrow bubble size distribution and radially uniform gas holdup; and the heterogeneous (churnturbulent ow) regime observed at higher gas velocities and characterized by the appearance of large bubbles, formed by coalescence of the small bubbles and bearing a higher rise velocity hence leading to relatively lower gas holdup values

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(Joshi et al., 2002; Camarasa et al., 1999; Zahradnik et al., 1997). The two regimes differ from one another in their hydrodynamic and transport characteristics. Depending on the type of the gas distributor and the properties of the liquid phase, both regimes can be obtained in the same equipment by varying the gas input ow rate. Various types of gas spargers, the most common of which are perforated plate, membrane and ne porous plate, are in use. Among the above sparger types, the perforated plate requires a minimum gas velocity in order to produce a uniform bubble distribution over the whole sparger area. On the other hand, bubble columns equipped with porous spargers offer a greater gas/liquid contact area for efcient mass and heat transfer, because the bubbles created by this type of gas distributor are numerous and far smaller. Finally, the membrane, even though it is able to maintain a homogeneous ow up to greater ow rates, generates a greater pressure drop (Hebrard et al., 1996). As a result, the use of a ne porous plate as a gas sparger seems to be advantageous over the other types of multiple injection point distributors. To the authors best knowledge, limited information is available in the literature regarding the behavior of ne porous plate spargers. Hebrard et al. (1996), who studied the inuence of gas sparger characteristics on the hydrodynamic behavior of bubble columns, concluded that bubble size and holdup values depend primarily on the physico-chemical properties of the liquid phase and the type of gas distributor. On the other hand, Parthasarathy and Ahmed (1996), who conducted their experiments with non-coalescing liquids, stated that there is confusion regarding the average size value and size distribution of bubbles generated by ne pore spargers. Zahradnik et al. (1997) investigated the effect of various parameters (i.e., column geometry, distributor type, liquid properties) on the gasliquid ow regime stability and gas holdup in bubble column reactors equipped, among others, with porous spargers. Camarasa et al. (1999), who examined the inuence of the liquid properties and of the gas sparging method on hydrodynamics and bubble characteristics in a bubble column, used water-alcohol solutions to simulate the behavior of non-coalescing organic liquids and compared their data with those concerning standard airwater systems. Kaji et al. (2001) studied experimentally the behavior of bubble formation using various porous spargers with pore diameter 5400 m and investigated the effect of surface tension on the gas holdup distribution. The purpose of this work is to study the effect of liquid properties on bubble size distribution in a bubble column equipped with two different ne porous spargers. Various liquids covering a range of surface tension and viscosity values are employed, while atmospheric air is used as the gas phase for all experiments. Experimental data on average gas holdup, bubble size distribution and mean Sauter diameter, obtained from image analysis of fast video recordings, are

reported. A correlation is also proposed for the prediction of average gas holdup.

2. Experimental set-up and procedures The experimental set-up (Fig. 1) consists of a vertical rectangular Plexiglas column 1.5 m height, having a square cross-section (side length 10 cm). The column is equipped with appropriate rotameters for gas phase ow measurement and control. The rectangular geometry was preferred over the cylindrical one, because it facilitates both the direct ow visualization and the use of optical measuring methods by minimizing optical distortion. For the injection and uniform distribution of the gas phase, a gas sparger, i.e., a round metal porous disk, 2.0 cm in diameter, is installed at the center of the bottom plate. In the present experiments, two 316L SS porous disks (made by Mott Corp.) with nominal pore size of 20 and 40 m were alternatively used as gas spargers. However, in order to check the effect of the usage time on sparger performance various porous disks were employed during the period of the experiments. Several liquids, whose physical properties are presented in Table 1, were employed as liquid phase, whereas the gas phase was atmospheric air for all runs. All the experiments were conducted at ambient pressure and temperature conditions. Each experimental run started by rst lling the column with the appropriate liquid phase up to 80 cm above the sparger. All the experiments were performed with no liquid throughput, while the gas phase was injected and distributed into the liquid phase by passing through the porous disk sparger. A high-speed digital video camera (Redlake MotionScope PCI 1000S) is used both for direct ow visualization and for bubble size and gas holdup measurements. The camera is xed on a stand very close to the area of observation in such a way that the test section is located between the camera and an appropriate lighting system placed behind a diffuser to evenly distribute the light. Although the imaging system used was capable of recording up to 1000 full frames per second, a speed of 500 fps is considered a suitable recording rate for the present experiments. The shutter rate employed was of 1/10 000. It must be pointed out that the optical system used offers a very narrow depth of eld (few mm). The recorded images were also used to extract quantitative information on bubble size distribution and gas holdup values. Using proper lighting, the gasliquid interface around the bubble circumference can be clearly outlined on the pictures. The calibration of the measuring system, needed to ensure the accurate measurement of the bubbles, is accomplished by measuring a microscale placed at the focusing plane. Subsequent image processing (e.g. noise reduction, brightness improvement, contrast enhancement, shadow and double images removal) results to a sharp bubbleliquid interface. A detailed description of the technique can be also

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Fig. 1. Experimental set-up.

Table 1 Liquid phase properties at 20 C Index Liquid phase Viscosity, L (mPa s) 1.0 0.9 0.9 3.5 8.2 22.5 Density, 3 L (kg/m ) 998 994 991 1081 1126 1173 Surface tension, L (mN/m) 72 60 48 70 68 67

3. Results 3.1. Visual observations As already mentioned, depending on the gas ow rate, the two ow regimes observed in bubble columns are the homogeneous bubbly ow regime encountered at low gas velocities and the heterogeneous (churn-turbulent ow) regime observed at higher gas velocities. The photos in Fig. 2 give a visual image of the ow patterns observed in a bubble column according to the gas ow rate when the liquid phase is either water or 50% glycerin solution. At the beginning the bubbles are gathered at the core of the ow, but after the rst 20 cm they are spread uniformly covering the whole column area. It is also worth noticing that after the rst 40 cm of the column height the gas phase distribution does not seem to change signicantly. For the lower gas velocities applied the homogeneous ow regime is encountered, where relatively small gas bubbles are formed and almost uniformly distributed throughout the whole column area (Figs. 2a and b). The bubbles have a symmetric ellipsoid shape and rise almost vertically with the same speed and without coalescence drifting an amount of liquid to the top of the column. As it is also described by Ruzicka et al. (2001), the amount of liquid carried up by the bubbles hinders the uprising bubbles on its way down, resulting in an increase of gas holdup. By increasing the gas ow rate the bubbles begin to grow in size and large bubbles appear to coexist with the smaller ones. The uprising bubbles begin to exhibit also a reciprocative movement which retards their upward movement enhancing coalescence. The above observations correspond to an intermediate transition regime. By further increasing the

w b1 b2 g1 g2 g3

Water n-butanol 0.6% w/w n-butanol 1.5% w/w Glycerin 33.3% w/w Glycerin 50.0% w/w Glycerin 66.7% w/w

found in a recent paper by Colella et al. (1999). Image analysis, using appropriate software (SigmaScan Pro ), allows bubble size prediction. The bubbles were approximated by ellipses whose major and minor axes were computed by the software. The equivalent diameter of a sphere with the same volume as the ellipsoid was computed (Colella et al., 1999; Polli et al., 2002). Approximately 800 bubbles were measured in each experimental run, a number considered to be adequate for statistical calculations (Tse et al., 2003; Hebrard et al., 1996). The advantage of the method is that it permits both in situ and non-intrusive measurements. The uncertainty of the measurements has been estimated to be less than 10%. The average gas holdup is estimated by the bed expansion. The liquid level is measured on two different pictures taken prior to gas inow and after gas is injected and steady state is established. The difference in liquid level, measured by superposition of the two pictures, gives a measure of the average gas holdup. The uncertainty of the measurements is estimated to be less than 15%.

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Fig. 2. Flow patterns in homogeneous (QG = 0.8 105 m3 /s) and heterogeneous (QG = 7.7 105 m3 /s) regimes for waterair (a, c) and glycerin 50.0%air (b, d) systems (dp = 40 m).

gas ow rates (Figs. 2c and d) the heterogeneous ow regime is encountered where big gas masses, presumably formed by coalescence, begin to rise resulting in a kind of churn ow pattern. In this regime velocities display pronounced radial proles resulting to strong circulations and enhancing bubble rise speed. This results to a further decrease of gas holdup value. A detailed and comprehensive description of the ow regimes in bubble columns is also given by Ruzicka et al. (2001). The ow patterns observed for some of the liquids used (i.e., water, 50% glycerin and 1.5% butanol) are presented in Fig. 3. It is worth noticing that the bubble shape and concentration obtained by the glycerin solutions is practically the same with that of water (Figs. 3a and b). The bubbles observed in the low surface tension non-coalescing butanol solutions (Fig. 3c) differ signicantly from those encountered in the coalescence promoting media (i.e., water and glycerin solutions). The former are spherical, considerably smaller in size and hence, for a given gas ow rate, far more numerous than those of water (Papatzika, 2002). These bubbles form a kind of plume that quickly covers the whole column area providing an interfacial area much greater than that obtained with water. A radial circulation is also observed, which becomes more pronounced by increasing gas ow rate, resulting in a decrease of holdup value (transition regime). 3.2. Gas holdup In this section the measured gas holdup values are given. The ow regimes can be distinguished by plotting the average gas holdup ( G ) versus the gas ow rate (QG ). Fig. 4

shows the dependence of gas holdup on corresponding gas supercial velocity for the two spargers used. A typical ow regime map (Ruzicka et al., 2001) is also included for comparison. The gas supercial velocity is dened as UGS = QG , A (1)

where QG is the gas ow rate and A the column cross section area. A rst observation is that for the two spargers tested the gas holdup is not signicantly affected by the sparger pore size, a remark that is in agreement with previous observations (e.g. Kaji et al., 2001). The rst part of the curve corresponds to the homogeneous regime, where the gas holdup increases with the gas velocity. A transition regime follows where a slight decrease in gas holdup is observed. Finally, at the heterogeneous regime the gas holdup continues to increase but with a lower slope than the homogeneous regime. As it is also pointed out by Ruzicka et al. (2003), if the bubbles could travel unaffected at their terminal velocity, the gas holdup would increase linearly with the gas ow rate. In the homogeneous regime, as the gas holdup increases the hindrance progressively reduces the bubble velocity leading to a further increase of the gas holdup. The opposite holds true for the heterogeneous regime, where the bubble velocity increases in the central core of the column resulting in a decrease of the gas holdup value with gas ow rate. In Fig. 5 the data are plotted in terms of gas holdup versus gas phase supercial velocity for airwater, airbutanol and airglycerin systems. As it is expected, gas holdup increases with gas ow rate. A slight increase in gas holdup

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Fig. 3. Characteristic photos of the homogeneous regime for various liquids (a) water, (b) glycerin 50.0% and (c) butanol 1.5% (QG = 1.5 105 m3 /s, dp = 40 m).

4.0

5 w dp, m b1 4 b2 g1 g2 3 g3

3.0

20 40

G, %

2.0

G, % 2 1 dp=40m 0.2 0.4 0.6 UGS, cm/s 0.8 1.0 0 0.0

1.0

0.0 0.0

0.2

0.4

0.6

0.8

1.0

UGS, cm/s
Fig. 5. Effect of type of liquid on gas holdup (dp = 40 m).

Fig. 4. Effect of pore diameter on gas holdup for the waterair system.

values is also observed when the lower surface tension butanol solutions are used as liquid phase, whereas airwater and airglycerin solutions have almost identical gas holdup values. It is evident that the effect of viscosity is negligible. The present experimental data are compared with correlations included in a comprehensive review paper by Shah et al. (1982) and in general they are found to deviate considerably from the proposed empirical models. For instance, the prediction by the correlations of Akita and Yoshida (1973) and Hikita et al. (1980) exhibit for airwater systems a 20% deviation from the present data and those of

Camarasa et al. (1999) for porous spargers, whereas for glycerin (Fig. 6) and butanol solutions the corresponding deviations exceed 40%. This can be attributed to the fact that the aforementioned correlations are based on data obtained with single and multi-nozzle spargers (Shah et al., 1982). 3.3. Bubble size distributions The number frequency of the bubble size was calculated at ve distances above the sparger surface (i.e., 3, 10, 20, 30

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3.0 exp data present work Eq.8 Akita & Yoshida (1973) 2.0 G, % Hikita et al. (1980)
number frequency, %

50

L=3.5 mPa.s
40

dp, m 20 40 h=40 cm 30

1.0

20

0.0
(a)

10

0.1

0.2 UGS, cm/s

0.3

0.4

3.0 exp data present work Eq.8 Akita & Yoshida (1973) 2.0 G , % Hikita et al. (1980) L=22.5 mPa.s

0 0 1 2 3 d, mm 4 5 6

Fig. 7. Effect of pore diameter on bubble size distribution (waterair system, h 40 cm, QG = 0.8 105 m3 /s).

1.0

0.0
(b)

0.1

0.2 UGS, cm/s

0.3

0.4

Fig. 6. Comparison of the present experimental data with values calculated by proposed Eq. (8) and the models of Hikita et al. (1980) and Akita and Yoshida (1973) for two glycerin solutions: (a) 33.3% and (b) 66.7%. Error bars correspond to 10 deviation.

and 40 cm) for the homogeneous regime. In Fig. 7 the bubble size distribution curve is presented for the airwater system and for both sparger types used. The measurements were performed at a height of 40 cm above the sparger surface where the ow was found to be developed. It seems that for the spargers tested the sparger pore size has practically no effect on the distribution curve and this holds true for all the liquids tested. The above observation agrees with the results of Parthasarathy and Ahmed (1996), who reported that below a sparger pore diameter of 50 m there is a negligible change in bubble size. Fig. 8 shows bubble size distributions at two locations i.e., just above the sparger surface and 40 cm away from it, for water and for the glycerin solutions. In all cases it is obvious that the form of bubble size distribution curve does not

practically change with height, an observation that is also reported by Colella et al. (1999) for airwater systems. The water data, both in the vicinity of (h 3 cm) and away from (h 40 cm) the sparger area, are well tted by a lognormal distribution curve (Fig. 8a). Similarly, the two glycerin solutions (i.e., g 1 and g 2) data obtained close to the sparger follow a log-normal distribution curve (Figs. 8a and b). However, the g 1 and g 2 solutions data away from the sparger (h 40 cm) cannot be tted by such type of curve because a second peak makes its appearance (presumably due to coalescence), which becomes more distinct for the higher viscosity glycerin solution (g 3). In these cases the data are best tted by the summation of two normal distribution functions (Figs. 8a and b). It must be noted that the bubble size distributions of the butanol solutions were not calculated due to the limitations of the measuring technique applied. In this case the problems arise from bubble overlapping on the focusing plane due to high bubble concentration. It is believed that the limited available data on bubble size distribution for low surface tension liquids is due to the difculty in performing such measurements. The visual observations reveal a behavior for the butanol solutions similar to that of the low viscosity glycerin solutions. Moreover, Camarasa et al. (1999) report that for non-coalescing alcohol solutions a narrow distribution of small bubbles is observed and that the bubble size within the column is nearly the same as that of bubbles formed at the porous distributor. For the rst two glycerin solutions (Figs. 8a and b) the unimodal bubble size distribution curve suggests that the majority of the bubbles have the same size. This implies that the bubbles, after detaching from the sparger surface,

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50 h, cm 40 number frequency, % 3 40 3 40 L, mPa.s 1.0 3.5

Table 2 Mean Sauter diameter (d32 ) and standard deviation ( ) for the 40 m pore sparger at h 40 cm Liquid phase QG = 0.8 105 m3 /s QG = 1.5 105 m3 /s d32 (mm) Water n-butanol 0.6% w/w n-butanol 1.5% w/w Glycerin 33.3% w/w Glycerin 50.0% w/w Glycerin 66.7% w/w
a Not available.

(mm) 0.5
a a

d32 (mm) 3.8 1.7 1.3 2.8 3.5 4.8

a a

(mm) 0.9

30

20

3.1 1.5 1.1 2.2 2.4 3.0

0.6 0.8 1.0

0.8 1.0 1.5

10

0 0 (a) 50 h, cm 40 number frequency, % 3 40 3 40 L, mPa.s 8.2 22.5 1 2 3 d, mm 4 5 6

the distributor region. Finally, the broad distribution curve of the water, which retains its initial shape through the column, may be attributed to the fact that coalescence occurs onto the sparger surface but does not continue during the bubble course through the bulk of the liquid. The mean Sauter bubble diameter (d32 ), dened as d32 =
N 3 i =1 di N 2 i =1 di

(2)

30

20

10

0 (b)

3 d, mm

Fig. 8. Bubble size distributions in the homogeneous regime (QG = 1.5 105 m3 /s) for: (a) water, glycerin 33.3% and (b) glycerin 50.0%, glycerin 66.7%.

retain their initial size and neither a coalescence nor a breakage process occurs during their course to the column exit. The bimodal distribution observed at the higher viscosity value (Fig. 8b) can be attributed to coalescence phenomena that seem to commence onto the sparger surface. The more pronounced bimodal distribution observed at h 40 cm implies that the bubbles continue to coalesce as they rise towards the liquid surface. This is in agreement with the observations of Zahradnik et al. (1997), who noticed an unfavorable effect of liquid viscosity that they ascribed to the existence of drag forces promoting bubble coalescence in

is a popular representation of the mean bubble size. Its values and the standard deviation of the drop size distribution ( ) for all liquids as well as for two gas ow rates are given in Table 2. Values for the low surface tension solutions are only a rough estimation, because they are calculated from a series of small samples (e.g. 30 bubbles) taken from areas with low bubble concentration and for this reason values for the butanol solutions are not included in Table 2. As it is expected the mean bubble size increases with increasing gas ow rate but it is worth noticing that the increase is more pronounced for the high-viscosity glycerin solutions (3060%) than it is for the low viscosity butanol solutions ( 15%). It is evident that d32 also increases with viscosity. The only exception is water which, despite its relatively low viscosity value, exhibits a d32 comparable to that of the high-viscosity glycerin solutions. It must be noted that the calculated d32 value of the glycerin solutions is much greater than the more frequent bubble diameter (< 1 mm), as it can be seen in Fig. 8, a fact that is also reported by Tse et al. (2003), who found that during coalescence the formation of large bubbles is accompanied by a great number of small daughter bubbles (100200 m). 3.4. Homogeneousheterogeneous regime transition A common procedure to locate the transition point between the homogeneous and heterogeneous regime is to apply the drift ux analysis, which is based on mass conservation equations and relates velocities and concentrations of the phases (Wallis, 1969). The model looks at the relative motion of the two phases and is suggested for ows with at radial proles. The basic quantity is the drift ux, j, which

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0.010

0.008

drift flux, m/s

0.006 w 0.004 b1 b2 g1 0.002 trans 0.000 0 1 2 G, %

Fig. 9. Regime transition using the drift ux model.

tion point to slightly higher velocities. The only exception is water whose transition velocity is lower than that of butanol solutions despite its slightly higher viscosity. This behavior can be attributed to the simultaneous effects of both relatively low viscosity and high surface tension. The difference between the calculated transition velocities and the ones reported in the literature (e.g. Zahradnik et al., 1997; Camarasa et al., 1999; Ruzicka et al., 2001, 2003) is not unexpected since it has been reported (e.g. Hebrard et al., 1996; Zahradnik et al., 1997) that differences in size and type of the distributor shifts the limit of the homogeneous regime.

g2 g3 4 5

4. Result interpretation The optimum operating conditions of a bubble column would be the ones that enhance mass transfer and this is accomplished by maximizing the gas/liquid interfacial area, a measure of which is given by a= 6G , d32 (4)

Table 3 Transition between homogeneous and heterogeneous regime (dp = 40 m) Liquid phase Water n-butanol 0.6% w/w n-butanol 1.5% w/w Glycerin 33.3% w/w Glycerin 50.0% w/w Glycerin 66.7% w/w
trans (%)

Utrans (cm/s) 0.20 0.23 0.23 0.29 0.28 0.28

js (cm/s) 6.4 7.3 7.3 9.2 8.9 8.9

1.2 2.2 2.2 1.1 1.1 1.2

represents the gas ux through a surface moving at the average velocity of the mixture and is given by j = UGS (1
G ),

(3)

where UGS is the supercial gas velocity and G the average gas holdup. If the drift ux is plotted versus the gas holdup, the change in the slope of the curve indicates the transition from the homogeneous to the heterogeneous regime (Shah et al., 1982). Fig. 9 presents the calculated j values (Eq. (3)) versus the corresponding gas holdup experimental data for all the liquids tested. The points where the change of the slope occurs are located and the corresponding supercial velocities (UGS ) are calculated and presented in Table 3. A general comment is that for all cases the transition occurs at a liquid supercial velocity between 0.2 and 0.3 cm/s. These supercial velocity values correspond to gas uxes through the sparger, js , 6.0 to 9.0 cm/s (Table 3), which are in the same order of magnitude with those reported in the literature (e.g. Camarasa et al., 1999; Zahradnik et al., 1997). It has been determined that (for the two spargers employed) the transition point does not depend on the pore size. It is also evident that an increase in liquid phase viscosity shifts the transi-

where G is the gas holdup and d32 the mean Sauter diameter. Consequently, the homogeneous bubbly ow regime encountered at the lower gas ow rates is most desirable for mass transfer operations, since, by exhibiting a large gas holdup value accompanied by relatively small bubble size, provides a greater interfacial area. As it is already mentioned the mean bubble size depends on the liquid properties which may either promote or inhibit coalescence of the primary bubbles formed on the sparger surface. It is generally admitted that coalescence occurs in three steps, i.e., collision, liquid lm drainage and rupture. When two bubbles collide, the liquid lm formed by the small amount of liquid trapped between them begins to drain until it becomes sufciently thin to be ruptured due to an instability mechanism. The above described sequence is leading to a coalesced bubble. It is also believed that the liquid lm drainage is the rate controlling step while the rupturing step is almost instantaneous (Chaudhari and Hofmann, 1994). Bubble coalescence is also a function of the contact time between two bubbles that depends on the bubble rising velocity, which in turn is a function of the bubble size and the turbulence intensity. It is evident that, when a porous sparger is used, the proximity of the pores promotes coalescence on the sparger surface as soon as the bubbles enter the column. The viscosity seems to play a dual role. At relatively low viscosity values, an increase in viscosity hinders lm drainage during the thinning process and thus inhibits coalescence. This remark is also supported by the shape of the distribution curves of the two lower viscosity glycerin solutions tested (Fig. 10) and the photos in Figs. 11a and b from which is evident that the bubbles away from the sparger area retain their relative monodispersity and coalescence mechanism plays a minor role. However, a further increase of

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50 L, mPa.s 40 1.0 3.5 8.2 22.5 h=40 cm

number frequency, %

30

coalescence on the sparger surface as the bubbles enter the column. An attempt was made to formulate a correlation that would permit the prediction of gas holdup, a variable that greatly affects the bubble column operation. From the visual observations and the careful inspection of the experimental results (from various investigators) it can be concluded that the gas holdup value is the result of the interaction of several parameters, the most important of which are: the gas phase supercial velocity, the physical properties of the liquid phase (i.e., surface tension, viscosity), the column cross section and the sparger cross section. The experimental results of this study show that the sparger pore size used does not practically affect the holdup values, a remark that is also supported by other investigators (e.g. Parthasarathy and Ahmed, 1996; Kaji et al., 2001). It must be also noted that the use of several porous disks with the same nominal porosity during the period of the experiments proved that the data are quite reproducible and that the porous disk usage time does not signicantly affect its performance. In order to formulate a generalized correlation that would incorporate the relative effect of all the above factors, dimensional analysis was performed. The results show that the effect of gas velocity and column dimensions can be taken into account by dening a Froude number: Fr =
2 UGS , dC g

20

10

0 0 1 2 3 d, mm 4 5 6

Fig. 10. Effect of liquid viscosity on the form of bubble size distribution curve (QG = 0.8 105 m3 /s, h 40 cm).

liquid viscosity leads to a decrease of turbulence in the liquid phase favoring large bubble formation by coalescence (Figs. 10 and 11c) which leads to an increase of the larger bubble number in expense of the smaller ones. This explanation is also supported by other authors (e.g. Ruzicka et al., 2003). Thus at higher viscosity values the wide shape of the bubble size distribution curve implies that the smaller bubbles coalesce, an assumption also supported by the bimodal bubble size distribution observed. It is noted that Parthasarathy and Ahmed (1996) believe that in a coalescing medium bubbles continue to coalesce as they rise. The water is an exception to the above trends and the bubbles formed have larger sizes than that expected by considering only the physical properties, i.e., the mean bubble size has a higher value than that of the 50% glycerin solution whose viscosity value is 8.2 mPa s (Fig. 10). This peculiar behavior can be attributed to the simultaneous effects of both low viscosity and relatively high surface tension that favor

(5)

where UGS is the gas supercial velocity and dC the column diameter or, in case of non-circular cross-sections, the hydraulic diameter. Similarly, the effect of the liquid phase properties can be included in the appropriate Archimedes (Ar) and Etvos (Eo) numbers dened as follows: Ar =
3 dC 2g L , 2 L

(6)

Fig. 11. Images illustrating the effect of viscosity on bubble size distribution for: (a) glycerin 33.3%, (b) glycerin 50.0% and (c) glycerin 66.7%. (QG = 0.8 105 m3 /s, dp = 40 m).

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25

20

present work Kaji et al.(2001) Camarasa etal. (1999) correlation

15 G, %

10

0 103

104

105 Fr0.5Ar0.1Eo2.2 (dS/dC)

106

107

Fig. 12. Gas holdup correlation for the homogeneous regime.

Eo =

2 dC

Lg L

(7)

where L , L and L are the liquid density, viscosity and surface tension respectively. Finally, the ratio (dS /dC ) of sparger to column diameter was also included to account for the different geometrical congurations of the gas entrance. The attempt to formulate a generalized relation that would be valid for both homogeneous and heterogeneous regimes was unsuccessful. Finally, a correlation is formulated that is valid only for the homogeneous regime:
G

bubble sizes. An increase in liquid viscosity favors larger bubble formation by decreasing turbulence, a fact that both promotes bubble coalescence and hinders breakage. On the other hand, an increase in liquid surface tension favors small bubble formation by promoting breakage and demoting coalescence. The bubble size distribution data are generally unimodal. Only for the relatively high-viscosity liquids a second peak arises as a result of bubble coalescence, and therefore the data are best tted by the summation of two normal distribution functions. It is found that for the geometry studied the supercial velocity that marks the homogeneous regime limit does not exceed 0.3 cm/s. Finally, a new correlation based on dimensionless groups for the prediction of gas holdup in the homogeneous regime is proposed and found to be in good agreement with available data. It is generally accepted that porous plates hold advantages over the other types of gas distributors used. It has been also proved that bubble size distribution in bubble columns equipped with ne porous spargers depends mostly on coalescence/breakage phenomena, which take place either directly onto or in the vicinity of the sparger surface. Delhaye and McLaughlin (2003) stated that both experimental and theoretical analyses are needed in order to establish rigorous criteria for the coalescence and breakage of uid objects at the microscopic level. Consequently, future experimental work must be focused on the phenomena occurring onto the sparger surface with the intention to gain an insight on the bubble formation mechanisms. Moreover, the knowledge of the range of parameters over which a particular regime is encountered and the conditions under which a transition occurs would facilitate the design of a bubble column reactor. References
Akita, K., Yoshida, F., 1973. Gas Holdup and Volumetric Mass Transfer Coefcient in Bubble Columns. Ind. Eng. Chem. Proc. Des. Dev. 12, 7680. Camarasa, E., Vial, C., Poncin, S., Wild, G., Midoux, N., Bouillard, J., 1999. Inuence of coalescence behaviour of the liquid and of gas sparging on hydrodynamics and bubble characteristics in a bubble column. Chemical Engineering and Processing 38, 329344. Chaudhari, R.V., Hofmann, H., 1994. Coalescence of gas bubbles in liquids. Reviews in Chemical Engineering 10 (2), Colella, D., Vinci, D., Bagatin, R., Masi, M., Bakr, E.A., 1999. A study on coalescence and breakage mechanisms in three different bubble columns. Chemical Engineering Science 54, 47674777. Deckwer, W.-D., Schumpe, A., 1993. Improved tools for bubble column reactors and scale up. Chemical Engineering Science 48, 889911. Delhaye, J.-M., McLaughlin, J.B., 2003. Appendix 4: report of study group on microphysics. International Journal of Multiphase Flow 29, 11011116. Hebrard, G., Bastoul, D., Roustan, M., 1996. Inuence of gas sparger on the hydrodynamic behaviour of bubble columns. Transactions of the Institution of Chemical Engineers 74, 406414. Hikita, H., Asai, S., Tanigawa, K., Segawa, K., Kitao, M., 1980. Gas Holdup in Bubble Column. Chemical Engineering Journal 20, 5967. Joshi, J.B., Vitankar, V.S., Kulkarni, A.A., Dhotre, M.T., Ekambara, K., 2002. Coherent ow structures in bubble column reactors. Chemical Engineering Science 57, 31573183.

= 0.001 F r 0.5 Ar 0.1 Eo2.2

dS dC

2/3

(8)

and it is plotted in Fig. 12, where the data of Camarasa et al. (1999) and Kaji et al. (2001) are also included for comparison. It seems that the proposed correlation is in fairly good agreement (10%) with all the available data for the homogeneous regime.

5. Concluding remarks In bubble column reactor design the homogeneous ow regime is usually the most desirable, because it enhances the efciency of the equipment by providing a greater gasliquid interfacial area. For this regime new data concerning average gas holdup values, bubble size distributions and Sauter diameters are given for a number of liquids covering a range of surface tension and viscosity values. It was found that bubble size depends on the gas ow rate and is affected by the liquid properties and that an increase in gas ow rate increases bubble collision probability resulting in greater

A.A. Mouza et al. / Chemical Engineering Science 60 (2005) 1465 1475 Kaji, M., Sawai, T., Mori, K., Iguchi, M., 2001. Behaviors of bubble formation from a bottom porous nozzle bath. Proceedings of the 5th ExHFT, Thessaloniki, Greece. Parasu Veera, U., Joshi, J.B., 1999. Measurement of gas hold-up proles by gamma ray tomography: effect of sparger design and height of dispersion in bubble columns. Transactions of the Institution of Chemical Engineers 77, 303317. Papatzika, E., 2002. Experimental study of a bubble column. Diploma Thesis, Department of Chemical Engineering, AUTh (in Greek). Parthasarathy, R., Ahmed, N., 1996. Size distribution of bubbles generated by ne pore spargers. Journal of Chemical Engineering of Japan 29, 10301034. Polli, M., Di Stanislao, M., Bagatin, R., AbuBakr, E., Masi, M., 2002. Bubble size distribution in the sparger region of bubble columns. Chemical Engineering Science 57, 197205. Ruzicka, M.C., Zahradnik, J., Drahos, J., Thomas, N.H., 2001. Homogeneousheterogeneous regime transition in bubble columns. Chemical Engineering Science 56, 46094626.

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