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ENHANCEMENT IN GAS HOLDUP IN BUBBLE COLUMNS THROUGH USE OF VIBRATING INTERNALS

V. Balamurugan, D. Subbarao and Shantanu Roy*
1. Department of Chemical Engineering, Indian Institute of Technology Delhi, Hauz Khas, New Delhi 110 016, India

Including internals in bubble columns is known to enhance the gas holdup. In this paper, a method to achieve this objective substantially has been proposed via the use of vibrating helical spring internals. Experimental observations on effect of vibrating internals such as vibrating helical springs on gas holdup in bubble columns are presented. Effects of supercial gas velocity, H/D ratio (height of the static liquid to column diameter ratio), volume fraction of helical springs, and thickness of the helical spring wires on hydrodynamics parameters are studied. Increase in gas holdup up to 135% is observed by using vibrating helical spring internals in bubble columns compared to bubble columns without internals. This method offers a simple, cost-effective, and easy way to enhance gas holdup even at high gas uxes. It has been reported that this enhancement stems from the fact that the vibrating springs breakup the gas into ne bubbles, which effectively reduces their rise velocity and enhances their average residence time in the liquid column. ` bulles accro On sait quinclure des composantes internes dans les colonnes a t le volume mort. Dans ce document, une m ethode pour atteindre en t substance cet objectif a e e propos ee par lutilisation de composantes internes de ressorts h elico daux vibrants. Des observations exp erimentales ` bulles ont e t sur leffet des composantes internes vibrantes comme les ressorts h elico daux vibrants sur le volume mort dans les colonnes a e pr esent ees. Les effets sur la vitesse supercielle du gaz, le rapport H/D (rapport de hauteur du liquide statique au diam` etre de la colonne), la tudi fraction du volume des ressorts h elico daux et l epaisseur des ls des ressorts h elico daux sur les param` etres hydrodynamiques sont e es. Une augmentation du volume mort jusqu` a 135 % est observ ee au moyen des composantes internes de ressorts h elico daux vibrants dans les colonnes ` bulles, en comparaison avec les colonnes a ` bulles sans composantes internes. Cette m conomique daccro a ethode offre une fac on simple et e tre lev le volume mort m eme lors de ux de gaz e es. On a rapport e que cet accroissement d ecoule du fait que les ressorts vibrants divisent le gaz en nes bulles, ce qui r eduit de mani` ere efcace leur vitesse dascension et accro t leur temps de s ejour moyen dans la colonne de liquide. Keywords: bubble column, gas holdup, volume fraction, vibrating internals, springs, churn-turbulent ow

INTRODUCTION

ubble columns are generally cylindrical vessels where gas is sparged into a pool of liquid or liquidsolid suspension in the form of bubbles. Bubble columns serve as multiphase reactors and contactors in chemical, petrochemical, biochemical processes, efuent/waste-water treatment process, and metallurgical industries. As reactors, bubble columns are encountered in a wide range of applications in chemical processes involving oxidation, chlorination, alkylation, polymerization, and hydrogenation reactions (Shah et al., 1982; Fan, 1990). Bubble columns are also used in processes such as hydrotreating and conversion of petroleum residues (Lunin et al., 1985), coal gasication, and coal liquefaction (Tarmy et al., 1984). Other processes that utilize bubble columns are gas conversion processes involving the production of liquid fuels from synthesis gas, for example, Fisher Tropsch process (Kolbel and Ralek, 1980), synthesis of methanol (e.g., LPMEOHTM technology for liquid-phase methanol synthe-

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Author to whom correspondence may be addressed. E-mail address: roys@chemical.iitd.ac.in Can. J. Chem. Eng. 9999:1, 2010 2010 Canadian Society for Chemical Engineering DOI 10.1002/cjce.20362 Published online in Wiley InterScience (www.interscience.wiley.com)

sis from Air Products and Chemicals), and other synthetic fuels. In a world increasingly interested in bio-fuels and fuels from renewable sources, bubble columns are thus expected to play an increasingly dominant role as process equipment. As separation units, bubble columns are utilized in the form of bubble cap tray towers. Bubble columns are used as fermenters, in wastewater treatment and in variety of metallurgical operations such as leaching of metal ores. Bubble columns are preferred over other types of reactors due to their simplicity in operation, compactness, low operating cost, maintenance cost, lack of mov-

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ing parts and therefore reduced wear and tear, high durability of catalyst, and good heat and mass transfer characteristics. The gas holdup and consequently the gasliquid interfacial area is the single-most important variable governing the operation of bubbles columns as process vessels. The gas holdup drives the liquid circulation and the multiphase turbulence eld, and thus determines to a large extent the gasliquid interfacial area and associated mass transfer rates as well. Provided that the reactions are not all kinetically controlled, whenever inter-phase and intraphase transport are governing phenomena, having optimal gas holdup is the rst priority for smooth and economically viable operation. The numerous reviews that have appeared suggest that the bottleneck in further improvement in bubble column performance comes because of our inability to control and enhance the gasliquid interfacial area and the gas holdup at high gas uxes (e.g., JoshiQ1 and Shah, 1981; Shah et al., 1982; Deckwer, 1992; Koide, 1996; Wild et al., 2003). Thus, if we are able to enhance these two physical parameters, we will be successful in enhancing volumetric mass transport rate between the gas and liquid phases, and hence enhance all those reactions which are limited by the interfacial transport rate. Unfortunately, this wish is not easily realizable going forward, because the use of better designed spargers, distributors as well as various kinds of internals has already been attempted. These modications have provided marginal improvement in gas holdup and interfacial area but have not been game-changers in bubble column technology. With a broader perspective, the need to enhance gas holdup and interfacial area is in line with the global objective of process intensication that is likely to dene the chemical and rening industry of the future (Dautzenberg and Mukherjee, 2001), Therefore, improved gasliquid contacting in bubble columns is not only a future need for these reactors alone but also a demand of the process industry of the future, in general. One proposed method of improving gasliquid contacting in bubble columns has been by introducing appropriately designed internals (Fair et al., 1962; Patil et al., 1984; Yamashita, 1987a; Pradhan et al., 1991). These internals (e.g., horizontal bafes, vertical rods, helical coils, KATAPAK-S, Sulzer SMV type) improve gasliquid contacting by intensifying the process parameters through enhanced phase holdups, higher specic gasliquid interfacial area, better heat and mass transfer characteristics, all at higher throughputs. The last point is of particular importance, because while it is possible to improve holdup when gas ow rates are small, as soon as the gas supercial velocity increases, the complex multiphase turbulence takes over and widespread bubble coalescence leads to the formation of larger bubbles. These are more buoyant, have a higher rise velocity, and hence the effective holdup of gas in the vessel tends to level off. In other words, the further enhancement of gas holdup is very marginal and certainly not commensurate with the imposed increase in gas ow rate. The internals that have been considered in the past include heat exchanger tubes, inserted into the reactor for cooling/heating the system and maintaining isothermal conditions, especially for highly exothermic/endothermic reactions. In some cases, bubble columns are also sectionalized using bafes to reduce back mixing (Shah et al., 1982; Deckwer and Schumpe, 1993; Pandit and Doshi, 2005). Even though these internals improve the bubble column performance, they are too expensive and occupy space inside the reactor (high volume fraction of internals). This constitutes the valuable real estate in the reactor, that is, the volume that would have been otherwise used for the desired reaction. Perhaps the rst reported instance for process intensication in bubble columns using some sort of vibrational mode was the

Author Proof

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(i) (ii) (iii) (iv) (v)

work of Baird and Garstang (1967), wherein they reported that pulsing the inlet air ow leads to enhancement of mass transfer. In recent years, some researchers have reported vibration of bubble columns as a possible means of improving the gasliquid contacting. Vibrating or shaken bubble columns have been shown to be advantageous over conventional bubble columns by reducing the mean bubble size (Ellenberger and Krishna, 2003a; Ellenberger et al., 2003), and enhancement of gas for the same overall operating conditions. Vibrations in the liquid phase at a frequency of 40120 Hz have been achieved by a vibration exciter (Ellenberger and Krishna, 2003b) and by an oscillating plate connected to the vibration exciter. These vibrations are generated by externally controlled vibration excitement devices. Consequently, an external energy input is required to generate vibration inside the bubble columns and also mechanical difculties associated with the moving parts are the main drawbacks of these vibrating bubble columns. In summary, a wish list of what one expects from internals in bubble columns can be listed as follows: low volume fraction of internals; high surface area of internals; no external energy input; high-throughput operation; minimum maintenance cost of internals and other bubble column hardware.

In this paper, one way of addressing some of the points raised in the above wish list is presented. Specically, use of simple springs as internals in bubble columns is proposed, with the underlying idea that vibrations in the springs caused by gas ow can be harnessed to modify the gasliquid contacting in the columns. The objective of the work is to experimentally study the effect of vibrating helical spring internals on gas holdup.

EXPERIMENTAL

A schematic diagram of the facility used in the present study is shown in Figure 1a. A bubble column made of Perspex was designed, fabricated, and erected for the measurements. The bubble column has an internal diameter of 15 cm and a height of 125 cm. Gas is sparged into a pool of liquid in the column through a gas distributor, which is a 1 cm thick perforated plate made of Perspex with 126 holes of 0.2 cm diameter each on a 1-cm pitch. The internals employed in this work can be characterized by their volume fraction and surface area of contact with the uid around them. The internals investigated in this work are essentially straight or coiled structures positioned vertically along the vertical axis of the bubble column, and xed at both ends. In one geometrical limit, they are straight vertical rods while in the other, they are coiled springs. In all that follows, the term internal is used to describe in general any such structure. For a given total volume occupied by internals, the surface area of the internals increases with decrease in diameter or thickness of the internals. However, there is a limit on thickness/diameter at which mechanical strength of the internal declines to such an extent that it cannot maintain its own structural integrity. Further decrease can make the internals collapse unless supported otherwise. As the internals thickness is reduced (they being xed at both ends), depending on their effective stiffness constant and damping coefcient, they can vibrate notably when subjected to a time-varying force eld. The amount of vibration (amplitude and frequency) rendered is a function of the nature of the time-varying

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Figure 1. Schematic diagram of bubble column with spring internals. a: Set-up; (b) helical spring holderisometric view; (c) helical spring internal holdertop view.

force eld, and modulating it for enhancing the bubble column reactor performance is desirable. In this work, the vibrating internals used are helical springs of different diameters and thickness. Vertical rod internals are also employed in the present study for the comparison purposes. Details of helical springs and vertical rods internals used in the study are given in Table 1. The helical spring internals are held in position with the help of holder as shown in Figure 1b,c. The spring holder consists of two circular rings, one at the base and other at the top, held in position by three tie rods. The circular rings are tted with wire mesh and the helical springs are supported at the nodal points of the wire mesh at the top and bottom. The number of circular rotation of the springs is kept constant, 105 rotation for all types springs. Similar to spring holder, rod holder consists of a skeleton of two circular rings supported by four tie rods. The circular rings are provided with supporting holders (2 cm diameter and 2 cm height) for location of a rod at the centre r/R = 0 and symmetric location of eight more rods at r/R = 0.5. Top and front views of the internals holders are shown in Figure 2.

Table 1. Details of internals used

Type of internals Springs (S1005)

Springs (S19005) Springs (S4005) Springs (S1901) Springs (S401) Rods (R19)

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Gas Holdup Measurement
Diameter of internals (cm) 1.0 1.9 1.9 1.9 1.9 4.0 4.0 1.9 1.9 4.0 1.9 1.9 Wire thickness (cm) 0.05 0.05 0.05 0.05 0.05 0.05 0.05 0.1 0.1 0.1 1.9 1.9 Number of internals 39 1 9 21 41 14 21 11 41 19 1 9 Volume fraction of internals 2.29 103 5.57 105 5.01 104 1.70 104 2.28 103 2.25 103 3.37 103 2.26 103 8.42 103 8.35 103 0.016 0.144 Spring constant (N/m) 20.82 0.68 1.15 1.4 0.41 0.63 11.13 1.98 2.15 0.65

In order to estimate the spring constant in the current work, a spring is suspended from a support as shown in Figure 3 and its unstretched (no-load) length is noted. Some known weight is added to one end of the spring. The spring stretches and comes into equilibrium at a length x beyond the springs unstretched length. The experiment is repeated for different loads. By measuring and plotting the spring force, F (=mg, where m is the mass loaded), against the extension in the spring, x, a straight-line graph with slope k. In the present analysis, the damping factor of the spring has been ignored. The natural frequency of vibration of the springs is determined by hanging a known weight and pulling the weights down and releasing them. A springs vertical motion in cycles per second is measured and the same experiment is repeated for different weights and the average natural frequency is determined. Spring constant and natural frequency of the springs employed in the present study are also listed in Table 1.

Saturated air is passed into a pool of water in the column through a calibrated orice meter. The system is operated at ambient con-

Natural frequency (Hz)

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Figure 2. Photographs of internals. (a) Top view of column with springs. (b) Top view of rod frame. (c) Front view of spring internals. (d) Front view of rod internals.

ditions. Saturated air from the blower is passed into a pool of water in the column through a calibrated orice meter. Height of liquid dispersion to diameter ratio (H/D) is varied from 2 to 5. Supercial gas velocity used in the present study ranged from 3.6 to 54.2 cm/s. At the higher gas velocities, there is some ambiguity in determining exactly the height of the expanded bed because the disengaging bubbles cause liquid splashing at the top, so that

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g = Hd H Hd

the top surface of the liquid is highly dynamic. To overcome this ambiguity, average dispersion height is taken into consideration, which is measured by noting the dispersion height at three different locations (located on the circumference of the column) and taking the average of the time averages at these locations. The time-averaged gas holdup (g ) is estimated by noting the height of dispersion Hd as a function gas ow rate for each clear liquid height H using the following equation: (1)

RESULTS AND DISCUSSION

Experiments are carried out for different internals and different operating parameters (supercial gas velocity and H/D ratio) in bubble columns, and the representative data of bubble columns without and with internals are presented for discussion.

Gas Holdup in Bubble Columns Without Internals

Figure 3. Schematic characterization of springs.

The gas holdup in bubble columns without internals is measured to benchmark the gas holdup of the bubble columns with internals. Here, the effect of supercial gas velocity and H/D ratio (height of the static liquid to column diameter ratio) on gas holdup is investigated. In the homogeneous bubbling regime, the size of the bubbles is entirely dictated by the sparger design and physical properties of the gasliquid phases. In contrast, in the heterogeneous regime the role of sparger design diminishes depending upon the column height. The total height of the liquid in the column is divided into two regions, the sparger region and the bulk region (Thorat et al., 1998). The size of the bubbles in the bubbly regime is totally dictated by the sparger (primary bubble size) and mainly depends on the sparger design. In the sparger (gas distributor) region, the size of the bubbles changes with respect to height

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Figure 4. Effect of supercial gas velocity on gas holdup for bubble column without internals.

depending upon the coalescence nature of the liquid phase (surface tension of liquid), the level of turbulence, and bulk motion (Thorat et al., 1998). At the end of the sparger region the bubble attains an equilibrium size referred by Thorat et al. (1998) as the secondary bubble size. The equilibrium bubble size is governed by the breaking forces due to bulk motion (turbulent and viscous stresses) and the stabilizing force due to surface tension. The height of the sparger region depends upon the difference between the primary and secondary bubble size, the coalescence nature of the liquid phase and liquid circulation in heterogeneous or churnturbulent regime. The relative proportion of the sparger region in the total column height decides the effect of H/D ratio on gas holdup. If the sparger region is small, the effect of H/D ratio on gas holdup is minimum, and vice versa (Thorat et al., 1998). In Figures 4 and 5, the effect of the supercial gas velocity and H/D ratio on gas holdup with internals is presented. The measured average gas holdup increases steadily with supercial gas velocity for all H/D ratios. With increase in H/D ratio gas holdup decreases to a limiting value, beyond which H/D ratio has negligible effect on gas holdup. Observation indicates for H/D 3, there is no perceivable effect on gas holdup. Thus, the role of the sparger region above H/D 3 is minimal. For comparison, the range of experimental data of Thorat et al. (1998) is shown on the same graph (Figure 4). It is clear that our experimental data also fall within the acceptable range. The experiments carried out in this work are repeated several times and the

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Gas Holdup in Bubble Columns With Internals Gas holdup in bubble columns with vertical rod internals (R19) Gas holdup in bubble columns with helical spring internals
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Figure 6. Effect of supercial gas velocity and H/D ratio on gas holdup for bubble column with vertical rod internals (number of rods = 9, diameter of each rod = 1.9 cm, total volume fraction of nine rods = 0.144).

maximum relative error is observed to be 5%. The moderate deviation in the gas holdup of the present study to the literature data of Thorat et al. (1998) can be ascribed to the fact that the column diameter used by Thorat et al. (1998) was 38.2 cm.

Effect of supercial gas velocity and H/D ratio on gas holdup for vertical rod internals (number of rods = 9, diameter of rod = 1.9 cm, total volume fraction of nine rods = 0.144) in bubble columns is shown in Figure 6. Similar to bubble columns without internals, the gas holdup increases with supercial gas velocity and decreases with H/D ratio to a limiting value for H/D 3. The data for various H/D ratios fall within the error range. The same observations regarding relative insensitivity of the measured holdup to H/D ratio were made with different numbers of rod internals. This fact was essential to establish so that data for average gas holdup using volume displacement method (Equation 1) can be taken with condence. Effect of volume fraction of vertical rod internals on gas holdup is shown in Figure 7. Clearly, the gas holdup increases substantially with increase in volume fraction of rod internals. A single vertical rod does not have much effect on gas holdup, when compared to a bubble column without internals. However, the enhancement in gas holdup is signicant for a higher number of internals (e.g., nine vertical rods), whence the internals signicantly reduce the cross-sectional area available for ow, resulting in higher interstitial gas velocity and promoting radial mixing and circulation of bubbles. This observation of higher gas holdup for internals due to the reduction in the cross-sectional area for ow was also reported by Yamashita (1987b) and Pradhan et al. (1991, 1993).

Figure 5. Effect of H/D ratio on gas holdup for bubble columns without internals.

Experiments are carried out for different helical spring internals and different operating parameters (supercial gas velocity and H/D ratio) in bubble columns and the representative data of bubble columns with helical spring internals and the amount of vibration of springs inside the bubble columns are presented here.

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Figure 7. Effect of volume fraction of internals on gas holdup for bubble column with rod internals (H/D ratio = 3, diameter of each rod = 1.9 cm).

Peak-to-peak displacement and frequency of vibrating spring internals. The motion of any simple harmonic oscillator (as the helical springs have been reasonably assumed to be) is characterized by two quantities: the amplitude and the time period (or frequency). The peak-to-peak displacement (two times of amplitude), the maximum upward (compressive) and downward movement (expansive) of the springs from a specic reference point, and the frequency of the vibrating springs (number of cycles per second) in the bubble columns are analysed by photographic imaging. Figure 8 shows the pictorial representation of peak-topeak displacement of the helical spring internals from a specic reference point. A reference point is a marking made to the one edge coil of the springs which is as close as to the wall. A camera (Silicon Graphics model: INDY CMNB0060) is focused at the reference point and used to measure the movement of the springs inside the column, and is interfaced with a computer. The camera acquires 30 frames per second, and IRISTM software is loaded for image processing. The camera records the vibration of the springs with respect to time for various supercial gas velocities. The time interval of the entire observation is 20 s. A frame-by-frame analysis is done using the IRISTM software to determine displacement

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and the frequency of the vibrating springs. The liquid height used for this study is 75 cm (H/D ratio = 5). When the bubble column is in operation, the springs are subjected to an external forcing function generated by the gas ow. Note that in stationary liquid the springs would not oscillate, and this periodic motion is brought about by the chaotic and random motion of the bubbles in the bubble column. The bubble motion involves a multitude of frequencies and this spectrum of frequencies serves to induce a multiple harmonics in the springs. In turn, these harmonics induce periodic motions (at various frequencies) in the liquid and indeed the two-phase (gasliquid) mixture. Thus, clearly, the coupling is two-way: gas ow induces vibrations in the springs at multiple frequencies, which in turn modulates the ow eld in the liquid, and through the drag and other interphase forces, the ow eld, and conguration of the gas phase. Earlier authors (e.g., Krishna et al., 2000; Krishna and Ellenberger, 2002; Ellenberger et al., 2005) have also highlighted the notion of external frequencies modulating the ow eld; however, in their case the external vibration source affects the ow eld, but the ow eld does not change the vibrations in any way (one-way coupling). In the present work, the coupling is two-way. In addition to the above effects, the spring internals play a role of physically chopping up the bubbles because of direct mechanical interaction with the gas phase as the bubbles make their way up the column. Note that this is in addition to the modulation of spring oscillations by the gas phase (gas bubbles), since that effect would have occurred even if the bubbles were rigid entities. The physical disintegration and redispersion of the bubbles by the internals is a complex phenomenon which clearly is an undertone to the present work. The effect of the external force (supercial gas velocity) on the amplitude and frequency of the springs of the type S19005 (springs made of 0.05 cm wire thickness and 1.9 cm diameter) is shown in Figure 9. This is typical for the behaviour of the spring internals in bubble columns studied in this work. The graph shows that the amplitude increases slowly in the supercial gas velocity range of 010 cm/s, following which there is a sharp increase of the amplitude in the range of 1036 cm/s. Further increase of the supercial gas velocity (beyond 36 cm/s)

Figure 8. Pictorial representation of peak-to-peak displacement of springs.

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Figure 9. Effect of supercial gas velocity on vibration displacement and frequency of the springs (number of springs = 41, diameter of springs = 1.9 cm, wire thickness = 0.05 cm).

has no signicant effect on the amplitude of the vibrating springs inside the bubble column. On the other hand, the frequencies of the oscillating spring are very high at the bubbly regime (gas velocities below 6 cm/s) then drop sharply in the supercial gas velocity range of 615 cm/s, then remain almost constant up to supercial gas velocity 36 cm/s, and then increase slowly with further increase in the supercial gas velocity. While clearly there is a multitude of frequencies involved in the process and the physics is quite complex and warrants a separate study under more controlled conditions of gas ow than what exist in a bubble column, one may still attempt to rationalize the observations of Figure 9 as follows. At low gas supercial velocities, the bubbling at the orice is a rapid process and each bubble is small and all bubbles are of fairly uniform size with minimal coalescence and redispersion. The kinetic energy associated with the gas ow is low, thus when this gas interacts with the springs they can only cause a small displacement in them and consequently low amplitude (Figure 9). Further, since the bubbles are rising in well-dened layers with a fairly uniform characteristic rise time, successive layers of bubbles interact at regular intervals with the springs resulting in a high frequency of vibration. Above a gas supercial velocity of 6 cm/s, we believe (based on visual observations and photography, though admittedly these images are not clear and it is hard to see through the wall) that coalescence sets into the bubble ensemble, and large bubbles begin to be formed as a result of this coalescence. This initiates larger displacements in the springs because of the presence of these large bubbles, which is shown in the sudden and steep rise in amplitude starting from about supercial gas velocity 10 cm/s. It seems that the range 610 cm/s is a transition regime in which this begins to occur. Associated with the formation of large bubbles, smaller bubbles are lost from the system so that the upward motion of bubbles is not as regular as it is at lower gas velocities. In other words, if one focuses attention on a single point along the spring internal, one does not see bubbles arriving at such a regular interval as one observe in bubbly regime. This causes a rapid drop in frequency as shown in Figure 9. Subsequently, as the typical characteristics of churn-turbulent regime properly establish themselves beyond a supercial gas velocity of 10 cm/s, the amplitude rises steadily as more and more large bubbles are formed and more kinetic energy is associated with the gas. We feel that in this regime in a bubble column with internals, there is no preference for any frequency and all

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Figure 10. Effect of supercial gas velocity and H/D ratio on gas holdup for bubble column with spring internals (number of springs = 41, diameter of springs = 1.9 cm, wire thickness = 0.05 cm, volume fraction of springs = 2.28 103 ).

frequencies are equally preferred in the gasliquid dispersion. In this white-noise scenario, the springs are perhaps forced by all frequencies uniformly so that the net frequency that is observable with the experimental techniques employed in this work limits us to observation of a fairly constant frequency. Note that it is in this region (discussed later) that the gas holdup tends to peak under all ow conditions. Beyond 36 cm/s, we would observe a fairly uniform gasliquid dispersion, which is stabilized on its own (based on the forces of interaction between the gas and the liquid phases), as well as the physical constraints put by the vessel dimensions. Thus, the amplitude, which is basically governed by the large bubbles in these conditions, levels off. Further increase in gas velocities adds to more bubbles of smaller sizes, hence a marginal and steady increase in frequency is observed. Effect of supercial gas velocity and H/D ratio of helical spring internals. Figure 10 shows the effect of supercial gas velocity and H/D ratio on gas holdup for 41 helical spring internals of the type S19005. Gas holdup increases with supercial gas velocity and decreases with H/D ratio. The gas holdup is seen to be higher at H/D ratio of 2 and decreases by 1012% as H/D ratio is increased from 3 to 5. This is due to the steady-state bubble size obtained at higher H/D ratio (>3) due to coalescence/dispersion (Thorat et al., 1998). Similar effect of supercial gas velocity and H/D ratio on gas holdup is observed for other helical springs differing in thickness of wire, helical spring diameter, and volume fraction of helical spring internals. Effect of volume fraction of helical spring internals. Effect of volume fraction of helical spring internals (i.e., number of springs) for S19005 on gas holdup for H/D ratio equal to 3 is shown in Figure 11. The numbers of helical springs used are 1 (volume fraction = 5.57 105 ), 9 (volume fraction = 5.0 104 ), 21 (volume fraction = 1.7 104 ) and 41 (volume fraction = 2.28 103 ). For comparison, data on bubble columns without internals are also included (where volume fraction of spring internals is zero). Gas holdup increases with increase in volume fraction of helical spring internals. For larger number of springs, it seems to go through a maximum around 20 cm/s gas supercial velocity, while the other trends seem to be monotonically increasing. At low volume fraction of internals, the main effect brought in by the springs is the acoustic vibration effect causing enhance-

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Figure 11. Effect of volume fraction of internals on gas holdup for bubble column with spring internals (H/D ratio = 3, diameter of springs = 1.9 cm, wire thickness = 0.05 cm, volume fraction of 1 spring = 5.57 105 , volume fraction of 9 springs = 5.0 104 , volume fraction of 21 springs = 1.7 104 , and volume fraction of 41 springs = 2.28 103 ).

ment of gas holdup because of the vibrations. This effect has been discussed by some earlier authors, notably in the paper of Ellenberger et al. (2005). Following the theory reported in that work, it can be argued that this enhancement of holdup stems from the Bjerknes force. The Bjerknes force arises because the existing gradient in pressure eld interacts with volume pulsations in bubbles, which in turn are created when bubbles are subjected to an acoustic pressure eld. Ellenberger et al. (2005) argue that along with drag, buoyancy and Bjerknes force lead to formation of standing pressure waves, at the antinodes of which the bubbles tend to accumulate leading to the enhancement of holdup. One may speculate here that similar phenomena occur in the present case as well. However, the situation is far more complex because unlike the case of Ellenberger et al. (2005), where in a given experiment the excitation frequency was kept constant, in the present case there is a spectrum of frequencies emanating from the complex interactions of the gas bubbles and the springs. Thus, one expect many antinodes to form based on the harmonics, or rather a diffuse region in the bubble column where enhancement of holdup occurs. As the volume fraction of the internals is increased, the above effect is enhanced. At higher volume fractions, say for the case 41 springs, in addition to the effect discussed earlier, an effect of steric hindrance also becomes important. Because of the physical obstruction of the rising bubbles and the ensuing chopping action, the larger bubbles are broken into small bubbles due the vibrating springs and their close packed conguration. The springs do not allow the larger bubbles to escape freely and breaks them into smaller entities. The increase (or enhancement) in the gas holdup for 41 helical springs (p = 2.285 103 ) is as much as 135% at a gas velocity of 7 cm/s when compared to the bubble columns without internals, at the same gas supercial velocity. Similar effect on gas holdup for various volume fractions of helical spring internals is observed for S4005 and S1901 type helical spring internals. The enhancement of gas holdup is calculated by gas holdup of bubble column with helical spring internals divided by the gas holdup of bubble column without internals. The enhancement of the gas holdup for bubble column with spring internals (S19005, 41 springs) is 2.3 times than the bubble column without internals at supercial gas velocity 14 cm/s as shown in Figure 12. The enhancement

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Figure 12. Effect of supercial gas velocity on percentage enhancement in gas holdup for bubble column with spring internals (number of springs = 41, diameter of springs = 1.9 cm, wire thickness = 0.05 cm, volume fraction of springs = 2.28 103 ).

of gas holdup increases rapidly up to supercial gas velocity of 14 cm/s and then decreases gradually at higher supercial gas velocity. In line with our earlier arguments, around 1214 cm/s the formation of larger bubbles by coalescence is just initiated, and all bubbles are of small size and occupy the entire column. Visual observation of the column under these conditions reveals a froth-like gasliquid suspension (even though it was ensured that the system is clean prior to the experiment, hence negating the possibility of any stray surfactants), almost occupying the entire column. As the velocity is further increased, the steady-state coalescence rate picks up (even with the spring internals present) and larger bubbles are formed. These bubbles rise quicker, thus the enhancement is gas holdup is reduced. In summary, one may argue that the presence of the spring internals effectively delays the transition from bubbly to churn-turbulent ow regime (i.e., the transition occurs now at a higher gas supercial velocity), and also enhances the average gas holdup at any given gas supercial velocity. Effect of diameter of helical spring internals. The earlier sub-section described the effect of overall volume fraction of the springs on the gas holdup, without any direct reference to the

Figure 13. Comparison of gas holdup for bubble column with different diameters of spring internals and nearly equal volume fractions = 2.3 103 (wire thickness = 0.05 cm, H/D ratio = 3).

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Author Proof

Figure 14. Comparison of gas holdup for bubble column with different wire thickness of spring internals and nearly equal volume fractions = 2.3 103 (diameter of helical springs = 1.9 cm, H/D ratio = 3).

geometry (diameter, pitch, and wire thickness) of the springs. Figure 13 compares the gas holdup observed with helical springs made of different spring diameters (wire thickness of springs being constant at 0.05 cm and H/D ratio of unexpanded bed being xed at 3). Experimental observations indicate that gas holdup is maximum for 1.9 cm diameter helical springs when compared to the 4 and 1 cm diameter helical springs. The 4 cm helical springs provide enough space for the larger bubbles to escape without breakage while that is not the case in bubble column with 1.9 cm springs. The 1 cm helical springs are too rigid (spring constant = 20.82 N/m) and do not vibrate as compared to 1.9 cm helical springs. Higher gas holdup for 1.9 cm springs is due to lower stiffness (spring constant = 0.68 N/m) of 1.9 cm springs over 4 cm (spring constant = 0.41 N/m) and 1 cm springs. Similar effect of maximum gas holdup with good bubble breakage is observed for springs of type S1901 as compared to S401. These observations also corroborate our hypothesis that both the vibration in the springs as well as the steric hindrance offered by them to the bubbles determine the average bubble size and hence the nal gas holdup. Effect of thickness of helical spring wires. Figure 14 compares the gas holdup as a function of wire thickness (for equal spring diameter and H/D ratio of 3). Gas holdup is higher for 0.05 cm wire diameter springs than the 0.1 cm wire diameter

Table 2. Comparison of gas holdup for bubble columns with internals Uog = 7 cm/s g

Refs.

Patil et al. (1984) Yamashita (1987a) Pradhan et al. (1991) PradhanQ2 et al. (1994) Urseanu et al. (2001) Birrer and Bohm (2004) Present work (S19005, 41 Springs)

g,i , gas holdup with internals; g , gas holdup without internals.

A
Uog = 18 cm/s g Uog = 35 cm/s g g , i % increase 10.0 38.5 27.3 36.4 38.5 12.5 135.7 g ,i % increase g,i 0.11 0.18 0.14 0.15 0.18 0.18 0.33 0.10 0.13 0.11 0.11 0.13 0.16 0.14 0.27 0.22 22.7 0.35 0.3 0.25 0.29 0.52 0.24 0.23 0.24 4.2 26.1 116.7 0.35 0.34 0.53 0.33

Figure 15. Comparison of gas holdup for bubble column with helical spring internals with vertical rod internal internals (H/D ratio = 3, total volume fraction of internals = 2.3 103 ).

springs, since 0.05 cm wire diameter helical springs vibrates better due to their lower spring constant. The 0.1 cm thickness wire is too rigid (spring constant = 20.82 N/m), that is higher spring constant and vibrates less than the 0.05 cm thickness wire. Vibration of helical springs breaks the larger bubbles into smaller ones and increases the gas holdup. It is clear from the above observations that the stiffness of the springs as well as their physical dimensions (diameter, thickness of wire) plays an important role in determining the local hydrodynamics and the gas holdup. Also the packing or volume fraction (number) of springs play an equally, if not more, important role in providing steric limitations to the bubbles and causing them to disintegrate, thus limiting their size. Comparison of helical spring and vertical rod internals. Figure 15 compares gas holdup for helical springs with vertical rod internals. Volume fraction of one vertical rod and helical springs (S19005, 41 springs) used are 16 103 and 2.25 103 , respectively (Table 1). The maximum possible number of helical springs that can be placed/positioned in the spring holder is 41. It can be seen that even a single thin rod has a volume fraction of 16 103 and results in a much lower enhancement in holdup compared to any of the spring internals. Reasons for this are twofold. First, in terms of providing steric hindrance to the passage of bubbles and hence limiting their size, the rods are practically ineffective because they do not change the cross-sectional area through which bubbles rise, appreciably. In terms of vibrations, too, the

% increase

16.7

2.9

60.6

Bold and underlined values indicate maximum gas holdup achieved for the respective supercial gas velocity using different internals by the authors.

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single rod is too stiff and hence its motion is essentially unmodulated by the passing gas (whose kinetic energy is too low to induce any vibrations in the rod). Thus, clearly the springs occupy less space inside the bubble columns and also lead to higher gas holdup than vertical rods. The message is that internals of regular shape, like rods, enhance gas holdup only to a limited extent while the use of potentially vibrating internals (like springs) would signicantly enhance their potential. This is shown through a comparison of the literature gas holdup with the present work in Table 2. It can be seen clearly from the table that the present helical spring internals are far better choice of internals compared to any other internals used in the literature. The increase of gas holdup is around 135% for 7 cm/s, while the maximum reported gas holdup at this supercial gas velocity is only 38.5%.

Author Proof
NOMENCLATURE

CONCLUSIONS

One of the holy grails of bubble column research has been to obtain high gas holdups at high gas uxes. In conventional bubble columns (either empty or with conventional internals like rods), these two requirements are contradictory. This is because as gas ux (supercial gas velocity) is increased, it leads to coalescence forming larger bubbles which have in general a lower residence time and higher rise velocity. Consequently, while the increase of gas ow leads to increase in holdup, the enhancement is not proportional and indeed it tends to level off at high values of gas ux. The experimental results presented in this paper indicate that the vibrating structures like springs have a strong potential for use as internals in industrial bubble columns. The results indicated that at supercial gas velocities of around 12 cm/s, the percentage enhancement of gas holdup is around 230%. Even at higher throughput of gas, the percentage enhancement of gas holdup is more than 150% for supercial gas velocity 40 cm/s. Industrially, the current trend is to use bubble columns at higher gas throughputs, so the presented results indicate a promising option for industrial practitioners to harness high gas holdups are high gas uxes. It is also clear that the geometry, material of construction, and properties of the spring internals have a marked effect on their role in holdup enhancement. The experimental observations indicate that gas holdup is maximum for 1.9 cm diameter helical springs compared to the 4 and 1 cm diameter helical springs. Gas holdup is higher for 0.05 cm wire diameter springs than the 0.1 cm wire diameter springs, all other parameters being constant. This point clearly needs further investigation and is a topic of ongoing research in our group. The helical spring internals satises the wish list as one expects from internals in bubble columns are low volume fraction of internals, high surface area of internals, no external energy input, high-throughput operation, and minimum maintenance cost of internals and other bubble column hardware. Fact is that in spite of its good points, such ne structures like springs (which seem so promising in cold ow experiments) will either be inadequate for purposes of heat transfer (for instance, it is difcult to envision that the tubes which carry a heat transfer uid to be so ne that they can also serves the cause of being vibrating structures). However, the point we wish to highlight through our contribution is the importance of vibrating structures in enhancing gas holdup, not necessarily springs. Any other vibrating or exible structure (not necessarily a simple harmonic oscillator like a spring) would also serve to enhance the gas holdup, albeit our understanding of structures whose oscillation

A
END NOTES
Please refer to Table 1 for listing of various internals used.

frequencies may have multiple modes may be more limited as compared to a humble spring. An alternate suggestion may be to have microtubes which can double up as springs, much as the contemporarily prevalent idea of microheat exchangers. These would be designed to provide the same heat transfer area offered by the conventional bubble column heat exchanger tubes by adjusting the number of (vibrating) microtubes. To make such concepts operational and realizable, the material of construction of the vibrating microtubes would be very important. Clearly, this is going to be a challenge for material scientists, since the microstructures should have corrosion and erosion resistance offered by the sometimes harsh environment of a industrial bubble column.

D column diameter (m) F force exerted by a spring (N) H static liquid height (m) Hd liquid dispersion height (m) k spring constant (N/m) r radial coordinate R radius of the rod holder (m) Uogsupercial gas velocity (m/s) x displacement of the end of the spring from its equilibrium position (m) g gas holdup

REFERENCES

Baird, M. H. I. and J. H. Garstang, Power Consumption and Gas Hold-Up in a Pulsed Column, Chem. Eng. Sci. 22, 16631673 (1967). Dautzenberg, F. M. and M. Mukherjee, Process Intensication Using Multifunctional Reactors, Chem. Eng. Sci. 56, 251267 (2001). Deckwer, W. D., Bubble Column Reactors, Wiley, Chichester (1992). DeckwerQ3 , W. D. and A. Schumpe, Bubble ColumnsThe State of Art and Current Trends, Int. Chem. Eng. 27, 405422 (1987). Deckwer, W. D. and A. Schumpe, Improved Tool for Bubble Column Reactor Design and Scale-Up, Chem. Eng. Sci. 48, 889911 (1993). Ellenberger, J. and R. Krishna, Shaken, Not Stirred, Bubble Column Reactors: Enhancement of Mass Transfer by Vibration Excitement, Chem. Eng. Sci. 58, 705710 (2003a). Ellenberger, J. and R. Krishna, Intensication of Slurry Bubble Columns by Vibration Excitement, Can. J. Chem. Eng. 81(34), 655659 (2003b). Ellenberger, J., J. M. van Baten and R. Krishna, Intensication of Bubble Columns by Vibration Excitement, Catalysis Today 7980, 181188 (2003). Ellenberger, J., J. M. van Baten and R. Krishna, Exploiting the Bjerknes Force in Bubble Column Reactors, Chem. Eng. Sci. 60, 59625970 (2005). Fair, J. R., A. J. Lambright and J. W. Anderson, Gas Holdup in Sparged Contactors, Ind. Eng. Chem. Proc. Des. Dev. 1, 3336 (1962).

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Fan, L. S., GasLiquid Solid Fluidization Engineering, Butterworth-Heinemann, Boston (1990). Koide, K., Design Parameters of Bubble Column Reactors With and Without Solid Suspensions, J. Chem. Eng. Jpn. 29, 745759 (1996). Kolbel, H. and M. Ralek, The Fischer Tropsch Synthesis in the Liquid Phase, Catalysis Rev. Sci. Eng. 21, 255274 (1980). Krishna, R. and J. Ellenberger, Improving GasLiquid Mass Transfer in Bubble Columns by Applying Low-Frequency Vibration, Chem. Eng. Technol. 25, 159162 (2002). Krishna, R., J. W. A. de Swart, J. Ellenberger, G. B. Martina and C. Maretto, Effect of Column Diameter and Slurry Concentrations, Am. Inst. Chem. Eng. J. 33, 311316 (1997). Krishna, R., J. Ellenberger, M. I. Urseanu and F. J. Keil, Utilization of Bubble Resonance Phenomena to Improve GasLiquid Contact, Natureissenschaften 87, 455459 (2000). Lunin, G., L. Lamarree and K. Whitman, Paper Presented at the UNITAR Third International Conference Heavy Crude and Tar Sands, Long Beach, CA, July 1985, pp 2231. Pandit, A. B. and Y. K. Doshi, Mixing Time Studies in Bubble Column Reactor With and Without Internals, Int. J. Chem. React. Eng. 3(A22), 125 (2005). Patil, V. K., J. B. Joshi and M. M. Sharma, Sectionalized Bubble Column: Gas Holdup and Wall Side SolidLiquid Mass Transfer Coefcient, Can. J. Chem. Eng. 62, 228232 (1984). Pradhan, A. K., R. K. Parichha and P. De, Flow Behavior and Gas Holdup in Two-Phase Bubble Column, Inst. Eng. (India) 72, 69 (1991). Pradhan, A. K., R. K. Parichha and P. De, Gas Holdup in Non-Newtonian Solutions in a Bubble Column With Internals, Can. J. Chem. Eng. 71, 468471 (1993). Saxena, S. C., Bubble Column Reactors and Fischers-Tropsch Synthesis, Cat. Rev. Sci. Eng. 37, 227309 (1995). Shah, Y. T., B. G. Kelkar, S. P. Godbole and W. D. Deckwer, Design Parameter Estimations for Bubble Column Reactors, Am. Inst. Chem. Eng. J. 28, 353379 (1982). Tarmy, B. L., M. Chang, C. A. Coulaloglou and P. R. Ponzi, The Three Phase Hydrodynamic Characteristics of the EDS Coal Liquefaction Reactors: Their Development and Scale-Up, Proceedings of the Eighth International Symposium on Chemical Reaction Engineering, Elsevier Scientic, NY 1984. Thorat, B. N., A. V. Shevade, K. N. Bhilegaonkar, R. H. Aglawe, U. Parasu Verra, S. S. Thakre, A. B. Pandit, S. B. Sawant and J. B. Joshi, Effect of Sparger Design and Height to Diameter Ratio on Fractional Gas Holdup in Bubble Columns, Trans. Inst. Chem. Eng. 76(Part A), 823834 (1998). Wild, G., S. Poncin, H. Z. Li and E. Olmos, Some Aspects of the Hydrodynamics of Bubble Columns, Int. J. Chem. React. Eng. 1(Review 7), 136 (2003). Yamashita, F., Effect of Liquid Depth, Column Inclination and Bafe Plates on Gas Holdup in Bubble Columns, J. Chem. Eng. Jpn. 18, 349353 (1985). Yamashita, F., Effect of Shape of Bafe Plates and Mesh and Cross Sectional Area of Wire Gauzes on Gas Holdup and Pressure Drop in a Bubble Column, J. Chem. Eng. Jpn. 20, 201204 (1987a). Yamashita, F., Effect of Vertical Pipes and Rod Internals on Gas Holdup in Bubble Columns, J. Chem. Eng. Jpn. 20, 204206 (1987b). Manuscript received April 22, 2009; revised manuscript received January 10, 2010; accepted for publication January 11,

2010.

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Q1: Please add Joshi and Shah (1981) in the reference list. Q2: Please add Pradhan et al. (1994), Urseanu et al. (2001), Birrer and Bohm (2004) in the reference list. Q3: Please cite the following references in the list: Deckwer and Schumpe (1987), Krishna et al. (1997), Saxena (1995), Yamashita (1985).

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