1.

Introduction Multiphase reactors are encountered in several industrial processes, for instance, in the chemical, biochemical, environmental, pharmaceutical, or petrochemical industries and are therefore of practical importance. Among multiphase reactors, bubble columns are widely used for several reasons: simple construction (no mechanically moving part), low maintenance cost, good mass and heat transfer [1]. Gasliquid systems and bubble columns are of paramount importance to the chemical process industry and the dynamics of these systems have been researched extensively. However, still now the lack of accurate relationships for the gasliquid interfacial forces makes it difcult to simulate the uid dynamics of this type of equipment with condence [2]. In the modelling of dispersed two-phase ow, a correct modelling of the inter-phase forces is needed to represent the momentum transfer between the phases. This usually consists of simple correlations for the forces acting on a single uid particle in an innite medium, which are derived either empirically or theoretically, and that can be extended to very dilute dispersed system.

Industrial processes are normally carried out at higher phase fractions, where the mutual inter- action among the uid particles has a signicant inuence. Hence, it is the objective of this study to identify the effect of the inter-particle interaction on the drag force acting on a bubble in a gasliquid system [2]. The knowledge of the closure terms in the NavierStokes equations such as the turbulence Reynolds stresses or the interaction forces between the bubbles and the liquid phase: drag, lift, added mass, or Basset forces. To close these last terms, empirical correlations giving drag or lift coefcients for an isolated bubble rising in a quiescent liquid are generally used. But many authors emphasize the fact that those coefcients are no more appropriate as soon as the bubble is surrounded by other bubbles [1]. For solid particles the drag coefcient depends only on the characteristics of the ow surrounding the particle and it is primarily a function of the particle Reynolds number and of the turbulence intensity of the

continuous phase. In the case of uid particles, the drag coefcient is also dependent on other uid properties, which are characterized by Etvs number, determining the ratio between gravitational

..................................................................................... uid surrounding the bubble:

(1)

and Morton number, which involves only the physical parameters of the

...................................................................................... As well as on the ratios of uid densities and viscosities [2]. 1.1 Topic Description

(2)

This paper tries to explore the information about the effects of drag coefficient and the momentum transfer process in a swarm of bubbles based on the work of Simonnet et al [1], Bertola et al [2] and Nguyen-Van et al [3]. The topics that shall be discussed in this report includes the experimental variation of the drag coefficient with the local void fraction, the behaviour of a swarm of bubbles under conditions similar to those accurring in the bubble columns operating in the homogenous regime (i.e., at low gas flow rate).

2. Overview 2.1 Creeping Flow Of Liquid Near The Bubble Surface In The Bubble Swarm For the creeping flow regime of bubbles, the solution to the Navier-tokes equations for the stream function of fluid flow is given generally. .............................................................. the relationship between r and gas holdup can be derived as follows: ........................................................... (4) where Nis the actual number of bubbles in the pulp phase of volume Vcell, (3)

For a swarm of bubbles, the radius of the outer boundary is finite and

R is the dimensional radius of the outer boundary, and Vgas is the volume of the gas phase actually present in the pulp phase. By using the expressions given in Eq. (3) and (4), the radial component of water velocity near the bubble surface is reduced into the following form [3]: ................................................................ (5) where ................................................. (6) 2.2 Flow of Liquid Near The Bubble Surface at The Intermediate Reynolds Number of Bubble in The Bubble Swarm The water flow pattern near the bubble surface in this case is quantified by using the results of numerical solution to the Navier-Stokes equations. Like the results of the semi-analytical solution to the NavierStokes equations for fluid flow around a single rigid sphere, the dimensionless vorticity at the surface of the front hemisphere of a bubble in this case can be estimated by: (7) where the parameters Xand Y are obtained by using a curve-fitting technique and least-square method: ........................... (8a) . (8b) where is given in fraction up to 0.30. The surface vorticity given by Eq. (7) is in agreement with that from the numerical solution of the Navier-Stokes

equations (e.g. LeClair, 1970). It is also known from fluid-dynamics (Krasnov, 1985) that .. (9a) . (9b) where V is the Laplacian operator. Eq. (9b) is the continuity equation.

Recognizing that when the dimensionless tangential liquid velocity wo= 0 at

the bubble surface, the expansion of velocity in a Taylor series reads:

the dimensionless

tangential

liquid

(9c) where = r- 1. The velocity wr can be obtained by using Eqs. ( 9a ) - ( 9c ). The result is simplified by using the polar spherical system of coordinates and Eq. (7) for surface vorticity: (10) It is obvious that when Re= 0 the radial velocity of water flow near the bubble surface given by Eq. ( 10 ) is identical with that described by Eq. (5) [3].

2.3 Bubble velocity The bubble velocity is calculated by inter-correlating the signal obtained from the rst probe to that emitted by the second probe. The maximum of the inter- correlation function corresponds to the most likely residence time of bubble between the two probes. Dividing the vertical distance separating the probe tips by this time gives the mean vertical bubble velocity. Vg has been checked by comparison with the more precise results obtained with a high-speed cam- era; uncertainty found was about 15% [1]. 2.4 Bubble equivalent diameter The average cut chord length of a bubble crossing the dual optical probe can be calculated from ... (11) Eq. (7) is based on a statistical calculation of the mean vertical chord of an ellipsoidal object. From the analysis of pictures obtained with the high-speed camera, in the range of bubble diameters studied, the ratio E between the vertical and horizontal bubble diameter is found to be constant and approximately equal to 0.6. This aspect ratio is comprised between the values obtained in pure water and the ones measured in contaminated media (Clift et al., 1978). The knowledge

of E and of the vertical diameter nally leads to the mean volume equivalent diameter of the bubble [2]: (12)

2.5 Determination of the mean relative velocity and the drag coefficient The knowledge of the bubble velocity, measured by the optical probe, and the liquid velocity, measured by LDV, allows the calculation of a mean bubble relative velocity by .............................................................................. (13) The relative velocity is thereby a local value with respect to space and a mean value with respect to time. In commercial CFD codes, the buoyancy expression is based on the pressure gradient, and includes consequently the modication of the continuous phase apparent density due to the bubble presence. Equilibrium between the buoyancy and drag forces in the axial equation of momentum conservation leads to the drag coefcient: .................................................................... (14) Expression (13) shows that to take the inuence of surrounding bubbles into account, the corrective term (1 loc) is needed in the drag formulation compared to the isolated bubble case. This drag coefcient, based on local time averaged values of the void fraction, of the dispersed phase diameter and of the gas and liquid velocities, should improve CFD prediction of bubble column hydrodynamics; in particular, for the simulation of the heterogeneous regime, where local inhomogeneities govern the ow [2].

3. Momentum Transfer and Effect of The Drag Coefficient in a Swarm of Bubble 3.1 Rise of a Single Bubble To evaluate the quality of the VOF predictions applied to a gasliquid system, at rst we have simulated the rise of a single bubble of air in quiescent water. A bubble of diameter de moves in a vertical cylinder of diameter 5de and height 8de . In order to mimic a reference frame moving with the bubble, water is fed downwards from the top of the cylinder. Since the bubble and its wake should remain in the computational domain during the simulation, the inlet velocity ofthe water has been set close to the bubble terminal velocity; the proper value has been determined by trial and error. These simulations have been performed by means of the code Fluent (version 6.0), using an unstructured grid. Different grid sizes have been tested; the number of cells used to characterize the bubble was varied. Up to a value of250 cells/bubble the results continue changing increasing the grid density; over 250 cells/bubble the difference in the results increasing the grid resolution becomes very small. A grid density that allowed 300 cells/bubble was thus chosen in or- der to be close to the grid independence condition. The time step adopted was 105 s for all the simulations. No differences were found with simulations performed with smaller time steps. With this set of the parameters of simulation, the loss of volume of the bubble at the end of the calculations was always below 1%. The results showed that the simulations are capable of capturing the main features of the bubbles of the considered size range, such as the ellipsoidal shape and the oscillations both in shape and in trajectory. For instance, Fig. 1 plots velocity components vs. time for a 4 mm bubble with counter- current water at 20 cm/s. The graph indicates the occurrence of a zigzagging motion, typical of the considered size. Fig. 2 shows the evolution of the bubble shape and the velocity vectors. The obtained bubble shape (ellipsoidal) is in agreement with the one expected based on the experimental observation.

Fig. 1 Velocity vs Time for a 4 mm Bubble of air in clean water (at vertical axis; x, y; horizontal axis)

Fig. 2 Four milimetre air bubble in water flowing downwards at; 20 cm/s; frames at a time step of 0.i s A more detailed evaluation of the simulations can be obtained from the predicted terminal velocities. For air bubbles larger than 1.3 mm rising in clean water, the following experimental phenomenon: relationship describes accurately the

................................................. (15) Where is the surface tension, de the equivalent diameter of the bubble and the bubble/cylinder ratio (0.2 in our case). The rst factor is known to predict

accurately the terminal velocity in an unbounded uid; the second one is a corrective term for the wall effect in the simulated cylinder. Fig. 3 compares Eq. (15) with the results of our simulations, indicating good agreement. This conrms the ability of computational uid dynamics to simulate effectively such a system.

Fig. 3 Comparison between the terminal velocity predicted by CFD simulation, squares, and Eq. (15), continuous line.

3.2 Rise of a swarm of bubbles The swarm of bubbles has been modelled as a periodic repetition of identical cells, each one containing a single particle. The simulations have been carried out in 3D domains. The domain is a cubic box with periodical boundary conditions on each face. In this way the bubble goes out of the domain on one side, and it comes back in the domain again from the opposite side. Considering as one of the variables of the system, the periodical boundary conditions are implemented in the following way:

................................................................................... (16) The size of the domain L has been calculated from the bubble diameter in such a way as to obtain the desired hold-up value = /6 (de / L)3 . The computational domain has 53 cells in each direction; the number has been kept constant for every condition investigated. This means that even at the smallest considered hold-up (0.5%) the bubble includes approximately 600 cells, while at the largest hold-up (5%) it includes about 6000 cells. At the beginning of the simulations a spherical bubble has been placed in the centre of the domain and its

evolution due to gravity has been calculated. The slip velocity in the vertical direction has been evaluated as the difference between the domain-averaged gas and liquid velocities, Uslip = Ugas Uliq . The drag coefcient is evaluated by the following relationship, obtained from considering a balance of forces on the bubble in steady conditions of ow: ..................................................................... (17) In our simulations bubbles do not normally reach a constant slip velocity, because of the onset of zigzagging or spiralling motion. In this case an effective value of drag coefcient has been evaluated, based on the time averaged vertical slip velocity. The analysis has been applied to the airwater system and to a gas hydrocarbon system.

3.3 Relative velocity of bubbles: influence of the void fraction In Fig. 4, the inuence of the local void fraction on the relative velocity of bubbles is shown (133 capillaries fed and Jl = 9cm/s). This variation exhibits two distinct behaviors. First, for a local void fraction less than a critical value, crit around 15%, the relative velocity decreases slowly when the void fraction increases. For such conditions, the relative velocity is below the velocity of an isolated bubble with the same diameter correlation (17) with the bubble diameter from Fig. 5). (calculated from

................................................................................. (17)

Fig. 4 Bubble Relative Velocity vs Local Void Fraction

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Fig. 5 Local Bubble Diameter vs Local Void Fraction This means that for loc < crit , measurements integrate the well-known hindrance effect caused by the presence of other bubbles in the surrounding. This decrease can also be related to the turbulent intensity of the liquid phase which can reduce the bubble velocity up to 50% in comparison to that in quiescent liquid (this phenomenon has been observed when bubbles are located behind a grid generating homogeneous and isotropic turbulence). This can be linked to the fact that these authors report smaller bubble sizes for high void fractions, than the sizes obtained with our injection conguration, leading to an enhanced hindrance effect. But this decreasing variation can be perfectly tted by correlation (18) in a swarm of 5 mm diameter bubbles. ................................................................ (18) Secondly, for loc > crit, the variation of relative velocity presents a sudden change: it increases rapidly with the local void fraction and becomes much greater than V . This increase is mainly due to three main effects:

coalescence of bubbles; aspiration of bubbles in wakes of the preceding ones leading to a rapid acceleration; and the turbulence induced by bubbles.

3.4 Drag Correlation The previous measurements allow to propose a new correlation describing the bubble relative movement over a wide range of void fractions. From the values of loc , Vrel and db obtained previously, the drag coefcient can be

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calculated (see Eq. (14)). Its variation with the local void fraction is shown in Fig. 6 for the 133 capillaries conguration and all the values of Jl imposed.

Fig. 6 Bubble Drag Coefficient vs. Local Void Fraction The drag coefcient obviously presents an opposite trend with the local void fraction, compared to the one of the relative velocity (Eq. (14)): it increases until crit and decreases beyond. The tting of this experimental curve let us obtain a new drag correlation, function of the local void fraction and of the mean bubble diameter (Table 1). Table 1. Drag Coefficient in a air bubbles in pure water

Finally, to drive the simulation of a bubble column under industrial conditions, where gas distribution systems are often such that bubble diameters are greater than 7 mm for loc > 15%, the following drag correlation can be used for the airpure water system: ........................................ (19) It is valid for bubble diameters ranging from 5 to 10 mm (on condition that db > 7 mm for loc > 15%) and local void fraction less than 30%. The exponent m is chosen in such a way that the transition between the increasing and decreasing drag coefcient occurs for a given crit . For instance, Fig. 6 shows data

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with m = 25, which lead to crit = 15%.

4. Final Remark The case of a single air bubble rising in quiescent water has been considered in order to dene the correct simulation conditions and to validate the VOF approach for this application. Different bubble dimensions, corresponding to different shape and ow regimes, have been considered in the range between 2 and 10mm of diameter. The bubble terminal velocity, the shape and the rising path of the bubbles have been compared with data available in the literature, and the comparison showed good agreement. In addition the simulations indicate that the effect of the swarm is to shift the transition between the non-oscillating and the oscillating regime towards larger bubble size (about7mm vs. 1.3mm for a single bubble). This phenomenon could have implications on mass transfer as well. The experimental study of the relative velocity in a swarm of bubbles has been carried out. It has led to the determination of the inuence of the local void fraction on the bubble relative velocity. For bubble diameters larger than 7mm,it is found that, for a gas holdup lower than a critical value near 15%, the relative velocity is subjected to the hindrance effect and decreases when the void fraction increases. Beyond this critical value, the aspiration in the bubbles wakes results in an increasing relative velocity with the local void fraction. The role played by the bubble diameter in these variations is determined by keeping it constant (modication of the number of capillaries aerated) and varying the void fraction. Most of the papers dealing with this subject have measured a decreasing relative velocity when the void fraction increases, whatever its value, provided that the bubble diameter was smaller than 7mm. This phenomenon has been checked hereby experiments performed in presence of butanol, but would need to be investigated for a pure waterair system.

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5. References 1. M. Simonnet, C. Gentric, E. Olmos, N. Midoux; Experimental determination of the drag coefcient in a swarm of bubbles, France. 2006. 2. Francesco Bertola, Giancarlo Baldi, Daniele Marchisio, Marco Vanni; Momentum transfer in a swarm of bubbles: estimates from uid -dynamic simulations, Italy. 2004. 3. Nguyen-Van, A. and Kmet, S., 1992. Probability of collision between particles and bubbles in flotation: the theoretical inertialess model

involving a swarm of bubbles in pulp phase, Slovak Republic. 1993.

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