Investigations on hydrodynamics and mass transfer in gas–liquid stirred reactor using computational fluid dynamics

In this work, the hydrodynamics and mass transfer in a gas–liquid dual turbine stirred tank reactor are investigated using multiphase computational fluid dynamics coupled with population balance method (CFD–PBM). A steady state method of multiple frame of reference (MFR) approach is used to model the impeller and tank regions. The population balance for bubbles is considered using both homogeneous and inhomogeneous polydispersed flow (MUSIG) equations to account for bubble size distribution due to breakup and coalescence of bubbles. The gas–liquid mass transfer is implemented simultaneously along with the hydrodynamic simulation and the mass transfer coefficient is obtained theoretically using the equation based on the various approaches like penetration theory, slip velocity, eddy cell model and rigid based model. The CFD model predictions of local hydrodynamic parameters such as gas holdup, Sauter mean bubble diameter and interfacial area as well as averaged quantities of hydrodynamic and mass transfer parameters for different mass transfer theoretical models are compared with the reported experimental data of [Alves et al., 2002a] and [Alves et al., 2002b] . The predicted hydrodynamic and mass transfer parameters are in reasonable agreement with the experimental data.     

Quantifying sub-grid scale (SGS) turbulent dispersion force and its effect using one-equation SGS large eddy simulation (LES) model in a gas–liquid and a liquid–liquid system

The one-equation SGS LES model has shown promise in revealing flow details as compared to the Dynamic model, with the additional benefit of providing information on the modelled SGS-turbulent kinetic energy (Niceno et al., 2008). This information on SGS-turbulent kinetic energy (SGS-TKE) offers the possibility to more accurately model the physical phenomena at the sub-grid level, especially the modelling of the SGS-turbulent dispersion force (SGS-TDF). The use of SGS-TDF force has the potential to account for the dispersion of particles by sub-grid scale eddies in an LES framework, and through its use, one expects to overcome the conceptual drawback faced by Eulerian–Eulerian LES models. But, no work has ever been carried out to study this aspect. Niceno et al. (2008) could not study the impact of SGS-TDF effect as their grid size was comparable to the dispersed bubble diameter. A proper extension of research ahead would be to quantify the effect of sub-grid scale turbulent dispersion force for different particle systems, where the particle sizes would be smaller than filter-size. This work attempts to apply the concept developed by Lopez de Bertodano (1991) to approximate the turbulent diffusion of the particles by the sub-grid scale liquid eddies. This numerical experimentation has been done for a gas–liquid bubble column system (Tabib et al., 2008) and a liquid–liquid solvent extraction pump-mixer system ( [Tabib et al., 2010] and [28] ). In liquid–liquid extraction system, the organic droplet size is around 0.5 mm, and in bubble columns, the bubble size is around 3–5 mm. The simulations were run with mesh size coarser than droplet size in pump-mixer, and for bubble column, two simulations were run with mesh size finer and coarser than bubble diameter. The magnitude of SGS-TDF values in all the cases were compared with magnitude of other interfacial forces (like drag force, lift force, resolved turbulent dispersion force, force due to momentum advection and pressure). The results show that the relative magnitude of SGS-TDF as compared to other forces were higher for the pump-mixer than for the coarser and finer mesh bubble column simulations. This was because in the pump-mixer, the ratio of “dispersed phase particle diameter to the grid-size” was smaller than that for the bubble column runs. Also, the inclusion of SGS-TDF affected the radial hold-up, even though the magnitudes of these SGS-TDF forces appeared to be small. These results confirms that (a) the inclusion of SGS-TDF will have more pronounced effect for those Eulerian–Eulerian LES simulation where grid-size happens to be more than the particle size, and (b) that the SGS-TDF in combination with one-equation-SGS-TKE LES model serves as a tool to overcome a conceptual drawback of Eulerian–Eulerian LES model.     

On the numerical study of isothermal vertical bubbly flow using two population balance approaches

Two population balance approaches based on the MUltiple-SIze-Group (MUSIG) model and one-group average bubble number density (ABND) model for handling the bubble size distribution of gas-liquid bubbly flows under isothermal conditions are assessed. Three forms of coalescence and breakage mechanisms by Wu et al. [1998. One-group interfacial area transport in vertical bubbly flow. International Journal of Heat Mass Transfer 41, 1103-1112], Hibiki and Ishii [2002. Development of one-group interfacial area transport equation in bubbly flow systems. International Journal of Heat Mass Transfer 45, 2351-2372] and Yao and Morel [2004. Volumetric interfacial area prediction in upwards bubbly two-phase flow. International Journal of Heat Mass Transfer 47, 307-328] are incorporated in the ABND model. To examine the relative merits of both approaches, local radial distributions of five primitive variables in bubbly flows: void fraction, Sauter mean bubble diameter, interfacial area concentration, and gas and liquid velocities, are compared against the experimental data of Liu and Bankoff [1993a. Structure of air-water bubbly flow in a vertical pipe—I. Liquid mean velocity and turbulence measurements. International Journal of Heat Mass Transfer 36, 1049-1060; 1993b. Structure of air-water bubbly flow in a vertical pipe—II. Void fraction, bubble velocity and bubble size distribution. International Journal of Heat Mass Transfer 36, 1061-1072] and Hibiki et al. [2001. Axial interfacial area transport of vertical bubble flows. International Journal of Heat Mass Transfer 44, 1869-1888]. In general, both of the ABND model and MUSIG model predictions yield close agreement with experimental results. To account for the range of different bubble sizes in the gas-liquid bubbly flows, the resolution required is achieved through the application of the MUSIG model. Nevertheless, computational times increase by a factor of two when compared to applying the simpler ABND model. To further exploit the models’ capabilities, investigations are carried out by extending the two population approaches beyond the bubbly flow regime of higher void fraction, particularly in the transition regime. The numerical results are found to be grossly over-predicted, which expose the inherent limitations of the models. It is known that bubbles in this regime are generally highly distorted and closely packed instead of spherical shape and allowed to move freely in bubbly flow regime.     

群体平衡模型对复杂气液泡状流数值模拟

引言 气液泡状流广泛出现于航空航天、石油化工、核工程技术等领域,且多为复杂湍流泡状流.在工程领域中,准确预测这种复杂泡状流的含气率、气一液速度、气泡直径等参数对工业设备安全与优化分析十分重要.     

Dynamics of bubble breakup in a microfluidic T-junction divergence

The aim of this work is to investigate experimentally the bubble breakup in a microfluidic T-junction divergence using a high-speed digital camera and a micro-Particle Image Velocimetry (micro-PIV) system. The breakup and non-breakup of N₂ bubbles in glycerol–water mixtures with several concentrations of sodium dodecyl sulphate (SDS) as surfactant were studied with capillary number ranging from 0.001 to 0.1. The cross section of PMMA square microchannel is 400 μm wide and 400 μm deep. Four various flow patterns were observed at the T-junction by changing gas and liquid flow rates. The dynamics of three various types of symmetric breakup of bubbles were investigated. The symmetric breakup of bubbles type I is mainly controlled by the augmented pressure in liquid phase. The symmetric breakup of bubbles type II is controlled by both the increased pressure and viscous forces. In the symmetric breakup of bubbles type III, a scaling law for the minimum bubble neck and the remaining time during bubble breaking process were found. The transitions between breakup and non-breakup of bubbles were investigated, and a power–law relationship between bubble extension and capillary number was proposed to predict the transitions between adjacent regimes. Our experimental results reveal that the bubble breakup in a microfluidic T-junction divergence is similar to the droplet behaviours in such a device ( [Jullien et al., 2009] , [Leshansky and Pismen, 2009] and [Link et al., 2004] ).     

Effect of spent grains on flow regime transition in bubble column

It is well known that two main flow regimes are present in bubble columns, being the evaluation of transition between homogeneous and heterogeneous regimes of crucial importance for reactor design. For air–water systems, several models have been satisfactorily proposed to explain this phenomenon. However when gas–liquid–solids systems are considered, solid particles influence on regime transition is not yet clear, in spite of the amount of research developed over the past years.The objective of this work is to evaluate the effect of a specific solid phase – spent grains – on homogeneous regime stability and regime transition. Spent grains are cellulose-based particles that have been used to immobilize cells on biotechnology process. These particles are wettable and have a density close to water and its influence on bubble column reactors is particularly important in order to establish the limits were both regimes prevail.A cylindrical Plexiglax BC of 18 L volume was used with air, water and spent grains at different concentrations (0–20% (wt._{WET BASIS}/vol.)) as gas, liquid and solid phases. Regime transition was determined according to the drift-flux and slip speed concept.It was found that at studied concentrations of spent grains, critical gas hold-up decreases as solids concentration increases. At the highest solids concentration and lowest gas flow rates no fluidization of the solid phase was observed. It is believed that the critical hold-up decrease was mainly due to bubble coalescence, as larger bubbles were observed when heterogeneous regime was present. This coalescence may be caused by the non-uniform distribution of solid phase on the column and the interaction of spent grains with bubbles in the liquid–gas interface     

Behavior of a single coherent gas bubble chain and surrounding liquid jet flow structure

The motion of a single nitrogen gas bubble chain and the structure of water flow field surrounding the chain were experimentally studied. We developed a bubble generator that can control both the bubble diameter and the generation frequency independently. Experimental conditions of bubble Reynolds number and bubble distance divided by bubble diameter were from 300 to 650 and from 6.5 to 300, respectively. We discuss the interaction effects on the motion of each bubble rising in a chain, as compared to the effects of a single rising bubble. The bubble trajectories and the surrounding water flow fields in the state of bubbles rising in a chain were investigated using a high-speed digital video camera and an analog single-lens-reflex camera. We observed two important physical phenomena. First, bubbles passed through a nearly identical path in the case of low frequency of bubble production. On the contrary, at a height of approximately 50 mm from the nozzle, the bubbles in the case of high frequency deviated and scattered from this path due to bubble-bubble interaction. Second, with higher bubble production frequency, coherent bubble chain and the characteristic structure of the surrounding water flow called “liquid jet” were observed near the nozzle. The direction of liquid jet flow differed from the bubble trajectory. We theoretically investigated the relation of coherent bubble chain and liquid jet by applying the conservation of liquid momentum.     

Transient gas–liquid mass transfer model for thin liquid films on structured solid packings

This paper describes a model for gas–liquid mass transfer through thin liquid films present on structured packings for gas–liquid operations under dispersed gas flow regime. The model has been derived for two cases: the absorption (or desorption) of a gaseous component into the liquid film and the transfer of the gaseous component through the liquid film to the packing surface where an infinitely fast reaction takes place. These cases have been solved for three bubble geometries: rectangular, cylindrical, and spherical. For Fourier numbers below 0.3, the model corresponds to Higbie’s penetration theory for both cases. The Sherwood numbers for cylindrical and spherical bubbles are 20% and 35% higher, respectively, than for rectangular bubbles. In case of absorption and Fourier numbers exceeding 3, the effect of bubble geometry becomes more pronounced. The Sherwood numbers for cylindrical and spherical bubbles now are 55% and 100% higher, respectively, than for rectangular bubbles. In case of an infinitely fast reaction at the packing surface, the Sherwood number corresponds to Whitman’s film theory (Sh=1$Sh=1$) for all bubble geometries. In this paper also practical approximations to the derived Sherwood numbers are presented. The approximations for both cases and all bubble geometries describe all the model data within an error of 4%. The application of the model has been demonstrated for three examples: (1) gas–liquid mass transfer for a structured packing; (2) gas–liquid mass transfer in a microchannel operated with annular flow; (3) gas–liquid mass transfer in a microchannel with Taylor flow.     

Bubble flow in trickle beds: investigations using resistive sensors

The local hydrodynamics of co-current gas-liquid down-flow through porous media are investigated in a quasi two-dimensional regular arrangement by means of a network of resistive sensors. The investigations are focused on a liquid continuous flow regime, the dispersed bubble flow, where the gas is divided into elongated bubbles. Due to the variation of the local flow channel orientation and the local void fraction, the average bubble velocity strongly depends on the local geometry. The flow is more coherent in vertical constrictions, compared to all other types of sites, this is probably due to bubble stagnation in the flow channel enlargements. At a given liquid superficial velocities and for sufficiently high superficial gas velocities, the average bubble size is independent of the gas flow rate; it is of the order of magnitude of the volume of the enlargements of the porous medium. The maximum bubble size is about three times its average size, corresponding thus to the coalescence of three average sized bubbles.     

Population balance modelling for bubbly flows with heat and mass transfer

Population balance equations combined with a three-dimensional two-fluid model are employed to predict bubbly flows with the presence of heat and mass transfer processes. Subcooled boiling flow belongs to this specific category of bubbly flows is considered. The MUSIG (MUltiple-SIze-Group) model implemented in CFX4.4 is further developed to account for the wall nucleation and condensation in the subcooled boiling regime. Comparison of model predictions against local measurements near the test channel exit is made for the radial distribution of the bubble Sauter diameter, void fraction, interfacial area concentration and gas and liquid velocities covering a range of different mass and heat fluxes and inlet subcooling temperatures. Additional comparison was also performed against existing boiling model in CFX4.4 and the modified model developed in our previous work (Int. J. Heat Mass Transfer 45 (2002) 1197). Good agreement is better achieved with the local radial bubble Sauter diameter, void fraction, interfacial area concentration and liquid velocity profiles against measurements using the newly formulated MUSIG boiling model over the simpler boiling models. However, significant weakness of the model is still evidenced in the prediction of the vapour velocity. Work is in progress to circumvent the deficiency of the model by the consideration of additional momentum equations or an algebraic slip model to account for bubble separation.     

Effect of a dispersed immiscible liquid phase on the hydrodynamics of a bubble column and ebullated bed

Secondary undesired reactions in ebullated bed resid hydroprocessors can generate an additional dispersed liquid phase, referred as mesophase, which is denser and more viscous than the continuous liquid phase and affects the operation and transport phenomena of the fluidized bed. This study investigates the effect of a dispersed immiscible liquid phase on the overall phase holdups, bubble properties, and fluidization behavior in a bubble column and ebullated bed. The experimental system consisted of biodiesel as the continuous liquid phase, glycerol as the dispersed liquid phase, 1.3 mm diameter glass beads, and nitrogen. The addition of dispersed glycerol reduced the gas holdups in the bubble column for the studied gas and liquid superficial velocities. Dynamic gas disengagement profiles reveal a rise in the large bubble population and reductions to the small and micro bubble holdups when increasing the glycerol concentration. Liquid–liquid–solid bed expansions at various liquid flowrates confirm particle agglomeration in the presence of a more viscous dispersed liquid phase. Overall phase holdups in a gas–liquid–liquid–solid ebullated bed were obtained while varying the gas and liquid flowrates as well as the glycerol concentration. A coalesced bubble flow regime was observed in the bed region without glycerol whereas the addition of glycerol resulted in the dispersed bubble flow regime due to particle clustering and a greater apparent particle size. The resulting bubble flow regime increased the bed and freeboard region gas holdups due to enhanced bubble break-up. Observations of the fluidized bed behavior following the addition of the dispersed glycerol are also discussed.     

Gas-liquid flow and bubble size distribution in stirred tanks

This work is aimed at investigating the turbulent two-phase flow and the bubble size distribution (BSD) in aerated stirred tanks by experiments and computational fluid dynamics (CFD) modelling. The experimental data were collected using a two-phase particle image velocimetry technique and a digital image processing method based on a threshold criterion. With the former technique, the liquid and the gas phase ensemble-averaged mean and r.m.s. velocities are measured simultaneously, while with the latter the dimensions of the bubbles dispersed inside the liquid are evaluated. On the modelling side, a CFD approach, based on the solution of Reynolds average Navier-Stokes equations in an Eulerian framework for both phases, is adopted. As for the bubble dimensions modelling, besides the mono-dispersed assumption, a population balance method, named MUSIG, with bubble break-up and coalescence models is considered. The BSD and the axial and radial velocity of the gas and the liquid phase are presented and discussed. The outcomes of the computational work are evaluated on the basis of the experimental results.     

Modeling of turbulent gas–liquid bubbly flows using stochastic Lagrangian model and lattice-Boltzmann scheme

In this paper we present detailed, three-dimensional and time-resolved simulations of turbulent gas–liquid bubbly flows. The continuous phase is modeled using a lattice-Boltzmann (LB) scheme. The scheme solves the large-scale motions of the turbulent flow using the filtered conservation equations, where the Smagorinsky model has been used to account for the effects of the sub-filter scales. A Lagrangian approach has been used for the dispersed, bubbly phase. That is we update the equations of motion of individual bubbles. It is shown that the incorporation of the sub-filter scale fluid fluctuations along the bubble trajectory improves the predictions. Collisions between bubbles are described by the stochastic inter-particle collision model based on kinetic theory developed by Sommerfeld (2001). It has been found that the collision model not only dramatically decreases computing time compared to the direct collision method, but also provides an excellent computational efficiency on parallel platforms. Furthermore, it was found that the presented modeling technique provides very good agreement with experimental data for mean and fluctuating velocity components.     

Theoretical prediction of flow regime transition in bubble columns by the population balance model

Theoretical prediction of flow regime transition in bubble columns was studied based on the bubble size distribution by the population balance model (PBM). Models for bubble coalescence and breakup due to different mechanisms, including coalescence due to turbulent eddies, coalescence due to different bubble rise velocities, coalescence due to bubble wake entrainment, breakup due to eddy collision and breakup due to large bubble instability, were proposed. Simulation results showed that at relatively low superficial gas velocities, bubble coalescence and breakup were relatively weak and the bubble size was small and had a narrow distribution; with an increase in the superficial gas velocity, large bubbles began to form due to bubble coalescence, resulting in a much wider bubble size distribution. The regime transition was predicted to occur when the volume fraction of small bubbles sharply decreased. The predicted transition superficial gas velocity was about 4 cm/s for the air-water system, in accordance with the values obtained from experimental approaches.     

Adhesion of solid particles to gas bubbles. Part 2: Experimental

In slurry bubble columns, the adhesion of solid catalyst particles to bubbles may significantly affect the G-L mass transfer and bubble size distribution. This feature may be exploited in design by modifying the hydrophilic or hydrophobic nature of the particles used. Previously we have proposed a generalised model, describing the adhesion of particles to G-L interface under stagnant conditions. In this work, we studied the adhesion of particles characterised by different degree of hydrophobicity and porosity: non-porous polystyrene and glass beads, unmodified and hydrophobised mesoporous silica, and activated carbon particles. Images recorded at high optical magnification show the particles adhering to gas bubbles individually or as aggregates. In aqueous media, higher liquid surface tension and particle surface hydrophobicity increase the adhesion strength and the tendency of particles to agglomerate, in agreement with the model. The adhesion of non-porous rough-surface particles to gas bubbles can be characterised by the receding contact angle. The advancing contact angle represents better the adhesion of the same particles to liquid droplets. We found that the “effective” contact angle of porous particles is much lower than an “intrinsic” contact angle calculated from the heat of immersion in water, or measured by sessile drop method. An equivalent contact angle derived from the Cassie rule explains the wetting behaviour of particles having the pores filled with liquid.     

Use of models for lift, wall and turbulent dispersion forces acting on bubbles for poly-disperse flows

Closure laws are needed for the qualification of CFD codes for two-phase flows. In case of bubbly and slug flow, forces acting on the bubbles usually model the momentum transfer between the phases. Several models for such forces can be found in Literature. They show, that these forces depend on the liquid flow field as well as on the size and the shape of the bubbles. A validation of consistent sets of bubble force models for poly-disperse flows is given, basing on a detailed experimental database for vertical pipe flows, which contains data on the radial distribution of bubbles of different size as well as local bubble size distributions. A one-dimensional (1D) solver provides velocity profiles and bubble distributions in radial direction. It considers a large number of bubble size classes and is used for the comparison with the experiments. The simplified model was checked against the results of full 3D simulations done by the commercial code CFX-5.7 for simplified monodisperse cases. The effects of the number of bubbles classes as well as the effect of the lateral extension of the bubbles were analyzed. For the validation of bubble force models measured bubble size distributions were taken as an input for the calculation. On basis of the assumption of an equilibrium of the lateral bubble forces, radial volume fraction profiles were calculated separately for each bubble class. In the result of the validation of different models for the bubble forces, a set of Tomiyama lift and wall force, deformation force and Favre averaged turbulent dispersion force was found to provide the best agreement with the experimental data. Some discrepancies remain at high liquid superficial velocities.     

On the drag force of bubbles in bubble swarms at intermediate and high Reynolds numbers

An accurate and fast simulation of large-scale gas/liquid contact apparatusses, such as bubble columns, is essential for the optimization and further development of many (bio)chemical and metallurgical processes. Since it is not feasible to simulate an entire industrial-scale bubble column in full detail from first principles (direct numerical simulations), higher-level models rely on algebraic closure relations to account for the most important physical phenomena prevailing at the smallest length and time scales, while keeping computational demands low. The most important closure for describing rising bubbles in a liquid is the closure for the drag force, since it dominates the terminal rise velocity of the bubbles.Due to the very high gas loadings used in many industrial processes, bubble–bubble (or ‘swarm’) interactions need to be accounted for in the drag closure. An advanced front-tracking model was employed, which can simulate bubble swarms up to 50% gas hold-up without the problem of (numerical) coalescence. The influence of the gas hold-up for mono-disperse bubble swarms with different bubble diameters (i.e. Eötvös numbers) was quantified in a single drag correlation valid for the intermediate to high Reynolds numbers regime . Also the physical properties of the liquid phase were varied, but the simulation results revealed that the drag force coefficient was independent of the Morton number. The newly developed correlation has been implemented in a larger-scale model, and the effect of the new drag closure on the hydrodynamics in a bubble column is investigated in a separate paper (Lau et al., this issue).     

Hydrodynamic and mass transfer in inertial gas–liquid flow regimes through straight and meandering millimetric square channels

Heat-exchanger reactors are an important part of process intensification technology. For plate geometries, one solution for intensifying transfer and increasing residence times is to construct two-dimensional meandering channels. Supported by this scientific context, the present work aims at characterising gas–liquid mass transfer in the same square millimetric meandering channel, as in Anxionnaz (2009), this constituted the preliminary step required for performing exothermic gas–liquid reactions. Firstly, the gas–liquid hydrodynamics were characterised for a water/air system. When compared to a straight channel of identical compactness and sectional-area (2×2 mm²), the meandering channel induced (i) a delay in the transition from Taylor to annular-slug regimes, (ii) a rise of 10–20% in bubble lengths while conserving almost identical slug lengths, (iii) higher deformations of bubble nose and rear due to centrifugal forces (bends). Secondly, an original method for verifying the relevancy of the plug flow model and accurately determining k_la was used (measurements of concentrations in dissolved oxygen along the channel length). For the Taylor flow regime, k_la increased coherently when increasing j_g, and the meandering geometry had a small influence. On the contrary, this effect was found no more negligible for the slug-annular flow regime. Whatever the channels, the NTU_l remained low, thus showing that, even if millimetric channels allowed to intensify k_la, a special attention should be paid for generating sufficient residence times. At identical compactness, the meandering channel was found to be the most competitive. Finally, results on gas–liquid interfacial areas and mass transfer coefficients were confronted and discussed with respect to the predictions issued from the model developed by Van Baten and Krishna (2004).     

Bubble lengths in the gas–liquid Taylor flow in microchannels

Experimental results of measurements of the bubble and slug lengths in Taylor (slug) flow are presented. The experiments were carried out using 3 different straight microchannels (microreactor with square cross-section made of polydimethyloxosilane (PDMS); microreactor with circular cross-section made of glass; microreactor with rectangular cross-section made of polyethylene terephthalate modified by glycol (PETg)) and 4 different liquids (water, ethanol propanol and heptane). The results have been compared with the available literature correlations. It is concluded, that the values obtained from the correlation proposed by Laborie et al. [Laborie, S., Cabassud, C., Durant-Bourlier, L., Laine, J.M., 1999. Characterization of gas–liquid two-phase flow inside capillaries. Chem Eng Sci 54, 5723–5735] do not agree with the results of measurements, while the agreement of these results with the predictions obtained using the correlation proposed by Qian and Lawal [Qian, D., Lawal, A., 2006. Numerical study on gas and liquid slugs for Taylor flow in a T-junction microchannel. Chem Eng Sci 61, 7609–7625] is good. New, corrected values of the pre-exponential constant and the exponents in the Qian and Lawal [Qian, D., Lawal, A., 2006. Numerical study on gas and liquid slugs for Taylor flow in a T-junction microchannel. Chem Eng Sci 61, 7609–7625] correlation are proposed.