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.     

Effects of viscosity and relaxation time on the hydrodynamics of gas–liquid systems

Effects of liquid properties on the hydrodynamics of gas–liquid systems were investigated in lab-scale bubble column (BC) and internal loop airlift (ILA). Alginate solutions, a glycerol solution and a Boger fluid were adopted to separately address the effects of viscosity and of surface tension for Newtonian fluids, and the effects of relaxation time for non-Newtonian fluid characterized by approximately constant viscosity (low shear thinning). Hydrodynamic regimes were characterized in terms of overall gas holdup, gas–liquid mass transfer coefficient, drift-flux and liquid circulation velocity. The superficial gas velocities at the transition between hydrodynamic regimes (homogenous regime–vortical-spiral regime–heterogeneous regime) as a function the liquid viscosity was characterized by a maximum. The same behavior was observed for the maximum stable gas holdup and gas–liquid mass transfer coefficient in BC. Viscosity enhances homogeneous regime stability for μ<4.25 mPa s, in BC, and μ<7.68 mPa s, in ILA. For non-Newtonian fluids the transition velocity increases with liquid elasticity. The stabilization mechanism related to the relaxation time of Boger fluids has been discussed.     

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.     

Tomographic measurement of liquid hold up and effective interfacial area distributions in a column packed with high performance structured packings

In this paper, we report on the use of a high energy and high resolution X-ray tomograph to visualize and quantify the distribution of liquid hold up and of gas–liquid interfacial area in a 0.1 m diameter column filled with MellapakPlus 752.Y packing elements. A standard air–water system at room temperature and atmospheric pressure were used. Tomographic measurements have been carried out in a large number of packing cross sections situated at different heights between the top and the bottom of the packed column, giving access to the evolution of axial profiles of liquid hold up and of gas–liquid interfacial area as a function of the operating conditions. Gas–liquid interfacial area values were also measured by a chemical method (CO₂ absorption from air into a caustic solution). For the first time, a whole set of gas–liquid interfacial area values evaluated from tomographic images are interestingly compared with values measured by a chemical method. A comparison is also presented with literature models.     

Gas–liquid interfacial area and mass transfer coefficient in a co‐current down flow contacting column

The gas–liquid interfacial area and mass transfer coefficient for absorption of oxygen from air into water, aqueous glycerol solutions up to 1.5% (w/w) and fermentation medium containing glucose up to a 3% concentration were determined in a co‐current down flow contacting column (CDCC; 0.05 m i.d. and 0.8 m length). Experimental studies were conducted using various nozzle diameters at different gas and re‐circulation liquid rates. Specific interfacial area (a) is determined from the fractional gas hold‐up (ε_G) and the average bubble diameter (d_b). Once the interfacial area is determined, the volumetric mass transfer coefficient (k_La) is then used to evaluate the film mass transfer coefficient in the CDCC. The effects of operating conditions and liquid properties on the specific interfacial area were investigated. The values of interfacial area in air–aqueous glycerol solutions and fermentation media were found to be lower than those in the air–water system. As far as experimental conditions were concerned, the values of interfacial area obtained from this study were found to be considerably higher than those of the literature values of conventional bubble columns. The penetration theory is used to interpret the film mass transfer coefficient and results match the experimental k_L data reasonably well. Copyright © 2006 Society of Chemical Industry     

Gas–liquid mass transfer in periodically operated trickle-bed reactors: Influence of the liquid-phase physical properties and flow modulation

The influence of periodic operation on trickle-bed reactor (TBR) hydrodynamics and gas–liquid mass transfer was investigated. Two-phase pressure drop, dynamic liquid hold-up and gas–liquid mass transfer coefficient (k_La) were determined at various liquid flow rates and for different modes of liquid flow variation (increasing and decreasing liquid flow rate). The results reveal the considerable influence of type of liquid flow rate modulation on k_La values (deviations of up to 80% in k_La). Simulation studies on gas-limited reaction in a periodically operated TBR indicate that an enhancement in conversion of about 14% can be expected from an appropriate selection of the operating mode, thus clearly demonstrating the quantitative process intensification feasible through increased gas–liquid mass transfer.     

Carbon Dioxide Absorption in Triethanolamine Aqueous Solutions: Hydrodynamics and Mass Transfer

The carbon dioxide absorption process by triethanolamine aqueous solutions was analyzed in a bubble‐column reactor taking into account the chemical reaction mechanism, gas‐liquid interfacial area, and mass transfer rate. A speciation study of this gas‐liquid system was developed by ¹H and ¹³C NMR spectroscopy in order to obtain the reaction mechanism and stoichiometry. The gas‐liquid interfacial area was evaluated considering the variations of bubble size distribution and gas holdup during the operation time. The liquid‐phase mass transfer coefficient was calculated from the carbon dioxide absorption rate data by interfacial area evolution and reaction stoichiometry.     

Determination of the interfacial area and mass transfer coefficients in the Taylor gas–liquid flow in a microchannel

The interfacial area in the Taylor (slug) gas–liquid flow in a microchannel was measured by the Danckwerts' (chemical) method, using CO₂ absorption from the CO₂/N₂ mixture into KHCO₃/K₂CO₃ buffer solutions, containing NaOCl as a catalyst. The rate of absorption was determined and the Danckwerts' plots were constructed. Reasonable agreement with the geometrical area measured photographically was obtained. This fact allowed to determine for the first time the mass transfer coefficients separately for liquid film and liquid caps. A correlation for the calculation of mass transfer coefficients has been proposed.     

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).     

Effects of surface active agents on hydrodynamics and mass transfer characteristics in a split-cylinder airlift bioreactor with packed bed

The effects of three types of surface active agents (containing SDS, HCTBr and Tween 40) with various concentrations (0–5 ppm) on the hydrodynamic and oxygen mass transfer characteristics in a split-cylinder airlift bioreactor with and without packing were investigated. It was observed that in the surfactant solutions, surface tension of the liquid decreased and smaller bubbles were produced in comparison with pure water. So, surfactants presence strongly enhanced mixing time and gas hold-up although oxygen mass transfer coefficient and the liquid circulation velocity reduced. Furthermore, the packing installation enhanced the overall gas–liquid volumetric mass transfer coefficient by increasing flow turbulency and Reynolds number compared to an unpacked column. The packing increased gas hold-up and decreased bubbles size and liquid circulation velocity.     

Interfacial area and mass transfer in gas-liquid cocurrent upflow and countercurrent flow in reciprocating plate column

The volumetric mass transfer coefficient and the interfacial area were measured for carbon dioxide absorption into water using a reciprocating plate column of plate geometry different from a Karr column. The specific interfacial area was governed by a change in bubble size at low agitation rates and by a variation in gas holdup at high agitation rates. The liquid phase mass transfer coefficient was strongly influenced by the agitation rate, the phase velocities and the plate geometry.     

Impact of Surfactant Addition on Oxygen Mass Transfer in a Bubble Column

The impact of sparger design and surfactant addition on the oxygen transfer rate in a bubble column was examined. Additionally, measurements were also made of the holdup and bubble size distribution, allowing both the interfacial area for mass transfer and the liquid film mass transfer coefficient to be determined for a range of industrially relevant superficial velocities. It was found that for the velocity range examined changes in the superficial velocity had a minimal impact on the observed value of liquid film mass transfer coefficient. In contrast, addition of both hydrophilic and hydrophobic surface‐active compounds led to an approximately threefold reduction in liquid film mass transfer coefficient.     

Mass transfer with chemical reaction in liquid foam reactors

Mass transfer studies were conducted in a stable liquid foam reactor under various operating conditions to evaluate gas holdup, effective interfacial area, liquid-phase mass transfer coefficient and a modified interfacial mass transfer coefficient to include the surface-active agents employed. Gas holdup and effective interfacial area were evaluated experimentally. The interfacial mass transfer coefficient was evaluated semitheoretically, by considering the interfacial region as a separate phase and using the experimental data developed for mass transfer accompanied by a fast first-order chemical reaction. The liquid-phase mass transfer coefficient was also evaluated semitheoretically, using Danckwert's theory for the liquid phase and the experimental data on mass transfer accompanied by a slow pseudofirst-order chemical reaction. An experimental unit was set up to provide a stable flowing foam column, simulating the foam reactor. Mass transfer rates were studied for superfacial gas velocities in the range from 1.5 × 10⁻² m/s to 5 × 10⁻² m/s, giving gas residence times in the range from 20 to 55 seconds. A cationic and nonionic surface-active agent and three different wire mesh sizes, giving bubble size distributions in the range from 2.2 to 5.4 mm Sauter mean diameters, were employed. It is observed that gas holdup is insensitive to the type of surface-active agent; it is however, dependent on wire mesh size and gas velocity. The bubble diameter and, hence, the interfacial area are found to be insensitive to gas velocity in the range studied; they are, however, strong functions of wire mesh size. The liquid-phase mass transfer coefficient increases with increase in gas velocity. The surface-active agent introduces additional resistance to mass transfer in both reaction cases, this being the controlling one in the case of the fast reaction. A comparison with conventional packed bed contactors indicates the mass transfer rates to be about 8 times lower for the foam reactor, for the fast reaction case; for slow reactions, the foam reactor has mass transfer rates approximately 2-4 times higher than those for conventional packed bed contactors.     

Influence of Chitosan and Chitosan Derivatives on Hydrodynamics and Mass Transfer in a Bubble Contactor

The behavior of chitosan and two kinds of chitosan derivatives in carbon dioxide absorption in a bubble column contactor is analyzed. The effects of absorption type (physical or chemical), polymer type, concentration, and liquid‐phase physical properties on hydrodynamics (bubble size, gas holdup, and specific interfacial area) and mass transfer (absorption rate and mass transfer coefficient) are evaluated.     

Multi-scale analysis of gas–liquid interaction and CFD simulation of gas–liquid flow in bubble columns

The ratio of effective drag coefficient to bubble diameter is of critical importance for CFD simulation of gas–liquid flow in bubble columns. In this study, a novel model is proposed to calculate the ratio on the basis of the Dual-Bubble-Size (DBS) model. The motivation of the study is that a stability condition reflecting the compromise between different dominant mechanisms can serve for a closure in addition to mass and momentum conservative constraints, and the interphase momentum transfer should be related to different paths of energy dissipation. With the DBS model, we can first offer a physical interpretation on macro-scale regime transition via the shift of global minimum point of micro-scale energy dissipation from one potential trough to the other. Then the proposed drag model is integrated into a CFD simulation. Prior to this integration, we investigate the respective effects of bubble diameter and correction factor and found that the effect of bubble diameter is limited, whereas the correction factor due to the bubble swarm effect is eminent and appropriate correction factor has to be selected for different correlations of standard drag efficient to be in accord with experiments. By contrast, the DBS drag model can well predict the radial gas holdup distribution, the total gas holdup as well as the two-phase flow field without the need to adjust model parameters, showing its great potential and advantage in understanding the complex nature of multi-scale structure of gas–liquid flow in bubble columns.     

Impact of Cellulose and Surfactants on Mass Transfer of Bubble Columns

The effects of cellulose, surfactants, and their combination on the hydrodynamic behavior and the liquid‐side mass transfer coefficient of a bubble column were evaluated. For that purpose, different aqueous solutions containing surfactants (sodium dodecyl sulfate) and cellulose (microcrystalline cellulose, MCC) were investigated. The interfacial areas were calculated from the bubble diameters, the bubble frequencies, and the terminal bubble rising velocities. The liquid‐side mass transfer coefficients were determined from the volumetric mass transfer coefficients measured by the dynamic method. In the concentration range under test, the experimental results proved that the addition of MCC to the studied liquid phases did not affect the mass transfer coefficient.     

Hydrodynamics and mass transfer study of aliphatic alcohols in airlift reactors

Gas holdup and gas–liquid mass transfer coefficient were considered in an external airlift reactor. Air was sparged through some aliphatic alcohols (methanol, ethanol, n-propanol, and n-butanol) with different concentrations (0–1%, v/v). It was observed that gas holdup and mass transfer coefficient increased with increasing the number of carbons in alcohols. Furthermore, an increment in alcohols concentration increased gas holdup and mass transfer coefficient. The same behavior was observed in external and internal loop airlift reactors although gas holdup and mass transfer coefficient values were less than those of internal airlift reactor. According to the experiments, two correlations for gas holdup and mass transfer were developed.     

A CFD-based approach to the interfacial mass transfer at free gas–liquid interfaces

A novel computational fluid dynamics (CFD) based approach is suggested, which incorporates interfacial mass transfer at moving interfaces. This approach is general and able to govern multicomponent systems as well as interfacial boundary conditions in an arbitrary form. This is important in order to properly handle the typical concentration jump at the phase interface and to avoid an assumption of a constant distribution coefficient, which is seldom met in real processes. A test case study is carried out for a gas bubble rising in a stagnant liquid phase, whereas two different liquids, namely water and water–carboxymethylcellulose solution, are used. The gas bubble contains 99% of oxygen diffusing into continuous phase. The movement of the bubble is simulated using the level set method. Both velocity vectors and concentration contours are demonstrated and analysed.     

Effects of surfactants on hydrodynamics and mass transfer in a split‐cylinder airlift reactor

Effects of various concentrations (0–5 ppm) of anionic (sodium dodecyl sulfate, SDS) and non‐ionic (Tween‐80 and Triton X‐405) surfactants on gas hold‐up and gas–liquid mass transfer in a split‐cylinder airlift reactor are reported for air–water. Surfactants were found to strongly enhance gas hold‐up. Non‐ionic surfactants were more effective in enhancing gas hold‐up compared to the anionic surfactant SDS. An enhanced gas hold‐up and a visually reduced bubble size in the presence of surfactants implied an enhanced gas–liquid interfacial area for mass transfer. Nevertheless, the overall gas–liquid volumetric mass transfer coefficient was reduced in the presence of surfactants, suggesting that surfactants greatly reduced the true liquid film mass transfer coefficient and this reduction outweighed the interfacial area enhancing effect. Presence of surfactants did not substantially affect the induced liquid circulation rate in the airlift vessel.     

Design and selection of sparger for bubble column reactor. Part II: Optimum sparger type and design

Bubble columns are widely used for conducting gas–liquid and gas–liquid–solid mass transfer/chemical reactions. Sparger is the most important accessory because it decides the bubble size/rise velocity distribution. These, in turn, govern the radial and axial hold-up profiles, the liquid phase flow pattern and hence the performance of bubble columns. In particular, the sparger design is critical if the aspect ratio is low and the sparger design dominates the performance of the bubble column. However, systematic procedure for the selection of sparger design and type are not available in the published literature. This is the specific objective of the present work. In Part I, the performance of different spargers, including the newly developed wheel type of sparger is discussed. Thus the important considerations required for the sparger design are highlighted. The bubble column used in the manufacture of hydrogen peroxide has been considered as a case for illustration.