Numerical study of the coupling between reaction and mass transfer for liquid‐liquid slug flow in square microchannels

While the benefits of miniaturization on processes have been widely demonstrated, its impact on microfluidics and local mechanisms such as mass transfer is still little understood. The coupling between reaction and mass transfer in microchannels is simulated for liquid‐liquid slug flow. First, the extrapolation to confined flow of the classical model used to calculate interfacial mass fluxes in reactive infinite media was studied. This model consists in estimating transferred fluxes between two phases as a function of the enhancement factor E. Its expression depends on the model used to represent interfacial mass transfer. In infinite media, Lewis and Whitman's stagnant film theory is generally preferred for its simplicity and its reliability. In the case of confined slug flow, the limitation of such a model to predict interfacial fluxes is highlighted. Second, the case of liquid‐liquid competitive consecutive reactions in microchannels is considered. The unfavorable impact of the length between droplets on selectivity is emphasized. This is a direct consequence of mass‐transport mechanisms in microchannels. © 2010 American Institute of Chemical Engineers AIChE J, 2011     

CFD studies coupling hydrodynamics and solid‐liquid mass transfer in slug flow for matter removal from tube walls

Organic matter deposition on internal surfaces constitutes a drawback that impairs the efficiency of several industrial processes. To overcome this problem, sparging a train of bubbles could be useful since its presence strongly increases the wall shear stress. A detailed numerical mass‐transfer study between a finite soluble wall and the liquid around a rising Taylor bubble was performed, simultaneously solving velocity and concentration fields. The bubble passage throws solute backward and is responsible for radial dispersion. There is also an increase in the transfer rate with enhancements between 10 and 20% (depending on liquid average velocity and bubble length) compared to single‐phase flow. Mass‐transfer coefficients along the different hydrodynamic regions around the bubble nose, liquid film, and wake were characterized and their values compared with those from literature. The results suggest a promising potential of bubble train flow to enhance organic matter removal from walls in biological systems. © 2016 American Institute of Chemical Engineers AIChE J, 63: 2420–2439, 2017     

Measurements of horizontal three‐phase solid‐liquid‐gas slug flow: Influence of hydrate‐like particles on hydrodynamics

Gas hydrate formation is a main flow assurance concern in oil and gas production. Understanding the effects of the introduction of solid particles in the slug flow is essential to improve the efficiency and safety of multiphase production. The purpose of the present work is the experimental characterization of solid‐liquid‐gas slug flow with the presence of dispersed hydrate‐like particles. Experimental tests were carried out with inert polyethylene particles of 0.5‐mm diameter with density similar to gas hydrates (938 kg/m³). The test section comprised a 26‐mm ID, 9‐m length horizontal duct of transparent Plexiglas. High Speed Imaging and resistivity sensors was used to analyze the slug flow unit cell behavior due to the introduction of the solid particles and to measure the unit cell translational velocity, the slug flow frequency, the bubble and slug lengths, and the phase fractions. Two distinct concentrations of solid particles were tested (6 and 8 g/dm³). © 2018 American Institute of Chemical Engineers AIChE J, 64: 2864–2880, 2018     

Direct numerical simulations of mass transfer in square microchannels for liquid-liquid slug flow

Microreactors for the development of liquid-liquid processes are promising technologies since they are supposed to offer an enhancement of mass transfer compared to conventional devices due to the increase in the surface/volume ratio. But impact of the laminar flow should be negative and the effect is still to be evaluated. The present work focuses on the study of mass transfer in microchannels by means of 2D direct numerical simulations. We investigated liquid-liquid slug flow systems in square channel of depth. The droplet velocity ranges from 0.0015-0.25 m/s and the ratio between the channel depth and the droplet length varies between 0.4 and 11.2. Droplet side volumetric mass transfer coefficients were identified from concentration field computations and the evolution of these coefficients as a function of the flow parameters and the channel size is discussed. This study reveals that mass transfer is strongly influenced by the flow structure inside the droplet. Moreover, it shows that the confinement of the droplets due to the channel size leads to an enhancement of mass transfer compared to cases where the droplets are not constrained by the walls.     

Hydrodynamics and mass transfer of gas–liquid flow in a falling film microreactor

In this article, flow pattern of liquid film and flooding phenomena of a falling film microreactor (FFMR) were investigated using high‐speed CCD camera. Three flow regimes were identified as “corner rivulet flow,” “falling film flow with dry patches,” and “complete falling film flow” when liquid flow rate increased gradually. Besides liquid film flow in microchannels, a flooding presented as the flow of liquid along the side wall of gas chamber in FFMR was found at high liquid flow rate. Moreover, the flooding could be initiated at lower flow rate with the reduction of the depth of the gas chamber. CO₂ absorption was then investigated under the complete falling flow regime in FFMR, where the effects of liquid viscosity and surface tension on mass transfer were demonstrated. The experimental results indicate that k_L is in the range of 5.83 to 13.4 × 10^?5 m s^?1 and an empirical correlation was proposed to predict k_L in FFMR. © 2009 American Institute of Chemical Engineers AIChE J, 2009     

Gas–liquid mass transfer of aqueous Taylor flow in monoliths

The gas–liquid mass transfer of a monolith operating in the Taylor flow regime is presented. Mass transfer measurements are compared with a literature model derived for single capillaries. The comparison resulted in a prediction of the unit cell length (gasbubble+liquidslug). Independent measurements of the liquid slug length showed that the predicted unit cell length is close to the measured ones. This leads to the conclusion that mass transfer models for single capillaries may indeed be used for monoliths. Additionally, it is shown that the liquid slug length may also be estimated from pressure drop measurements.     

High‐throughput microporous tube‐in‐tube microreactor as novel gas–liquid contactor: Mass transfer study

High‐throughput microporous tube‐in‐tube microchannel reactor (MTMCR) was first designed and developed as a novel gas–liquid contactor. Experimentally measured k_Lα in MTMCR is at least one or two orders of magnitude higher than those in the conventional gas–liquid contactors. A high throughput of 500 L/h for gas and 43.31 L/h for liquid is over 60 times higher than that of T‐type microchannel. An increase of the gas or liquid flow rate, as well as a reduction of the micropore size and annular channel width of MTMCR, could greatly intensify the gas–liquid mass transfer. The interfacial area, α, in MTMCR was measured to be as high as 2.2 × 10⁵ m²/m³, which is much higher than those of microchannels (3400–9000 m²/m³) and traditional contactors (50–2050 m²/m³). The artificial neural network model was proposed for predicting α, revealing only an average absolute relative error of <5%. © 2010 American Institute of Chemical Engineers AIChE J, 2011     

An experimental study of air-water Taylor flow and mass transfer inside square microchannels

Flow and mass transfer properties under air-water Taylor flow have been investigated in two square microchannels with hydraulic diameters of 400 and 200 μm. Experimental data on Taylor bubble velocity, pressure drop and liquid side volumetric mass transfer coefficient (k_La) have been presented. It was shown that the measured Taylor bubble velocity in square microchannels could be well interpreted based upon an approximate measurement of the liquid film profile therein. Then, the obtained two-phase frictional pressure drop values in both microchannels were found to be significantly higher than the predictions of the correlation proposed by Kreutzer et al. [2005b. Inertial and interfacial effects on pressure drop of Taylor flow in capillaries. A.I.Ch.E. Journal 51, 2428-2440] when the liquid slug was very short, which can be explained by the inadequacy of their correlation to describe the excess pressure drop caused by the strong inner circulation in such short liquid slugs. An appropriate modification has been made to this correlation in order to improve its applicability in microchannels. Finally, the experimental (k_La) values in the microchannel with hydraulic diameter of 400 μm were found to be in poor agreement with those predicted by the existing correlations proposed for capillaries with diameters of several millimeters. The observed deviation was mainly due to the fact that mass transfer experiments in this microchannel actually corresponded to the case of short film contact time and rather poor mixing between the liquid film and the liquid slug, which was not in accordance with mass transfer assumptions associated with these correlations. A new empirical correlation has been proposed to describe mass transfer data in this microchannel.     

Modelling of transient mass transfer in liquid and liquid‐solid pulsating systems: Applications and extension to heat transfer

The dynamic surface renewal model of Maucci et al. (2001) is applied to transient mass transfer problems and extended to transient heat transfer measurements in pulsating, two‐phase flows. The model is also used to simulate mass transfer for square‐wave liquid velocity pulses in a liquid‐solid column. Experiments and simulation show that, when flow reversal occurs, the average mass transfer for a pulsating flow can be significantly higher than for steady state flow at the same bulk flow rate. This increase depends mainly on the relative pulse magnitude. The influence of pulse frequency and symmetry is second‐order. Apparent differences between various published studies are resolved.     

气液传质理论研究进展

文内对气液传质的理论研究进行了评述，并预测了未来的发展方向     

Chemical conversion and liquid–liquid extraction of 5‐hydroxymethylfurfural from fructose by slug flow microreactor

A dehydration of fructose in the water/methyl isobuthyl ketone (MIBK) biphasic system can yield 5‐hydroxymethylfurfural (HMF) to be successfully extracted into the organic MIBK phase. The HMF production and yield in MIBK phase was discussed by using a simplified model taking into consideration of the slug flow. The extraction resistance of HMF across the interface between water and MIBK depended on the line velocity and the flow rate ratio. It was likely that the velocity field generated in the slug flow contributed to an increase in the mass transfer of HMF. © 2016 American Institute of Chemical Engineers AIChE J, 62: 2135–2143, 2016     

填料塔气液传质参数研究（Ⅰ）──有效传质面积及容积传质系数

用化学吸收法测定了拉西环填料的有效传质表面积和容积传质系数，并进一步用物理法比较测定了容积传质系数。实验证明，用化学法测得的容积传质系数大于物理法测定值。并得出有效传质表面积及容积传质系数与喷淋密度的关系式。     

Design and operation of gas–liquid slug flow in miniaturized channels for rapid mass transfer

The influences of operating parameters such as channel size, flow rate, and void fraction on the mass transfer rate in the gas–liquid slug flow are investigated to establish a design method to determine the parameters for rapid mass transfer. From the experimental results, the turnover index, including the slug linear velocity, its length, and the channel size that represents the turnover frequency of the internal circulation flow, is proposed. For PTFE tube in which no liquid film exists in slug flow, a master curve is derived from the relationship between the mass transfer coefficient and the turnover index. For each channel material, the Sherwood number is also roughly correlated with the Peclet number. These correlations make it possible to arbitrarily determine a set of operating parameters to achieve the desired mass transfer rate. However, the turnover index and the Peclet number include the slug length, which cannot be controlled directly. The relationship between the slug length and the operating parameters is also investigated. The slug volume mainly depends on the inner diameter (i.d.) of a union tee. At a fixed union tee i.d., the slug length is controlled through the exit i.d. of the channel connected to the union tee and the void fraction. Thus, the final slug length depends on the union tee and exit channel inner diameters. At low flow rates, the gas and liquid collision angle is significant in determining the slug length.     

Influence of hydrodynamics on liquid mixing during Taylor flow in a microchannel

The miscible liquid‐liquid two phases based on Taylor flow in microchannels was investigated by high‐speed imaging techniques and Villermaux/Dushman reaction. The mixing based on Taylor flow was much better compared with that without introducing gas in microchannels, even the ideal micromixing performance could be obtained under optimized superficial gas and liquid velocities. In the mixing process based on Taylor flow, the superficial gas and liquid velocities affected the lengths and the velocities of Taylor bubble and liquid slug, and finally the micromixing performance. The formation process of Taylor flow in the inlets, the initial uniform distribution of reactants and the internal circulations in the liquid slug, and the thin liquid films all improved the mixing performance. Furthermore, a modified Peclet number that represented the relative importance of diffusion and convection in the mixing process was proposed for explaining and anticipating micromixing efficiency. © 2011 American Institute of Chemical Engineers AIChE J, 58: 1660–1670, 2012     

表面张力对传质过程的影响

表面张力对传质过程的影响主要是影响传质界面积,当物系为正物系时,对板式塔有较小较稳定的汽泡,对填料塔和湿壁塔,有较稳定的液膜,结果使二者均有较大的传质界面积,传质效果较好;负物系的情况相反。当液体混合物的平均表面张力较小时,也有利于形成较小较稳定的汽泡,从而有利于传质。表面张力对传质过程的影响机理相当复杂,这方面的研究工作有待深入开展。     

Absorption methods for the determination of mass transfer parameters of packing internals: A literature review

Methods for the determination of mass‐transfer coefficients and effective interfacial areas in packed absorption columns are reviewed. For each parameter, the methods are grouped into categories on the basis of their physical principle; the chemical systems used, experimental protocol, and the advantages and inconveniences are discussed. The treatment of end effects, the influence of packed bed height, and the recent efforts in standardization of measurement methods are also treated. The aim of the review is to give a broad overview of the methods used in literature in the last eight decades, some of which might be reconsidered in the light of modern measurement techniques and to evaluate them in relation to precision, practicality and hazardousness thereby to facilitate the search for reliable, precise, and convenient experimental practices. © 2017 American Institute of Chemical Engineers AIChE J, 63: 3246–3275, 2017     

Effect of channel size on liquid‐liquid plug flow in small channels

The hydrodynamic properties of plug flow were investigated in small channels with 0.5‐, 1‐, and 2‐mm internal diameter, for an ionic liquid/aqueous two‐phase system with the aqueous phase forming the dispersed plugs. Bright field Particle Image Velocimetry combined with high‐speed imaging were used to obtain plug length, velocity, and film thickness, and to acquire velocity profiles within the plugs. Plug length decreased with mixture velocity, while for constant mixture velocity it increased with channel size. Plug velocity increased with increasing mixture velocity and channel size. The film thickness was predicted reasonably well for Ca > 0.08 by Taylor's (Taylor, J Fluid Mech. 1961;10(2):161–165) model. A fully developed laminar profile was established in the central region of the plugs. Circulation times in the plugs decreased with increasing channel size. Pressure drop was predicted reasonably well by a modified literature model, using a new correlation for the film thickness derived from experimental values. © 2015 American Institute of Chemical Engineers AIChE J, 62: 315–324, 2016     

Influence of impeller type on hydrodynamics and gas‐liquid mass‐transfer in stirred airlift bioreactor

The influence of impeller type in a mechanically stirred airlift bioreactor was analyzed in relation to the non‐Newtonian viscous fluids. The agitation was carried out through a marine impeller (axial impeller) and a paddle impeller (radial impeller) located along with the gas sparger in the region comprised by the riser. The bioreactor was sparged with air under different velocities (0.036–0.060 m s^?1). Carboxymethylcellulose 1.94% and xanthan 1.80% were used as a fluid model. The gas holdup and volumetric mass‐transfer coefficient increased in up to five and three times, respectively, when compared to a conventional airlift bioreactor; however, better results were obtained when the straight paddle impeller type was used. The results suggest that the studied bioreactor can be used successfully in viscous fluid, and it can be more efficient than conventional airlift bioreactors. The results obtained suggest the use of radial impellers. © 2015 American Institute of Chemical Engineers AIChE J, 61: 3159–3171, 2015     

Effect of interfacial mass transfer on the dispersion in segmented flow in straight capillaries

The effect of interfacial mass transfer on the extent of dispersion in liquid‐liquid segmented flow in straight capillaries is studied. In the absence of interfacial mass transfer, dispersion coefficient was seen to go through a minimum with increasing flow rates. In the presence of mass transfer, physicochemical properties of both the phases and slug lengths were seen to vary along the capillary length. The extent of dispersion was always higher in the presence of interfacial mass transfer. The predictions using axial dispersion model deviated noticeably for larger capillaries as the model does not account for varying buoyancy, dynamic contacting, and Marangoni convection. Simulations of a first‐order interfacial reaction considering varying slug lengths showed a significant change in optimum operating parameters than the conventional approach. A special case of “drop‐on‐demand” type of controlled two‐phase flow in capillaries was also studied. © 2015 American Institute of Chemical Engineers AIChE J, 61: 4294–4308, 2015     

Studies on the hydrodynamic behavior and mass transfer in a down‐flow jet loop reactor with a coaxial draft tube

The effects of certain pertinent parameters such as gas and liquid flow rates and nozzle position on the behavior of a down‐flow jet loop reactor (DJR) have been studied. The mean residence times of gas and liquid phases and the gas holdup within the reactor have been measured. In addition, the overall volumetric mass transfer coefficient, and the influence of the gas flow rate and the position of the nozzle inside the draft tube on the latter has been determined. Correlations have been presented for the gas holdup and k_La which take into account the length of the draft tube and the nozzle immersion height. The k_La values obtained at different power per unit volume (P/V) values in the DJR used in the present study compare favorably with data presented for stirred tanks and bubble columns in the literature. The liquid residence time distribution (RTD) within the reactor has been studied by tracer analysis for various operating conditions and nozzle immersion height and the results are indicative of the high mixing intensities that can be obtained in such reactions. © 2001 Society of Chemical Industry