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     

微通道内气-液弹状流动及传质特性研究进展

气-液弹状流,又称Taylor流,是一种以长气泡和液弹交替形式流动的流动形态。微通道内气-液弹状流因其气泡与液弹尺寸分布均一、停留时间分布窄、径向混合强等优点,是一种适于强化气-液反应的理想流型。本文首先介绍了微通道内气泡的生成机理、气泡和液弹长度,以及气泡生成阶段的传质特征。其次系统综述了主通道中弹状流动及传质过程的研究进展,包括气泡形状与液膜厚度、液弹内循环和泄漏流特征、气-液传质系数的测量与预测,以及物理与化学吸收过程中的传质特性等方面内容。最后阐述了当前研究的不足并展望了气-液弹状流的研究方向。     

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     

微通道内气-液两相传质过程行为及其应用

微通道内气-液两相体系中Taylor流和泡状流具有气泡尺寸均一、停留时间分布窄、可调控性强和比表面积高等优点,具有广泛的应用前景。从Taylor气泡和泡状气泡的传质过程出发,系统综述了微尺度下气泡的溶解规律、传质过程机理和传质/溶解模型等方面的研究进展,并介绍上述流型在反应或过程强化、基础物性及动力学数据测量和微纳材料合成方面的应用。最后总结并展望了技术领域的研究难点与研究方向。     

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     

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.     

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     

Aerobic oxidation of benzyl alcohol in a slug flow microreactor: Influence of liquid film wetting on mass transfer

Homogeneous Co/Mn/Br catalyzed aerobic oxidation of benzyl alcohol in acetic acid to benzaldehyde was performed in polytetrafluoroethylene microreactors operated under slug flow at temperatures up to 150°C and pressures up to 5 bar. Depending on the bubble velocity and length, a wetted or dewetted slug flow was observed, characterized typically by a complete or partially wetting liquid film around the bubble body. The latter flow suffered from a limited interfacial area for mass transfer. Experiments at temperatures up to ca. 90°C were under kinetic control given no product yield difference under wetted and dewetted slug flows and were used to establish a simplified kinetic expression (first order in benzyl alcohol and zero order in oxygen). This allows to develop a mass transfer model combined with an instantaneous reaction regime that well described the experimental results at higher temperatures where mass transfer was limiting in the dewetted slug flow.     

壁面润湿性对微通道内二氧化碳-水两相流流动及传质性能的影响

在1 mm×1 mm矩形截面下微通道内,以二氧化碳-水为工作流体,研究壁面润湿性和气液表观流速对气-液两相流型和气液传质的影响,并研究了气、液表观流速对弹状流流体力学性质的影响。在亲水微通道中观测到了泡状流、泡状-弹状流、弹状流;在疏水微通道中观测到了非对称弹状流、拉长的非对称弹状流、分层流。实验表明亲水微通道中弹状流区域下气泡长度大体上随气相表观流速的增大而增大,随液相表观流速的增大而减小;液弹长度大体上随气相表观流速的增大而减小,随液相表观流速的增大先增大后减小;液侧体积传质系数k_La均随气、液相表观流速的增大而增大,随通道壁面润湿性的增强而增大。     

微通道中钒的液-液流型和萃取传质动力学研究

采用伯胺N1923萃取剂在微通道中研究V(V)的液-液流型和萃取传质动力学,以15vol% N1923作为连续相、钒氧酸根水溶液作为分散相,研究不同流速下两不混溶相的流型变化规律及两相停留时间和微通道管径作为流速的函数对传质的影响。随两相流速增大,段塞流长度和比界面面积基本不变,且两相流体由Raydrop微通道流入外接毛细管微通道时由于微通道的扩张会改变两相流动方式,使同一实验条件下在微通道中同时出现多种流型,与此同时两相流速和总体积传质系数(kLa)呈正相关,表明流型在本研究体系中对传质的影响可忽略。在相同管径通道内,停留时间与总体积传质系数呈负相关,表明在两相接触通道入口处发生了显著传质。在相同的两相混合速度和相比下,254 μm的管径传质效果是750 μm的9倍,表明小管径内传质效果更加,循环强度更大。最后将实验总体积传质系数结果与总体积传质系数的经验式进行了关联,有望为实现将微通道放大的绿色冶金技术提供理论基础。     

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     

微通道内CO2吸收与传质及资源化利用的研究进展

由于在流体流动、传质、传热及反应等方面良好的调控能力,微化工技术成为化工学科重要的发展领域。综述了近年来以CO₂应用为背景的微化工系统中的多相流与传质的研究进展。从流体流动和传质机理出发,分别介绍了物理吸收和化学吸收过程的传质规律。总结了二氧化碳资源化利用的应用进展。展望了微化工技术在二氧化碳吸收与传质方面的发展前景。     

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.     

微通道内液-液两相流流型及传质的研究进展

微通道内液-液两相流流动在微化工系统中占有重要的地位,了解微通道内液-液两相流体流动和传质规律对推动其工业化应用有重要作用。本文以微通道内液-液两相流系统为研究对象,简述了不同工况下微通道内液-液两相流流型和混合传质效率,分析了微通道特征、流体性质和流体流动速度等对流型形成和传质效率的影响。指出目前对于微通道内液-液两相流的研究多处于定性研究,定量研究仅针对某一体系展开,所得结果具有一定的局限性。关于微通道内液-液两相流传质研究实验较多而数值模拟方法相对较少,接下来的研究工作中应该考虑建立微通道内液-液两相流基础研究的数据库,通过分析大量的数据获得有效的流型划分准则和相关经验式以此推动微通道内液-液两相流的工业化应用。同时在传质研究过程中应研究开发相应的数值模拟模型,保证实验和数值模拟相结合,提出有效的传质效率评价机制。     

垂直及倾斜上升管内气液两相弹状流壁面切应力的模拟

用VOF模型对垂直及倾斜上升管内弹状流壁面切应力进行数值模拟。计算结果表明,垂直上升流动时,液膜厚度始终小于对应位置倾斜上升弹状流的液膜厚度,壁面切应力从气弹头部至尾部逐渐增大至恒定不变,在尾流区呈杂乱无章状态。倾斜上升流动时,气泡头部顶点偏向管中心线上方,倾角越小,相同轴向位置处测得的液膜厚度越大。当FrTB较小时,倾斜管内弹状流上管壁面的切应力曲线在液膜区有明显波动,而下管壁面在对应区域的切应力分布则比较光滑。随着FrTB的增大,上下壁面切应力分布曲线越来越靠近。     

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.