Mixing and residence time distribution in ultrasonic microreactors

Intensification of liquid mixing was investigated in domestic fabricated ultrasonic microreactors. Under the ultrasonic field, cavitation bubbles were generated, which undergo vigorous translational motion and surface oscillation with different modes (volume, shape oscillation, and transient collapse). These cavitation phenomena induce intensive convective mixing and reduce the mixing time from 24–32 s to 0.2–1.0 s. The mixing performance decreases with the channel size, due to the weaker cavitation activity in smaller channel. The energy efficiency is comparable to that of the conventional T‐type and higher than the Y‐type and Caterpillar microreactors. Residence time distribution was also measured by a stimulus‐response experiment and analyzed with axial dispersion model. Axial dispersion was significantly reduced by the ultrasound‐induced radial mixing, leading to the increasing of Bo number with ultrasound power. © 2016 American Institute of Chemical Engineers AIChE J, 63: 1404–1418, 2017     

Liquid–liquid two‐phase flow in ultrasonic microreactors: Cavitation,emulsification, and mass transfer enhancement

The effects of ultrasound on the hydrodynamic and mass transfer behaviors of immiscible liquid–liquid two‐phase flow was investigated in a domestic ultrasonic microreactor. Under ultrasonic irradiation, cavitation bubble was generated and underwent violent oscillation. Emulsification of immiscible phases was initiated by virtue of oscillating bubbles shuttling through the water/oil interface. The pressure drop was found to decrease with increasing ultrasound power, with a maximum decrement ratio of 12% obtained at power 30 W. The mass transfer behavior was characterized by extraction of Rhodamine B from water to 1‐octanol. An enhancement factor of 1.3–2.2 on the overall mass‐transfer coefficient was achieved under sonication. The mass transfer performance was comparable to passive microreactor at similar energy dissipation rate (61–184 W/kg). The extraction equilibrium was reached under a total flow velocity 0.01 m/s and input power 20 and 30 W, exhibiting its potential use in liquid‐liquid extraction process. © 2017 American Institute of Chemical Engineers AIChE J, 64: 1412–1423, 2018     

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     

Automated measurements of gas‐liquid mass transfer in micropacked bed reactors

Gas‐liquid mass transfer in micropacked bed reactors is characterized with an automated platform integrated with in‐line Fourier transform infrared spectroscopy. This setup enables screening of a multidimensional parameter space underlying absorption with chemical reaction. Volumetric gas‐liquid mass‐transfer coefficients (k_La) are determined for the model reaction of CO₂ absorption in a methyl diethanolamine/water solution. Parametric studies are conducted varying gas and liquid superficial velocities, packed bed dimensions and packing particle sizes. The results show that k_La values are in the range of 0.12～0.39 s^?1, which is about one‐to‐two orders of magnitude larger than those of conventional trickle beds. An empirical correlation predicts k_La in micropacked bed reactors in good agreement with experimental data. © 2017 American Institute of Chemical Engineers AIChE J, 64: 564–570, 2018     

Bubble/droplet formation and mass transfer during gas–liquid–liquid segmented flow with soluble gas in a microchannel

Microchannels have great potential in intensification of gas–liquid–liquid reactions involving reacting gases, such as hydrogenation. This work uses CO₂–octane–water system to model the hydrodynamics and mass transfer of such systems in a microchannel with double T‐junctions. Segmented flows are generated with three inlet sequences and the size laws of dispersed phases are obtained. Three generation mechanisms of dispersed gas bubbles/water droplets are identified: squeezing by the oil phase, cutting by the droplet/bubble, cutting by the water–oil/gas–oil interface. Based on the gas dissolution rate, the mass transfer coefficients are calculated. It is found that water droplet can significantly enhance the transfer of CO₂ into the oil phase initially. When bubble‐droplet cluster are formed downstream the microchannel, droplet will retard the mass transfer. Other characteristics such as phase hold‐up, bubble velocity and bubble dissolution rate are also discussed. The information is beneficial for microreactor design when applying three‐phase reactions. © 2016 American Institute of Chemical Engineers AIChE J, 63: 1727–1739, 2017     

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.     

Gas-liquid-liquid slug flow and mass transfer in hydrophilic and hydrophobic microreactors

Gas-liquid-liquid three-phase slug flow was generated in both hydrophilic and hydrophobic microreactors with double T-junctions. The bubble-droplet relative movement and the local mass transfer within the continuous slug and the dispersed droplet were investigated. It was found that bubbles moved faster than droplets under low capillary number (Ca), while droplets moved faster upon the increase of Ca due to the increased inertia. For the first time, we observed that the increased viscosity of droplets fastened the droplet movement. The mass transfer in the continuous slug was dominated by convection, leading to nearly constant global mass transfer coefficient (k_La); while that in the dispersed droplet was dominated by diffusion, resulting in k_L decreasing along the channel. Such features are analogical to the corresponding gas-liquid or liquid-liquid two-phase slug flow, but the formation of bubble-droplet clusters caused by relative movement lowered the absolute mass transfer coefficient. These results provide insights for the precise manipulation of gas-liquid-liquid slug flow in microreactors towards process optimization.     

The effect of system pressure on gas‐liquid slug flow in a microchannel

Characteristics of gas‐liquid two‐phase flow under elevated pressures up to 3.0 MPa in a microchannel are investigated to provide the guidance for microreactor designs relevant to industrial application. The results indicate that a strong leakage flow through the channel corners occurs although the gas bubbles block the channel. With a simplified estimation, the leakage flow is shown to increase with an increase in pressure, leading to a bubble formation shifting from transition regime to squeezing regime. During the formation process, the two‐phase dynamic interaction at the T‐junction entrance would have a significant influence on the flow in the main channel as the moving velocity of generated bubbles varies periodically with the formation cycle. Other characteristics such as bubble formation frequency, bubble and slug lengths, bubble velocities, gas hold‐up, and the specific surface area are also discussed under different system pressures. © 2013 American Institute of Chemical Engineers AIChE J, 60: 1132–1142, 2014     

Bubble shape,gas flow and gas–liquid mass transfer in pulp fibre suspensions

Gas–liquid mass transfer in pulp fibre suspensions in a batch‐operated bubble column is explained by observations of bubble size and shape made in a 2D column. Two pulp fibre suspensions (hardwood and softwood kraft) were studied over a range of suspension mass concentrations and gas flow rates. For a given gas flow rate, bubble size was found to increase as suspension concentration increased, moving from smaller spherical/elliptical bubbles to larger spherical‐capped/dimpled‐elliptical bubbles. At relatively low mass concentrations (C_m = 2–3% for the softwood and C_m ? 7% for the hardwood pulp) distinct bubbles were no longer observed in the suspension. Instead, a network of channels formed through which gas flowed. In the bubble column, the volumetric gas–liquid mass transfer rate, k_La, decreased with increasing suspension concentration. From the 2D studies, this occurred as bubble size and rise velocity increased, which would decrease overall bubble surface area and gas holdup in the column. A minimum in k_La occurred between C_m = 2% and 4% which depended on pulp type and was reached near the mass concentration where the flow channels first formed.     

Hydrodynamics of gas–liquid flow in micropacked beds: Pressure drop,liquid holdup,and two‐phase model

Hydrodynamics of gas–liquid two‐phase flow in micropacked beds are studied with a new experimental setup. The pressure drop, residence time distribution, and liquid holdup are measured with gas and liquid flow rates varying from 4 to 14 sccm and 0.1 to 1 mL/min, respectively. Key parameters are identified to control the experimentally observed hydrodynamics, including transient start‐up procedure, gas and liquid superficial velocities, particle and packed bed diameters, and physical properties of the liquids. Contrary to conventional large packed beds, our results demonstrate that in these microsystems, capillary forces have a large effect on pressure drop and liquid holdup, while gravity can be neglected. A mathematical model describes the hydrodynamics in the micropacked beds by considering the contribution of capillary forces, and its predictions are in good agreement with experimental data. © 2017 American Institute of Chemical Engineers AIChE J, 63: 4694–4704, 2017     

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.     

Application of extended quadrature method of moments for simulation of bubbly flow and mass transfer in gas‐liquid stirred tanks

In the present paper, two gas‐liquid stirred tanks, one agitated by a radial impeller and another by an axial impeller, are modelled using the open‐source computational fluid dynamic (CFD) package OpenFOAM (open source field operation and manipulation). The combined effect of the bubble break‐up and coalescence in the tank is considered by a population balance model (PBM) called extended quadrature method of moments (EQMOM). The three‐dimensional simulation is made using a multiple reference frame (MRF), a well‐established method for the modelling of mixers. Dispersed gas and bubble dynamics in the turbulent flow are modelled using the Eulerian‐Eulerian approach (E‐E) with mixture k‐epsilon turbulent model and the modified Tomiyama drag coefficient for the momentum exchange. The model is developed to predict the spatial distribution of gas phase fraction, Sauter mean bubble diameter (), number density function (NDF), dissolved oxygen (DO) evolution, and flow structure. The numerical results are compared with experimental data and a fair agreement is achieved. The results of the axial impeller are discussed based on four impeller rotational speeds with different volumetric mass transfer coefficients.     

Gas-liquid mass transfer in taylor flow through a capillary

The gas-liquid mass transfer in two-phase flow through a capillary has been measured for water-air, ethanol-air and ethylene glycol-air systems. A semi-theoretical model has been developed and compared with experimental results. and a full computer simulations of the flow pattern and mass transfer using a flow simulation program have been made. The measured values are about 30% less than the calculated values.     

超声微反应器内气液传质过程的介尺度强化机制

采用CFD方法对超声微反应器内的Taylor气液两相流的传质过程进行了模拟。针对传质过程中主要的介尺度结构,包括气泡表面波、空化声流、液相内的局部浓度,分析了其空间分布和时间演化规律。模拟结果有效捕捉了实验难以观测的液膜区域,并将液膜厚度与气泡表面波振动进行了关联,阐释了气液界面附近的空化声流对传质过程的强化作用。根据超声微反应器内Taylor流的传质特点,分别研究了不同流动和超声条件对液弹内和液膜处传质过程的影响,比较了各局部传质对整体传质效率的贡献。通过分析整体/局部Sherwood数与Peclet数间的关系,研究了超声效应对气液传质速率的影响。分析结果从介尺度角度验证了文献关于超声微反应器传质系数的计算,完善了超声微反应器内气液传质过程的强化理论。     

Liquid-liquid two-phase flow patterns and mass transfer characteristics in rectangular glass microreactors

The flow of two immiscible fluids was investigated in rectangular glass microchannels with equivalent diameters of 269 and . Deionised water, dyed toluene and hexane were selected as probe fluids. Flow patterns were obtained for Y- and T-junction of two micro-channels and monitored by a photo-camera. Volumetric velocities of water and organic phase varied between 1 and 6 ml/h. The formation mechanism of slug and parallel flow was studied and the mass transfer performances of two flow patterns were compared. The shape of the interface between the immiscible liquids was controlled by a competition between the viscous forces and the local interfacial tension. The flow patterns could be correlated with the mean Capillary and Reynolds numbers. The mass transfer coefficients for parallel and slug flow were determined using instantaneous neutralisation (acid-base) reaction. The two flow patterns showed the same global volumetric mass transfer coefficients in the range of , being affected mainly by the base concentration in water for parallel flow and by the linear velocity in the case of the slug flow.     

整体式床层中液体分布与气-液传质的关系

With a particular focus on the connection between liquid flow distribution and gas-liquid mass transfer in monolithic beds in the Taylor flow regime, hydrodynamic and gas-liquid mass transfer experiments were carried out in a column with a monolithic bed of cell density of 50 cpsi with two different distributors (nozzle and packed bed distributors). Liquid saturation in individual channels was measured by using self-made micro-conductivity probes. A mal-distribution factor was used to evaluate uniform degree of phase distribution in monoliths. Overall bed pressure drop and mass transfer coefficients were measured. For liquid flow distribution and gas-liquid mass transfer, it is found that the superficial liquid velocity is a crucial factor and the packed bed distributor is better than the nozzle distributor. A semi-theoretical analysis using single channel models shows that the packed bed distributor always yields shorter and uniformly distributed liquid slugs compared to the nozzle distributor, which in turn ensures a better mass transfer performance. A bed scale mass transfer model is proposed by employing the single channel models in individual channels and incorporating effects of non-uniform liquid distribution along the bed cross-section. The model predicts the overall gas-liquid mass transfer coefficient with a relative error within ±30%.     

毛细管中泰勒流液侧传质特性及其强化机理的CFD模拟

采用计算流体力学（CFD）的方法,研究了圆管中泰勒流的液侧传质特性,分析了泰勒气泡上局部传质特性,并研究了气泡上升速度、液膜长度和液栓长度对液膜处和气泡半球帽处平均传质系数的影响。结果表明,泰勒气泡表面局部传质系数存在3个峰值,液膜处的平均传质系数随气泡上升速度增大显著增大,随液膜长度增大而减小,而半球帽处的平均传质系数随气泡速度和液膜长度的增大变化较小,即膜接触时间增加时,液膜处的传质系数降低,而半球帽处传质系数变化较小。另外,引入场协同原则对单元胞内速度场和浓度场进行分析,解释了局部传质特性及强化机理。最后,给出了分别预测短和长膜接触时间下泰勒流液侧体积传质系数的关联式,该式在较宽的管径尺度范围（0.25～3 mm）内的预测误差在±20%以内。