Characterization of liquid–liquid mass transfer performance in a capillary microreactor system

Liquid–liquid mass transfer performance in a capillary microreactor system was studied with an improved experimental method. Proper sampling modes were chosen to eliminate the effect of the sampling zone on the mass transfer characterization in capillary microreactor systems. The overall volumetric mass transfer coefficients in the T‐micromixer and the capillary microreactor system were found to smoothly increase and then significantly increase with increasing the Reynolds number of two immiscible liquid phases. Other factors such as the inlet mode and inner diameter of T‐micromixer, the capillary length, and the volumetric flux ratio of the aqueous phase to the organic phase affected the mass transfer performance in the T‐micromixer and the capillary microreactor system. Furthermore, the contribution of the mass transfer in the T‐micromixer zone to the capillary microreactor system was found to be in a range of 34–78% under the involved experimental conditions, which was emphasized in the proposed empirical correlations. © 2017 American Institute of Chemical Engineers AIChE J, 64: 1106–1116, 2018     

Process intensification of high viscosity extraction system in microreactor via ultrasound-driven microbubbles

Aiming at the problem of weak mass transfer ability in high-viscosity-liquid systems, this paper carried out a study to introduce an inert gas into the ultrasonic microreactor to enhance the mass transfer process of the high-viscosity-liquid extraction system. Extraction of vanillin from aqueous solution to toluene was employed as a model to investigate the oscillation behavior of gas bubbles with varying shape and size as well as elucidate the enhancement mechanism of ultrasound-driven slug and microbubble on mass transfer process, respectively. The results can provide theoretical basis for the utilization of introducing gas on accelerating mass transfer between high viscous liquids. Finally, on the basis of the dimensionless Reynolds number of immiscible liquid and gas phase, and ultrasound input power, an empirical model was put forward to correlate the overall mass transfer coefficients, which shows good agreement with the measured values.     

声驱动微气泡强化微反应器内高黏体系萃取过程

针对高黏液-液体系中所存在的传质能力弱等问题,开展了在超声微反应器内导入惰性气体以强化高黏液-液萃取体系传质过程的研究。以甲苯萃取水相中香草醛过程为模型体系,研究了超声激发作用下,不同形状、尺寸气泡的振动行为,揭示了声驱动气弹与声驱动微气泡对该体系传质强化机制,为导入气体辅助超声强化高黏液体间的传质过程提供了理论基础。基于液相Reynolds数、气相Reynolds数和声能密度等参数,提出了预测超声微反应器内液-液总体积传质系数的经验关联式,预测值与实验值吻合良好。     

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。     

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     

Investigating the liquid film characteristics of gas–liquid swirling flow using ultrasound doppler velocimetry

A novel gas–liquid two‐phase flow metering method was proposed. A spiral vane mounted in the inner pipe was used to transform inlet flow patterns into gas–liquid swirling annular flow. The thickness and velocity profile of liquid film were measured by ultrasound Doppler velocimetry. The liquid flow rates were obtained by integrating of velocity profile during the liquid film zone. Experiments were carried out in an air–water two‐phase flow loop and an ultrasonic transducer was installed under the bottom of the test section with the Doppler angle of 70°. The flow patterns included stratified wavy, annular, and slug flows. Compared with non‐swirling flow, the liquid film thickness at the bottom reduces greatly. The measurement accuracy of liquid flow rate was independent of inlet flow patterns, gas and liquid velocities. © 2016 American Institute of Chemical Engineers AIChE J, 63: 2348–2357, 2017     

Hydrodynamics and mass transfer of oscillating gas‐liquid flow in ultrasonic microreactors

Ultrasonic microreactors were used to intensify gas‐liquid mass‐transfer process and study the intensification mechanism. Fierce surface wave oscillation with different modes was excited on the bubble. It was found that for slug bubbles confined in smaller microchannel, surface wave oscillations require more ultrasound energy to excite due to the confinement effect. Cavitation microstreaming with two toroidal vortices was observed near the oscillating bubble by a streak photography experiment. Surface wave oscillation at the gas‐liquid interface increases the specific surface area, while cavitation microstreaming accelerates the interface renewal and thus improves the individual mass‐transfer coefficient. With these two reasons, the overall mass‐transfer coefficient was enhanced by 3–20 times under ultrasonication. As for gas‐liquid flow hydrodynamics, ultrasound oscillation disturbs the bubble formation process and changes the initial bubble length and pressure drop. © 2015 American Institute of Chemical Engineers AIChE J, 62: 1294–1307, 2016     

Gas-liquid flow mass transfer in a T-shape microreactor stimulated with 1.7 MHz ultrasound waves

This paper describes the application of ultrasound waves on hydrodynamics and mass transfer characteristics in the gas-liquid flow in a T-shape microreactor with a diameter of 800 μm.A 1.7 MHz piezoelectric transducer (PZT) was employed to induce the vibration in this microreactor.Liquid side volumetric mass transfer coefficients were measured by physical and chemical methods of CO2 absorption into water and NaOH solution.The approach of absorption of CO2 into a 1 mol· L-1 NaOH solution was used for analysis of interfacial areas.With the help of a photography system,the fluid flow patterns inside the microreactor were analyzed.The effects of superficial liquid velocity,initial concentration of NaOH,superficial CO2 gas velocity and length of microreactor on the mass transfer rate were investigated.The comparison between sonicated and plain microreactors (microreactor with and without ultrasound) shows that the ultrasound wave irradiation has a significant effect on kLa and interfacial area at various operational conditions.For the microreactor length of 12 cm,ultrasound waves improved kLa and interfacial area about 21％ and 22％,respectively.From this study,it can be concluded that ultrasound wave irradiation in microreactor has a great effect on the mass transfer rate.This study suggests a new enhancement technique to establish high interfacial area and kLa in microreactors.     

Liquid–liquid two-phase flow and mass transfer characteristics in packed microchannels

In this work, the flow hydrodynamic characteristics and the mass transfer performance of immiscible fluids in the packed microchannels are investigated experimentally. Water–kerosene system is used for visually identifying the flow hydrodynamic characteristics in PMMA microchannels, and water–succinic acid–n-butanol is chosen for investigating mass transfer performance in stainless steel microchannels. Quartz sand micro-particles are used as packing particles. In packed microchannels, high liquid–liquid dispersions can be obtained, and the diameter of droplets produced in the packed microchannel can be even less than 10 μm. It ensures better mixing performance and larger effective interfacial area of two immiscible fluids, and improves the mass transfer performance obviously. Compared to the extraction efficiency (46–61%) in the non-packed microchannel, it can reach 81–96% in the packed microchannel. The effects of packing length, micro-particle size on liquid–liquid dispersions and extraction efficiency are investigated. The pressure drop and the specific energy dissipation in the packed microchannels are also discussed.     

不同强化方法对超临界CO2萃取人参皂甙的影响

为改善超临界CO2在萃取极性物质和传质方面的缺点,用自行设计的超声强化超临界CO2萃取设备,研究了夹带剂、超声和反相微乳技术对超临界CO2萃取人参皂甙的强化效果。实验条件设定为:萃取压力、温度与时间分别为25 MPa、45℃、4 h,CO2流量为2.0 L/h,分离压力与温度分别为6 MPa和55℃,超声频率、功率密度和辐照方式分别为20 kHz、100 W/L和6 s/6 s。实验结果发现,超声联合超临界CO2反相微乳萃取的人参皂甙萃取率分别是SC、MSC、UMSC和SCRM的13.9、4.9、3.1和1.8倍,其萃取固形物中皂甙的质量分数分别是SC和MSC的4.5和2.1倍;MSC、UMSC、SCRM和USCRM的人参皂甙萃取速率大小顺序依次为:USCRM>SCRM>UMSC>MSC;超声的加入不会改变对萃取人参皂甙的选择性和人参皂甙的结构。     

A continuous ultrasound‐assisted packed‐bed bioreactor for the lipase‐catalyzed synthesis of caffeic acid phenethyl ester

BACKGROUND: The focus of this paper is the ultrasound‐assisted synthesis of caffeic acid phenethyl ester (CAPE) from caffeic acid and phenyl ethanol in a continuous packed‐bed bioreactor. Immobilized Novozym^® 435 (from Candida antarctica) is used as the catalyst. A three‐level–three‐factor Box–Behnken design and a response surface methodology (RSM) are employed to evaluate the effects of temperature, flow rate, and ultrasonic power on the percentage molar conversion of CAPE. RESULTS: Based on ridge max analysis, it is concluded that the optimum condition for synthesis is reaction temperature 72.66 °C, flow rate 0.046 mL min^?1, and ultrasonic power 1.64 W cm^?2. The expected molar conversion value is 97.84%. An experiment performed under these optimal conditions resulted in a molar conversion of 92.11 ± 0.75%. The enzyme in the bioreactor was found to be stable for at least 6 days. CONCLUSIONS: The lipase‐catalyzed synthesis of CAPE by an ultrasound‐assisted packed‐bed bioreactor uses mild reaction conditions. Enzymatic synthesis of CAPE is suitable for use in the nutraceutical and food production industries. Copyright © 2011 Society of Chemical Industry     

超声场对栀子甙提取过程的强化

测定了在栀子果实中栀子甙在水溶液中浸取的固液平衡关系,不同强度超声场作用下栀子甙相平衡关系,研究比较了机械搅拌法和超声场介人下栀子甙的浸取率和浸取速率。实验结果表明：超声场可以改变浸取相平衡,超声场强度越大,固体中栀子甙吸附容量越小：超声场作用下使浸取率达到最高、浸取速率达到最大。超声场可有效强化液膜传质、粒内扩散,提高浸取率、加快浸取速率,能达到机械搅拌无法达到强化传质的效果。     

Investigation of multiphase hydrogenation in a catalyst‐trap microreactor

BACKGROUND: Multiphase hydrogenation plays a critical role in the pharmaceutical industry. A significant portion of the reaction steps in a typical fine chemical synthesis are catalytic hydrogenations, generally limited by resistances to mass and heat transport. To this end, the small‐scale and large surface‐to‐volume ratios of microreactor technology would greatly benefit chemical processing in the pharmaceutical and other industries. A silicon microreactor has been developed to investigate mass transfer in a catalytic hydrogenation reaction. The reactor design is such that solid catalyst is suspended in the reaction channel by an arrangement of catalyst traps. The design supports the use of commercial catalyst and allows control of pressure drop across the bed by engineering the packing density. RESULTS: This paper discusses the design and operation of the reactor in the context of the liquid‐phase hydrogenation of o‐nitroanisole to o‐anisidine. A two‐phase ‘flow map’ is generated across a range of conditions depicting three flow regimes, termed gas‐dominated, liquid‐dominated, and transitional, all with distinctly different mass transfer behavior. Conversion is measured across the flow map and then reconciled against the mass transfer characteristics of the prevailing flow regime. The highest conversion is achieved in the transitional flow regime, where competition between phases induces the most favorable gas–liquid mass transfer. CONCLUSION: The results are used to associate a mass transfer coefficient with each flow regime to quantify differences in performance. This reactor architecture may be useful for catalyst evaluation through rapid screening, or in large numbers as an alternative to macro‐scale production reactors. Copyright © 2008 Society of Chemical Industry     

Intensification of liquid–liquid two-phase mass transfer in a capillary microreactor system

A convenient strategy to intensify the liquid–liquid mass transfer performance in a capillary microreactor system was developed by narrowing the inlet channel of T-micromixer or adding baffles into the capillary. Various geometrical parameters such as the inlet mode and diameter of the modified T-micromixer, the number of baffles and interval distance between baffles in the modified capillary were investigated to elaborate the mass transfer intensification mechanism. The liquid–liquid two-phase flow patterns in new capillary microreactors were captured by a high-speed camera. Moreover, pressure drops and specific energy dissipation of these modified microreactor systems were studied and a new parameter indicating the ratio of the mass transfer coefficient to the energy dissipation was proposed. This work highlights the modified capillary microreactor systems with embedding baffle units for achieving high mass transfer rates with its advantages over other types of reactors or microreactors considering specific energy dissipation and effective energy utilization efficiency. © 2018 American Institute of Chemical Engineers AIChE J, 65: 334–346, 2019     

气升式反应器超声破碎海带提取硫酸酯多糖

在内径8cm、有效容积为1L的气升式循环超声破碎浸提装置中,进行了超声波强化海带硫酸酯的多浸提实验。在pH5．0、提取温度40℃、液固比45、提取时间25min、通气量75L/h、超声功率120W、超怕作用时间百分比为100％的工艺条件下,硫酸酯多糖的提取率可达1．86％,比传统水提法高,且大地缩短了提取时间,比相同条件下不用超声时的提取率（1．11％）高得多。此法所得多糖的SO4^2－含量（26．5％）比水法浸提（20．8％）和相同条件下不用超声时（21．3％）都要高,显示出超声波在强化海带硫酸酯多糖浸提方面的良好应用前景。     

Mass transfer and hydrodynamic characteristics in a co‐current downflow contacting column

Hydrodynamic and mass transfer characteristics of water–air system in a co‐current downflow contacting column (CDCC) were studied for various nozzle diameters at different superficial gas velocities and liquid re‐circulation rates. Gas hold‐up and liquid‐side mass transfer coefficient increased with increasing superficial gas velocity and liquid flow rate but decreased with increasing nozzle diameter. It is shown that correlations developed, which are based on liquid kinetic power per liquid volume present in the column, and superficial gas velocity explains gas hold‐up and the mass transfer coefficient within an error 20% for all gas and liquid flow rates and nozzle diameters used. The constants of correlations for gas hold‐up and mass transfer coefficient were found to be considerably different from other gas–liquid contacting systems. © 2003 Society of Chemical Industry     

Prediction of Concentration Profiles in an L‐Shaped Pulsed Extraction Column

The L‐shaped extraction pulsed plate column is believed to be able to perform under operating conditions between those of the vertical and the horizontal pulsed plate columns. It has an extraction efficiency similar to the vertical pulsed plate column. Here, the mass transfer performance of this novel column type was investigated and the application of three different models, i.e., the plug flow, the axial dispersion, and the back flow models, was evaluated to predict the solute concentration profile along the column length. The water‐acetone‐n‐butyl acetate and the water‐acetone‐toluene systems were used. The influence of the operational parameters on the height of the mass transfer unit and the back flow coefficients was evaluated using the back flow model. New correlations were proposed to predict the height of the mass transfer unit along with the back flow coefficients in each phase, which were in satisfactory agreement with the experimental data.     

微通道中气-液-液三相流流型及传质研究

使用双T型微通道,以体积分数为30%的磷酸三丁酯（TBP）的环己烷溶液-乙酸水溶液为萃取体系,研究了不同油水两相流量比及油水两相总流量条件下,气相的引入及气相流量分率α对流型及传质的影响,并获得总体积传质系数k_La与油水两相流量比q、气相雷诺数Re_g、液相平均雷诺数Re_M的关系式。研究结果表明,第1个T型接口处气相的引入所带来的气相剪切作用能促进第2个T型接口处分散相液滴的形成,可使液-液并行流转化为气-液-液三相弹状流;同时,由于气-液-液弹状流具有较高的相接触面积及内循环作用,传质系数k_La得到显著提高。     

Aerobic oxidation of 2-tert-butyl phenol within gas–liquid segmented flow: Mass transfer characteristics and scale-up

Quantifying the mass transfer of gas–liquid segmented flow in practical reactions is of significant for the scale-up design. However, there is a lack of theoretical guidance to predict operational conditions to meet required the mass transfer in a selective dimension-enlarged microreactor. Herein, the oxidation of 2-tert-butyl phenol (2-TBP) was performed in a selective dimension-enlarged capillary microreactor of 4.35 mm i.d. and optimal operation conditions were obtained. A high 2-tert-butyl-1,4-benzoquinone (2-TBQ) yield of 73% was achieved within 6 min. Moreover, a quantitative method to assess the mass transfer of gas–liquid segmented flow in practical reaction was developed by introducing a circulation frequency, f_cir, which could provide theoretical guidance to predict operating conditions for the scale-up production. The 2-TBQ productivity is significantly increased from 0.0061 to 0.5068 kg/h, that is, an increase of 83 times, by selective dimension enlarging from 2 mm to 4.35 mm with predicted operating conditions.     

Gas‐Liquid Mass Transfer in Fibrous Bed Reactor with Counter‐Current Liquid Recycle

In this work, the gas‐liquid mass transfer in a lab‐scale fibrous bed reactor with liquid recycle was studied. The volumetric gas‐liquid mass transfer coefficient, k_La, is determined over a range of the superficial liquid velocity (0.0042–0.0126 m.s^–1), gas velocity (0.006–0.021 m.s^–1), surface tension (35–72 mN/m), and viscosity (1–6 mPa.s). Increasing fluid velocities and viscosity, and decreasing interfacial tension, the volumetric oxygen transfer coefficient increased. In contrast to the case of co‐current flow, the effect of gas superficial velocity was found to be more significant than the liquid superficial velocity. This behavior is explained by variation of the coalescing gas fraction and the reduction in bubble size. A correlation for k_La is proposed. The predicted values deviate within ± 15 % from the experimental values, thus, implying that the equation can be used to predict gas‐liquid mass transfer rates in fibrous bed recycle bioreactors.