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。     

Comparison of hydrodynamic and mass transfer performances of an emulsion loop-venturi reactor in cocurrent downflow and upflow configurations

Hydrodynamic parameters (gas-induced flow rate and gas hold-up) and mass transfer characteristics (k_La, k_L and a) have been investigated in a gas–liquid reactor denoted “Emulsair” in which the distributor is an emulsion-venturi and the gas phase is self-aspired by action of the kinetic energy of the liquid phase at the venturi throat. Two configurations, respectively cocurrent downflow and cocurrent upflow were compared. A chemical method involving the dispersion of a CO₂–air mixture in a monoethanolamine (MEA) aqueous solution was used to measure mass transfer parameters. Experimental results showed that only the homogeneous bubbling regime prevailed in the upward configuration, while an annular regime could also be observed for cocurrent downflow at low liquid flow rate. Gas-induced flow rate and gas hold-up were usually smaller for cocurrent upflow, both at constant liquid flow rate and specific power input. The same stood for mass transfer properties. Conversely, specific power requirements were lower at constant liquid flow rate and mass transfer characteristics were enhanced at constant gas-induced flow rate for cocurrent upflow. A comparison with other gas–liquid contacting devices showed that the Emulsair reactor is a versatile tool avoiding the presence of mechanically moving parts when high and quickly adaptable dissolved gas supply is required. The cocurrent upflow configuration can be preferred when high gas flow rates are desired because the evolutions of gas-induced flow rate and mass transfer characteristics exhibit a stronger dependence on specific power input in the homogeneous bubbling regime for this configuration.     

Calculation of flow fields in two and three-phase bubble columns considering mass transfer

The dimension of bubble column reactors is often based on empirical correlations. Very popular is the axial dispersion model. However, the applicability of these models is limited to the experimental conditions for which the dispersion coefficients are measured, because backmixing depends strongly on the columns dimension and the flow regime. This paper presents a numerical method for the calculation of the three-dimensional flow fields in bubble columns based on a multi-fluid model. Therefore, the local bubble size distribution is considered by a transport equation for the mean bubble volume, which is obtained from the population balance equation. For comparison with experimental results, the axial dispersion coefficients in the liquid and gas phase are calculated from the instationary, three-dimensional concentration fields of a tracer. The model is then extended to include mass transfer between the gas and liquid phase. Increasing mass transfer rates significantly influence the flow pattern. For several applications, a dispersed solid phase is added. For the calculation of three-phase gas-liquid-solid flow, the solid phase is considered numerically by an additional Eulerian phase.     

筛型塔板在喷射及混合状态操作下三相传质性能

以空气-水-油(煤油及白油)为介质在600mm×150mm矩形冷模塔内测试了筛型塔板气液液三相传质性能。研究喷射及混合状态下,气速、液流强度、油水比等操作条件和塔板结构参数(孔径、开孔率)对塔板效率的影响。气膜和液膜控制的2种物系的实验表明,三相传质的板效率在喷射状态下明显高于混合状态。对测试数据进行关联,获得适用于喷射及混合状态下三相传质板效率的估算式。     

Mass Transfer In Trickle‐Bed Reactors With Structured Packing

An experimental investigation was carried out to examine the fluid dynamic and mass transfer behavior of structured packing, with the liquid and gas phase flowing co‐currently downwards in the column. Liquid to packing mass transfer coefficients for three positions within the pack were measured by an electrochemical method, varying both the liquid and gas loads as well as the physical properties of the liquid phase. Due to the high void fraction of structured packing, much higher liquid flow rates can be used than in traditional particle trickle‐beds. It was found that in the range studied, the gas superficial velocity has no effect on the mass transfer rate and thus, a general mass transfer correlation in terms of liquid Reynolds number only, was developed. Wetted areas and the radial distribution of liquid through the packing element were determined by a colorimetric method. Within the range of liquid flow rates investigated, complete wetting is not achieved, even with the low viscosity solutions. The measured ratios of hydraulic to geometric area, agree reasonably well with values predicted by existing relationships.     

假塑性流体的雾化研究：Ⅱ.二流式喷嘴的结构与尺寸参数

本文以气流式喷嘴的雾化机理为基础，研究了用于雾化高粘度物料（假塑性流体）的二流式喷嘴的结构形式和尺寸参数。通过雾化试验研究，初步得到了以较小的气液比雾化高粘度物料，并具有良好雾化特性的二流式喷嘴。     

RADIAL DISPERSION AND BUBBLE CHARACTERISTICS IN THREE-PHASE FLUIDIZED BEDS

The effects of gas and liquid velocities, liquid viscosity and particle size on the radial dispersion coefficient of liquid phase (D_r) and the bubble properties in three-phase fluidized beds have been determined. A new flow regime map based on the drift flux theory in three-phase fluidized beds has been proposed.

In three-phase fluidized beds, D, increases with increasing gas velocity in the bubble coalescing and in the slug flow regimes, but it decreases in the bubble disintegrating regime. The coefficient exhibits a maximum value in the bed of small particles with increasing liquid velocity at lower gas velocities. However, it increases with increasing liquid velocity at higher gas velocities. In two and three-phase fluidized beds of larger particles (6,8 mm), D_r exhibits a maximum value with an increase in liquid viscosity at lower gas velocities, but it increases at higher gas velocities. The mean bubble chord length and its rising velocity increase with increasing gas velocity and liquid viscosity. However, the bubble chord length decreases with an increase in liquid velocity and it exhibits a maximum value with increasing particle size in the bed. The radial dispersion coefficients in the bubble coalescing and disintegrating regimes of three-phase fluidized beds in terms of the Peclet number in the present and previous studies have been well represented by the correlations based on the concept of isotropic turbulence theory.     

Mass transfer in trickle-bed reactors at low reynolds number

Mass transfer rates were determined in a 3.4 cm i.d. trickle-bed reactor in the absence of reaction by absorption measurements and in presence of reaction. Gas flow rates were varied from 0-100 l/h and liquid flow rates from 0-1.5 l/h. The catalyst particles were crushed to an average diameter of 0.054 and 0.09 cm. Mass transfer coefficients remained unaffected by change in gas flow rate but increased with liquid rate. The data from absorption measurements were evaluated with predictions based upon plug-flow and axial dispersion model. Mass transfer coefficients were found greater in case of axial dispersion model than that of plug-flow model specially at low Reynolds number (Re₁ < 1).Hydrogenation of α-methylstyrene to cumene using a Pd/Al₂O₃ catalyst was taken as a model reaction. Intrinsic kinetic studies were made in a laboratory-stirred-autoclave. Mass transfer coefficients were determined using these intrinsic kinetic data from the process kinetic measurements in trickle-bed reactor. Mass transfer coefficients under reaction conditions were found to be considerably higher than those obtained by absorption measurements.Correlations were suggested for predicting mass transfer coefficients at low Reynolds number.The gas to liquid mass transfer coefficients for lower gas and liquid flow rates were determined in a laboratory trickle-bed reactor. The effect of axial dispersion on mass transfer was considered in order to evaluate the experimental data. Three correlations were formulated to calculate the mass transfer coefficients, which included the effect of liquid loading, particle size and the properties of the reacting substances. The gas flow rate influences the gas to liquid mass transfer only in the region of low gas velocities. In the additional investigations of gas to liquid mass transfer without reaction in trickle-bed reactor, the mass transfer coefficients were determined under reaction conditions and the intrinsic kinetics was studied in a laboratory scale stirred autoclave with suspended catalyst. A few correlations are formulated for the mass transfer coefficients. A comparison with the gas-liquid mass transfer coefficient obtained by absorption measurements showed considerable deviations, which were illustrated phenomenologically.     

Interpretation of mass transfer measurements in bubble columns considering dispersion of both phases

Mass transfer measurements in two bubble columns with an inner diameter of 100 resp. 140 mm with the systems air/water/carbon dioxide and nitrogen/n-propanol/carbon dioxide have been evaluated with the axial dispersion model. The dispersion coefficients of both phases have been determined in separate investigations. As the results revealed a strong influence of the liquid viscosity, additional dispersion coefficient measurements have been carried out with the system air/glycol. It could be shown that the liquid phase dispersion coefficient decreases with increasing viscosity while the gas phase dispersion coefficient increases with increasing liquid viscosity. Both coefficients are strongly dependent on the gas throughput and the column diameter. Using these coefficients, the mass transfer coefficients have been calculated by fitting the calculated concentration profile to the measured values and by splitting the volumetric mass transfer coefficient with the experimental value of the interfacial are a. The results agree best with a correlation of Calderbank and Moo-Young.     

Distillation tray efficiency and interfacial area

Three pure liquids, viz. water, ethanol and toluene were evaporated in air on a 10 cm dia. sieve plate to ascertain the effect of liquid properties on the mass transfer in the gas phase.

It was found that two extreme forms of dispersion exist on the tray, viz. a liquid dispersion (droplets) at high air velocity and low liquid hold-up, and an air dispersion (bubbles) at lower air velocity and higher liquid hold-up.

The mass transfer outside the jetting droplets is found to increase with increasing air velocity and with decreasing surface tension.

The mass transfer of the cellular foam is found to decrease as the air velocity increases, and is correlated with an internal circulation Re-number and a Fo-number for the contact time.

The difference in bubbling mechanism between bubbles rising from a single orifice and those rising from closely spaced orifices is discussed.     

Gas Holdup and Solid‐Liquid Mass Transfer in Newtonian and non‐Newtonian Fluids in Bubble Columns

Gas holdup and surface‐liquid mass transfer rate in a bubble column have been experimentally investigated. De‐mineralized water, 0.5 and 1.0% aqueous solutions of carboxy methyl cellulose (CMC), and 60% aqueous propylene glycol have been used as the test liquids. Effects of column diameter, liquid height to column diameter ratio, superficial gas velocity and liquid phase viscosity on gas holdup and mass transfer rate are studied. Generalized correlations for the average gas holdup and wall to liquid heat and mass transfer coefficients are proposed. These are valid for both Newtonian and pseudoplastic non‐Newtonian fluids.     

Liquid phase axial mixing in a bubble column with viscous non-newtonian liquids

This paper presents some new data for the liquid phase axial dispersion coefficient in a bubble column with highly viscous non-Newtonian liquids (μ_L > 0.03 Pa · s). The data were obtained in a 0.15 m diameter column operating in the slug flow regime, and the dispersion measurements were conducted using heat aas a tracer. The experimental results show that the dispersion coefficients increase with both gas and liquid velocities and quantitatively they are about three times higher than those obtained for the air-water system. The results are explained based on a known hydrodynamic model of vertical gas-liquid slug flow.     

EFFECT OF VISCOSITY ON HYDRODYNAMIC PROPERTIES OF PULSING FLOW IN TRICKLE BEDS

New data on pulsing flow onset, properties of pulses (frequency, celerity, length), liquid holdup and pressure drop are presented for aqueous glycerol solutions of viscosity 6.7 and 20.2 mPa s and compared with similar measurements from an air-water (1.0 mPas) system. With the exception of viscosity, all other physical properties of the liquid phase are kept constant and fairly close to those of water, thus allowing a direct assessment of the effect of viscosity. Pulse formation and propagation with viscous liquids is examined on the basis of time records from a conductance type technique. A striking effect due to increased liquid viscosity is the reduction of the pulsing flow regime; in particular, the pulsing-to-bubbling transition boundary is shifted towards higher gas flow rates. Pulse frequency and celerity appear to decrease only slightly with increasing liquid viscosity, whereas the two-phase pressure gradient increases significantly. Liquid holdup also tends to increase with viscosity. Moreover, holdup with viscous liquids tends to increase significantly with the liquid flow rate, whereas an insignificant effect is found for water. A new correlation for estimating liquid holdup is proposed, and a simple model for predicting pulsing flow characteristics is modified in order to take account of the aforementioned effects.     

Gas-Liquid mass transfer in fixed beds with two-phase cocurrent downflow: Gas/newtonian and non-newtonian liquid systems

New data of gas-liquid mass transfer for cocurrent downflow through packed beds of porous and non-porous particles are presented. Mass transfer parameters for air/carbon dioxide/water, air/carbon dioxide/carboxymethylcellulose solution and air/carbon dioxide/sodium hydroxide systems were evaluated by least square fit of the calculated CO₂ concentration profiles in gas phase to the experimental values. The volumetric liquid-side mass transfer coefficient increases with the increase of the flow consistency index of the liquid. A comparison of the volumetric liquid-side mass transfer coefficient values evaluated with and without taking into account the axial dispersion shows that the influence of the liquid axial dispersion is significant at low liquid velocity and high CMC concentrations, and the influence of the gas axial dispersion is insignificant.     

Microstructured reactors and supports for ionic liquids

Different types of microstructures and their applications with respect to the synthesis and the use of ionic liquids are presented. Microstructured reactors are suitable for reactions with fast intrinsic kinetics, requiring high mass and heat transfer performances. Chemical synthesis can be performed safely under operating condition (e.g. high temperature, pressure, etc.) difficult to obtain in traditional reactors. The examples presented clearly indicate that microstructured reactors offer superior performance for the synthesis of ionic liquids in comparison to conventional equipment. For the use of ionic liquids as reaction media, existing ionic liquids show some limitations due to their higher viscosity compared to conventional solvents. Therefore, future research should be focused on the development of low viscosity ionic liquids.The approaches to use ionic liquids in microstructured reactors and in combination with microstructured supports for catalytic reactions show many advantages in view of high product selectivity and yield. The use of supported ionic liquids on microstructured materials seems to be particularly promising for gas phase as well as for gas/liquid reactions.     

Experimental investigation of fast-mode liquid modulation in a trickle-bed reactor

Unsteady-state operation of trickle-bed reactors (TBRs) is a promising technique to improve reactor performances especially when mass transfer phenomena are rate controlling. Among the different techniques, fast-mode modulation of the liquid flow rate seems to be one of the most successful. In fact cycling the liquid flow rate at very low frequencies can induce the reactor to work at the high-interaction regime where mass and heat transfer phenomena are strongly enhanced. Fast-mode periodic operation, then, can be considered an extension of the natural high-interaction regime at a mean range of gas and liquid flow rate normally associated with trickling regime in steady-state conditions.Experimental tests have been performed in a TBR employing α-methyl styrene hydrogenation on Pd/C catalyst in unsteady-state conditions by “on-off” fast-mode liquid modulation. Results have been compared with the steady-state experiments at the corresponding average liquid flow rate, revealing a conversion rate improvement up to 60%. All experiments have been performed in isothermal conditions, so conversion improvement can be ascribed only to mass transfer increase and not to thermal effects. The variation of gas and liquid flow rates and liquid cycle parameters presented several important implications about the optimal working conditions.     

Internal Mass Transfer during Isothermal Drying of a Porous Solid Containing Multicomponent Liquid Mixtures

Internal mass transfer in a porous solid partially saturated with multicomponent liquids has been experimentally and theoretically studied. Isothermal drying experiments were performed using a jacketed wind tunnel where the transient composition profiles and total liquid content of a cylindrical sample were determined. Sand samples wetted with the ternary liquid mixtures water-methanol-ethanol and 2-propanol-methanol-ethanol were dried at two different initial compositions and temperatures. A mathematical model including mass transfer by capillary movement of the liquid and interactive diffusion in both gas and liquid phase was developed. To simulate the capillary movement of liquid mixtures, parameters experimentally determined for single liquids where weighed according to liquid composition. A fairly good agreement between theoretical and experimental liquid composition profiles was obtained provided that axial dispersion is included in the model.     

Internal Mass Transfer during Isothermal Drying of a Porous Solid Containing Multicomponent Liquid Mixtures

Abstract

Internal mass transfer in a porous solid partially saturated with multicomponent liquids has been experimentally and theoretically studied. Isothermal drying experiments were performed using a jacketed wind tunnel where the transient composition profiles and total liquid content of a cylindrical sample were determined. Sand samples wetted with the ternary liquid mixtures water-methanol-ethanol and 2-propanol-methanol-ethanol were dried at two different initial compositions and temperatures. A mathematical model including mass transfer by capillary movement of the liquid and interactive diffusion in both gas and liquid phase was developed. To simulate the capillary movement of liquid mixtures, parameters experimentally determined for single liquids where weighed according to liquid composition. A fairly good agreement between theoretical and experimental liquid composition profiles was obtained provided that axial dispersion is included in the model.     

Phase inversion and mass transfer during liquid–liquid dispersed flow through mini-channel

The present study aims to identify means of process intensification during liquid–liquid flow through a mini-channel. During liquid–liquid flow, depending on the flow conditions either the organic or the aqueous phase can be dispersed and with increase in flow velocity the dispersed phase can spontaneously invert to form the continuous phase or vice-versa. The present study aims to investigate the phenomena of phase inversion and its influence on mass transfer during toluene/acetic acid-water flow in a 1.98 mm glass mini-channel. It is observed that for organic phase as dispersed regime, higher mass transfer efficiency is achieved when the liquid–liquid mixture is in the phase inversion zone which marks the transition from organic to aqueous phase dispersion. The mixture velocities as well as the inlet concentration of diffusing species influence mass transfer characteristics in this zone. The results have indicated some interesting observations which can be exploited for process intensification in monolith and micro-reactor.     

Liquid back-mixing in packed-bubble column reactors: a state-of-the-art correlation

The extent of liquid back-mixing in gas–liquid concurrent upflow packed-bubble column reactors is quantified in terms of an axial dispersion coefficient or its corresponding dimensionless Péclet number. Effects of reactor operating conditions on the axial dispersion coefficient are not properly accounted for by the available literature correlations, wherein most often the Péclet number is expressed solely in terms of the gas and liquid Reynolds numbers or superficial velocities. Based on the broadest experimental databank (1322 measurements, 11 liquids, four gases, 28 packing materials, 14 columns diameters, Newtonian, non-Newtonian, aqueous, organic, coalescing and non-coalescing liquids, high pressure, bubble and pulsing flow regime conditions), a state-of-the-art liquid axial dispersion coefficient correlation is obtained by combining neural network modeling and dimensional analysis. Thorough qualitative and quantitative analyses of the constructed databank demonstrate the robustness of the proposed correlation to restore the variety of trend variations of liquid Péclet numbers reported in the literature.