用可视化方法实验研究规整填料的局部传质(英文)

A chromochemical reactive mass transfer technique has been employed to study local mass transfer characteristics of structured packing. This technology adopted by experiment is an Ammonia Adsorption Method (AAM) that yields the surface distribution of transferred mass by analyzing the color distribution on a filter paper with the results of the color chemical reaction. A digital image processing technology is applied for data visualiza-tion. The three-dimensional plot of the local mass transfer coefficients shows that there exist three peak values on different positions of a unit cell of structured packing. In order to improve mass transfer efficiency of the structured packing, one piece of baffle is added between packing sheets. As a result, the average mass transfer coefficient in-creases by (10-20)% and the pressure drop decreases by (15-55)%.     

Axial Mixing and Mass Transfer Performance of an Annular Pulsed Disc-and-Doughnut Column

The annular pulsed disc-and-doughnut column (APDDC) is an important type of extraction equipment in the PUREX process, which has been used in several commercial reprocessing plants. As there are few mass transfer experimental results reported in the literature, the axial mixing and mass transfer performance of an APDDC was studied for both extraction and stripping processes in the present work. Two parameters in the axial dispersion model (ADM), namely, the axial dispersion coefficient of the continuous phase and the number of mass transfer units, were regressed by correlating ADM with experimental concentration profiles. The influence of flow rate and pulsation intensity on these parameters was also investigated. Models developed for the PDDC were tested for correlation with APDDC experimental data and suitable models and conditions were determined. The height of a mass transfer unit was also calculated, which highlights the impact of axial mixing on mass transfer performance. Moreover, the influence of internal wettability on mass transfer performance was discussed.     

Investigation of hydrodynamic and mass transfer of mercaptan extraction in pulsed and non-pulsed packed columns

We investigated the hydrodynamic behavior and mass transfer characteristics of a pilot-scale conventional packed bed extraction column of mercaptan removal from liquid propane. The extraction column was filled with pall rings structured packing where mercaptan was extracted from the continuous phase to the dispersed phase, accompanied by a chemical reaction in propane-mercaptan-caustic system. The pulsing was introduced into the column to enhance the mass transfer rate. Hydrodynamic parameters such as hold up, flooding velocity and mean drop size were studied together with the effect of chemical reaction on increasing mass transfer performance. Finally, the mass transfer and axial mixing coefficients were obtained from the optimization of data by ADM. It was found that at the pulsation intensity from 0.003 to 0.007 m/s, the maximum mass transfer and minimum axial mixing occurred and it can be concluded that pulsation improves the efficiency of mass transfer just at low intensities.     

Mass transfer with chemical reaction in liquid foam reactors

Mass transfer studies were conducted in a stable liquid foam reactor under various operating conditions to evaluate gas holdup, effective interfacial area, liquid-phase mass transfer coefficient and a modified interfacial mass transfer coefficient to include the surface-active agents employed. Gas holdup and effective interfacial area were evaluated experimentally. The interfacial mass transfer coefficient was evaluated semitheoretically, by considering the interfacial region as a separate phase and using the experimental data developed for mass transfer accompanied by a fast first-order chemical reaction. The liquid-phase mass transfer coefficient was also evaluated semitheoretically, using Danckwert's theory for the liquid phase and the experimental data on mass transfer accompanied by a slow pseudofirst-order chemical reaction. An experimental unit was set up to provide a stable flowing foam column, simulating the foam reactor. Mass transfer rates were studied for superfacial gas velocities in the range from 1.5 × 10⁻² m/s to 5 × 10⁻² m/s, giving gas residence times in the range from 20 to 55 seconds. A cationic and nonionic surface-active agent and three different wire mesh sizes, giving bubble size distributions in the range from 2.2 to 5.4 mm Sauter mean diameters, were employed. It is observed that gas holdup is insensitive to the type of surface-active agent; it is however, dependent on wire mesh size and gas velocity. The bubble diameter and, hence, the interfacial area are found to be insensitive to gas velocity in the range studied; they are, however, strong functions of wire mesh size. The liquid-phase mass transfer coefficient increases with increase in gas velocity. The surface-active agent introduces additional resistance to mass transfer in both reaction cases, this being the controlling one in the case of the fast reaction. A comparison with conventional packed bed contactors indicates the mass transfer rates to be about 8 times lower for the foam reactor, for the fast reaction case; for slow reactions, the foam reactor has mass transfer rates approximately 2-4 times higher than those for conventional packed bed contactors.     

Hydrodynamik und Stofftransport in einem Perlschnurreaktor für Gas/Flüssig/Fest‐Reaktionen

In this work, a pellet string reactor was characterized with respect to hydrodynamics and mass transfer. The catalyst packing consists of a cylindrical channel with a diameter of 1.41 mm, which was filled with spherical catalyst particles, having an outer diameter of 0.8 mm. Under reaction conditions (liquid phase hydrogenation of α‐methylstyrene) overall (gas‐liquid‐solid) volumetric mass transfer coefficients for hydrogen between 0.8 and 5.5 s^–1 were computed. Due to high mass transfer rates and simple reactor geometry, pellet string reactors can be applied in industry as highly efficient reaction units.     

Influence of mass transfer direction on efficiency of a pulsed perforated plate column

The purpose of this paper is to give a complete analysis of the influence of mass transfer direction on the performance of a pulsed perforated plate-column.The ternary system studied was water—iodine—carbon tetrachloride. Both mass transfer directions were considered, i.e. iodine transfering from continuous aqueous phase to dispersed organic phase and vice versa.Parameters considered are overall efficiency, hold up, true number of transfer units, Peclet number for both phases, drop size, interfacial area and overall mass transfer coefficient.     

微孔射流毛细管反应器内液-液两相传质和反应选择性

微反应技术在化工过程强化领域已得到广泛应用,尤其适用于快速复杂竞争反应体系。对于液-液两相快速竞争反应,反应过程受传质限制,显著影响反应转化率和收率。本文开发了一种新型的微孔射流毛细管反应器（MJCM）,采用微孔射流强化进口处液-液两相传质性能,分别采用水-苯甲酸-煤油体系和水-氢氧化钠-甲苯-苯甲酸-氯乙酸乙酯体系研究了不同操作参数（流量、流量比、表面活性剂浓度、温度）和结构参数（孔径、管长）下液-液两相传质特性和反应选择性,并获得了舍伍德数Sh的关联式。结果表明：随着两相流量的增加,传质效率E呈下降趋势,总体积传质系数k_La呈增加趋势,反应选择性指数X_s则先减小后增大;孔径的增大则会减弱液液传质和反应选择性;随着毛细管长的增加,E和X_s逐渐增大,k_La则逐渐减小;水相-有机相流量比的变化对E和k_La会产生不同影响,而温度的适当升高则可以提升反应选择性,表面活性剂的加入降低了传质和反应选择性。与其他液液传质设备对比,MJCM在液-液两相传质、反应选择性方面性能良好,可以用于工业生产进行液液传质与反应过程的强化。     

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.     

Sulphur dioxide absorption into sodium sulphite solutions in a cable contactor

An experimental investigation of the rate of sulphur dioxide absorption into sodium sulphite solutions in a cable contactor was made at room temperature for several gas velocities, liquid flow rates and pH values. Correlations were derived giving the overall gas mass transfer coefficients, enhancement factors and heights of transfer units for a cable-bundle scrubber. It was found that the enhancement factors are very high and that the absorption rate is mainly controlled by the gas film mass transfer resistance. Modelling of the operation according to the two-film theory of absorption with chemical reaction allowed the calculation of theoretical values of the overall mass transfer coefficient, which were found to be in good agreement with experimental results.     

双搅拌釜中脱硫催化剂再生的传质反应过程

在双搅拌釜中,考察了ＴＨＳ、ＡＤＡ、ＴＦ三种催化剂的再生氧化传质速度随液相传质数变化的规律,并以效果最好的ＴＨＳ的对象,进一步考察了催化剂浓度、温度、ｐＨ等因素对其再生氧化传质速度的影响。研究了用液相催化氧化法脱硫化氢的催化剂再生的传质反应过程。     

运动颗粒对传质过程影响的格子Boltzmann模拟

颗粒的主动运动对传质过程有重要影响.以表面恒浓度的二维球形颗粒为研究对象,采用耦合传质的格子Boltzmann方法(LBM)模拟了颗粒在自旋和振动两种情况下的相间传质过程.选择浸入运动边界法和非平衡态外推法处理运动颗粒边界,研究了颗粒自旋速度、颗粒振幅及振动频率对传质过程的影响.结果表明,中等雷诺数的自旋颗粒绕流中,随...     

EXPERIMENTAL DETERMINATION AND MODELLING OF LIQUID-SOLID MASS TRANSFER COEFFICIENTS IN A THREE-PHASE REACTOR

Apparent mass transfer coefficients for solid dissolution in a liquid with and without a chemical reaction were experimentally determined in a fixed bed three phases reactor with downward cocurrent gas and liquid flows. The chemical system selected was benzoic acid, sodium hydroxide in aqueous solution, and atmospheric air. Continuous gas, pulse and dispersed bubble regimes were studied and the results were correlated obtaining apparent mass transfer coefficient as a function of liquid and fluid volumetric flow. It was found that gas flow effect on mass transfer coefficient was small over continuous gas and dispersed bubble regimes, but appreciable over pulse regime. Additionally, it was found that the mathematical model that best described the mass transfer process under pulse regime, by using the increment factor due to the instantaneous chemical reaction, is the film theory     

圆盘反应器中的PET缩聚过程

利用薄膜实验研究了PET缩聚过程反应和传质规律 ,建立了链增长、链降解反应动力学模型和泡沫脱挥时的传质速率方程 ;通过冷模实验研究了圆盘反应器中PET的混合、流动、成膜、膜表面更新以及传质规律 ;综合了反应和反应器研究结果 ,建立了圆盘反应器中的PET缩聚过程模型 ,对圆盘反应器中的PET缩聚过程进行了仿真分析 ,考察了温度、压力、停留时间、转速、催化剂浓度、负荷大小等各种因素的影响     

Recovery of carbon monoxide from flue gases by reactive absorption in ionic liquid imidazolium chlorocuprate(I):Mass transfer coefficients

Recovery of carbon monoxide from flue gases by selective absorption of carbon monoxide in an imidazolium chlorocuprate(I) ionic liquid is considered in this work as an alternative to the use of molecular volatile solvents such as aromatic hydrocarbons. The present work evaluates the CO mass transfer rates from the gas phase to the ionic liquid solutions in the absence of chemical reaction. To that end, carbon dioxide was employed as an inert model gas and absorption experiments were performed to assess the influence of different process variables in a batch reactor with flat gas–liquid interface. The experimental mass transfer coefficients showed significant var-iation with temperature, (3.4–10.9) × 10-7 m·s-1 between 293 and 313 K; stirring speed, (10.2–33.1) × 10-7 m·s-1 between 100 and 300 r·min-1;and concentration of copper(I), (6.6–10.2) × 10-7 m·s-1 between 0.25 and 2 mol·L-1. In addition, the mass transfer coefficients were eventually found to follow a poten-tial proportionality of the type kL∝μ-0.5 and the dimensionless correlation that makes the estimation of the mass transfer coefficients possible in the studied range of process variables was obtained:Sh=10-2.64·Re1.07·Sc0.75. These results constitute the first step in the kinetic analysis of the reaction between CO and imidazolium chlorocuprate(I) ionic liquid that determines the design of the separation units.     

Some aspects of the mechanism of cellular convection

The mechanism of cellular convection during absorption accompanied by chemical reaction was investigated. It was found that the reaction rate had a considerable effect on the occurrence of the phenomenon in the case studied. The effect was proved to be quite analogous to that of the gas phase mass transfer coefficient on the cellular convection accompanying physical absorption. This conclusion explains the occurrence of the cellular convection during chemisorption even when there is a negligible resistance to mass transfer in the gas phase, i.e. with mass transfer coefficients in this phase approaching infinity.     

Transport and reaction in catalytic wall-flow filters

Diesel particulate filters composed of so-called wall-flow monoliths are well established devices for diesel particulate abatement. Recent improvements in production technology allow implementation of full-featured catalyst functionality in the filter walls.

From a reactor engineering point of view such wall-flow reactors with wall-integrated catalyst show fundamental differences compared to conventional flow-through monoliths. The complex interactions of convection, diffusion and reaction in the wall-flow monolith are studied by means of numerical simulation. A two-dimensional model for the flow in one pair of inlet/outlet channels with a generic first order reaction in the catalytic filter wall is developed. Concentration profiles in the reactor and a conventional flow-through catalyst are compared.

It is found that in the range of moderate reactor conversion concentration gradients along the inlet channel of the filter are small. Thus the reactor can be described by an approximate one-dimensional model, taking into account only the radial flux through the filter wall and assuming a constant inlet concentration in axial direction along the inlet channel.

Light-off curves are computed for the wall-flow and for the conventional flow-through monolith. Significantly better conversion is found for the wall-flow configuration. This can be explained by mass transfer limitation in the conventional flow-through monolith.     

Reactive mass transfer at gas-liquid interfaces: impact of micro-scale fluid dynamics on yield and selectivity of liquid-phase cyclohexane oxidation

The impact of single-bubble wake dynamics on the reaction-enhanced mass transfer and on the yield and selectivity of the cyclohexane oxidation reaction was studied using a two-dimensional CFD-reaction model that was developed by our group. Temperature and the concentrations of the (desired) intermediate and (undesired) final products of this autocatalytic reaction were the parameters of this study. Two bubble types were studied: (a) a circular bubble with closed wake, and (b) an elliptical bubble with an unsteady, vortex-shedding wake. The main results of our work are: (1) Film theory over-predicts reaction-enhanced mass transfer since the assumption of an average film thickness is not justified. In order to study fast reaction systems on a reactor scale using coarse-grid CFD codes, a full bubble model, or correlations based on it, should be incorporated as a sub-grid micro model. (2) The bubble wake does not contribute to mass transfer in systems where reaction rates are low. For fast reactions, the local mass transfer rate in the wake can increase by several thousand percent. (3) Vortex shedding causes qualitatively different mixing since patches rich in the dissolved gas are quickly convected away from the bubble. Bubbles that cause vortex shedding will lead to a significantly higher conversion per volume than spherical bubbles. (4) Parallel-consecutive reactions with a high liquid-phase reactant concentration and with reaction rates that depend in an identical way on the dissolved gas concentration, are not micro-mixing sensitive in terms of selectivity. Since bubble shapes and sizes can be controlled by changing operating and design parameters, the yield of this reaction can be controlled.     

Kinetics of sunflower oil methanolysis catalyzed by calcium oxide

The methanolysis of sunflower oil was studied in the presence of CaO previously calcined at various temperatures and the optimal temperature for CaO calcination was determined. The sigmoidal process kinetics was explained by the initial triglyceride (TG) mass transfer controlled region, followed by the chemical reaction controlled region in the latter reaction period. The TG mass transfer limitation was due to the small available active specific catalyst surface, which was mainly covered by adsorbed molecules of methanol. In the later phase, the adsorbed methanol concentration decreased, causing the increase of both the available active specific catalyst surface and the TG mass transfer rate, and the chemical reaction rate become smaller than the TG mass transfer rate.     

化工原理传质单元操作工程研究的方法论

基于对化工原理课程中各传质单元操作工程研究方法的分析,笔者论述了各传质单元操作的研究方法,在相平衡描述、传质速率描述、物料衡算、极限处理法和技术经济性分析等几个方面存在着共同的特征。掌握这一共性特征,对于整体上把握传质单元操作的教学内容和教学方法,具有认识论和方法论上的意义。     

Nitration of nitrobenzene at high‐concentrations of sulfuric acid: Mass transfer and kinetic aspects

This article reports studies on mass transfer and kinetics of nitration of nitrobenzene at high concentrations of sulfuric acid in a batch reactor at different temperatures. The effects of concentration of sulfuric acid, speed of stirring, and temperature on mass transfer coefficient were investigated. The kinetics of nitration under homogenized conditions was studied at different sulfuric acid concentrations at these temperatures. The reaction rate constants were determined. The variation of rate constant with sulfuric acid concentration was explained by the M_c function. The activation energies of the reactions were determined from the Arrhenius plots. The regimes of the reactions were determined using the values of the mass transfer coefficients and the reaction rate constants. A model was developed for simultaneous mass transfer and chemical reaction in the aqueous phase. The yields of the three isomers of dinitrobenzene were determined, and the variation of isomer distribution with sulfuric acid concentration and temperature was analyzed. This work demonstrates that more than 90% conversion of nitrobenzene is possible at high‐sulfuric acid concentrations resulting in high yield of the product even at moderate temperatures and at low speeds of stirring. © 2009 American Institute of Chemical Engineers AIChE J, 2010