CO2-乙醇体系中界面对流的混合格子Boltzmann方法三维模拟及实验验证（英文）

By using a hybrid lattice-Boltzmann–finite-difference method (hybrid LBM–FDM method), three-dimensional simulations of solutal interfacial convection were conducted for the process of CO2 absorption into ethanol. A self-renewal interface model is adopted as an interfacial perturbation model. The simulation results revealed some three-dimensional features of the induced interfacial convection, such as the development of diverging cellular flow and Rayleigh plume-like convection in liquid phase. The concentration distribution of the simulation result is validated and found to be in wel agreement with the Schlieren visualization results qualitatively. Addi-tionally, the mass transfer enhancements by interfacial convection were investigated via both simulation and experiment for the absorption process, and the mass transfer is shown to be enhanced by the interfacial convec-tion by about two-fold comparing with that by diffusion.     

The Numerical Analysis of the Gas-Liquid Absorption Process Accompanied by Rayleigh Convection

Flow and concentration fields of liquid phase in a gas-liquid contacting system are simulated to show the Rayleigh convection by utilizing the finite-element method. The Schlieren images in CO2-ethanol system provided direct visual verification of the present simulation, and the simulated results were well consistent with the experimental observation. The influence of the Rayleigh convection on mass transfer is analyzed qualitatively and quantitatively based on the simulated and the experimental results.     

伴有Rayleigh对流的气液吸收过程数值模拟

Flow and concentration fields of liquid phase in a gas-liquid contacting system are simulated to show the Rayleigh convection by utilizing the finite-element method. The Schlieren images in C02-ethanol system provided direct visual verification of the present simulation, and the simulated results were well consistent with the experimental observation. The influence of the Rayleigh convection on mass transfer is analyzed qualitatively and quantitatively based on the simulated and the experimental results.     

Entransy dissipation analysis of interfacial convection enhancing gas–liquid mass transfer process based on field synergy principle

An exploration of the gas CO2 absorbed into liquid ethanol accompanied with Rayleigh convection is performed by analyzing the mass entransy dissipation; this new statistical quantity is introduced to describe the irreversibility of mass transfer potential capacity. Based on the general advection–diffusion differential equation for an unsteady mass transfer process, the variation of the included angle between the velocity vector and concentration gradient fields is investigated to reveal the underlying mechanism of interfacial convection enhancing mass transfer. Results show some identical characteristics with the qualitative analyses of the synergy effects generated by the concentration and velocity fields after interfacial convection occurring for a boundary condition of fixed surface concentration. And the equivalent mass resistance for convective mass transfer process presents the similar variation with the reciprocal of instantaneous mass transfer coefficient. Accordingly, it is reasonable to be seen that mass transfer dissipation rate could be provided to assess the convection strength and explain fundamentally how Rayleigh convection improves mass transfer performance through establishing a close relationship between the mass transfer capacity and field synergy principle from the view of mass transfer theory.     

精馏塔板液相流场三维模拟

The liquid flow on a single-pass sieve distillation tray is simulated with a three-dimensionM computational fluid dynamics (CFD) program with the K-e turbulence model. In the model, a source term SMi is formulated in the Navier-Stokes equations to represent the interfacial momentum transfer and another term Sc is added to the mass transfer equation as the source of interfacial mass transfer. The simulation provides the detailed information of the three-dimensionM distribution of liquid velocity on the tray, the circulation area and the concentration profile along the height of liquid layer.     

Three Dimensional Simulation of Liquid Flow on Distillation Tray

The liquid flow on a single-pass sieve distillation tray is simulated with a three-dimensional computational fluid dynamics (CFD) program with the K-ε turbulence model. In the model, a source term SMi is formulated in the Navier-Stokes equations to represent the interfacial momentum transfer and another term SC is added to the mass transfer equation as the source of interfacial mass transfer. The simulation provides the detailed information of the three-dimensional distribution of liquid velocity on the tray, the circulation area and the concentration profile along the height of liquid layer.     

A Reynolds mass flux model for gas separation process simulation:I. Modeling and validation

Separation process undertaken in packed columns often displays anisotropic turbulent mass diffusion. The aniso-tropic turbulent mass diffusion can be characterized rigorously by using the Reynolds mass flux (RMF) model. With the RMF model, the concentration and temperature as well as the velocity distributions can be simulated numerical y. The modeled Reynolds mass flux equation is adopted to close the turbulent mass transfer equation, while the modeled Reynolds heat flux and Reynolds stress equations are used to close the turbulent heat and mo-mentum transfer equations, so that the Boussinesq postulate and the isotropic assumption are abandoned. To val-idate the presented RMF model, simulation is carried out for CO2 absorption into aqueous NaOH solutions in a packed column (0.1 m id, packed with 12.7 mm Berl saddles up to a height of 6.55 m). The simulated results are compared with the experimental data and satisfactory agreement is found both in concentration and temper-ature distributions. The sequel Part II extends the model application to the simulation of an unsteady state ad-sorption process in a packed column.     

MASS TRANSFER IN TURBULENT PULSATING FLOWS

The effect of flow oscillation to the mass transfer between turbulent fluid and solid wall was investigatedby measuring the mass transfer rate between fluid and pipe wall with imposed oscillating flow usingelectrochemical method.The velocity and concentration field in the viscous sublayer which controls the mass trans-fer in such a process was simulated by a simple wave model of single harmonics.Experimental results confirmthat the flow oscillation has no influene on time averaged mass transfer rate,but the phase difference betweenphase averaged velocity field and concentration field shifts with the frequency of imposed oscillating flow.Numeri-cal analysis reveals that the concentration boundarylayer which is responsible for the mass transfer is muchthinner than the viscous sublayer which greatly weakens the influence of imposed oscillating flow on mass transfer.     

两液层体系传质引发的Marangoni效应的数值模拟

The Marangoni effect induced by mass transfer at the interface between two immiscible liquids displays important influence on laboratory and industrial operation of solvent extraction. A systematic numerical study of the two-dimensional Marangoni effect in a two liquid layer system was conducted. The linear relationship of the inter- facial tension versus the solute concentration was incorporated into a mathematical model accounting for liquid flow and mass transfer in both phases. The typical cases analyzed by Sternling ＆ Scriven （AIChE J., 1959） using the linear instability theory were simulated bv the finite difference method and good agreement between the theory and the numerical simulation was observed. The simulation suggests that the Marangoni convection needs certain time to develop sufficiently in strength and scale to enhance the interphase mass transfer, the Marangoni effect is dynamic and transient, and remains at some stabilized level as long as the mass transfer driving force is kept con- stant. When certain level of shear is imposed at the interface as in most cases of practical significance, the Maran- goni effect is suppressed slightly but progressively as the shear is increased gradually. The present two-dimensional simulation of the Marangoni effect provides some insight into the underlying mechanism and also the basis for further theoretical study of the three-dimensional Marangoni effect in the real world and in chemical engineering applications.     

Prediction of mass transfer coefficients in an asymmetric rotating disk contactor using effective diffusivity

Mass transfer characteristics have been investigated in a 113 mm diameter asymmetric rotating disk contactor of the pilot plant scale for two different liquid–liquid systems. The effects of operating parameters including rotor speed and continuous and dispersed phase velocities on the volumetric overall mass transfer coefficients are investigated. The results show that the mass transfer performance is strongly dependent on agitation rate and interfacial tension, but only slightly dependent on phase flow rates. In this study, effective diffusivity is used instead of molecular diffusivity in the Gr?ber equation for estimation of dispersed phase overall mass transfer coefficient.The enhancement factor is determined experimentally and there from an empirical expression is derived for prediction of the enhancement factor as a function of Reynolds number. The predicted results compared to the experimental data show that the proposed correlation can efficiently predict the overall mass transfer coefficients in asymmetric rotating disk contactors.     

伴有Rayleigh对流的气液传质理论

浓度梯度导致的Rayleigh对流会对界面传质产生重要影响。采用格子Boltzmann方法(LBM)对吸收过程伴有Rayleigh对流的气液传质理论进行了分析。针对表面更新理论,提出了将近界面处羽状对流结构的宽度作为特征尺度来求得表面更新时间。结果表明,Rayleigh对流的发生能够有效减小双膜理论中的液膜厚度;液相传质系数的LBM模拟值与表面更新理论预测值吻合较好。     

水溶解CO2过程界面对流现象的PIV/LIF测量及传质系数预测

建立了用于观测水溶解CO₂过程界面Rayleigh对流现象的粒子成像测速（PIV）和激光诱导荧光（LIF）技术联用方法,同时获得了该对流传质过程的液相速度场及浓度分布,定量观测了Rayleigh对流的发展过程。经界面对流发生条件下传质过程的分析,指出Rayleigh对流过程的涡量是影响传质过程的主要因素,给出了传质系数随涡量的变化关系和相应的关联式,进而为通过液相速度场的测量预测Rayleigh对流条件下的液相传质系数提供了一种有效的方法。     

采用格子Boltzmann方法模拟解吸过程中的Rayleigh对流

应用二维非稳态格子Boltzmann方法研究了异丙醇-水溶液和丙酮-乙酸乙酯溶液解吸过程中Rayleigh对流的临界开始时间、流动特征及其对界面传质的影响,并与相关文献对比. 结果表明,临界开始时间随界面浓度增加呈先缓慢增大再迅速增大最后趋于稳定的变化趋势. Rayleigh对流结构经历了从有序到无序的发展过程,是不断更新的耗散结构. Rayleigh对流主要作用于液相主体,使液相主体具有较大的湍动速度(10-4~10-3 m/s). 液相主体中存在许多循环流动,促进了界面更新及界面与液相主体之间液体的交换与混合. 传质增强因子(介于2~6之间)表明Rayleigh对流能有效提高解吸过程传质速率,强化界面传质过程.     

PIV Measurement for Rayleigh Convection and Its Effect on Mass Transfer☆

The velocity distribution in Rayleigh convection caused by acetone volatilization in acetone-ethyl acetate binary system was observed in a vertical cross section of an initially quiescent liquid layer ...     

气相第2组分对水溶解CO2过程界面对流影响的LIF观测

采用激光诱导荧光（LIF）观测方法考察了在气相中分别添加乙醇和二氯甲烷分别对CO₂在水中溶解过程界面对流的影响,得到了液相中CO₂浓度分布及其演化的观测结果,通过物料衡算得到了相应条件下的液相传质系数。CO₂溶解过程会出现由密度梯度引起的Rayleigh对流。实验结果表明,当添加的乙醇含量小于8.47 mg·L^-1时,Rayleigh对流会被增强,进而促进了CO₂的溶解;随着气相中乙醇含量的增大,Rayleigh对流反而被抑制;气相添加二氯甲烷会显著增强Rayleigh对流,提高了CO₂的传质速率,随着气相二氯甲烷含量的增大,CO₂在水中溶解过程的液相传质系数呈现先加强后恒定的趋势。     

格子Boltzmann方法模拟咸水吸收CO2的Rayleigh对流过程

由溶解的CO₂引发的Rayleigh对流,对咸水层中CO₂的捕获与封存至关重要。为了更加直观地了解该过程的混合规律和盐浓度变化带来的影响,本文采用格子Boltzmann方法（LBM）对该过程进行了模拟。通过建立包含密度和浓度分布函数的双分布模型,同时引入静电力和体积力等外力项,对293.15K、101kPa下有多个离散的CO₂扩散源时的浓度分布进行了模拟。结果表明,模拟得到的Rayleigh对流结构、对流发生时间、流场速度和瞬时传质通量的数量级与前人研究结果一致;在咸水吸收CO₂过程中,Rayleigh对流结构可有效强化传质;瞬时传质通量随着时间增长先减小后增大再减小,对应了Rayleigh对流结构产生、发展、稳定的变化过程。同时模拟CO₂在纯水和不同盐浓度咸水中的溶解过程结果表明,盐浓度的增加会延迟Rayleigh对流的开始时间、降低传质效率,这与前人的实验结果一致,模拟结果可为不同盐浓度咸水层中CO₂的封存提供指导。     

界面传质中Rayleigh对流的定量分析

通过纹影光路观察了特定气液传质装置中乙醇吸收CO₂过程所引发的Rayleigh对流在垂直界面方向上的发展过程。随着溶质吸收的进行,液层的流体稳定性变弱,扰动加剧气液界面失稳并发生湍动,进而发展为羽状流并逐步向液相主体发展,在此过程中伴随着对流胞的融合与增长。液层的浓度分布可通过对相应液层纹影图像进行定量分析获得。液层浓度分布和瞬时传质系数变化表征了Rayleigh对流的引发与发展及其对传质过程的强化效果,界面浓度分布及临界Rayleigh数解释了非均匀传质对湍动的引发机理。羽状流将高浓度液体快速带入主体,加速了近界面液层与主体液层的混合,增强了气液传质。     

Spatial Scale Effects on Rayleigh Convection and Interfacial Mass Transfer Characteristics in CO2 Absorption

Concentration gradient‐induced Rayleigh convections in the CO₂ absorption process were investigated by the hybrid Lattice‐Boltzmann/finite‐difference method (LBM‐FDM). The spatial scale effects on Rayleigh convection were studied by simulating Rayleigh convections with different liquid layers. The scale of convection increased with the liquid layer height but the average mass transfer coefficient showed the adverse tendency. The Rayleigh convection had a pronounced effect on the surface renewal. For better assessment of the renewal intensity, two statistical quantities were proposed. The transient variations of these quantities provided a good following feature with the mass transfer coefficient which confirms their accuracy and precision in characterizing the mass transfer process.