三相鼓泡淤浆床环氧乙烷合成反应器数学模拟及工程分析

建立了加压三相鼓泡淤浆床环氧乙烷合成反应器的数学模型 ,计入了催化剂颗粒在床层中沉降形成沿床高浓度分布对反应的影响以及由于惰性液相载体部分返混对传递的影响 ,进一步利用经实验验证的上述数学模型模拟不同表观气速、床高、反应器直径 (扣除传热元件截面积 )、进口乙烯摩尔分数等参数对床层中催化剂浓度随床高的分布、出口环氧乙烷摩尔分数、环氧乙烷选择率以及单位质量催化剂环氧乙烷年产量的影响 .通过模拟分析预示了工业三相床环氧乙烷反应器的合理尺寸、表观气速、环氧乙烷选择率以及时空产率 ,为工业化提供必要的设计依据     

矩形鼓泡塔流体动力学数值模拟

鼓泡塔反应器内流体动力学特性预测对于鼓泡塔的设计和发展具有重要意义。文中应用CFX4.4商业软件,采用k-ε模型中气泡诱发湍流模型,对较高鼓泡塔中湍流弥散力影响和Tomiyama模型的作用进行了数值模拟。研究发现,目前通用的湍流弥散力对所研究的气泡流体动力学影响很小,引入带有气泡诱发湍流模型的Tomiyama模型能获得较好的速度分布。在这种情况下,Pfleger&Becker的模型要优于Troshko&Hassan模型,原因在于后者高估气泡诱发湍流时间尺度。     

网格和数值格式对TBPBM-CFD模型模拟鼓泡塔的影响

基于气泡动力学属性的现有认识,把气泡分成大、小气泡,首次建立了完整的双气泡相-群平衡模型(TBPBM)以预测气泡尺寸.通过编写用户自定义程序实现了TBPBM模型、Luo破碎模型以及Prince 聚并模型,并耦合TBPBM与CFD双流体模型对直径440 mm鼓泡塔进行数值模拟,详细考察了网格与数值格式对TBPBM-CFD模型模拟结果的影响.结果表明,网格与数值格式对各物理变量的模拟结果影响非常大,特别是网格和体积分数方程对流项离散格式的影响最为显著.随着计算精度的提高,湍流耗散率和整体气含率分布梯度增大,气泡平均直径减少,大气泡所占气相比率降低,液相速度及气含率径向分布与实验值更趋吻合.     

CFD simulation of gas-liquid contacting in tubular reactors

Gas-liquid contacting in tubular reactors was simulated using an Eulerian-Eulerian CFD approach in which accurate interphase momentum closure relations are incorporated, bubble-induced turbulence is accounted for, and population balance equations are used to describe bubble breakage and coalescence. The ability of two breakup kernels (Luo, H., Svendsen, H.F., 1996. Theoretical model for drop and bubble breakup in turbulent dispersions. A.I.Ch.E. Journal 42, 1225-1233; Lehr, F., Millies, M., Mewes, D., 2002. Bubble size distributions and flow fields in bubble columns. A.I.Ch.E. Journal 48, 2426-2443) and three coalescence kernels (Prince, M.J., Blanch, H.W., 1990. Bubble coalescence and breakup in air sparged bubble columns. A.I.Ch.E. Journal 36, 1485-1499; Luo, H., 1993. Coalescence, breakup and liquid recirculation in bubble column reactors. Ph.D. Thesis, Norwegian University of Science and Technology, Trondheim; Lehr, F., Millies, M., Mewes, D., 2002. Bubble size distributions and flow fields in bubble columns. A.I.Ch.E. Journal 48, 2426-2443) to accurately predict several flow parameters in pipe flow was tested.Good agreement between simulation and experimental results (radial profiles of gas holdup, turbulence intensity, and local Sauter bubble diameter) was achieved without the use of empirically derived relationships (such as Drift flux) by adjusting a single parameter which accounts for the deviation in the coalescence behaviour of tap water from that of pure water. The approach adopted in this investigation may thus be applicable to more complex hydrodynamic situations such as those encountered in mechanically agitated tanks and the need for extensive experimental testing may be replaced by single measurement of the effect interfacial properties have on coalescence rates.     

Studies on hydrodynamics of turbulent slurry bubble column（Ⅲ）Effect of vertical pipe bundles

浆态床反应器内部往往安装有密集的竖直列管换热内构件,有关列管束对流场分布的影响还少有研究。本文在Φ500 mm×5000 mm的大型冷模实验装置中测定了安装不同密度列管束时的速度分布和气含率分布。实验表明,列管的存在一方面会显著提高浆料轴向速度,促进大尺度流体循环,另一方面也抑制了液体与气泡的径向湍动,使速度和气含率的径向分布更不均匀,造成液体与气体轴向返混加剧,增大了有列管束的浆态床反应器的放大风险。在低气速湍动鼓泡条件下,列管加入造成的“烟囱效应”将更为显著。     

湍动浆态床流体力学研究（Ⅲ）垂直列管内构件的影响

浆态床反应器内部往往安装有密集的竖直列管换热内构件,有关列管束对流场分布的影响还少有研究。本文在Φ500 mm×5000 mm的大型冷模实验装置中测定了安装不同密度列管束时的速度分布和气含率分布。实验表明,列管的存在一方面会显著提高浆料轴向速度,促进大尺度流体循环,另一方面也抑制了液体与气泡的径向湍动,使速度和气含率的径向分布更不均匀,造成液体与气体轴向返混加剧,增大了有列管束的浆态床反应器的放大风险。在低气速湍动鼓泡条件下,列管加入造成的“烟囱效应”将更为显著。     

CFD modeling of slurry bubble column reactors for Fisher-Tropsch synthesis

Industrial bubble column reactors for Fischer-Tropsch (FT) synthesis include complex hydrodynamic, chemical and thermal interaction of three material phases: a population of gas bubbles of different sizes, a liquid phase and solid catalyst particles suspended in the liquid. In this paper, a CFD model of FT reactors has been developed, including variable gas bubble size, effects of the catalyst present in the liquid phase and chemical reactions, with the objective of predicting quantitative reactor performance information useful for design purposes. The model is based on a Eulerian multifluid formulation and includes two phases: liquid-catalyst slurry and syngas bubbles. The bubble size distribution is predicted using a Population Balance (PB) model. Experimentally observed strong influence of the catalyst particles concentration on the bubble size distribution is taken into account by including a catalyst particle induced modification of the turbulent dissipation rate in the liquid. A simple scaling modification to the dissipation rate is proposed to model this influence in the PB model. Additional mass conservation equations are introduced for chemical species associated with the gas and liquid phases. Heterogeneous and homogeneous reaction rates representing simplified FT synthesis are taken from the literature and incorporated in the model.Hydrodynamic effects have been validated against experimental results for laboratory scale bubble columns, including the influence of catalyst particles. Good agreement was observed on bubble size distribution and gas holdup for bubble columns operating in the bubble and churn turbulence regimes. Finally, the complete model including chemical species transport was applied to an industrial scale bubble column. Resulting hydrocarbon production rates were compared to predictions made by previously published one-dimensional semi-empirical models. As confirmed by the comparisons with available data, the modeling methodology proposed in this work represents the physics of FT reactors consistently, since the influence of chemical reactions, catalyst particles, bubble coalescence and breakup on the key bubble-fluid drag force and interfacial area effects are accounted for. However, heat transfer effects have not yet been considered. Inclusion of heat transfer should be the final step in the creation of a comprehensive FT CFD simulation methodology. A significant conclusion from the modeling results is that a highly localized FT reaction rate appears next to the gas injection region when the syngas flow rate is low. As the FT reaction is exothermal, it may lead to a highly concentrated heat release in the liquid. From the design perspective, the introduction of appropriate heat removal devices may be required.     

CFD simulation of bubble columns incorporating population balance modeling

A computational fluid dynamics (CFD)-code has been developed using finite volume method in Eulerian framework for the simulation of axisymmetric steady state flows in bubble columns. The population balance equation for bubble number density has been included in the CFD code. The fixed pivot method of Kumar and Ramkrishna [1996. On the solution of population balance equations by discretization—I. A fixed pivot technique. Chemical Engineering Science 51, 1311-1332] has been used to discretize the population balance equation. The turbulence in the liquid phase has been modeled by a k-ε model. The novel feature of the framework is that it includes the size-specific bubble velocities obtained by assuming mechanical equilibrium for each bubble and hence it is a generalized multi-fluid model. With appropriate closures for the drag and lift forces, it allows for different velocities for bubbles of different sizes and hence the proper spatial distributions of bubbles are predicted. Accordingly the proper distributions of gas hold-up, liquid circulation velocities and turbulence intensities in the column are predicted. A survey of the literature shows that the algebraic manipulations of either bubble coalescence or break-up rate were mainly guided by the need to obtain the equilibrium bubble size distributions in the column. The model of Prince and Blanch [1990. Bubble coalescence and break-up in air-sparged bubble columns. A.I.Ch.E. Journal 36, 1485-1499] is known to overpredict the bubble collision frequencies in bubble columns. It has been modified to incorporate the effect of gas phase dispersion number. The predictions of the model are in good agreement with the experimental data of Bhole et al. [2006. Laser Doppler anemometer measurements in bubble column: effect of sparger. Industrial & Engineering Chemistry Research 45, 9201-9207] obtained using Laser Doppler anemometry. Comparison of simulation results with the experimental measurements of Sanyal et al. [1999. Numerical simulation of gas-liquid dynamics in cylindrical bubble column reactors. Chemical Engineering Science 54, 5071-5083] and Olmos et al. [2001. Numerical simulation of multiphase flow in bubble column reactors: influence of bubble coalescence and breakup. Chemical Engineering Science 56, 6359-6365] also show a good agreement for liquid velocity and gas hold-up profiles.     

A scale-up strategy for low-temperature methanol synthesis in a circulating slurry bubble reactor

Slurry bubble column reactors are being increasingly utilized in the large-scale conversion of coal or natural gas to liquid hydrocarbons and alcohols. A new suite of tools for developing low-temperature methanol synthesis in circulating slurry bubble reactors is explored in this study. The scale-up strategy consisting of hydrodynamics in cold flow units, catalyst performance evaluation in an autoclave, and process investigation in a pilot-scaled circulating slurry bubble reactor is presented. This methodology should be helpful for designing and scaling-up the low-temperature methanol synthesis and other related processes in slurry bubble column reactors, which will enhance and speed them towards commercial application.     

湍动浆态床流体力学研究（Ⅱ）轴向浆料速度的径向分布

对高气速、大塔径条件下的湍动浆态床轴向速度进行了实验测定,提出了简化的一维流体力学模型。实验结果表明：固含率对浆料速度的径向分布影响不明显;采用中心速度和塔径作为参考量,则不同条件下的量纲1流速分布相似;高气速下中心速度随塔径的变化可近似用Nottenkamper关联式描述。提出了一维流体力学模型预测浆态床液速分布,模型计算结果与实验数据符合较好,模型较好地反映了浆态床反应器内液速分布随表观气速、固含率及塔径变化的规律。     

SOLIDS DISTRIBUTION IN A BATCH BUBBLE COLUMN

This paper presents some new experimental data for axial solid distribution in batch slurry reactors. The effects of liquid and solid properties on the solid dispersion behavior in 0.076 m and 0.305 m diameter slurry bubble columns are outlined. The effects of gas distributor, column internals and particle size distribution on the solids concentation profiles are also examined. Critical gas velocity for complete suspension of solids are measured and compared with those predicted from the available literature correlations. It is shown that when the particles are completely suspended, the Peclet number obtained from the sedimentation-dispersion model depends very significantly on the assumed boundary conditions. The effect of gas velocity on the particle Peclet number depends on the nature of the liquid-solid system.     

撞击流反应器用于甲醇合成反应

撞击流反应器用于气液固三相甲醇合成反应可以充分发挥其优良的传热、传质性能。在撞击流反应器内,催化剂浆料经喷嘴雾化后成微米尺度的液滴,气液相间接触面积远大于其他三相合成反应器。考察了温度、压力、气体流量、浆料循环量以及喷嘴个数对甲醇合成反应的影响,结果表明,当压力从3.8 MPa上升到5 MPa时,反应器的时空产率增长了近1倍,气体流量达22.4 L·min^-1后时空产率几乎不再变化,增加浆料循环量以及在同一循环量下采用多喷嘴对置都可以增加催化剂时空产率。同时,与固定床、搅拌釜和浆态鼓泡床甲醇合成进行了对比,结果表明,在低空速下撞击流反应器与其他反应器时空产率相当,而在高空速下要优于其他反应器。     

计及气泡诱导与剪切湍流的气泡破碎、湍流相间扩散及传质模型

在以鼓泡塔为代表的气液鼓泡流动中,存在着气泡诱导湍流（BIT）和剪切湍流两种湍流机制,并且二者在不同的时间、空间范围内既相互竞争又共同作用。受制于BIT动能能谱的形式和特性不够完整清晰,过去的研究中关于BIT如何对气泡破碎聚并、相间作用力、相间传热传质等相间相互作用过程产生影响的结论比较模糊。因此,本文在具有波数κ^-3特性的BIT能谱的基础上,提出了在不同工况下考虑BIT与剪切湍流共同作用的研究思路。研究结果表明,考虑两种湍流机制的气泡破碎模型和湍流相间扩散模型对BIT在整体或局部占据不同程度主导地位的情况,都能很好地捕捉气液鼓泡流动的动力学特性,为进一步准确揭示气液相间传质过程的内在机理提供了基础。     

Effect of interfacial forces and turbulence models on predicting flow pattern inside the bubble column

The numerical approaches have been used in many studies to predict the flow pattern inside the bubble column reactors because of the difficulties that are still found in designing and scaling-up the bubble columns. This review makes an effort to show suitable interfacial forces i.e., drag force, lift force, turbulent dispersion models and virtual mass and turbulence models such as standard k–ɛ model, Reynolds Stress Model, Large Eddy Simulation to predict flow pattern inside the bubble column using Eulerian–Eulerian. The effect of various interfacial forces and turbulence models on gas–liquid velocity and gas hold-up in bubble column is critically reviewed.     

A dual-scale turbulence model for gas-liquid bubbly flows☆

A dual-scale turbulence model is applied to simulate cocurrent upward gas–liquid bubbly flows and validated with available experimental data. In the model, liquid phase turbulence is split into shear-induced and bubble-induced turbulence. Single-phase standard k-εmodel is used to compute shear-induced turbulence and another transport equation is added to model bubble-induced turbulence. In the latter transport equation, energy loss due to interface drag is the production term, and the characteristic length of bubble-induced turbulence, simply the bubble diameter in this work, is introduced to model the dissipation term. The simulated results agree well with experimental data of the test cases and it is demonstrated that the proposed dual-scale turbulence model outperforms other models. Analysis of the predicted turbulence shows that the main part of turbulent kinetic en-ergy is the bubble-induced one while the shear-induced turbulent viscosity predominates within turbulent vis-cosity, especially at the pipe center. The underlying reason is the apparently different scales for the two kinds of turbulence production mechanisms:the shear-induced turbulence is on the scale of the whole pipe while the bubble-induced turbulence is on the scale of bubble diameter. Therefore, the model reflects the multi-scale phe-nomenon involved in gas–liquid bubbly flows.     

鼓泡塔反应器气液两相流CFD数值模拟

对圆柱形鼓泡塔反应器内的气液两相流动进行了三维瞬态数值模拟,模拟的表观气速范围为0.02～0.30 m•s^-1; 模拟采用了双流体模型,并耦合了气泡界面密度单方程模型预测气泡尺寸,该模型考虑了气泡聚并与破碎对气泡尺寸的影响。液相湍流采用考虑气相影响的修正k-ε模型,两相间的动量传输仅考虑曳力作用。模拟获得了轴向气/液相速度分布、气含率分布、湍流动能分布以及气泡表面面积密度等,对部分模拟结果与实验值进行了定量比较,结果表明模拟结果与实验结果吻合较好。     

合成气制二甲醚三相淤浆床反应器的数学模型研究

A mathematical model for a bubble column slurry reactor is presented for dimethyl ether synthesis from syngas. Methanol synthesis from carbon monoxide and carbon dioxide by hydrogenation and the methanol dehydration are considered as independent reactions, in which methanol, dimethyl ether and carbon dioxide are the key components. In this model, the gas phase is considered to be in plug flow and the liquid phase to be in partly back mixing with axial distribution of solid catalyst. The simulation results show that the axial dispersion of solid catalysts, the operational height of the slurry phase in the bubble column slurry reactor, and the reaction results are influenced by the reaction temperature and pressure, which are the basic data for the scale-up of reactor.     

Estimation of mid‐distillates production rate in a low temperature Fischer–Tropsch process

BACKGROUND: The Fischer–Tropsch process is the most important path for converting natural gas to high quality liquid hydrocarbons. Low temperature Fischer–Tropsch synthesis in slurry bubble column reactors with cobalt‐based catalysts is used for mid‐distillates production. RESULTS: In this work the slurry bubble column reactor was simulated by applying the two‐bubble class mathematical model. In addition, the effect of operating parameters on synthesis gas conversion was studied. The distribution of products was also predicted from the simulation framework. CONCLUSIONS: The effect of synthesis gas inlet velocity on mid‐distillates production rate was studied in the present work. A maximum production rate for mid‐distillates of about 23 kg s^?1 was predicted from the simulation program. Copyright © 2011 Society of Chemical Industry     

Simulation of oscillatory baffled column: CFD and population balance

In the present work, an attempt has been made to combine population balance and a CFD approach for simulating the flow in oscillatory baffled column (OBC). Three-dimensional Euler-Euler two-fluid simulations are carried out for the experimental data of Oliveira and Ni [2001. Gas hold-up and bubble diameter in a gassed oscillatory baffled column. Chemical Engineering Science 56, 6143-6148]. The experimental data include the average hold-up profile and bubble size distribution in the OBC. All the non-drag forces (turbulent dispersion force, lift force) and the drag force are incorporated in the model. The coalescence and breakage effects of the gas bubbles are modeled according to the coalescence by the random collision driven by turbulence and wake entrainment while for bubble breakage by the impact of turbulent eddies. Predicted liquid velocity and averaged gas hold-up are compared with the experimental data. The profile of the mean bubble diameter in the column and its variation with the superficial gas velocity is studied. Bubble size distribution obtained by the model is compared with the experimental data.