催化裂化提升管反应器模型的建立

工业催化裂化提升管反应器内既存在着气固两相的湍流流动,又存在着传热和裂化反应,而且这些过程是相互影响,高度耦合在一起的。本文全面系统地考虑湍流气因两相流动,传质,传热及反应等复杂因素及其相互影响,建立了催化裂化提升管反应器三维气固两相流动反应模型,形成了相应的数值解法,编制了大型的模拟计算程序。由此可对工业催化裂化提升管反应器内湍流气固两相流动进行系统的数值模拟研究。     

Mathematische Modellierung von Wirbelschichtreaktoren

Mathematical modelling of fluidized bed reactors . Among the many fluidized bed models to be found in the literature, the two-phase model originally proposed by May has proved most suitable for accommodation of recent advances in flow mechanics: this model resolves the gas/solids fluidized bed into a bubble phase and a suspension phase surrounding the bubbles. Its limitation to slow reactions is a disadvantage. On the basis of the analogy between fluidized beds and gas/liquid systems, a general two-phase model that is valid for fast reactions has therefore been developed and its validity is confirmed by comparison with the experimental results obtained by other authors. The model describes mass transfer across the phase interface with the aid of the film theory known from gas/liquid reactor technology, and the reaction occurring in the suspension phase as a pseudo-homogeneous reaction. Since the dependence of the performance of fluidized bed reactors upon geometry is accounted for, the model can also be used for scale-up calculations. Its use is illustrated with the aid of design diagrams.     

Photophysikalische Meßverfahren zur Untersuchung von Gas/Flüssig-Reaktoren

Photophysical measuring techniques for the study of gas/liquid reactors . After a brief account of the fundamentals of photophysics, the authors describe various photophysical measuring procedures, with reference to available instrumentation, including prices. The measuring methods permit contactless and intertialess determination of various quantities in very small volumes (temperature, viscosity, concentration, pH, orientation of molecules, etc.). The authors examine which methods are available for the study of gas/liquid reactors. The most promising studies seem to involve the heat effects accompanying absorption with chemical reaction, study of interfacial effects (slowing mass transfer by accumulation of surface-active impurities, Marangoni effect), and the observation of complex reaction systems. Photophysical measuring techniques can also be used for measurements in industrial reactors; some of the known applications are described.     

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.     

Transient models for multiphase slurry reactors

Modelling of catalytic reactions is usually rather a complex task since several mass transfer and reaction effects take place simultaneously in gas, liquid and solid phases, not to mention the problems encountered when heat effects or changes in flow conditions cannot be excluded. Multiphase reactor models retrieved from existing literature are often not applicable as such for practical industrial problems. They might be oversimplified - or computationally too complicated, loaded with unidentifiable parameters. In this paper, a general set of dynamic model equations is presented, valid for a variety of non-catalytic gas-liquid or catalytic gas-liquid-solid reactors with simultaneous reaction and mass transfer. In order to decrease the number of model equations and parameters to be estimated from experimental data, analyses with simplified models are common. The simplified models are obtained as limiting cases, for example with respect to given reaction/diffusion parameters. We show how the validity of some simplifying hypotheses can be analysed in this paper by simulation with existing literature data of -methylstyrene hydrogenation. The procedure used here may further be used in the investigation of identifiability of parameters or model discrimination, for example to check whether joint assumption of rapid adsorption and intraparticle diffusion can be accepted in the view of experimental data.     

Experimental and Theoretical Studies on Hydrogenation in Multiphase Fixed‐Bed Reactors

Multiphase fixed‐bed reactors have complex hydrodynamic and mass transfer characteristics. The modeling and scale‐up are therefore difficult. The present work focuses on the role of mass transfer on the effective reaction rate. The catalytic 1‐octene hydrogenation was taken as a model reaction. The reaction rate in the trickle‐bed reactor is by a factor of 20 smaller than (theoretically) in the absence of any mass transfer limitations. For high octene concentrations (> 10 %), the effective reaction rate is limited by the H₂ consumption, above all by the gas/liquid and liquid/solid mass transfer. For lower octene concentrations the reaction is zero order with respect to H₂ and only depends on the octene consumption, i.e., on the interplay of chemical reaction, L/S and intraparticle mass transfer of octene.     

Effect of gassing rate on solid–liquid mass transfer coefficients and particle slip velocities in stirred tank reactors

While solid–liquid dispersion in mechanically agitated vessels has been widely investigated, the suspension of particles with simultaneous gas dispersion is, however, less well understood. A consideration of the gassing rate is of particular importance when designing “dead-end” batch reactors. Solid–liquid mass transfer coefficients were determined using the technique of dissolving a sparingly soluble solid, salicylic acid loaded onto silica gel, in water. Mass transfer was found to be dependent on a variety of geometric, physical and hydrodynamic properties; with the significant exception of agitation speed the influence of the latter properties was independent of gas dispersion. Flow visualisation with positron emission particle tracking has been used alongside the mass transfer measurements to study the effects of gas injection on the liquid flow patterns and the solid–liquid slip velocities. Time-averaged relative slip velocities were determined by simple subtraction of the data obtained using a neutrally buoyant particle. Gas dispersion was found to affect the particle–liquid slip velocity, explaining the mass transfer coefficient trends observed. While only a small diameter vessel has been used it does point to considerable non-uniformity of mass transfer in larger vessels.     

Classification and characterization of hydrodynamic and transport behaviors of three-phase reactors

According to axial profile of solid concentration, the cocurrent upward threephase reactors with liquid as continuous phase can be classified into three types (a) gassparged slurry reactors, (b) threephase bubble columns, and (c) threephase fluidized beds Comparative study shows that the gas hold up, bubble characteristics and mass transfer are significantly dependent on the type of threephase reactors Three types of reactors exhibit the different hydrodynamic and transport behaviors with particle size, solid concentration and gas holdup The structural analysis of the axial solid distribution indicates the bubble and bubble wake dynamics are the key factors to the hydrodynamic and transport behaviors of three-phase reactors.     

Novel Gas-Liquid-Solid Reactors

Multiphase reactors involving gas, liquid, and solid phases have several important applications in the chemical industry, particularly in catalytic processes. Some of the well-known examples are: hydrogenation and oxidation of organic compounds, hydro-processing coal-derived and petroleum oils, Fischer-Tropsch synthesis, and methanation reactions. Due to the presence of three phases, the problem of reactor design is often important to achieve effective mass and heat transfer as well as a mixing pattern favorable to the particular process. The reactors are mainly of two types: (a) solid catalyst is suspended either by mechanical agitation or gas-induced agitation and (b) solid catalyst is in a fixed bed with concurrent or countercurrent feed of gas and liquid re-actants. The reactor types conventionally used in industry are: (a) mechanically agitated or bubble column slurry reactors and (b) trickle-bed or packed-bed bubble reactor. The various design and modeling aspects of these reactors have been reviewed by Satterfield [1], Chaudhari and Ramachandran [2], Shah [3,4], Ramachandran and Chaudhari [5], Shah et al. [6], and Herskowitz and Smith [7]. In several industrial processes these reactor designs are modified to achieve a certain specific objective, such as better heat or mass transfer, higher catalyst efficiency, better reactor performance and selectivity, etc. Similarly, specially designed reactors are often used for laboratory kinetic studies or to understand a certain phenomenon. Thus, novel multiphase reactors are becoming important from both academic and industrial viewpoints. Some of the recently introduced novel gas-liquid-solid reactor types are: (a) loop recycle slurry reactors, (b) basket-type reactors, (c) ebullated-bed reactors, (d) internal or external recycle reactors, (e) multistage slurry or packed-bed reactors, (f) column reactors with sieve trays or multiple agitators, (g) gas-induced agitated reactors, and (h) horizontal-packed-bed reactors. are being used in several new commercial processes, and various design aspects, such as hydrodynamics and mass and heat transfer, have been the subject of investigations in the last few years. However, no attempt to review the scattered information on these novel gas-liquid-solid reactors has been made. Therefore, the main objective of this paper is to review important developments in novel gas-liquid-solid reactors. For each type of reactor, advantages, disadvantages, and applications are discussed. Further, the status of information on hydrodynamics and mass transfer parameters and scale-up considerations is reviewed. These novel reactor designs are being used in several new commercial processes, and various design aspects, such as hydrodynamics and mass and heat transfer, have been the subject of investigations in the last few years. However, no attempt to review the scattered information on these novel gas-liquid-solid reactors has been made. Therefore, the main objective of this paper is to review important developments in novel gas-liquid-solid reactors. For each type of reactor, advantages, disadvantages, and applications are discussed. Further, the status of information on hydrodynamics and mass transfer parameters and scale-up considerations is reviewed.     

Novel Gas-Liquid-Solid Reactors

Multiphase reactors involving gas, liquid, and solid phases have several important applications in the chemical industry, particularly in catalytic processes. Some of the well-known examples are: hydrogenation and oxidation of organic compounds, hydro-processing coal-derived and petroleum oils, Fischer-Tropsch synthesis, and methanation reactions. Due to the presence of three phases, the problem of reactor design is often important to achieve effective mass and heat transfer as well as a mixing pattern favorable to the particular process. The reactors are mainly of two types: (a) solid catalyst is suspended either by mechanical agitation or gas-induced agitation and (b) solid catalyst is in a fixed bed with concurrent or countercurrent feed of gas and liquid re-actants. The reactor types conventionally used in industry are: (a) mechanically agitated or bubble column slurry reactors and (b) trickle-bed or packed-bed bubble reactor. The various design and modeling aspects of these reactors have been reviewed by Satterfield [1], Chaudhari and Ramachandran [2], Shah [3,4], Ramachandran and Chaudhari [5], Shah et al. [6], and Herskowitz and Smith [7]. In several industrial processes these reactor designs are modified to achieve a certain specific objective, such as better heat or mass transfer, higher catalyst efficiency, better reactor performance and selectivity, etc. Similarly, specially designed reactors are often used for laboratory kinetic studies or to understand a certain phenomenon. Thus, novel multiphase reactors are becoming important from both academic and industrial viewpoints. Some of the recently introduced novel gas-liquid-solid reactor types are: (a) loop recycle slurry reactors, (b) basket-type reactors, (c) ebullated-bed reactors, (d) internal or external recycle reactors, (e) multistage slurry or packed-bed reactors, (f) column reactors with sieve trays or multiple agitators, (g) gas-induced agitated reactors, and (h) horizontal-packed-bed reactors. are being used in several new commercial processes, and various design aspects, such as hydrodynamics and mass and heat transfer, have been the subject of investigations in the last few years. However, no attempt to review the scattered information on these novel gas-liquid-solid reactors has been made. Therefore, the main objective of this paper is to review important developments in novel gas-liquid-solid reactors. For each type of reactor, advantages, disadvantages, and applications are discussed. Further, the status of information on hydrodynamics and mass transfer parameters and scale-up considerations is reviewed. These novel reactor designs are being used in several new commercial processes, and various design aspects, such as hydrodynamics and mass and heat transfer, have been the subject of investigations in the last few years. However, no attempt to review the scattered information on these novel gas-liquid-solid reactors has been made. Therefore, the main objective of this paper is to review important developments in novel gas-liquid-solid reactors. For each type of reactor, advantages, disadvantages, and applications are discussed. Further, the status of information on hydrodynamics and mass transfer parameters and scale-up considerations is reviewed.     

Cyclic mass transport phenomena in a novel reactor for gas–liquid–solid contacting

This study introduces a novel reactor concept, referred to as the Siphon Reactor, for intensified phase contacting of gas–liquid reactants on heterogeneous catalysts. The reactor comprises a fixed catalyst bed in a siphoned reservoir, which is periodically filled and emptied. This serves to alternate liquid–solid and then gas–liquid mass transfer processes. As the duration of each phase can be manipulated, mass transfer can be deliberately harmonized with the reaction. Residence time experiments demonstrate that, in contrast to periodically operated trickle‐bed reactors, the static liquid hold‐up is exchanged frequently and uniformly due to the complete homogeneous liquid wetting. A mathematical model describing the siphon hydrodynamics was developed and experimentally validated. The model was extended to account for a heterogeneously catalyzed gas–liquid reaction and capture the influence of siphon operation on conversion and selectivity of a consecutive reaction. © 2016 American Institute of Chemical Engineers AIChE J, 63: 208–215, 2017     

Tomography measurements of gas holdup in rotating foam reactors with Newtonian, non-Newtonian and foaming liquids

Rotating solid foam reactors have already proven to show high mass transfer rates and to be a potential alternative to slurry reactors. The rotation of a foam block stirrer results in a high mass transfer and in the development of different reactor sections showing specific hydrodynamics and gas holdup distributions. In order to optimize the reactor system the hydrodynamics in a lab scale reactor are studied using γ-ray tomography, a powerful method to measure the gas holdup in three-phase reactors. The influence of liquid properties, such as viscosity and surface tension, and the rotational speed on the gas/liquid distribution in the different reactor sections is investigated. Especially the viscosity has a strong effect on the entrapment of gas bubbles in the foam block structure, while the surface tension is the dominant parameter in the outer reactor section. The influence of these parameters on the inset of foaming and the collapse of the gas/liquid dispersion is investigated. Conclusions on the mass transfer performance are drawn and recommendations for further optimizations of the reactor design and the operational conditions depending on the liquid properties are developed.     

喷射式气-液反应器的型式及应用

气体和液体以喷射形式进料 ,是喷射式气液反应器的显著特征 ;喷射式气液反应器是一种多相反应器 ,具有较好的传热、传质和混合特性。对喷射式气—液反应器的型式及应用作了概要介绍     

翼形桨在气液固三相搅拌反应釜中的混合性能

<正>机械搅拌槽中高速旋转的叶轮产生的排出流中,径向速度主要用于气体的剪切分散,而其轴向速度是固体悬浮和液相轴向混合的主要动力。三相体系的混合不仅要求叶轮具有较强的径向剪切分散能力,而且要有一定的轴向混合能力,以此达到对气体和固体的同时分散。理想的混合水平不仅要求达到二者在宏观上的均匀,而且在微观混合上也要达到一定的均匀度,为此对搅拌桨的设计提出了较高的要求。在气液二相的混合操作中比较多的采用了盘式涡轮桨,而在液固二相的混合操作中比较多的使用螺旋桨,这都是为了利用各自不同的混合优势。涉及到气液固三相混合,由于气体和固体的分散是一个相互制约的问题,完全的径向     

PARTICLE-LIQUID MASS TRANSFER IN MULTI-IMPELLER AGITATED THREE PHASE REACTORS

The mass transfer coefficient between solid particle and liquid has been measured in high aspect ratio multiimpeller agitated three phase (gas-liquid-solid) reactors. Experiments were conducted in 0.15 and 0.30 m id acrylic columns of lm length each. Two types of impeller were used: disk turbine (DT) and pitched turbine downflow (PTD). Air used as the gas phase was introduced through a ring sparger of 0.8 D size located 0.1 T distance above the bottom. The interimpeller spacing was maintained at the tank diameter. The range of gas velocity used was 0-15 mm/s. A unique correlation between particle-liquid mass transfer coefficient and critical impeller speed for solid suspension has been presented.     

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.     

Revisiting shrinking particle and product layer models for fluid-solid reactions - From ideal surfaces to real surfaces

A general model based on an arbitrary geometry was developed for reactive solid particles which have surface defects and porosity. The model equations comprising intrinsic kinetics as well as mass transfer effects through the product layer and the fluid film surrounding the solid particle were derived for shrinking particle and product layer models. From the model equations, the fluid (gas or liquid) concentrations at the reaction surface can be calculated and the change of the solid phase can be predicted. The approach was illustrated with monodisperse particle distributions in batch reactors. Complex kinetics as well as simpler special cases were treated. In general, the model predicts a higher reaction order with respect to the solid component than the previous ideal models, which assume slab, cylindrical or spherical geometries for solid particles.     

Hydrogenation of 2‐ethylanthraquinone under Taylor flow in single square channel monolith reactors

The hydrogenation of 2‐ethylanthraquinone (EAQ) to 2‐ethylanthrahydroquinone (EAHQ) was carried out under Taylor flow in single square channel monolith reactors. The two opening ends of opaque reaction channel were connected with two circular transparent quartz‐glass capillaries, where Taylor flow hydrodynamics parameters were measured and further used to obtain practical flow state of reactants in square reaction channels. A carefully designed gas‐liquid inlet mixer was used to supply steady gas bubbles and liquid slugs with desired length. The effects of various operating parameters, involving superficial gas velocity, superficial liquid velocity, gas bubble length, liquid slug length, two‐phase velocity and temperature, on EAQ conversion were systematically researched. Based on EAQ conversion, experimental overall volumetric mass transfer coefficients were calculated, and also studied as functions of various parameters as mentioned earlier. The film model, penetration model, and existing semi‐empirical formula were used to predict gas‐solid, gas‐liquid, and liquid‐solid volumetric mass transfer coefficients in Taylor flow, respectively. The predicted overall volumetric mass transfer coefficients agreed well with the experimental ones. © 2009 American Institute of Chemical Engineers AIChE J, 2009     

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