Modeling and Simulation of a Bubbling SO2 Absorber with Granular Limestone Slurry and an Organic Acid Additive

The absorption of SO₂ into limestone slurry containing suspended reactive particles was performed in a bubble reactor with continuous feeding of both gas and liquid phases at a constant pH and high temperature (50 °C). An absorption model with a reaction plane based on the film model was developed. The effect of limestone particle size, concentration, acetic acid additives, and inlet SO₂ concentration on the concentration distribution of chemical species in the liquid film and SO₂ absorption rate were simulated. Increasing the concentration of limestone slurry, adding acetic acid additives into the system or decreasing the limestone particle size or inlet SO₂ concentration caused the reaction plane in the liquid film to shift towards the gas‐liquid interface. Model and experimental results were compared, and it was shown that the model fits the experimental data well.     

Hydrodynamics and mass transfer of gas–liquid flow in a falling film microreactor

In this article, flow pattern of liquid film and flooding phenomena of a falling film microreactor (FFMR) were investigated using high‐speed CCD camera. Three flow regimes were identified as “corner rivulet flow,” “falling film flow with dry patches,” and “complete falling film flow” when liquid flow rate increased gradually. Besides liquid film flow in microchannels, a flooding presented as the flow of liquid along the side wall of gas chamber in FFMR was found at high liquid flow rate. Moreover, the flooding could be initiated at lower flow rate with the reduction of the depth of the gas chamber. CO₂ absorption was then investigated under the complete falling flow regime in FFMR, where the effects of liquid viscosity and surface tension on mass transfer were demonstrated. The experimental results indicate that k_L is in the range of 5.83 to 13.4 × 10^?5 m s^?1 and an empirical correlation was proposed to predict k_L in FFMR. © 2009 American Institute of Chemical Engineers AIChE J, 2009     

CFD Simulation of Liquid Film Flow on Inclined Plates

A two‐phase flow CFD model using the volume of fluid (VOF) method is presented for predicting the hydrodynamics of falling film flow on inclined plates, corresponding to the surface texture of structured packing. Using the proposed CFD model the influence of the solid surface microstructure, liquid properties and gas flow rate on the flow behavior was investigated. From the simulated results it was shown that under the condition of no gas flow the liquid flow patterns are dependent on the microstructure of the plates, and proper microstructuring of the solid surface will improve the formation of a continuous liquid film. It was also found that liquid properties, especially surface tension, play an important role in determining the thin‐film pattern. However, there are very different liquid film patterns under the action of gas flow. Thinner liquid films break easily, but thicker liquid films can remain continuous even at higher gas flow rates, which demonstrates that all factors affecting the liquid film thickness will affect the liquid film patterns under conditions of counter‐current two‐phase flow.     

Mathematical Modeling and Genetic Algorithm Optimization of Reactive Absorption of H2S

A rate‐based mathematical model was developed for the reactive absorption of H₂S in NaOH, with NaOCl or H₂O₂ as the chemical oxidant solutions in a packed column. A modified mass transfer coefficient in the gas phase was obtained by genetic algorithm and implemented in the model to correct the assumption of instantaneous reactions. The effects of different operating variables including the inlet H₂S concentration, inlet gas mass flux, initial NaOH, concentrations of the chemical oxidants in the scrubbing solutions, and liquid‐to‐gas ratio on the H₂S removal efficiency were studied. A genetic algorithm was employed to optimize the operating variables in order to obtain maximum removal efficiency of H₂S. The model results were in good agreement with the experimental data.     

Mathematical Modeling,Simulation, and Experimental Verification of CO2 Removal in a Turbulent Contact Absorber

A highly efficient technique of contaminant gas reduction, Turbulent Contact Absorber (TCA), is applied to CO₂ removal from a typical flue gas. Aqueous K₂CO₃ sorbent was evaluated as a regenerable sorbent for CO₂ from the flue gas. In order to identify the system, momentum and mass balance equations were written for the TCA tower. A flat plate falling film model was employed to simulate the TCA tower and the effect of turbulence was included in mass and momentum transfer coefficients. To check the accuracy of the model, a pilot scale TCA was built and operated. A Testo type gas analyzer was used to detect gas concentrations at the inlet and outlet of the rig. The model was validated successfully with pilot plant data. The effect of velocity and K₂CO₃ concentration on the TCA performance has also been carried out. It was found that the bed pressure drop increases linearly with gas velocity and then remains constant. An increase in the liquid flow rate increases liquid holdup, which leads to a rise in bed pressure drop. Higher turbulence within the TCA causes a velocity peak to shift from hypothetical gas‐liquid interface towards the falling film plate. An increase of the K₂CO₃ concentration from 1.0 g mol/L to 2.0 g mol/L was found to give an increase in CO₂ removal by about 4 %.     

不同流型下离子液体-MEA复合工质降膜吸收CO2特性

以氨基酸离子液体和乙醇胺混合水溶液为吸收剂研究逆流气体对竖直平板降膜流型转换的影响,考察了3种流型下液体流量和入口温度、气体流量和进口CO₂浓度对CO₂吸收性能的影响。结果表明:随着液体流量的增加,液膜呈现溪流、片状流和完整流3种流型,降膜流型转换临界流量随逆流气体流量增大而增加;溪流和片状流时CO₂吸收速率随液体流量的增加而增加,但在完整流条件下基本不变;完整流下具有较高的CO₂吸收速率,然而溪流下的液相传质系数最高。     

DIRECT CONTACT CONDENSATION OF DILUTE STEAM/AIR MIXTURES ON WAVY FALLING FILMS

Condensation from air-steam mixtures on falling water layers is investigated experimentally and theoretically. The thin film flows on the inner surface of a 5cmi.d. vertical pipe. This film is wavy turbulent while the gas phase is kept saturated with steam. Experiments are conducted with the gas mixture effectively stagnant, compared with the fast moving liquid film. Measurements are also made under a mild vacuum applied on the gas phase. Heat transfer coefficients averaged over the entire length of the condensing surface, tend to increase by decreasing the liquid flowrate, by increasing the steam fraction, and by applying a mild vacuum on the gas phase. However, for the cases examined, there is a liquid flowrate above which the heat transfer coefficient becomes almost constant.

Numerical predictions are made for a fully developed turbulent film using an eddy diffusivity model. The results indicate that for a system with a large amount of noncondensable gases-as in this study-the temperature profile in the liquid film is nearly uniform and that the major resistance to condensation resides in the gas phase. The analysis also shows that the relative contribution of sensible heat transferred through the gas phase is small relative to the latent heat released upon condensation. Comparison of predictions with experimental data suggests that a significant parameter in these analyses is the gas diffusion boundary layer thickness which seems to be comparable in size with the liquid film thickness. Finally, the possibility is discussed of correlating condensation heat transfer coefficients with already available statistical characteristics of the falling wavy layer. Theoretical predictions based on this idea are in good agreement with data.     

Numerical investigation on CO2 absorbed in aqueous N‐methyldiethanolamine + piperazine

A multiphase and multicomponent mass transfer model of CO₂ absorbed in aqueous N‐methyldiethanolamine and piperazine (PZ) was built in the study. In the model, a simple method of mass transfer between phases was proposed. Besides, the hydrodynamics, thermodynamics, and complex reversible chemical reaction were considered simultaneously. The model was validated by comparing with the previous experimental data which showed that simulated results can represent the experimental data with reasonable accuracy. Based on the model, the effects of gas velocity, liquid load and CO₂ loading on the absorption rate, and enhancement factor were analyzed. Model results showed that the enhancement factor increased with a rising gas velocity while decreased with a rising liquid load or CO₂ loading. The change of enhancement factor with CO₂ loading was similar to that of equilibrium concentration of PZ which indicated that PZ was significant to the absorption process. Furthermore, the distributions of specie concentrations were discussed in detail. © 2016 American Institute of Chemical Engineers AIChE J, 63: 2386–2393, 2017     

Kinetic Model of Gas‐Liquid‐Liquid Reactive Extraction for Production of Hydrogen Peroxide

The kinetic aspects of the gas‐liquid‐liquid reactive extraction process for the production of hydrogen peroxide were investigated in a batch reactor. It was observed that the gas‐liquid reaction rate is strongly affected by mass transfer of oxygen across the liquid film and the reaction can be simplified to pseudo‐first order. The extraction rate is governed by both reaction and liquid‐liquid mass transfer, and is slightly lower than the reaction rate. In addition, a kinetic model of the reactive extraction process for the production of hydrogen peroxide was developed. Kinetic parameters under different conditions were determined by experiments. The data calculated from the kinetic model match experimental data well under different conditions for hydrogen peroxide production in gas‐liquid‐liquid reactive extraction.     

多排平直翅片管换热器表面气液降膜流动特性的三维数值模拟

基于VOF模型建立了考虑重力、表面张力及界面摩擦力源项的多排平直翅片管换热器表面气液两相降膜流动三维瞬态CFD模型。不同气流速度下液膜厚度模拟结果与文献中试验值吻合较好,最大偏差小于5%,表明所建立CFD模型是可靠的。通过研究壁面接触角为30°时不同气液Reynolds数下液膜流动特性,结果表明：翅片管表面满膜流的临界Reynolds数Re_l为239,临界喷淋密度为0.06 kg/(m·s);在239 ≤ Re_l ≤ 995内,其平均液膜厚度较Nusselt理论解高16.8%～35.1%;气液逆流和顺流时气相Reynolds数Re_g应分别小于2190.7和3286.0,其主要原因在于过高的Re_g会导致气液界面摩擦力快速增大,从而引发液膜破裂和液滴脱落等现象恶化设备性能。总之,气液顺流更有利于在较高气相Reynolds数下实现翅片管表面的较薄满膜流动。     

Comparison of Concentration Profiles for Boundary Layers in Absorption with Chemical Reaction Processes

An analysis of five different systems of absorption‐with‐chemical‐reaction in gas‐liquid reactors, commonly encountered in various industrial processes, is presented. To analyze the interphase mass transfer from gas to liquid, the rate limiting parameters and the concentrations at the gas‐liquid interface were determined on the basis of pertinent theories. The calculations presented, are based on the Whitman theory for gas and liquid phase mass transfer coefficients and Henry equilibrium constants. The necessary diffusion coefficients were calculated from existing correlations, and the corresponding chemical reaction rate constants were obtained from the literature, assuming pseudo first order chemical reaction. The process parameters required (pressure, temperature, and the gas‐liquid contact time) were within the values that occur in industrial processes. The results presented, are the concentration profiles in the boundary layers for the systems studied, calculated and graphically presented, together with the gas and liquid film thicknesses and Hatta numbers, obtained from calculations for the liquid phase mass transfer. The results may contribute to a better understanding of the absorption‐with‐chemical‐reaction processes in industrial plants, thus lowering the operational costs of these processes and alleviating the ecological problems of existing technologies.     

Rate‐based modelling of reactive absorption of acid gases in an aqueous methyldiethanolamine (MDEA) solution

In this work different tools for accurate prediction of acid gas absorption are used. At first, simulation of reactive absorption is carried out using the RATEFRAC module of Aspen Plus, which is tested against pilot plant data. The limitations and disadvantages of this module are presented. In order to present a more predictive approach a rate‐based model for the gas scrubbing process is developed. In this model the assumption of thermodynamic equilibrium is considered only at the gas–liquid interphase. Chemical equilibrium among the reacting species in the liquid phase is assumed just for the bulk phase. Mass transfer is modelled using mass transfer coefficients calculated from available correlations which are then improved using an enhancement factor to account for the chemical reactions. The validity of the suggested model is established by comparison of model results with published pilot plant data. The prediction results using the proposed model are improved by around 17% AAD for CO₂ and around 7.5% AAD for H₂S compared to simulation results using Aspen Plus.     

Mass Transfer and Liquid‐Film Formation in a Spray Tower for SO2 Removal in Sodium Hydroxide Solution

Spray towers allow for controlling air pollution in which a liquid is sprayed in small droplets to produce a large interfacial area for mass transfer between a gas and a liquid phase. An experimental study of a spray tower for removing SO₂ is described. The experiments were carried out under different operating conditions by varying the gas velocity, liquid flow rate, and SO₂ concentration. SO₂ removal efficiency, volumetric mass transfer coefficient, and liquid‐film formation as a result of the collision of droplets against the tower wall are investigated. Removal efficiency and volumetric mass transfer coefficient are analyzed as a function of gas velocity, liquid flow rate, and SO₂ concentration, while liquid‐film formation is evaluated as a function of tower height. The results indicate high removal efficiency. Correlations to predict the volumetric mass transfer coefficient are also proposed.     

Computational Fluid Dynamics Modeling of Gas‐Liquid Two‐Phase Flow around a Spherical Particle

Microscale studies, which can provide basic information for meso‐ and macroscale studies, are essential for the realization of flow characteristics of a packed bed. In the present study, the effects of gas velocity, liquid velocity, liquid‐solid contact angle, and liquid viscosity on the flow behavior were parametrically investigated for gas‐liquid two‐phase flow around a spherical particle, using computational fluid dynamics (CFD) methodology in combination with the volume‐of‐fluid (VOF) model. The VOF model was first validated and proved to be in good agreement with the experimental data. The simulation results show that the film thickness decreases with increasing gas velocity. This trend is more obvious with increasing operating pressure. With increasing liquid velocity, the film thickness tends to be uniform on the particle surface. The flow regime can change from film flow to transition flow to bubble flow with increasing contact angle. In addition, only at relatively high values does the liquid viscosity affect the residence time of the liquid on the particle surface.     

Practical identifiability analysis in dynamic gas–liquid reactors: Optimal experimental design for mass-transfer parameters determination

A dynamic gas–liquid transfer model without chemical reaction based on the unsteady film theory is analysed in order to confirm the possible identifiable parameters of the model from a given set of experimental data. The structural identifiability analysis of the model using the macroscopic concentrations at the gas and liquid phase shows that the identifiable parameters of the model are the gas hold-up, ?, the Henry's constant, H, the reciprocal of the diffusion time, D/δ², and the volumetric mass-transfer coefficient, k_La. A procedure for the optimal experimental design is proposed based on the analysis of the Fisher information matrix of the model. The analysis concludes that the measure of the dynamics of the concentration just in the liquid phase leads to important systematic errors in the determination of k_La. The importance of the concentration measurement simultaneously in the gas and the liquid phase for the parameter estimation is demonstrated and discussed.     

A refined model for ozone mass transfer in a semibatch stirred vessel

The mathematical model proposed by Anselmi et al. (1984) for a semibatch stirred gas‐liquid contactor is refined to describe the mass transfer of ozone absorption and decomposition in aqueous solution with the decomposition rate expression of general reaction orders (not necessarily integers). Three system equations are employed to describe the ozone concentrations in the bulk liquid (C_ALb), the hold‐up gas (C_AGi), and the outlet gas in the free volume above the liquid surface (C_AGe), respectively. The effect of ozone decomposition on the mass transfer, which is reflected by the enhancement factor (E_r) defined as the ratio of mass absorbed per unit area in time t with chemical reaction (r) to that without chemical reaction or of the purely physical absorption, is considered in the refined model. Furthermore, the refined model also takes into account the variation of E_r with C_ALb, which changes with time during the course of gas‐liquid contacting. Thus this analysis extends the applicability of the model of Anselmi et al. (1984) and is of special importance for ozone mass transfer in the cases of basic solutions and of low mass transfer coefficients, in which the effect of decomposition on absorption is significant, and in the system with variable liquid phase ozone concentration.     

Magnetically Stabilized Bed for Selective Hydrogenation of Benzene

The characteristics of a magnetically stabilized bed (MSB) were studied by cold‐model experiments, using water as liquid phase, hydrogen as gas phase, and γ‐Fe₂O₃ magnetic powder as solid phase. The fluidized state of different bed positions was investigated by testing the transmissible laser current. Effects of magnetic field intensity and gas flow rate on layer expansion states of the MSB were analyzed by color diagrams. A Ru‐Zn‐B amorphous alloy was prepared by chemical reduction. Selective hydrogenation of benzene was carried out in the MSB by adjusting the contact time between the catalysts and reactants through variations of reaction temperature, magnetic field current, and liquid hourly space velocity.