Experimental investigation of fast-mode liquid modulation in a trickle-bed reactor

Unsteady-state operation of trickle-bed reactors (TBRs) is a promising technique to improve reactor performances especially when mass transfer phenomena are rate controlling. Among the different techniques, fast-mode modulation of the liquid flow rate seems to be one of the most successful. In fact cycling the liquid flow rate at very low frequencies can induce the reactor to work at the high-interaction regime where mass and heat transfer phenomena are strongly enhanced. Fast-mode periodic operation, then, can be considered an extension of the natural high-interaction regime at a mean range of gas and liquid flow rate normally associated with trickling regime in steady-state conditions.Experimental tests have been performed in a TBR employing α-methyl styrene hydrogenation on Pd/C catalyst in unsteady-state conditions by “on-off” fast-mode liquid modulation. Results have been compared with the steady-state experiments at the corresponding average liquid flow rate, revealing a conversion rate improvement up to 60%. All experiments have been performed in isothermal conditions, so conversion improvement can be ascribed only to mass transfer increase and not to thermal effects. The variation of gas and liquid flow rates and liquid cycle parameters presented several important implications about the optimal working conditions.     

Hydrodynamics of trickle bed reactors at high pressure: Two-phase flow model for pressure drop and liquid holdup, formulation and experimental validation

A large experimental database has been established at IFP on the same experimental setup to measure simultaneously pressure drop and liquid holdup in packed bed reactor operated in trickle for a large range of operating conditions. The varying parameters are liquid viscosity and density, gas density, bed particle shape and size. The range for gas density range is particularly large (from 1.3 to ), thanks to the use of dense gas to simulate very high pressure conditions. This data bank has been first used to compare the prediction accuracy of the different models from the literature. Finally, the mechanistic model proposed by Attou et al. [1999. Modelling of the hydrodynamics of the cocurrent gas-liquid trickle flow through a trickle-bed reactor. Chemical Engineering Science 54, 785-802] has been improved by adding a new formulation for liquid film tortuosity in two-phase flow conditions. This model has been validated over the whole data range and the accuracy has been checked with data external to the data bank. The prediction accuracy is significantly increased when compared with the best available models for pressure drop and liquid retention in trickle flow reactors.     

Prediction of pressure drop and liquid holdup in trickle bed reactor using relative permeability concept in CFD

A Computational Fluid Dynamics (CFD) model based on porous media concept is presented to model the hydrodynamics of two-phase flow in trickle-bed reactors (TBRs). The aim of this study is to develop a comprehensive CFD based model for predicting hydrodynamic parameters in trickle-bed reactors under cold-flow conditions. The two-phase Eulerian model describing the flow domain as a porous region has been used to simulate the macroscale multiphase flow in trickle beds operating under trickle flow regime using FLUENT 6.2 software. The closure terms for phase interactions have been addressed by adopting the relative permeability concept [Sàez, A.E., Carbonell, R.G., 1985. Hydrodynamic parameters for gas-liquid cocurrent flow in packed beds. A.I.Ch.E. Journal 31, 52-62]. The model has been evaluated by comparing predictions with the data (collected under a varied set of laboratory conditions) available in the open literature. It is shown that while being relatively simple in structure, this CFD model is flexible and predictive for a large body of experimental data presented in the open literature.     

Cyclic variation of the liquid flow residence time in periodically operated trickle-bed reactors

The cyclic variation of the mean residence time of the liquid phase is investigated in a trickle-bed reactor operated with a liquid feed rate modulated in a periodic square wave pattern. Experiments made using a salt tracer method are compared to a residence time model, based on the concept of continuity shock waves. The model predicts accurately the mean residence times and their cyclic variation in case of a non-zero base liquid flow rate. A particular application of the model is the adjustment of the feed cycle parameters in order to obtain a constant residence time of the liquid, no matter the moment at which it enters the bed. This particular cycle duration depends, among others, on the feed rates, but also on the bed length.     

Hydrodynamics of a cocurrent downflow of gas and foaming liquid through the packed bed. Part II. Liquid holdup and gas pressure drop

In the present study the results of experiments have been presented whose aim was to determine the values of liquid holdup as well as gas pressure drop through the packing for systems foaming under the pulse flow regime. On the basis of 245 experimental points for the pulse flow regime the verification of the models describing the hydrodynamics of the system has been performed. Attention was focused on the models of Benkrid et al. (Chem. Eng. Sci. 52 (1997) 4021), Pina et al. (AIChE J. 47 (2001) 19) and Fourar et al. (Chem. Eng. Sci. 56 (2001) 5987). It has been concluded that none of the models analysed describes the hydrodynamics of the foaming systems with enough accuracy. Next, based on our own data-base the verification has been carried out of parameters of Benkrid et al. (Chem. Eng. Sci. 52 (1997) 4021) (‘drift flux’ model for _L and boundary layer model for ΔP/H) and Pina et al. (AIChE J. 47 (2001) 19) models as well as the estimation of the values of F*-functions of Fourar et al. (Chem. Eng. Sci. 56 (2001) 5987) model. Using as the criterion the accuracy of estimation of the values of (ΔP/H) the best results have been obtained by applying Fourar et al. (Chem. Eng. Sci. 56 (2001) 5987) model (for the Ergun constants determined experimentally). The introduction of the estimated F*-functions into the equations of the model (Eqs. 11 and 12) makes it possible to estimate the liquid holdup with the average absolute relative error not exceeding 9.8% and the pressure drop with an error less than 26%.     

Local liquid saturation measurements inside a trickle bed reactor operating near the transition between pulsing and trickling flow

A wire-mesh tomography device was used to study the liquid saturation at 78 points covering the cross-sectional area of a 0.30 m diameter trickle bed reactor. Measurements in the pulsing flow near the transition were done for glass beads and alumina cylinders using air and water as fluids. Local liquid saturation measurements allow identification of flow regime and pulse frequency for each of the 78 points considered. To the best of the authors’ knowledge this is the first time that such local measurements are done for the complete sectional area of a trickle bed reactor. Flow rate conditions at which different flow regimes coexist at the same horizontal plane of the column were identified. A remarkable influence of the initial liquid distribution on the observed flow regime was also observed.     

Effect of partial wetting on liquid/solid mass transfer in trickle bed reactors

The wetting efficiency of liquid trickle flow over a fixed bed reactor has been measured for a wide range of parameters including operating conditions, bed structure and physico-chemistry of liquid/solid phases. This data bank has been used to develop a new correlation for averaged wetting efficiency based on five different non-dimensional numbers. Finally liquid/solid mass transfer has been determined in partial wetting conditions to analyse what are the respective effects of wetting and liquid/gas flow turbulence. These effects appear to be separated: wetting being acting on liquid/solid interfacial area while the liquid/solid mass transfer coefficient is mainly connected to flow turbulence through the interstitial liquid velocity. A correlation has been proposed for liquid/solid mass transfer coefficient at very low liquid flow rate.     

Phenomenological approach to interpret the effect of liquid flow modulation in trickle bed reactors at the particle scale

This work analyzes the influence of liquid flow modulation on the behavior of a reaction occurring in a spherical porous particle within a trickle bed reactor. A single first-order reaction between a gaseous reactant and a non-volatile liquid reactant is considered. Non-steady-state mass balances for gas and liquid reactants are formulated and solved under isothermal conditions in order to focus the analysis on the mass transport effects. Dynamic reactant profiles inside the catalytic particle are obtained for different cycling and system conditions. The enhancement factor (ε) due to periodic operation is defined to evaluate the impact of induced liquid flow modulation on reaction rate. Influence of cycling and system parameters on the enhancement factor is also reported for a wide range of conditions. Experimental trends observed by several authors can be explained with this approach.     

CFD simulation and experimental measurement of gas holdup and liquid interstitial velocity in internal loop airlift reactor

This paper documents experiments and CFD simulations of the hydrodynamics of our two-phase (water, air) laboratory internal loop airlift reactor (40 l). The experiments and simulations were aimed at obtaining global flow characteristics (gas holdup and liquid interstitial velocity in the riser and in the downcomer) in our particular airlift configurations. The experiments and simulations were done for three different riser tubes with variable length and diameter. Gas (air) superficial velocities in riser were in range from 1 to 7.5 cm/s. Up to three circulation regimes were experimentally observed (no bubbles in downcomer, bubbles in downcomer but not circulating, and finally the circulating regime). The primary goal was to test our CFD simulation setup using only standard closures for interphase forces and turbulence, and assuming constant bubble size is able to capture global characteristics of the flow for our experimental airlift configurations for the three circulation regimes, and if the simulation setup could be later used for obtaining the global characteristic for modified geometries of our original airlift design or for different fluids. The CFD simulations were done in commercial code Fluent 6.3 using algebraic slip mixture multiphase model. The secondary goal was to test the sensitivity of the simulation results to different closures for the drag coefficient and the resulting bubble slip velocity and also for the turbulence. In addition to the simulations done in Fluent, simulation results using different code (CFX 12.1) and different model (full Euler–Euler) are also presented in this paper. The experimental measurements of liquid interstitial velocity in the riser and in the downcomer were done by evaluating the response to the injection of a sulphuric acid solution measured with pH probes. The gas holdup in the riser and downcomer was measured with the U-tube manometer. The results showed that the simulation setup works quite well when there are no bubbles present in the downcomer, and that the sensitivity to the drag closure is rather low in this case. The agreement was getting worse with the increase of gas holdup in the downcomer. The use of different multiphase model in the different code (CFX) gave almost the same results as the Fluent simulations.     

An investigation of liquid maldistribution in trickle beds

The influence of liquid maldistribution at the top of the packing on flow characteristics in packed beds of gas and liquid cocurrent downflow (trickle beds) is experimentally investigated. Particular attention is paid to the effect of gas and liquid flow rates on flow development. Tests are made in the trickling and pulsing flow regimes. A uniform, a half-blocked and a quarter-blocked liquid distributor is tested. Packings of various sizes and shapes are employed. Data are presented on pressure drop and liquid holdup as well as trickling to pulsing flow transition. Diagnosis of radial and axial liquid distribution is made by means of conductance probes. The effects of liquid foaming, bed pre-wetting, top-bed material, and blockage midway the bed on liquid distribution are also examined. Overall, liquid waves in the pulsing flow regime have a beneficial effect, promoting uniform liquid distribution in the bed cross section.     

Effects of internals on phase holdup and backmixing in a slightlyexpanded-bed reactor with gas-liquid concurrent upflow

Five different internals were designed, and their effects on phase holdup and backmixing were investigated in a gas-liquid concurrent upflow reactor where the spherical alumina packing particles of three diameters (3.0, 4.5 and 6.0 mm) were slightly expanded under the conditions of varied superficial gas velocities (6.77×10^-2-3.61×10^-1 m·s^-1) and superficial liquid velocities (9.47×10^-4-2.17×10^-3 m·s^-1). The experimental results show that the gas holdup increases with the superficial gas velocity and particle size, opposite to the variational trend of liquid holdup. When an internal component is installed amid the upflow reactor, a higher gas holdup, a less liquid holdup and a larger Peclet number characterizing the weaker backmixing are obtained compared to those in the bed without internals under the same operating conditions. Additionally, the minimal backmixing is observed in the reactor equipped with the internals with a novel multi-step design. Finally, empirical correlations were proposed for estimating gas holdup, liquid holdup and Peclet number with the relative deviations within 11%, 12% and 25%, respectively.     

Hydrodynamics and flow regime transition study of trickle bed reactor at elevated temperature and pressure

The hydrodynamics in a trickle bed reactor (TBR) in non-ambient conditions are studied for air-water and air-acetone (pure organic liquid of low surface tension) systems. A flow map experiments for air-water and air-acetone systems are performed in a pilot plant reactor of 0.05 m i.d. and 1.25 m height. It has been demonstrated from the experimental results that the pressure drop tends to increase with increasing superficial gas and liquid velocity and reactor pressure, while it tends to decrease with increasing bed temperature. The results also show that the dynamic liquid holdup increases with increasing liquid velocity and decreases with increasing superficial gas velocity, reactor pressure and bed temperature. The dynamic liquid holdup and pressure drop values are obviously higher than those measured for air-water system at the same fluid fluxes, reactor pressure and bed temperature due to the surface tension effects. For higher reactor pressure and temperature, the trickle to pulse transition boundary shifts towered higher superficial velocities of both gas and liquid.     

Hydrodynamics of a novel multi-stage external loop airlift reactor

In the present investigation a novel multi-stage external loop airlift reactor with hydro-dynamically induced continuous bubble generation, breakup and regeneration has been proposed. The system has been designed to operate with relatively large sized bubbles, so that interfacial circulation can be induced in the liquid-bubble interfaces and faster transfer of components can take place by turbulent diffusion through the interface of the bubbles and also due to the physical rupture and reformation of the bubbles. The system was also designed to operate in three stages operating in series so that in each stage completely deaerated liquid could be brought in contact with freshly generated bubbles. Detailed studies on the gas holdup and liquid circulation velocity have been carried out with respect to various values of superficial gas as well as liquid velocities. The gas holdup of the proposed multi-stage system is 45% higher than the single stage system, which results in better mass transfer characteristics. Empirical correlations describing the performance of the proposed reactor have been presented in this paper.     

Bed structure and its impact on liquid distribution in a trickle bed reactor

Trickle bed reactors, which has been a workhorse for the process and refining industry for many decades, are progressively being challenged to provide solutions to deep processing of feedstocks. It is known that the structure of the packed bed which is formed with a certain arrangement of catalyst particles in the three-dimensional space within the reactor modulates in an unknown fashion the flow of fluids in the trickle bed, and in turn affects the conversion and selectivity in the trickle bed. Under deep processing conditions, the impact of the bed structure in modulating the overall reactor performance in a trickle bed is not as yet established. The question begets three sequential studies: estimating and quantifying the bed structure, measuring the liquid distribution, and estimating transport parameters (that are dependent on the bed structure and liquid distribution) so that the overall performance metrics as a reactor may be quantified. This contribution relates to the second of these questions, the first being already addressed to some extent by our earlier work. The current investigation aims at quantifying the effect of structure of the packed bed on hydrodynamics of the reactor. The impact of various packing techniques is discussed along with the development of correlations for two-phase pressure drop and dynamic liquid holdup. Liquid distribution is studied in depth for various operating parameters such as gas and liquid superficial velocities and column aspect ratio for uniform and non-uniform packing methods. The packing devices consist of various inserts attached to a hopper which can generate packing structures having void fraction in the range of 37.2%–46.4%. The maldistribution factor and flow maps for various aspect ratio of column suggest that maldistribution rises along with the increased channeling effect along the height of the column. Uniformly packed bed were measurably less prone to maldistribution along the length than the non-uniformly packed beds.     

The influence of distributed reactant injection along the height of a fluidized bed reactor

A two-phase model is used to simulate spreading the introduction of reactant feed along the height of a fluidized bed reactor for oxidative dehydrogenation of ethane to ethylene. The reactor model is used to predict the reactor performance for different ethane-to-oxygen molar feed ratios, with premixed and non-premixed feed. The proposed model is used to simulate the premixed feed (without secondary injection), and for distributed feed with secondary injection at one, three and five injection levels above the primary distributor. Predictions from the model are shown to compare favourably with experimental data from an industrial pilot reactor of diameter 97 mm. A case study is then employed to explore a wider range of conditions than is possible experimentally. Oxidant distribution is shown to be beneficial in expanding the range of reactant compositions beyond those normally allowed by safety constraints. Distributing the feed over a number of levels improves the reactor performance, especially in reducing the selectivities of undesired by-products. Feeding gas at several levels is generally more promising than introducing feed at a single secondary injection level.     

Modelling of unsteady-state hydrodynamics in periodically operated trickle-bed reactors:Influence of the liquid-phase physical properties

Process intensification using periodic operation of trickle bed reactors (TBRs) is still a long way from replacing conventional steady-state operation in industrial use, despite the numerous benefits described in the literature. Complex interactions between hydrodynamics, mass transfer and reaction phenomena make the design of periodically operated TBRs an almost insurmountable challenge. The development of hydrodynamic models able to provide reliable quantitative predictions of flow behaviour and possessing a sound physical basis, is an essential prerequisite for obtaining the necessary insights into this complexity. In this work, the two-phase pressure drop and dynamic liquid hold-up during max/min and on/off periodical operation were predicted using a model based on the relative permeability concept. In order to demonstrate the utility of this approach, a systematic investigation of the quantitative influence of the liquid-phase physical properties was carried out. The results obtained show that the modelling of the hydrodynamics in periodically operated TBRs using the relative permeability concept is feasible. By selecting suitable permeability parameters, unsteady-state hydrodynamics for different periodic operating modes can be predicted successfully.     

Liquid holdup in columns packed with structured packings: Countercurrent vs. cocurrent operation

An experimental study of the liquid holdup and the liquid holdup axial profile in a square section column with structured packing is carried out. Both cocurrent and countercurrent operations are examined. A conductivity technique to estimate liquid holdups is proposed and calibrated against values measured by the drainage method. Liquid holdups estimated by this technique follow the same trends as those previously found by other methods. Axial profiles of liquid holdup in the cocurrent and countercurrent operation are illustrated for liquid velocities below the loading point, and for solutions of different viscosity and foaming character. Variations between operation modes are larger for the foaming liquid than for the other liquid solutions employed.     

CFD simulation of hydrodynamics of gas-liquid-solid fluidised bed reactor

A three dimensional transient model is developed to simulate the local hydrodynamics of a gas-liquid-solid three-phase fluidised bed reactor using the computational fluid dynamics (CFD) method. The CFD simulation predictions are compared with the experimental data of Kiared et al. [1999. Mean and turbulent particle velocity in the fully developed region of a three-phase fluidized bed. Chemical Engineering & Technology 22, 683-689] for solid phase hydrodynamics in terms of mean and turbulent velocities and with the results of Yu and Kim [1988. Bubble characteristics in the racial direction of three-phase fludised beds. A.I.Ch.E. Journal 34, 2069-2072; 2001. Bubble-wake model for radial velocity profiles of liquid and solid phases in three-phase fluidised beds. Industrial and Engineering Chemistry Research 40, 4463-4469] for the gas and liquid phase hydrodynamics in terms of phase velocities and holdup. The flow field predicted by CFD simulation shows a good agreement with the experimental data. From the validated CFD model, the computation of the solid mass balance and various energy flows in fluidised bed reactors are carried out. The influence of different interphase drag models for gas-liquid interaction on gas holdup are studied in this work.     

Gas–liquid mass transfer in periodically operated trickle-bed reactors: Influence of the liquid-phase physical properties and flow modulation

The influence of periodic operation on trickle-bed reactor (TBR) hydrodynamics and gas–liquid mass transfer was investigated. Two-phase pressure drop, dynamic liquid hold-up and gas–liquid mass transfer coefficient (k_La) were determined at various liquid flow rates and for different modes of liquid flow variation (increasing and decreasing liquid flow rate). The results reveal the considerable influence of type of liquid flow rate modulation on k_La values (deviations of up to 80% in k_La). Simulation studies on gas-limited reaction in a periodically operated TBR indicate that an enhancement in conversion of about 14% can be expected from an appropriate selection of the operating mode, thus clearly demonstrating the quantitative process intensification feasible through increased gas–liquid mass transfer.