Induced pulsing in trickle beds—characteristics and attenuation of pulses

Gas/liquid down-flow in packed beds is studied, under periodic liquid feeding (at sufficiently high frequencies to be classified as “fast” mode of pulsing), in a range of mean liquid and gas flow rates within the steady “trickling flow regime”. The aim is to identify periodic feeding conditions resulting in improved fluid-mechanical characteristics (e.g. uniform fluids distribution) and possibly enhanced transport rates in this flow regime, which is common in industrial processes. From instantaneous, cross-sectionally averaged holdup measurements, at various locations along the packed bed, quantitative information is obtained on the axial propagation and attenuation of induced pulses. A phenomenological treatment of the pulse decay process facilitates data interpretation and leads to the determination of a characteristic attenuation factor for the various conditions tested. Key parameters of the process studied include, in addition to dynamic holdup, pressure drop, pulse celerity and intensity, as a function of fluid feed rates (G,L) and liquid cyclic frequency. Under the conditions of these tests, and for fixed mean rates G,L, the time averaged holdup and the pulse celerity are practically constant along the bed; furthermore, these quantities as well as the pressure drop do not seem to be affected by the imposed cyclic liquid feeding frequency. An expression to tentatively correlate pulse celerity data is recommended.The computed attenuation factors indicate that there is a rather narrow band of mean gas and liquid rates (along the so-called “pseudo-transition” boundary to pulsing flow) where pulse decay is at a minimum. Based on these results as well as on pulse intensity vs. bed length data, recommendations are made on preferred conditions for induced pulsing (from the fluid-mechanical standpoint) which would maximize expected benefits.     

A study of particle shape and size effects on hydrodynamic parameters of trickle beds

Uniform-spherical and cylindrical-extrudate particles are employed to study air-water downflow in a packed bed of 14 cm i.d. The effect of particle shape, neglected in the literature so far, is shown to be very significant. A packed bed of extrudates displays significantly greater global dynamic liquid holdup h_d and pressure drop, as well as a trickling-to-pulsing transition boundary at higher gas flow rates, compared to beds of spheres of comparable size. Moreover, packed extrudates exhibit a significant increase of holdup, h_d, in the axial flow direction, a trend reported for the first time as there are no similar data available in the literature; on the contrary beds of spherical particles are characterized by practically constant h_d in the axial direction. Although an explanation for this h_d axial variation is not obvious, one might attribute it to the anisotropy and non-uniformity of interstitial voids of packed cylindrical particles. For beds of uniform spheres, in the diameter range examined (3-6 mm), the effect of size on both dynamic holdup and pressure drop, although quite pronounced, is not as significant as the effect of particle shape. An extensive survey of literature data, obtained with similar spherical particles, suggests that small bed diameters have an appreciable influence on trickling-to-pulsing transition boundary. Comparisons are reported with literature methods for predicting the measured parameters; discrepancies between data and predictions may be partly due to the inadequacy of a single “equivalent” diameter to represent both shape and size of non-spherical particles; predictive methods performing best are also identified.     

A study of local liquid/solid mass transfer in packed beds under trickling and induced pulsing flow

Induced pulsing flow (by cyclic liquid feeding) in packed beds, operated in the trickling flow regime, is studied as a method of overall improvement of catalytic reactor operation. In this paper results are reported of experiments aimed at determining local and global liquid/solid mass transfer rates, mainly for the so-called fast mode of ON-OFF periodic liquid feeding, with frequencies of order 0.1 Hz. Such mass transfer data for the fast mode of induced pulsing are not available in the literature. Uniform 6 mm glass spheres and alumina cylindrical extrudates, of 1.5 mm diameter and a narrow distribution of lengths, are employed in the tests. For completeness, results are also reported for single-phase (liquid) and trickling flow through the same packed beds. A well-known electrochemical technique is employed to measure instantaneous local mass transfer coefficients by means of quite a few probes distributed throughout the bed. The hydrodynamic characteristics under the above conditions, reported in companion papers, are helpful in interpreting the new mass transfer data.There is a wide spread of the time-averaged local mass transfer rates, in all cases tested, apparently due to packing and flow non-uniformities. This spread is much smaller in the case of packed uniform spheres. In general, the benefits of cyclic liquid feeding are more evident in the packed bed of spheres than in that of cylindrical extrudates; for instance, with increasing mean liquid rate, induced pulsing tends to reduce the spread of local mass transfer coefficients, which suggests that more uniform fluids distribution is promoted. The imposed liquid pulses are reflected in the observed periodic variation of local mass transfer coefficients; the latter appear to decay along the bed in the same manner as the liquid pulses. Other trends of local mass transfer rates are identified and discussed in relation to measured variation of liquid holdup, under the same conditions. For packed spheres, the measured global mass transfer rates are in fair agreement with literature correlations obtained for the trickling flow regime, unlike the case of packed extrudates where significant deviation is observed.     

Influence of temperature on fast-mode cyclic operation hydrodynamics in trickle-bed reactors

Despite the merits of periodic operation praised in the academic literature as one of the process intensification strategies advocated for trickle-bed reactors (TBRs), there is still reluctance to implement it in industrial practice. This can partly be ascribed to the lack of engineering data relevant to the elevated temperature and pressure characterizing industrial processes. Currently, the hydrodynamics of trickle beds under cyclic operation, especially in fast mode at elevated temperature and pressure, remains by and large terra incognita. This study proposes exploration of the hydrodynamic behavior of TBRs experiencing fast liquid flow modulation at elevated temperature and moderate pressure. The effect of temperature and pressure on the liquid holdup and pressure drop time series in terms of pulse breakthrough and decay times, pulse intensity and pulse velocity was examined for a wide range of superficial gas and liquid (base and pulse) velocities for the air-water system. The pulse breakthrough and decay times decreased, whereas the pulse velocity increased with temperature and/or pressure. The pressure drop was attenuated with increasing temperature for a given superficial gas, and base and pulse superficial liquid velocities. Experimental pulse velocity values were compared to the Giakoumakis et al. [2005. Induced pulsing in trickle beds—characteristics and attenuation of pulses. Chemical Engineering Science 60, 5183-5197] correlation which revealed that it could be relied upon at elevated temperature and close to atmospheric pressure.     

Hydrodynamics in a pilot‐scale cocurrent trickle‐bed reactor at low gas velocities

Hydrodynamic data obtained from laboratory‐scale trickle‐beds often fail to accurately represent industrial‐scale systems with high packing aspect ratios and column‐to‐particle diameter ratios. In this study, pressure drop, liquid holdup, and flow regime transition were investigated in a pilot‐scale trickle‐bed column of 33 cm ID and 2.45 m bed height packed with 1.6 mm × 8.4 ± 1.4 mm cylindrical extrudates for air‐water mass superficial velocities of 0.0023 – 0.094 kg/m²s and 4.5 – 45 kg/m²s, respectively, at atmospheric pressure. Significant deviation was observed from pressure drop and liquid holdup correlations at low liquid flows rates, corresponding to gravity‐driven flow limit. Likewise, liquid saturation is overestimated by correlations at high liquid flow rates, owing to significantly reduced wall effects. Lastly, trickle‐to‐dispersed bubble flow and trickle‐to‐pulsing flow regime transitions are reported using a combination of visual observations and analysis of the magnitude of local pressure fluctuations within the column. © 2018 American Institute of Chemical Engineers AIChE J, 64: 2560–2569, 2018     

EFFECT OF VISCOSITY ON HYDRODYNAMIC PROPERTIES OF PULSING FLOW IN TRICKLE BEDS

New data on pulsing flow onset, properties of pulses (frequency, celerity, length), liquid holdup and pressure drop are presented for aqueous glycerol solutions of viscosity 6.7 and 20.2 mPa s and compared with similar measurements from an air-water (1.0 mPas) system. With the exception of viscosity, all other physical properties of the liquid phase are kept constant and fairly close to those of water, thus allowing a direct assessment of the effect of viscosity. Pulse formation and propagation with viscous liquids is examined on the basis of time records from a conductance type technique. A striking effect due to increased liquid viscosity is the reduction of the pulsing flow regime; in particular, the pulsing-to-bubbling transition boundary is shifted towards higher gas flow rates. Pulse frequency and celerity appear to decrease only slightly with increasing liquid viscosity, whereas the two-phase pressure gradient increases significantly. Liquid holdup also tends to increase with viscosity. Moreover, holdup with viscous liquids tends to increase significantly with the liquid flow rate, whereas an insignificant effect is found for water. A new correlation for estimating liquid holdup is proposed, and a simple model for predicting pulsing flow characteristics is modified in order to take account of the aforementioned effects.     

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.     

滴流床中持液量及流型转变的一维流体力学模型

针对滴流床中均匀球形填料,在颗粒尺度上分析气液两相在颗粒空隙中的流动.从基本的流体力学方程出发,建立了微观流动模型,求得滴流区液相在填料表面上的分布,进而计算液相总持液量,并通过对液膜波的稳定性分析,提出了滴流区向脉动区转变的判据.模型与实验结果及文献值作了比较,符合程度较好.     

Hydrodynamics of a mobile bed contactor with ‘Low’ density packing particles of different shapes

Experimental studies have been reported on pressure drop, liquid holdup, bed expansion and minimum fluidization velocity in a 0.15 m ID mobile bed of relatively low density (53–183 kg m^?3) spherical and irregular shaped particles. The Kito-Tabei-Murata correlation has been adapted to fit the data on the liquid holdup and the pressure drop. The bed expansion was found to depend on the shape and density of the particles. It is shown that, in general, only a part of the liquid holdup in the bed is supported by the upward flow of gas. It was observed that in some regions the particles congregated at the wall, leaving a particle free core. The maps depicting these regions are presented.     

Rationalising MRI, conductance and pressure drop measurements of the trickle-to-pulse transition in trickle beds

Recent MRI data have shown that the transition from trickle to pulsing flow in trickle-bed reactors occurs over a range of liquid velocities at constant gas velocity. The transition is initiated by isolated local pulsing events, which increase in number with increase in liquid velocity until a maximum number exists. Above this liquid velocity, which we have termed the transition point, the individual pulses merge until a single macro-scale pulse is formed and the whole bed demonstrates pulsing flow. In this paper we compare the characterisation of the transition obtained using conductance and pressure drop measurements with that obtained using MRI. Using the insights gained from the 3-D MRI measurements, recorded with a data acquisition time of 280 ms, it is shown that the conductance and pressure drop measurements are sensitive to different stages of the evolution of the hydrodynamic transition, a factor important when using these different measurements in the development and validation of numerical and theoretical models. Conductance measurements identify unambiguously only the onset of the single macro-scale pulse regime, consistent with a determination of the transition point made by visual observation. In contrast, pressure drop measurements are sensitive to both the onset of formation of local pulses and the liquid velocity at which the maximum number of liquid pulses occurs. We also show how a combination of conductance and pressure drop measurements can be used to fully characterise the transition, thereby enabling translation of the insights gained by MRI into a robust measurement strategy for use on larger-scale reactors. Data are reported for a cylindrical column of length 70 cm and inner diameter 43 mm, packed with cylindrical porous γ-Al₂O₃ packing elements of length and diameter 3 mm. The bed was operated under conditions of co-current downflow of air and water, at ambient temperature and a pressure of 2 barg. Gas and liquid superficial velocities were in the range 25-300 and 0.9-, respectively.     

Multiple hydrodynamic states in trickle flow: Quantifying the extent of pressure drop, liquid holdup and gas-liquid mass transfer variation

It is well established that pressure drop and liquid holdup under trickle flow conditions are functions of the flow history. However, the extent of possible variation of these and other critical hydrodynamic parameters has not been fully quantified. In this study, specifically defined prewetting procedures are used as limiting cases for hydrodynamic hysteresis. These are:

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Non-prewetted.

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Levec prewetted: the bed is flooded and drained and after residual holdup stabilisation the gas and liquid flows are introduced.

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Kan_L prewetted: the bed is operated in the pulse flow regime (by increasing liquid velocity) after which liquid flow rate is reduced to the desired set point (all at the desired gas flow rate).

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Kan_G prewetted: the bed is operated in the pulse flow regime (by increasing gas velocity) after which gas flow rate is reduced to the desired set point (all at the desired liquid flow rate).

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Super prewetted: the bed is flooded and gas and liquid flows are introduced once draining commences.

It is shown that the upper limiting case for pressure drop is the Kan_L mode of operation. The lower limiting cases are the non-prewetted and Levec prewetted modes (these coincide). Pressure drop may vary by as much as 700% even for prewetted beds. Liquid holdup is different in all five prewetting modes. The upper limiting case is the Kan_G mode of operation, while the lower limiting case is the non-prewetted mode (Kan_G holdup is approximately 160% that of non-prewetted mode holdup at ). At low gas velocities the Kan_L holdup can be 400% of that of the non-prewetted beds. Importantly, the lower limiting case for prewetted beds is the Levec mode. Holdup in the Kan_G mode may be as much as 130% of the holdup in the Levec mode (at ).The effect of hydrodynamic multiplicity of the volumetric mass transfer coefficient is measured by the desorption of oxygen from water into nitrogen. In this case the different prewetting procedures result in three distinct regions, the upper region being the Kan and Super prewetted beds, the intermediate region being the Levec prewetted bed and the lower region being the dry bed. Mass transfer coefficients in the upper region can be as much as 600% of that of the lower region and 250% of that of the intermediate region. Evidently, prewetting (and even pulsing flow prewetting) does not guarantee that the bed is operating at the maximum values of pressure drop, holdup and mass transfer coefficient. Evidence of operation in between the limiting cases is presented. These non-limiting cases can be reached in multiple ways.     

A simple correlation for solids holdup in a gas-liquid-solid fluidized bed

A simple empirical model was established which allows solids holdup in a gas-liquid-solid fluidized bed containing large and dense particles to be readily predicted based on the equation of Richardson and Zaki (1954, Trans. Inst. Chem. Engrs32, 35) for liquid-solid fluidized bed systems. The approach is applicable both to monocompnent particle systems and to binary mixtures of particles. For a monocomponent system, a correlation for model parameters was proposed which is expressed as a function of particle diameter, particle density, bed diameter and liquid density. For a binary mixture of particles, the averaging and serial approaches were shown to predict the solids holdup equally well within the range of the gas and liquid velocities considered. Experiments were also performed using eight solid particles for the monocomponent system and five binary mixtures of particles differing in diameter and/or density for the mixture system to substantiate the model.     

Comparison of normal phase operation and phase reversal studies in a pulsed sieve plate extraction column

The hydrodynamic characteristics of a pulsed sieve plate extraction column (PSPEC) was studied experimentally using two different liquid phase systems, namely water/kerosene and 30%TBP (tributyl phosphate) in NPH (normal paraffin hydrocarbon)/0.3 M HNO₃. The aqueous phase as the dispersed phase and the organic phase as the continuous phase (phase reversal) and vice versa (normal phase operation) studies in a pulsed sieve plate extraction column 0.076 m in diameter and 1 m height are presented in this paper. The hydrodynamic properties like drop size and holdup are characterized as a function of various operating parameters namely pulse velocity, dispersed phase and continuous phase velocity and duty cycle of pulsing. Flooding in the column was also investigated for the changes involving flow ratio of continuous phase to that of the dispersed phase for both insufficient and excessive pulsing. It has been observed that phase reversal mode of operation is not efficient as compared to normal phase operation for the PSPEC.     

Effect of particles on hydrodynamics and mass transfer in a slurry bubble column: Correlation of experimental data

The effects of particle concentration and size on hydrodynamics and mass transport in an air–water slurry bubble column were experimentally studied. When the particle concentration α_s increased from 0% to 20%, the averaged gas holdup decreased by ~30%, gas holdup of small bubbles and gas–liquid volumetric mass transfer coefficient decreased by up to 50%, while the gas holdup of large bubbles increased slightly. The overall effect of particle size was insignificant. A liquid turbulence attenuation model which could quantitatively describe the effects of particle concentration and size was first proposed. Semi-empirical correlations were obtained based on extensive experimental data in a wide range of operating conditions and corrected liquid properties. The gas holdup and mass transfer coefficient calculated by the correlations agreed with the experimental data from both two-phase and three-phase bubble columns, with a maximum error <25%.     

滴流床反应器内脉冲流宏观流体力学的特性参数

引　言在石油化工工业的加氢处理中 ,滴流床反应器常操作在接近脉冲流流型区域[1] .脉冲流下气液流速都比较高 ,所以该操作方式适合催化剂活性高、反应速率快的反应[2 ] ,而且气液流量大有利于强放热反应的反应热从反应器移出。流体力学参数如脉冲速度、脉冲频率、持液量、气液分布、压力降等对于该类反应器的工业设计及操作具有很重要的意义 .Ｓａｔｏ等[3] 较早地对脉冲流的特性进行过定性的实验研究 .Ｂｌｏｋ等[4 ] 以及Ｔｓｏｃｈａｔｚｉｄｉｓ等[5] 通过电导法也对脉冲流宏观特性进行过研究 .本文用不同的实验方法对滴流床反应器内脉…     

Transition to pulsing flow,holdup and pressure drop in packed columns with cocurrent gas-liquid downflow

Trickle beds of 1 meter in length and resp. 5, 10 and 20 cm in diameter were operated in the so-called pulsing flow regime. The packing was 2.5 resp. 4 mm Raschig rings. Air was taken as the gas phase. Several liquids were used.In this contribution we describe the transition from gas-continuous to pulsing flow, the liquid holdup and the pressure drop over the column. The transition can be described by an effective Froude-number. Correlations are set up for the transition point as well as for the hold-up.Pressure drop is shown to be linearly dependent upon the pulse frequency. In a separate series of experiments the transition to pulsing flow was measured in a 5 mm capillary tube, used as a wetted wall column. It became clear, that the onset of pulsing flow in such a capillary is not determined by the same parameter as the onset of pulsing flow in a packed column.     

Hydrodynamics and mass transfer enhancement of gas–liquid flow in micropacked bed reactors: Effect of contact angle

Pressure drop, residence time distribution, dispersive behavior, liquid holdup, and mass transfer performance of gas–liquid flow in micropacked bed reactors (μPBRs) with different contact angles (CA) of particles are studied. The value of pressure drop for three types of beads can be obtained: copper beads (CA = 88.1°) > stainless steel beads (CA = 70.2°) > glass beads (CA = 47.1°). The liquid axial dispersion coefficient is 1.58 × 10⁻⁶ to 1.07 × 10⁻⁵ m²/s for glass beads and copper beads, which is smaller than those of trickle bed reactors. The liquid holdup of 400 μm copper beads is larger than that of 400 μm glass beads. The ratio of effective interfacial area enhancement is evaluated up to 55% for big contact angle beads compared with the hydrophilic glass beads. In addition, correlations of pressure drop, liquid holdup, and effective interfacial area in μPBRs with different wettability beads are developed and predicted values are in agreement with the experimental data.     

Pressure drop hysteresis in trickle bed reactors

An understanding of the hydrodynamics of trickle bed reactors (TBR) is essential for their design and prediction of their performance. Flow variables, packing characteristics, physical properties of fluids and operation modes influence the behavior of the TBR. The existence of multiple hydrodynamic states or hysteresis (pressure drop, liquid holdup, catalyst wetting, gas-liquid mass transfer) is due to the different flow structures in the packed bed and can be attained by a set of different operating procedures. Experiments were performed to study the effect of liquid and gas velocity, liquid surface tension, liquid viscosity and the particle diameter of the packing on two-phase pressure drop hysteresis. The parallel zone model for pressure drop hysteresis in the trickling flow was used for analysis of experimental data and flow structure. Theoretically predicted pressure drop hysteresis loop is in satisfactory agreement with experimental data.     

Trickle bed hydrodynamics and flow regime transition at elevated temperature for a Newtonian and a non-Newtonian liquid

Despite the hydrodynamics of trickle beds experiencing high pressures has become largely documented in the recent literature, trickle bed hydrodynamic behavior at elevated temperatures, on the contrary, largely remains terra incognita. This study's aim was to demonstrate experimentally the temperature shift of trickle-to-pulse flow regime transition, pulse velocity, two-phase pressure drop, liquid holdup and liquid axial dispersion coefficient. These parameters were determined for Newtonian (air-water) and non-Newtonian (air-0.25% Carboxymethylcellulose (CMC)) liquids, and the various experimental results were compared to available literature models and correlations for confrontation and recommendations. The trickle-to-pulse flow transition boundary shifted towards higher gas and liquid superficial velocities with increasingly temperatures, aligning with the findings on pressure effects which likewise were confirmed to broaden the trickle flow domain. The Larachi-Charpentier-Favier diagram [Larachi et al., 1993, The Canadian Journal of Chemical Engineering 71, 319-321] provided good predictions of the transition locus at elevated temperature for Newtonian liquids. Conversely, everything else being kept identical, increasingly temperatures occasioned a decrease in both two-phase pressure drop and liquid holdup; whereas pulse velocity was observed to increase with temperature. The Iliuta and Larachi slit model for non-Newtonian fluids [Iliuta and Larachi, 2002, Chemical Engineering Science 46, 1233-1246] predicted with very good accuracy both the pressure drops and the liquid holdups regardless of pressure and temperature without requiring any adjustable parameter. The Burghardt et al. [2004, Industrial and Engineering Chemistry Research 43, 4511-4521] pulse velocity correlation can be recommended for preliminary engineering calculations of pulse velocity at elevated temperature, pressure, Newtonian and non-Newtonian liquids. The liquid axial dispersion coefficient (D_ax) extracted from the axial dispersion RTD model revealed that temperatures did not affect in a substantial manner this parameter. Both Newtonian and power-law non-Newtonian fluids behaved qualitatively similarly regarding the effect of temperature.     

Flow through packed bed reactors: 2. Two-phase concurrent downflow

A model for the prediction of pressure drop and liquid holdup for trickling flow in packed bed reactors has been developed, based on the relative permeability concept. The relative permeabilities for gas and liquid as functions of corresponding phase saturations have been studied with 1300 newly measured data pairs of pressure drop and liquid holdup obtained for a wide range of commercially relevant operating conditions (including pressures up to 50 bar) as well as types of packing (both in terms of size and shape). The relative permeabilities are found to be solely the functions of corresponding phase saturations and it is shown that the functional form of the correlations developed, which are otherwise purely empirical by nature, has its roots in the physics of flow at the microscale level. The proposed model requires no prior experimental knowledge about the packed bed and is able to predict liquid holdup and pressure drop to within 5% and 20%, respectively, regardless of the type of packing or operating range investigated.