Article pubs.acs.

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A 3D CFD-DEM Methodology for Simulating Industrial Scale Packed Bed Chemical Looping Combustion Reactors
Mandar V. Tabib, Stein T. Johansen, and Shahriar Amini*
Flow Technology Group, SINTEF Materials and Chemistry, Trondheim 7034, Norway ABSTRACT: Design of industrial scale packed bed reactors can be aided by using computational uid dynamics (CFD)-discrete element method (DEM) simulation for understanding the transport phenomena. However, conducting CFD-DEM simulation for the whole large-scale packed bed reactor is computationally prohibitive, which limits the usage of this tool. Hence, a methodology has been developed to identify the segments of the bed, which can serve as a good representative for the CFD simulation of large industrial scale packed bed reactors. Two segments, a cylindrical cut-segment and a wall-segment, have been used to represent the core central region of packed bed and the near wall region of packed bed, respectively. The methodology determines the size (diameter and height) of the cylindrical bed cut-segment that can be a good representative for the large-scale packed bed reactor. The segments are then used to obtain the information on transport phenomena (friction factor coecients (pressure drop) and the heat transfer/mass-transfer coecients) for packed beds made of spherical particles and non-spherical particles. CFD simulations have been conducted on the DEM generated packing segments for a wide particle Reynolds number range (from laminar to turbulent regime) to develop the correlations. The proposed methodology (on cut-segment and wallsegment) has been validated for spherical particle packed bed by comparing results to well-established correlations (such as Ergun equation for pressure drop, Wakao correlation and multiparticle RanzMarshal correlation for particle heat transfer coecient, and DixonLubua and ColledgePaterson correlation for wall heat transfer coecient). The methodology is then applied to understand the transport phenomena and to develop correlations for long cylindrical pellet (aspect ratio 7) and utedring. The pressure drop correlation obtained for the long cylindrical pellet (aspect ratio of 7) packed bed has been compared to the correlation for cylindrical pellet with aspect ratio of 5.77 (obtained by Nemec; Nemec, D.; Levec, J. Chem. Eng. Sci. 2005, 60, 6947). The comparison shows that the eect of increasing aspect ratio on pressure drop is captured as per the expected trend. The methodology has been applied in a chemical looping combustion reactor based on the pressure drop and heat transfer results. Thus, the proposed CFD-DEM methodology oers a computationally ecient way of understanding the transport phenomena in an industrial scale reactor through simulating a methodically selected segment inside the reactor. This enables design and performance assessment of such reactors. reactor. The packing structure can have signicant eect on the pressure drop, the heat transfer, and the mass transfer characteristics of the system. Traditionally, these critical parameters required for the designing of packed bed reactors are obtained using empirical correlations (such as Ergun,5 Eisfeld,6 and Nemec1 for obtaining pressure drop; multiparticle Ranz and Marshal;7,38 Li and Finlayson8 and Dixon9 for obtaining heat transfer coecient; Leva10 and Dixon11 for computing void fraction). However, some of these correlations are valid only for certain operating conditions and for known particle shapes, such as Ergun is valid for spherical particles packing with tube to diameter ratio greater than 5. Nemec1 has modied Ergun correlation for dierent particle shapes, but the correlations are valid for cylindrical pellets up to aspect ratio of 5.77. Similarly, Ranz and Marshals7,38 heat transfer correlation is valid for spherical particles packing; while Li and Finlaysons8 heat transfer correlation for cylindrical pellets is valid up to particle Reynolds number of 800. Thus, every correlation has its range of applicability. In recent times, novel packed bed
Received: Revised: Accepted: Published:
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1. INTRODUCTION The packed bed chemical looping combustion (CLC) reactor has been envisaged as a cost-eective technology for transforming hydrocarbons into energy along with CO2 capture.14 The packed bed CLC process involves the utilization of the redox chemistry of a transition metal in a cyclic operation. The transition metal oxide acts as an oxygen carrier and forms the xed packing of the packed bed reactor. This xed packing is alternatively exposed to fuel gas stream (reduction cycle) and air streams (oxidation cycle). When exposed to the fuel gas stream (syngas), the metal oxide reduces. This reduction cycle results in production of hot stream of carbon dioxide and superheated steam, which can be used for energy generation. The reduced metal oxide bed is then exposed to the air stream, which reoxidizes it. This exothermic oxidation cycle produces a stream of hot gas that can also be used for energy production. The reductionoxidation cycle is then repeated continuously leading to power generation and CO2 capture (CO2 isolated by condensing steam). The ease of scale-up of packed bed reactors oers a possible early rollout for its use at commercial scale, provided the technology is rst shown to be feasible at a lower scale of operation. This work aims to contribute to the design and development of such a technology by developing a methodology for proper understanding of the transport phenomenon within the packing structure of a packed bed
2013 American Chemical Society

July 30, 2012 June 8, 2013 June 11, 2013 June 11, 2013
dx.doi.org/10.1021/ie302028s | Ind. Eng. Chem. Res. 2013, 52, 1204112058

Industrial & Engineering Chemistry Research chemical looping combustion reactors and many industrial scale packed bed reactors are using/testing some unique catalyst shapes (such as high aspect ratio cylindrical pellet and uted ring particle) at stringent reactor operating conditions (such as particle Reynolds number from 760 to 1500, 20 bar pressure, 1000 K). The currently available empirical correlations (as mentioned above) will not be valid in such cases. When the particle shape and size change, the packing structure (particle orientation and porosity) will change, and this will change the transport phenomenon within the bed. In such circumstances, computational uid dynamics (CFD)-discrete element method (DEM) can provide a cost-eective way of understanding the transport phenomena in the random packing structure of the packed bed. This is especially crucial, as it is dicult or timeconsuming to conduct experiments under such conditions and obtain appropriate correlations. Here, the DEM has been used to generate the random packing structure of the uted ring particles and the high aspect ratio cylindrical pellets. The CFD is then conducted on the DEM generated packing structure to understand the transport phenomena. However, the use of CFD-DEM model for simulating large-scale industrial reactors (tube to particle diameter ratio greater than 40) is computationally prohibitive. Hence, to meet our aims of aiding the design of packed bed reactor using CFD-DEM model, a new methodology needs to be developed and new correlations need to be obtained that can be used as closure by a simplied 1D model for designing. Hence, the current work aims to address these issues by meeting the following objectives: (a) Developing a methodology to overcome the diculties in the simulation of ow in the packed bed containing a huge number of particles. The current work aims to put forward a new methodology, involving the use of two segments: a cylindrical bed-segment with slip wall boundary condition (CBS-SW) for studying pressure drop and particle heat transfer and a wall-segment approach for studying wall heat transfer coecient. To be sure that the selected bed-segment is good representation of the industrial scale packed bed reactor, the methodology focuses on obtaining suitable dimensions of the bed-segment (diameter and height of the segment). The validation of methodology will be done by using a spherical particle where established correlations are available for comparison. (b) Developing correlations by understanding the transport phenomena: The proposed methodology will demonstrate its ability to obtain information on transport phenomena (friction factor (pressure drop) and heat transfer coecient) for unique particle shapes (uted ring and long-aspect ratio cylindrical pellets), which will also allow for design of packed bed reactor using a simplied and faster 1D model. (c) Enabling comparison of pellet shapes: To demonstrate that the understanding of transport phenomena (the ow proles, the heat transfer, and the pressure drop) gained by use of proposed CFD-DEM methodology can enable comparison of dierent packing structure (cylindrical pellet packing and uted ring packing) for design purposes. The development of this methodology has wider application as it encourages a potential serial by simplication multiscale modeling approach, wherein the correlation obtained by 3D CFD-DEM model on a representative volume of the packed bed is plugged into the 1D model to design the reactor. This methodology can also be in general applied to study dierent types of packings (such as trilobe, quadrulobe, monoliths,
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wagon wheels, hollow extrudates, discs) for which the correlations are not available in literature. To highlight the uniqueness of our proposed novel CFDDEM methodology and how this work lls some new knowledge gaps, a brief literature review is presented below.

2. LITERATURE REVIEW In literature, several notable contributions have been made toward understanding the transport phenomena in the packed bed using CFD for simplied geometry. One of the constraints in enabling CFD-DEM simulation of packed bed is the limitation with generating the computational mesh for the complex packing geometry. A ne mesh is required to capture the ow in the voidage, and the contact points between the particles and particle-wall have to be treated to avoid skewed cells. The huge meshing requirement limits the geometry size that can be simulated. To enable modeling, researchers have incorporated simplications to the sophisticated packed bed structure, and have come up with some notable contributions in this eld. The simplications involve: (a) use of eective porous medium in place of actual particle packing for both single phase and multiphase ows.1214 The porous media concept has been popularly used to design packed beds as it is computationally ecient. However, the porous media concept does not consider the solid phase to be made up of discrete particles but only as an eective phase with a dened void fraction. The void fraction distribution is provided as an input with additional terms implemented in the momentum balance to allow for the additional resistance to ow. For meeting our current objectives of accurately characterizing the eect of a particular particle shape on pressure drop and heat transfer coecient, this approach may not be suitable. (b) Another simplied approach applies the assumption of a quasihomogeneous reactor model, which involves the heat transfer and dispersion to be lumped.15 The lumping of transport processes conceals much physical phenomena, and this needs the introduction of an eective viscosity for the bed for obtaining agreement between computed and experimental velocity proles. Hence, this approach may not be applicable for our work. (c) Researchers from Dixons group1620 pointed out that it would be better to use the geometry of particle packing, and they have made some major notable contributions by taking this approach. Because of computational constrains, they simplied the actual packing structure, by use of wallsegment section as a representative of the entire geometry and by use of structured packing or a predened arrangement of particles in place of actual random packing. Dixons group have used a periodic 120 wall-segment model with symmetry side condition to understand the phenomena in vessels with a low tube to particle diameter ratio of 4. Here, the packing structure is arranged in a manner as observed by them frequently in their study of cylindrical pellets in a tube. However, in most real situations, the randomly generated packing structure (comprised of nonspherical particle shapes) may not lead to a repeatable pattern or any frequently seen arrangement. Hence, the use of periodic boundaries might not be possible for our case. (d) Recently, the DEM has been used to generate a very realistic packing structure.21 Bai22 used DEM to obtain the spherical particle and cylindrical pellet packing in their lab-scale, low tube-to-particle diameter vessel and used this for their CFD simulation. Others too have successfully used this approach with simple spherical particles at low tube-to-particle diameter.23,24 However, for large-scale packed bed reactors
dx.doi.org/10.1021/ie302028s | Ind. Eng. Chem. Res. 2013, 52, 1204112058

Industrial & Engineering Chemistry Research (with expected high tube-to-particle diameter ratio of around 40) involving nonspherical particles, it will be computationally prohibitive to generate mesh even for a smaller wall-segment as the walls are 40dp distance away. Also, in such cases, the actual wall eect of vessel can be neglected as the wall eect is conned to a smaller region (up to 35dp from wall). In such cases, the methodology presented in this work involving the cylindrical bed-segment with slip wall boundary condition (CBS-SW) can be widely used for studying the pressure drop in large-scale industrial packed bed reactors. For obtaining near wall information in an industrial scale reactor, a wall-segment can be constructed up to 35 particle diameter from the wall. This has also been attempted in this work by obtaining the wall heat transfer coecient. The section below explains the methodology, which is followed by details of simulation parameters and discussion on results.

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Figure 2. Particle shape generated using multiple spheres using scripts: (A) cylindrical pellets (aspect ratio: 7, sphericity 0.65), and (B) uted ring (aspect ratio: 1.4).

3. METHODOLOGY FOR ENABLING SIMULATION OF THE LARGE-SCALE PACKED BED CLC REACTOR The methodology determines the size of the bed cut-segment that can be a good representative for the large-scale reactor, which can enable meshing and the CFD simulations to be conducted. The bed cut-segment is a concentric cylindrical cutsection of size diameter (D*) and height (H*) carved out of the entire DEM generated packing bed (of diameter D and height H) (see Figure 1 for schematic representation). The following steps are carried out to select the bed-segment size D* and H*:

Table 1. Simulation Details and Particle Size

particle dimensions average external diameter (mm) average length (mm) equivalent particle diameter (dp, mm) uted ring particle 12.4 17.3 13.86 cylindrical pellet 3.6 24.9 7.4 spherical particle

10

Table 2. DEM Parameters Used in the Study

DEM parameters model to simulate particle collisions and motion particle density shear modulus, N/m2 Poissons ratio local damping coecient particleparticle and particlewall friction coecient uted ring/ cylindrical pellet HertzMindlin model 2300 kg/m3 1 108 0.25 0.7 0.3 spherical pellet HertzMindlin model 2300 kg/m3 1 108 0.25 0.7 0.4

Figure 1. Schematic of DEM generated packing structure and the bedsegment cut-section from it.

(a) First, discrete element modeling (DEM) is used to generate the packing structure for a given catalyst shape. The nonspherical catalyst shapes (such as cylinder pellet and uted ring particle) are generated by using a multisphere model, where the locations of spheres are determined through a user dened script. Figure 2 shows the cylindrical pellet and uted ring particle formed out of multiple spheres. The details of DEM simulations and particle sizes used in actual simulation are given in Tables 1 and 2. The simulation of the lling process becomes computationally prohibitive as the number of particles increases. So, the vessel dimensions for DEM generated packing (i.e., D and H) are xed out of constraints arising from computational requirements. The diameter D of the vessel for DEM generated packing is taken as 15 times the
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equivalent particle diameter (D = 15dp) for spherical pellets and 10 times the equivalent particle diameter (D = 10dp) for cylindrical and uted ring packing. The vessel height H is taken as 1.52 times the diameter D (or H = 15dp 20dp) for all. Figure 3 shows the packing structure obtained for spherical particle, cylindrical pellets, and uted ring using the DEM. The validation of DEM generated packing is done by measuring porosity and is covered in section 4. (b) Next, a cylindrical cut-section size has to be chosen as the bed-segment for CFD analysis. The cut-segment is cut out from the DEM generated packing. The CFD simulation applies a slip wall boundary condition (zero shear stress boundary condition) to the side cylindrical surfaces of the cylindrical cut-segment, while the top and bottom planar surfaces are the inlet and outlet boundary conditions, respectively. The details of the CFD simulation parameters and meshing details are given in section 4 and Tables 3 and 4. Figures 46 show the cutsegment and wall-segment for the spherical particle packing, the uted ring packing, and the cylindrical pellet packing, respectively. A decision has to be made about the minimum size that can be a good representative. Hence, the diameter (D*) and height (H*) of the concentric-cylindrical cut-segment are varied, and CFD is conducted to analyze the variation in the pressure prole. Initially, the height H* is taken as 8dp, and D*
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Figure 3. DEM generated packing for (A) spherical particle, (B) cylindrical pellets packing, and (C) uted ring packing.

Table 3. Meshing Details for Grid Used in the Study

meshing parameters mesh type mesh size for cut-segment case 1: 2dp diameter vessel case 2: 2.5dp diameter vessel case 3: 3dp diameter vessel mesh size for wall-segment particle treatment for avoiding skewed cells in grid generation uted ring/cylindrical pellet tetrahedral mesh element for uted ring (Figure 5) and Cartesian cut-cell for cylinder (Figure 6) approx. 1 million cells approx. 1.7 million cells approx. 2.2 million cells 0.32 million cells particle is shrunk by 2% spherical pellet tetrahedral mesh element (Figure 4)

approx. 0.3 million cells approx. 1.55 million cells approx. 2.83 million cells 0.33 million cells and 0.39 million cells neighboring spheres are bridged by a cylinder

is taken in increments of half particle diameter (2dp, 2.5dp, and 3dp). The H* value should be such that the bed has a substantial developed ow region devoid of the entrance eects. The height of bed-segment H* is selected on the basis of how many particle diameters are required to overcome the entrance eects of particles. This is determined from the axial prole of the cross-section area averaged pressure. The ow is said to be developed when the pressure drop varies linearly with the axial location. Figure 7 shows the averaged pressure prole for three dierent diameters (2dp, 2.5dp, and 3dp) for cylindrical packing (Figure 7A), for uted ring packing (Figure 7B), and for spherical packing (Figure 7C). The pressure prole is seen to be getting stabilized within one particle diameter. Hence, a minimum bed-segment height (H*) of 4dp will be sucient as it has ow regions free of entrance eect. Next, the diameter of cylindrical bed-segment (D*) is selected. D* is selected so that the pressure drop per unit length (in regions free of entrance eect) is stabilized and stops varying with diameter D*, and also the eect of wall region is avoided. The pressure drop per unit length [(P/L)D*] obtained for each diameter D* is plotted versus the diameter D* to see when it stops varying (or when the prole becomes at). Figure 8AC shows the slope (pressure drop per unit length) in the developed and entrance eect free region for three dierent cut-segment diameters for the uted ring packing (Figure 8A), the cylindrical pellet packing (Figure 8B), and the spherical packing (Figure 8C). The obtained slope (pressure drop per unit length) then is plotted versus the diameter D* as in Figure 9. For all of the packings, it can be seen that pressure drop stabilizes after 2.5dp particle diameters. Also, as per the literature, for spherical pellets, the eect of wall is felt upon the void fraction oscillations up to 35 particle diameters from the wall.21
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However, for cylindrical pellets and nonspherical, the radial void fraction shows less oscillation near wall and gets stabilized by 3 particle diameters from the wall (faster than the spherical pellets) as seen the in results by Giese.33 So, for avoiding the wall region, the maximum cut-segment diameter D* should be 5dp (D (2*5dp) = 15dp 10dp = 5dp) for spherical pellets, and for cylinder and uted ring packing, the maximum D* should be 4dp ((D (2*3dp) = 10dp 6dp = 4dp). Thus, the selected cut-segment diameter is away from the wall-region eect. Also, further checking for larger cut-segment diameter than 3dp is needless as with increasing size the meshing of geometry becomes prohibitive due to excessive use of computer resources. Thus, a cylindrical cut-segment dimension of diameter D* = 3dp and height H* = 4dp can give a good and aordable representation of a large-scale reactor. On the basis of this experience, a wall-segment of 3.5dp width (in radial direction) and 4dp height has been selected for studies pertaining to study of near wall eect. The wall-segment region is expected to capture the near wall physics more accurately. (c) The D* and H* decided on the basis of above calculations are used to obtain pressure drop and heat transfer coecients for the large-scale CLC reactor. Several simulations have been conducted using this cut-segment dimension to obtain the pressure drop and heat transfer correlation for dierent particle Reynolds numbers (varied from Rep = 1.75 to 1540), and correlations have been proposed. These correlations are useful for the prediction and scale-up of the industrial scale packed bed reactors. The correlations obtained are discussed later in this Article. The next section describes the CFD-DEM tools and the simulation parameters used to implement this methodology.
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Repf is varied from turbulent regime (Repf = 1520) to laminar region (Repf = 7) for developing pressure drop correlations for uted ring and cylindrical pellets and spherical pellets air and its properties are computed at 20 bar, 1000 K for all cut-segments, except for wall-segment study (where thermal conductivity of air is taken as 0.0242 W/m2K) mass ow rate per unit area is varied to achieve desired Reynolds number; hence, for each case (2dp, 3dp, 3.5dp having dierent cut-segment diameters), the mass ow rate changes as the cross-sectional area available for ow changes with the cut-section size; inlet temperature of air is 300 K one atmosphere (absolute) static pressure for cut-segment, the only side wall is specied as having slip wall (zero shear stress) and a constant temperature of 1000 K for wall-segment, the outer wall is no-slip boundary and the rest of the side-walls are slip wall boundary; two cases have been studied, one with constant temperature of 1000 K at side walls and second with a zero heat ux boundary condition at side wall no-slip momentum and a constant temperature of 1000 K

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4. VALIDATION AND IMPLEMENTATION DETAILS OF METHODOLOGY 4.1. DEM Simulation. a. Implementation. A Packed bed is generated by simulating the lling process of particles in the vessel. This can be enabled by using the DEM numerical method, which tracks the motion of each particle in free fall under gravity and its dynamic interactions/collisions with other particles and boundaries. The force arising during the interactions/collisions leads to newer particle positions and newer particle velocities, and is computed using the force displacement law. This particle contact behavior is simulated using a soft particle model involving springs, dashpots, and frictional sliders. In the soft particle model, the rigid particles are allowed to overlap at contact points. The magnitude of the overlap is related to the contact force via the force displacement law. All overlaps are small in relation to particle sizes. The spring expresses the hardness of particles through Youngs modulus parameter, while the dampener or dashpot expresses the particle energy dissipation through the coecient of restitution parameter. The friction sliders expressing the friction between contact points are dened with a Columbic type of friction and implemented with a friction factor. These parameters are based on physical properties of the material constituting the particle and the wall boundary. Tables 1 and 2 outline the parameter used in DEM simulation of cylindrical and uted ring packed bed. The commercial DEM software package PFC3D by ITASCA25 has been used in this work. PFC3D allows for implementation of arbitrary shape of particles using the clump logic feature. The arbitrary shape particle is formed from multiple spheres, which are clubbed to form a clump (Figure 2). A user-dened script is written for creating the particle shape. The script computes the location and number of spheres when the user inputs the dimensions of the particle and the size of a sphere. The higher number of sphere would lead to more accurate particle shape, but it will also lead to computational costs while running DEM. The multisphere particle (or clump) behaves as a rigid body (i.e., the particles comprising the clump remain at a xed distance from each other), although they can have a deformable boundary. Thus, they will not break apart, irrespective of the forces acting upon it. Particles within a clump may overlap to any extent, and the contact forces are not generated between these particles. During the calculation cycle, the contacts internal to the clump are ignored, resulting in a savings of computer time. However, contacts with particles external to the clump are considered. Such contacts develop when the particles comprising the boundary of a clump come into contact with other particles. At each cycle, a multisphere particle position is generated randomly within the vessel. To save computational time for the lling process, the particles are not generated at top of vessel but at random locations within vessel. The initial velocity of the multisphere particle (clump) is assigned on the basis of its axial location and its potential and kinetic energy. The calculation cycle in PFC3D is a time stepping algorithm that requires the repeated application of the law of motion to each particle, a forcedisplacement law to each contact, and a constant updating of the wall positions. The time-step is chosen so small that, during a single time-step, disturbances cannot propagate further from any particle than its immediate neighbors. At all times, the forces acting on any particle then are determined exclusively by its interaction with the particles with which it is in contact. Because the speed at which a
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Table 4. CFD Parameters Used in the Study

particle Reynolds number uid and properties inlet boundary condition for wall-segment and cut-segment outlet boundary condition for wallsegment and cut-segment outer wall/side wall boundary conditions

particle wall boundary conditions for wallsegment and cut-segment turbulence model time step

CFD parameters

realizable k- model with standard wall function 5 105 s

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Figure 4. (A,B) Two cut-segments of spherical particle packed bed: (A) 2dp diameter and 10dp height segment, (B) 3dp diameter and 4dp height. (C) The wall-segment used for obtaining the wall heat transfer coecient. The three gures in (B) and (C) show the outer surface of cut-section, the particles inside the cut-section, and the mesh used for CFD.

Figure 5. Fluted ring packing bed-segment cut-sections (2dp diameter and 8dp height). The diameter and height of this cut-section are varied as per methodology. The outer surface of cut-section and the particles inside the cut-section are shown on the left. The mesh used is shown on the right side.

disturbance can propagate is a function of the physical properties of the discrete system, so the time-step can be chosen based on the system. PFC3D uses a simplied way of
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computing the time-step by viewing the system as comprised of multiple bodies (masses) and springs (stiness). It computes the critical time step for each body in the system. The critical
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Figure 6. Cylindrical packing bed-segment cut-sections (2dp diameter and 8dp height) for pressure drop computation in (A) and the wall-segment for wall heat transfer coecient in (B). The diameter and height of this cut-segment are varied as per methodology. The outer surface of sections, the particles inside the sections, and the mesh used are shown.

time-step is a function of mass of the body and spring (stiness) associated with the contacts of the body. The stinesses are estimated by summing the contribution from all contacts, using only the diagonal terms of the contact stiness matrix. The nal critical time step is taken to be the minimum of all critical timesteps computed for all degrees of freedom of all bodies. The readers can refer to the PFC3D manual25 for the mathematical implementation of this scheme, as well as work by Cundall.26 Once the packing structure of the packed bed is predicted with DEM, the locations of particles in packing structure are transferred into the GAMBIT meshing software using script. b. Validation of DEM Simulation Results. Figure 3A shows the DEM obtained spherical packed bed for a vessel with a diameter around 15 times the particle diameter (D/dp = 15). The global porosity of this DEM generated spherical bed packing has been measured to be around 0.404, which is similar to the value obtained using Dixons correlation32 for bulk voidage for spherical bed packing. The porosity has been obtained at the center of the DEM generated bed using the measured sphere tool in PFC3D software. The cut-segment representing the core central region of the bed has this porosity (0.404). The porosity in the whole wall-segment is around 0.44, which is higher than the 0.405 porosity in the core region. This is in line with the near wall porosity reported by Zhang,34 who suggested that the porosity value is about 5% higher than bulk porosity at near wall region (of up to 2 particle diameters from the wall). This suggests that the setting of DEM parameter for particleparticle friction coecient and particlewall friction coecient (both around 0.4, see Table 2) is appropriate for the
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present case. The friction coecient can have an impact on porosity and bed structure; for example, when the friction coecient is high, then the particle will get balanced on each other and counteract the gravity. So, a higher friction coecient would cause a loose packing (leading to higher porosity). The bulk porosity is accurate in this case, and DEM generated bed can be considered for further studies. For uted ring and cylindrical pellets, the particle and ball friction of 0.3 is used. Generally, a value higher than spherical particles can be expected as nonspherical particles are expected to have a higher rolling friction at walls. However, one can expect some masking of the friction eects in these nonspherical cases because of the interlocking due to surface resolution. With the current friction coecient, the DEM generated packing was generated for cylindrical pellets at dierent aspect ratios (not shown here). The DEM was able to capture the trend that with increasing aspect ratio, the porosity was seen to be increasing (as reported by Nemec1). The resultant porosity for the cylindrical pellet of aspect ratio (AR = 2) is around 0.42, and for a higher aspect ratio of 7, this is around 0.55. The result is similar to that cited by Nemec1 in his work for an aspect ratio of 2. 4.2. CFD Simulation. 4.2.1. Implementation. Computational uid dynamics solves the conservation equations for momentum, mass, and energy using a nite volume method. Ansys Fluent 13 has been used for this CFD simulation. To enable CFD simulation for the complex packing geometry, the mesh has to be created on the complex packing structure. The regions of particle contact points and sharp angles at cutsection may often cause some skewed cells to appear. The occurrence of skewed cells leads to divergence of the solver. To
dx.doi.org/10.1021/ie302028s | Ind. Eng. Chem. Res. 2013, 52, 1204112058

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Figure 7. Axial prole of cross-section area averaged pressure for dierent cut-segment diameters for uted ring, cylindrical pellets, and spherical particle packing.

Figure 8. Slope (pressure drop per unit length) computed in the developed region for the three dierent diameters for uted ring, cylindrical pellets, and spherical particle.

overcome this, there are four methods suggested in the literature. Bai22 and Atmakidis and Kenig30 suggested shrinking the particles by a certain amount to remove the contact points. The shrinking of the particles increases the porosity, for which a correction factor has to be taken into account while computing pressure drop. Guardo24 suggested increasing the size of the particles by a certain value. The contact points then become contact areas, and the skewness of the cells is reduced. This method needs also a correction factor for pressure drop. Eppinger23 suggested attening of the particles locally in the proximity of the contact points if the distance between two particle surfaces falls below a predened value. This leads to a small gap between the particles, which can be lled with cells of good quality. Ookawara28 suggested bridging the spherical particles with small cylinders if the distance between the particles falls below a predened value, and the macroscopic ow properties such as the pressure drop are not inuenced by this. This bridged cylinder method has been adopted in this work for spherical particles, while for nonspherical particles, we shrink the particle size to enable meshing. However, because the geometry is so complex, we had to shrink the particle by about 2% to enable good quality mesh generation. A tetrahedral grid was used for the uted ring packing, and a Cartesian cutcell grid was used for the cylindrical and spherical particle packing (as seen in Figures 5 and 6). In both the cases, a Y+ of around 3 is obtained near the particle surface. The mesh size, boundary conditions, and simulation parameters for CFD simulations at three dierent diameters (2dp, 2.5dp, and 3dp) for dierent particle shapes are given in Tables 3 and 4. The
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particle shrinkage aects the voidage, which can aect the pressure drop results. To account for this eect, the pressure drop results are rescaled with void-fraction (using term 3/1 ) in accordance with Erguns5 nding. From the CFD results, the pressure drop correlation and heat transfer coecient correlation have been obtained in the equation form as shown below. 4.2.1.1. Equation for Pressure Drop (Friction Factor) Correlation. The dimensionless pressure drop (friction factor) correlation has been proposed in two forms: a linear Ergun equation form (eq 1) and in the form of equation proposed by Dalla Valle31 (eq 2).
fp = PDp 3 1 A = +B L 1 Vs 2 Repm

(1)

where A is known as the BlakeKozenyCarman constant and B is known as the BurkePlummer constant. The Ergun equation above is used in validation of the proposed methodology for pressure drops in spherical particles packing in regions away from the wall using A = 150 and B = 1.75. For uted ring and cylindrical pellet shapes, the Ergun equation is modied by changing values of A and B parameters. These parameters are determined by tting eq 1 to the results from the CFD-DEM methodology for these particle shapes. For the equation proposed by Dalla Valle31 (eq 2):
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Repm = VsDp (1 )

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(3)

4.2.1.2. Equation for Heat Transfer Correlation. The particle heat transfer coecient has been used in the form given by RanzMarshal and Wakao37 (eq 4):
Nu p = hpd p k = 2.0 + ARep xPr y
(4)

where Rep is the particle Reynolds number based on relative velocity. RanzMarshal proposed the parameters for a single sphere to be A = 0.6, x = 0.5, and y = 0.33. They later studied a multiparticle spherical packing and determined A to be 1.8 for packed bed. Wakao accounted for the eect of axial thermal and modied the RanzMarshal correlation by suggesting A to be 1.1 and x to be 0.6. Both Wakao and RanzMarshal correlations have been used in validation of the proposed methodology for obtaining particle heat transfer coecient in spherical particle packing. For uted ring and cylindrical pellet shapes, eq 4 is modied by changing values of A. These parameters are determined by tting eq 4 to the results from the CFD-DEM methodology for these particle shapes. The wall heat transfer coecient has been proposed in the form of eq 5 (originally given by Li and Finlayson).
Nu w = hw d p k = ARepf x
(5)

Figure 9. Slope (pressure drop per unit length) from Figure 7 versus the diameter of bed-segment for (A) uted ring, (B) cylindrical pellet, and (C) spherical particle.

fp =

PDp 3 1 A + 2 = L 1 Vs Repm

B +C Repm

(2)

where A, x, and y are the parameters that are determined by tting the equation to results of CFD CFD-DEM methodology in cylindrical pellets; Pr is the Prandtl number (Pr = Cp/k), and Repf is particle Reynolds number based on the supercial velocity. For validation of wall heat transfer coecient using the CFD-DEM methodology, the correlations proposed by Dixon Lubua and ColledgePaterson have been used. The particle heat transfer coecient (hp) and wall heat transfer coecient (hw) needed to develop the above correlations are computed from the CFD results using heat ux at particle surfaces and at wall and the average bulk temperature. a. Average Particle Heat Transfer Coecient.
hp,average =

where A, B, and C are the parameters that are determined by tting the equation to CFD-DEM methodology results. Vs is supercial velocity, and Repm is modied particle Reynolds number (varied from 3800 to 1.75 for establishing the correlation). In both equations, the modied particle Reynolds number is computed as:

qdSp T dV 1 , where Tbulk = dSp (Tp Tbulk) dV

(6)

q is the heat ow rate per unit particle surface area (W/m2) obtained from CFD results, Sp represents all particle surface elements (faces), and V represents all uid volume cells.

Figure 10. Mesh and geometry used for validation of uent for computing drag coecient over a single spherical particle.
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Industrial & Engineering Chemistry Research b. Wall Heat Transfer Coecient.

hw,average =

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qdSw T dV 1 , where Tbulk = dSw (Tp Tbulk) dV

(7)

q is the heat ow rate per unit area (W/m2) obtained from CFD results, Sw represents all wall surface elements, and V is for all uid volume cells. c. Validation. The CFD method is rst validated on the single sphere particle and then on the spherical particle packed bed at low tube-to-particle diameter. The CFD-DEM cutsegment methodology is validated on the spherical particle packing (where established correlations are available for comparison), and then the methodology is applied for developing correlations for unique particle shapes. 4.2.1.3. Validation of Drag Coecient for Single Spherical Particle. The drag coecients predicted by the 3D CFD for single sphere particle provide a fair agreement with those obtained by MorsiAlexander correlation.27 Figure 10 shows the geometry and planar cut-section of the spherical particle (of diameter dp = 6 mm) inside a box (wind-tunnel of dimension: 10dp 10dp 10dp) meshed with the Cartesian cut-cell approach. The CFD simulates the air ow over the stationary spherical particle (as in a wind-tunnel), and the drag experienced by the particle is obtained. The inlet air ow rate corresponds to the particle Reynolds number to be studied. The boundary condition at outlet is specied to be at one atmosphere (absolute) static pressure. The side walls of the box have zero shear stress (slip wall) boundary condition to generate the eect of far-away region, and the spherical particle inside the box (wind-tunnel) is a no-slip wall. In Figure 10A, the spherical particle diameter to grid size ratio (dp/X) is 5, and in Figure 10B, this ratio is 10 (ner grid, Y+ of around 0.5 1 at high Reynolds number of 6000). Table 4 and Figure 11

Figure 11. Comparison of the drag coecient as predicted by CFD and obtained by MorsiAlexander at dierent Reynolds number.

show the drag coecient obtained at dierent Reynolds number. The coarser grid (dp/X = 5) has given less than 3% deviation in drag prediction for Reynolds number up to 600, but at Re = 6000, the deviation is 16.7% (shown in parentheses in Table 4) as compared to that predicted by MorsiAlexander correlation.27 The ner grid (dp/X = 10) has been used at higher Reynolds number of 6000 and results in lower deviation of 5.89%. This could be because at higher Reynolds number, the boundary layer thickness reduces and ow undergoes separation. Hence, a ner grid is used to resolve
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the boundary layer and to capture the boundary layer physics and the resulting form and skin drag more accurately. 4.2.1.4. Validation of Pressure Drop in Spherical Particle Packed Bed. The pressure drop computed for spherical particle packed bed is validated with the Eisfeld equation6 for pressure drop. DEM has been used to generate the packing structure (Figure 12) and to enable good mesh at contact points; a bridged cylinder approach28,29 is used to treat the contact points as seen in Figure 12. A Cartesian-cut-cell mesh has been used. The Eisfeld correlation6 has been chosen for comparison as it considers the inuence of the tube-to-particle diameter ratio and therefore the inuence of the conning walls on the pressure drop. Table 5, Figure 12, and Figure 13 show that the deviation between CFD and Eisfeld predicted pressure drop is between 7% and 10% for the three Reynolds numbers (Re = 2532, 4302, and 5061). The Reynolds has been chosen such that the turbulence regime is encountered. The CFD uses the k- turbulence model based on results in the literature.22,23 The agreement between CFD and Eisfeld correlation has been quite good. The results do not change much with use of a ner grid, thus ensuring grid independence of results. The good agreements obtained with CFD for drag computation of single spherical particle and for pressure drop in spherical packed bed give us the condence to go ahead for applying it with dierent particle shapes. 4.2.1.5. Validation of Cut-Segment Methodology for Spherical Packing. The spherical packing packed bed has been chosen for validation of methodology as established correlations are available for comparison. The pressure drop results obtained using the cut-segment are validated by comparing it with the Ergun correlation for pressure drop. Further, a separate wall-segment approach has been used for obtaining the wall heat transfer coecient in the near wall region. The results of wall heat transfer coecient have been validated with the Dixon and Labua35 correlation and the ColledgePaterson correlation.36 The results on the particle heat transfer coecient have been validated with the established multiparticle RanzMarshal correlation and Wakao correlation for packed bed. The pressure drop has been computed at dierent Reynolds numbers varying from laminar regime to turbulent regime (Table 6). Figure 14 shows the pressure and the velocity prole at two particle Reynolds numbers (Rep 760 and Rep 380). Figure 15 compares the prediction of pressure drop obtained by CFD on a cut-segment (with mesh size of 0.39 million nodes) and Ergun correlation. The simulations were also conducted at slightly coarser mesh of 0.33 million nodes to check for grid independence at a particle Reynolds number of 350. The pressure drop results did not vary much. The deviation from Ergun is within 5% for Reynolds number lower than 350. However, at the higher Reynolds number of 750, the CFD underpredicts the pressure drop by around 13% as compared to Ergun correlation. The current results can be considered reasonably accurate to validate the use of cut-segment methodology for pressure drop studies. The cut-segment methodology is used to conduct thermal studies as well. The idea is to check whether it can be used to predict the particle and wall heat transfer coecient. The thermal boundary condition of constant specied temperature on the segment slip wall (zero shear stress wall) is not consistent as it suggests that the heat transfer is allowed on this boundary while the momentum ux is zero. Hence, a proper validation is required to check whether this thermal boundary condition will aect
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Figure 12. Pressure drop obtained by applying CFD over the DEM generated spherical particle packing (extreme left) at three dierent Reynolds numbers (Re of 2532, 4302, and 5061). The Cartesian mesh and bridged cylinder approach used can be seen at second from left.

Table 5. Comparison of Drag Coecient Predicted by CFD and MorsiAlexander for a Flow over Spherical Particle
Reynolds number 0.006 60 600 6000 drag coecient predicted by MorsiAlexander 4000 1.36 0.52 0.39 CFD predicted drag coecient 4103 1.33 0.51 0.36 (0.46) % deviation 2.5% 2.2% 2.73% 5.89% (16.7%)

Figure 13. Comparisons of pressure drop as predicted by CFD and as obtained by Eisfeld at three dierent Reynolds numbers (Re of 2532, 4302, and 5061).

Table 6. Pressure Drop Deviation from Flow over Spherical Particle Packed Bed
Reynolds number 2532 4302 5062 Eisfeld (2001) predicted pressure drop (Pa) 2194 6106 8415 CFD predicted pressure drop (Pa) 2383 6780 9353 % deviation 7.9 9.9 10

the region of interest and physics adversely. The cut-segment of spherical packed bed is validated for predicting the wall and particle heat transfer coecient using the DixonLabua35
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correlation and the ColledgePaterson36 correlation. The validation results pertaining to pressure drop correlations (hydrodynamics) do not change by simulating the cut-segment both with and without thermal calculations. This is mostly because the ow properties are not changed due to thermal calculations; hence, the pressure drop results are not aected by the thermal boundary condition. However, the wall heat transfer coecient value obtained from the cut-segment shows an overprediction of around 60% as compared to the ColledgePaterson36 correlation at a particle Reynolds number of 750. This could be because the cut-segment has slip wall boundary condition (where the wall heat transfer coecient is measured). As a result of this slip wall boundary condition, the hydrodynamic boundary layer does not exist, and there is a higher convection. This higher convection results in overprediction of wall heat transfer coecient. Thus, the cutsegment with slip wall boundary leads to inaccurate near wall physics. Also, the region near the slip wall does not have as high porosity as the regions near the actual wall, because this slip wall is actually a part of the cut-segment of the central region of the packed vessel. Hence, to obtain an accurate wall heat transfer coecient, a wall-segment approach has been tested (see Figure 4C). More importantly, the outer wall of this wallsegment, where the wall heat transfer is to be computed, has a no-slip wall with a specied constant temperature boundary condition. The inlet boundary condition for the wall-segment is specied by a mass-ow rate. The boundary condition at outlet is specied to be at one atmospheric (absolute) static pressure. We limit the wall-segment up to 3.5 particle diameter from the wall resulting in a inner wall surface. The boundary at this inner wall-surface and two other side-wall surfaces is specied to be a slip wall boundary with a zero heat ux boundary condition. Another wall-segment simulation case has been set up to test the eect of thermal boundary condition. Here, the boundary condition at inner wall and the two side surface has been changed to constant temperature boundary condition, while the rest is kept the same. The wall-segment region has 4% more porosity than the cut-segment zone (which is as observed by Zhang34). The mesh size for the wall-segment is around 1.07
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Figure 14. (A,B) Pressure and velocity proles at Reynolds number 760 and 380 for the cut-segment of spherical packing, and (C,D) show the temperature and velocity prole for heat transfer studies at Re 760 and 570.

Figure 15. Validation of methodology: Comparison of CFD predicted pressure drop for cut-segment of spherical particle packing with the pressure drop predicted by the Ergun correlation.

million nodes with the average Y+ at outer wall around 3 at a particle Reynolds number of 760. Figure 16 shows the wallsegment heat transfer coecient obtained from the CFD study. CFD results have been compared to that predicted by Dixon Labua35 correlation and ColledgePaterson36 correlation at two particles Reynolds numbers (Rep 760 and Rep 580). Figure 14C,D shows the temperature and velocity prole obtained at these two Reynolds numbers. Figures 16 and 17 compare the CFD prediction of the wall heat transfer coecient and the particle heat transfer coecient with established correlations. It was seen that by varying the boundary condition from constant temperature to zero heat ux at Rep of 750, the wall heat transfer coecient result did not change appreciably (only by 35%). The CFD predicted results underpredicts by 6% as compared to predictions by ColledgePaterson36 correlation, and it overpredicts by around 15% as compared to the Dixon Labua35 correlation. This wall heat transfer coecient result for the wall-segment is better than that predicted by the cut12052

Figure 16. Validation of methodology: Comparison of CFD predicted wall-heat transfer coecient for wall-segment of spherical particle packing with the wall-heat-transfer-coecient predicted by the Colledge and Paterson correlation36 and DixonLabua.35

segment with slip outer wall (where 60% overprediction is observed). This could be because the physics of heat transfer near the outer wall is accurately captured in the wall-segment simulation. It can be said that the boundary condition at outerwall (where wall heat transfer coecient is measured) will have a signicant eect on the wall heat transfer coecient. While the inner wall and side walls boundary condition inuences the bulk uid temperature, it does not have much inuence on the heat transfer mechanism near the outer wall. Thus, the wallsegment approach is a suitable approach for obtaining the wall heat transfer coecient. For obtaining particle heat transfer coecient, both of the segments (wall-segment and cut-segment) have been used. The particle heat transfer coecient obtained from CFD over cutsegment (see Figure 17A) overpredicts by around 515% ((hCFD hcorrelation)/hCFD) as compared to the Wakao and
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Figure 17. Comparison of CFD predicted particle-heat transfer coecient obtained from cut-segment and the wall-segment of spherical particle packing with that predicted by the Wakao and Ranz and Marshal correlations.7 The wall-segment cases have higher void fraction due to near wall-eect and have been simulated for uid with dierent thermal conductivity than the cut-segment.

multiparticle RanzMarshal correlation at low Reynolds number (Re 200). However, as the Reynolds number increases, the CFD begins to underpredict as compared to

Wakao correlation (by 1530%), and CFD overpredicts by 16% as compared to multiparticle RanzMarshal (see Figure 17A). When compared to prediction by single particle Ranz Marshal correlation, the CFD overpredicts by 6070%, which is along the expected lines. The single particle correlation gives much lower heat transfer coecient than the multiparticle systems. Thus, the CFD predicted particle heat transfer coecients results are reasonable. This could be because the heat transfer mechanism near the particle wall is not aected by the inconsistent boundary condition at the outer slip wall. This outer slip walls thermal boundary condition might only be aecting the bulk temperature of the uid but not the mechanism of heat transfer near the particle wall. For the wall-segment, the CFD predictions of particle heat transfer coecient at higher Reynolds number (Figure 17B) are overpredicted by around 1520% as compared to multiparticle RanzMarshal and underpredicted by around 4050% as compared to the Wakao correlation. The simulations at wallsegment are carried out for a uid having dierent thermal conductivity (see Table 4) than for the uid used in the cutsegment simulation; hence, the particle heat transfer coecient predicted from wall-segment is dierent from that of the cutsegment for the same supercial Reynolds number. Also, there is more voidage in the wall-segment region than in the cutsegment region due to the near wall eect, which aects the true velocity experienced by the particles in these segments (for the same supercial velocity). The CFD predictions are closer to the Wakao and multiparticle RanzMarshal correlations for the cut-segment than for the wall-segment region. This is expected as these particle heat transfer correlations do not specically consider the ow in near wall region (wallsegment). At higher Reynolds, the results can be improved by using a ner mesh near the particle wall. Thus, the results show that the cut-segment and wallsegment approach can be used for prediction of pressure drop

Figure 18. Contours in vertical cross-sectional plane for (A) velocity, m/s, (B) pressure, Pa, and contours in horizontal cross-sectional plane for (C) velocity, m/s, and (D) temperature, K, in cylindrical pellet packing of 3dp diameter cut-segment.
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Figure 19. Contours in vertical cross-sectional plane for (A) velocity, m/s, (B) pressure, Pa, and contours in horizontal cross-sectional plane for (C) velocity, m/s, and (D) temperature, K, in uted ring pellet packing of 3dp diameter cut-segment.

and heat transfer coecient as long as the physics is getting captured accurately. These approaches can be applied to obtain such information for unique particle shapes. The next section shows the application of this methodology to obtain information on long aspect ratio cylindrical pellet and uted ring, which are being tested for use in packed bed chemical looping combustion unit as oxygen carriers. The information for these unique shaped oxygen carriers is not available in the literature.

5. APPLICATION OF VALIDATED METHODOLOGY: TRANSPORT PHENOMENA IN LONG CYLINDRICAL PELLET AND FLUTED RING PACKING The pressure drop, the heat transfer/mass transfer coecient, and the ow features have been studied for both the uted ring particles and the cylindrical pellets. To develop the correlations for the heat transfer coecient and for the friction factor (pressure drop), many CFD simulations have been oated with the modied particle Reynolds number varying from 1.75 (laminar regime) to 3800 (turbulent regime). Figures 18 and 19 show the CFD simulation for the cylindrical pellets and for the uted ring at reactor conditions, respectively. As can be seen, the inclusion of actual packing structure makes the uid ow along a tortuous path. The uid prefers owing through channels that oer least ow resistance, and these are the regions of higher velocity in the contour plots. The corresponding uid temperatures in the regions of higher velocity are lower (Figures 18D and 19D), while higher temperatures are seen in the regions of low void fraction region (where ow is not high enough to induce high heat transfer coecient). These low velocity zones could be the region of potential hot-spots in the bed. Figures 18D and 19D show that after about 6dp from inlet, most of the inlet air has become hot enough to approach the wall temperature, and temperature contours in the cross-sectional area seem to be quite uniform.
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The CFD-DEM generated ow eld provides a good idea about the conditions in the packing. The results obtained here for a wide range of Reynolds number have been used to develop the correlations (described below). These correlations can be used in the 1D model to simulate the whole large-scale reactor. 5.1. Pressure Drop Correlations for Cylindrical Pellet Packed Bed and Fluted Ring. The pressure drop obtained for dierent Reynolds numbers has been plotted in Figure 20 for both the cylindrical pellet packing and the uted ring packing. The decrease in dimensionless pressure drop with

Figure 20. Comparison of friction factor (dimensionless pressure drop, f p) for uted ring and the cylindrical pellet packing for Rep from 1.75 to 3800. The black line (solid and dotted) represents the t from Linear equation (Ergun form) for pellet and uted ring respectively, and the red line (solid and dotted) in graph represents the t from Dalle Valle equation for pellet and uted ring respectively.
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Industrial & Engineering Chemistry Research increase in Reynolds number is along the expected lines. This trend is captured by means of correlations. Figure 20 shows the tting of two correlations (the Ergun linear form and the Dalla Valle31 form) for the CFD results. Equations 8 and 9 are the correlations obtained for cylindrical pellet. Equation 8 is a Ergun equation, with modied Blake Kozeny Carman constant value (A = 310) and the BurkePlummer constant (B = 4.56) providing the t for our high aspect ratio cylindrical pellets. Ergun had determined the constants for the spherical particle packing: 150 for the viscous term (often referred to as BlakeKozenyCarman constant) and 1.75 for the inertial term (BurkePlummer constant). The value obtained in our work varies substantially from the original Ergun parameters. This variation is expected. Nemec1 has shown that the higher is the aspect ratio of a cylindrical particle (in other words, a particle is nonspherical in shape), the higher are the Blake KozenyCarman and the BurkePlummer constants. However, Nemec1 has reported the values of A and B for cylindrical pellet to an aspect ratio of 5.77. In the current work, the cylindrical pellet aspect ratio to be used initially is 7, and the results of modied Ergun parameters obtained here will be useful for the 1-D model. However, the linear form is not giving a good t. Hence, a form proposed by Dalla Valle (eq 9) has been tested. The eq 9 form is shown to be giving a better t than the linear form (see Figure 20). The pressure drops obtained by these correlations are compared to the Nemec correlation (A and B parameters suggested by Nemec for pellet with an aspect ratio of 5.77) (see Figure 21). The slightly

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Hence, eq 9 is better suited for use for the 1-D model. This trend toward obtaining higher constant values (A,B) for nonspherical particles could be because in case of nonspherical particles, the eect of bed structure on heat transfer and pressure drop needs additional parameters (such as tortuosity, wetted surface) to represent the bed-structure. However, all of these additional bed-structure parameters are vague physical concepts, and they are hard to measure experimentally. So, for the time being, the only way around is to use constants for the nonspherical particles. For uted rings, eq 10 is a modied Ergun equation, with the BlakeKozenyCarman constant value (A = 253) and the BurkePlummer constant (B = 2.21) providing the t for the uted ring with an aspect ratio of 1.4. The values of constants (A and B) obtained for uted ring packing in our work are expectantly higher than the original Euler equations for spherical particle (A = 150, B = 1.75). These uted ring constant values are also higher than that of a corresponding cylindrical pellet with a similar aspect ratio of 1.4 (A = 210 and B = 1.9, as reported by Nemec1). However, these uted ring constant values are lower than the values obtained in this work for the long aspect ratio cylindrical pellet (AR = 7). These results are along the expected line as the higher is the nonsphericity of a particle (in other words, the more a particle has higher aspect ratio), the higher are the BlakeKozeny Carman and the BurkePlummer constants. For designing a reactor using uted rings as packing, the results of modied Ergun parameters obtained for uted ring will be useful for the 1-D model. However, the linear form is not giving a good t, as was the case with cylindrical pellet. Hence, the Dalla Valle form31 (eq 11) can be used.
PDp 3 1 310 = + 4.56 L 1 Vs 2 Repm

(8)

PDp 3 1 229.6 49.38 + + 1.78 2 = L 1 Vs Repm Repm

PDp 3 1 253 = + 2.21 L 1 Vs 2 Repm PDp 3 1 240 + 2 = L 1 Vs Repm
Figure 21. Comparison of pressure drop predicted by the correlation proposed for cylindrical pellet with aspect ratio 7 with the available Nemec correlation for cylindrical pellet with aspect ratio 5.77.

(9)

(10)

10.8 + 1.55 Repm

(11)

higher pressure drop obtained by our correlations as compared to Nemec (Figure 21) is along the expected lines as our correlations are for higher aspect ratio cylindrical pellets (aspect ratio 7) than the one by Nemec (aspect ratio 5.7). The deviation of the Dalla Valle31 form (eq 9) from the Nemec correlation is 15% at high supercial velocity (Vs > 1.5 m/s), which is due to the aspect ratio dierence of pellets. Further, the Dalla Valle equation form (eq 9) has been able to capture the linear variation of the pressure drop with Reynolds number at low Re, and the independence of pressure drop from Reynolds number at higher Re. This form is also asymptotically correct at both ends of Reynolds number (as Rep tends to zero and Rep tends to innity), and this asymptotic behavior is as expected and obtained with Nemec and Ergun correlations.
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As seen from Figure 20, the dimensionless pressure drop is lower for the uted ring than for the cylindrical pellet. For the same bed porosity, the same particle Reynolds number, and the same eective diameter, the long cylindrical pellets would result in a friction factor that is 2090% higher than the uted ring. One of the reasons for this could be the eect of the shape of catalyst on the orientation: the DEM generated packing of the high aspect ratio (7:1) cylindrical pellet (Figure 3A) shows that the majority of pellet orientations are either with cylindrical surface being horizontal or being inclined with respect to base, which oers more curvature for the owing uid to turn and twist and results in more pressure drop. In case of uted ring, if the grooves are oriented parallel or in an inclined way to the ow, then there will not be high resistance. The uid will ow across the grooves in such case. Yet, if the grooves are oriented perpendicular to the ow, then very high resistance would be oered to the ow. The DEM generated packing for this particular shape of uted ring particle with aspect ratio 1.4 is
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Industrial & Engineering Chemistry Research seen in Figure 3C. There is no particular bias for an arrangement that would cause higher resistance. There are many uted ring particles with grooves parallel or inclined to ow, and also there are grooves with perpendicular alignment to ow. The overall eect is a pressure drop that is lower than that obtained from the high aspect ratio pellets biased orientation. 5.2. Heat Transfer Correlations for Cylindrical Pellet and Fluted Ring Packed Bed. For cylindrical pellets, Figures 22 and 23 show the variation of particle Nusselt number and

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For uted ring, Figure 24 shows the variation of particle Nusselt number (dimensionless heat transfer coecient) with

Figure 24. Correlation obtained for particle Nusselt number as a function of particle Reynolds number (Rep) for uted ring packed bed for Rep from 17.5 to 3800.

Figure 22. Correlation obtained for particle Nusselt number as a function of particle Reynolds number (Rep) for cylindrical pellet packed bed for Rep from 17.5 to 3800.

particle Reynolds number for uted ring packing. Equation 14 is the correlation obtained for uted ring heat transfer coecient. Comparing eq 14 of uted ring to the equation obtained for cylindrical pellet (eq 12), it is seen that the uted ring particle packing arrangement gives higher heat transfer. The parameter A for uted ring (around 1.68 in eq 14) is slightly higher than cylindrical pellet but lower than that of spherical particle. The reason for this lies in the higher velocity within the packing structure of the uted ring, due to lower voidage inside the uted ring packing than the cylindrical pellets packing.
Nu p =
Nu w = Nu p =

hpd p k
hw d p k hpd p k

= 2.0 + 1.65Rep0.5Pr 0.33

= 7.37Repf 0.26 = 2.0 + 1.68Rep0.50Pr 0.33

(12)

(13)

(14)

Figure 23. Correlation obtained for wall Nusselt number as a function of particle Reynolds number (Repf) for cylindrical pellet packed bed for Repf from 7.5 to 760.

wall Nusselt number with the particle Reynolds number for cylindrical pellets. Equations 12 and 13 have been proposed as correlation for obtaining particle heat transfer coecient and wall heat transfer coecient, respectively. Comparing eq 12 for cylindrical pellet to the equation proposed by mulit-particle Ranz and Marshall7 for spherical particle packing, it is seen that a lower value of constant (A = 1.65) is required to t the heat transfer correlation for pellets as compared to the A = 1.8 for the multiparticle RanzMarshall7 correlation. Similarly, for wall heat transfer coecient, eq 13 is obtained for our pellet, and this is compared to the equation proposed by Li and Finlayson8 for cylindrical pellet. Li and Finlaysons correlation is valid up to a particle Reynolds number of 800. As compared to their correlation, the present correlation has a higher value of constant (A = 7.37), as compared to A = 0.16 by Li and Finlayson8) and lower dependence on particle Reynolds number (to the power of 0.26 in eq 11 as compared to 0.93 in Li and Finlayson8). This variation could be because of the lower range of applicability of the Li and Finlayson8 correlation.
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The next section uses the pressure drop and heat transfer information to enable an oxygen carrier comparison for the proposed reactor operating conditions of the packed bed chemical looping combustion system. 5.3. Comparison of Pressure Drop and Heat Transfer Coecient for the Two Packings at a Given CLC Operating Condition. The operating inlet ow rate of fuel gas (syn gas) in the reduction cycle of pilot scale packed bed chemical looping combustion is equivalent to 500 kW of caloric value, and air ow rate in the oxidation cycle is expected to be 10 times the syn-gas ow rate. At the same inlet ow rate, the particle Reynolds number for uted ring packing is higher than the particle Reynolds number of cylindrical pellet (due to the dierence in pellet eective diameter and bed porosities). At the operating condition for air ow rate, the friction factor for the cylindrical pellet packing is 120% higher than the uted ring packing. Hence, uted ring packing would provide less resistance to uid ow and will oer lower pressure drop. Also, the volume average of ow velocity in the uted ring packing structure (obtained from CFD) is 2% higher than that in the cylindrical pellet, and the volume average turbulent kinetic energy is 5% higher than that in cylindrical pellet packing (obtained from CFD). This is due to lower porosity in uted ring (AR 1.4) packing than cylindrical pellet (AR 7)
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Industrial & Engineering Chemistry Research packing, which results in higher velocity and slightly high heat transfer/mass transfer coecient for uted ring pellet arrangement. Hence, uted ring packing looks promising as it can provide lower pressure drop and higher external heat/mass transfer. However, the uted ring should have enough mechanical strength to withstand the thermal and chemical stresses within the reactor. A more eective comparison can be enabled by incorporating the reaction kinetics and understanding the diusion limitations within these pellet shapes, which can help in obtaining the conversion versus pressure drop study for these packing (using the correlations developed in this work). This additional work is subjected to the understanding/development of a reaction kinetics model for the high pressure CLC packed bed system. Thus, the proposed CFD-DEM methodology enables understanding of transport phenomena in large industrial scale packed bed reactor, and helps to overcome the diculties related to the ow simulation for packed bed with huge number of particles. This work has validated the proposed methodology for obtaining information on unique shaped packing. This information on transport phenomena is useful for designing the reactor and for the packing/catalyst selection. The methodology can also be extended and applied to demonstrate a serial by simplication multiscale approach for reactor design. Further development of CFD-DEM methodology could involve incorporating reaction kinetics and to simulate for reactiondiusion inside the particles, but this would need more computational requirements and can make the model computationally expensive.

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model on a representative volume of packed bed is plugged into the 1D model to design the reactor. The correlations on pressure drop, particle heat transfer coecient, and the wall heat transfer coecient can be used for designing the reactors. Thus, the development of the current methodology serves as a potential tool for simple, accurate, and fast modeling of the reactors.

AUTHOR INFORMATION

Corresponding Author

*Tel.: +4746639721. E-mail: shahriar.amini@sintef.no.

Notes

The authors declare no competing nancial interest.

ACKNOWLEDGMENTS

The authors would like to acknowledge the nancial support from the European Commission under the seventh framework. The authors are also grateful for suggestions from John Morud, Paal Skjetne, and Wei Yang from SINTEF Materials and Chemistry.

REFERENCES

6. CONCLUSIONS A novel 3D CFD-DEM-based methodology has been developed to identify segments of the bed that can serve as a good representative for the CFD simulation of large industrial scale packed bed. This approach helps to overcome the diculties in the simulation of ow in the packed bed containing a huge number of particles. Two segments, a cutsegment and a wall-segment, have been proposed to represent the core central region of packed bed and near wall region of packed bed, respectively. The methodology has been validated for the spherical packed bed where established correlations are available for comparison. The pressure drop results are validated with the Ergun equation, the particle heat transfer coecients are validated with the RanzMarshal correlation, and the wall heat transfer coecients are validated with Dixon Labua35 and ColledgePaterson36 correlations. The validated methodology can be applied in general for obtaining information on dierent types of packing (such as trilobe, quadrulobe, monoliths, wagon wheels, hollow extrudates, discs). This has been shown in the work by obtaining information on correlations for friction coecients (pressure drop) and the heat transfer coecients for a long cylindrical pellet (aspect ratio: 7) packing and for a uted ring pellet packing (aspect ratio: 1.4). The information on these unique particle shapes is not available in the literature. This information enables comparison between these two packings, which are under investigation for possible use in packed bed chemical looping combustion units. However, an eective comparison will need inclusion of intra-particle reaction diusion phenomena. The development of such a methodology also encourages a potential serial by simplication multiscale modeling approach, wherein the correlation obtained by 3D CFD-DEM
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(1) Nemec, D.; Levec, J. Flow through packed bed reactors: 1. Singlephase flow. Chem. Eng. Sci. 2005, 60, 69476957. (2) Noorman, S.; Van Sint Annaland, M.; Kuipers, H. Packed bed reactor technology for chemical-looping combustion. Ind. Eng. Chem. Res. 2007, 46, 42124220. (3) Noorman, S.; van Sint Annaland, M.; Kuipers, J. A. M. Experimental validation of packed bed chemical-looping combustion. Chem. Eng. Sci. 2010, 65, 9297. (4) Noorman, S.; Gallucci, F.; Van Sint Annaland, M.; Kuipers, J. A. M. Experimental investigation of chemical-looping combustion in packed beds: A parametric study. Ind. Eng. Chem. Res. 2011, 50, 1968 1980. (5) Ergun, S. Fluid flow through packed columns. Chem. Eng. Prog. 1952, 48, 89. (6) Eisfeld, B.; Schnitzlein, K. The influence of confining walls on the pressure drop in packed beds. Chem. Eng. Sci. 2001, 43214329. (7) Ranz, W. E.; Marshall, W. R. Evaporation from drops, part II. Chem. Eng. Prog. 1952, 48/4, 173. (8) Li, C. H.; Finlayson, B. A. Heat transfer in packed beds: A reevaluation. Chem. Eng. Sci. 1977, 32, 1055. (9) Dixon, A.; Cresswell, D. Theoretical prediction of effective heat transfer parameters in packed beds. AIChE J. 1979, 25, 663676. (10) Leva, M.; Grummer, M. Pressure drop through packed tubes: Part III prediction of voids in packed tubes. Chem. Eng. Prog. 1947, 43, 713718. (11) Dixon, A. G. Correlations for the wall and particle shape effects on fixed bed voidage. Can. Chem. Eng. 1988, 66, 705708. (12) Arnab, A.; Shantanu, R.; Nigam, K. D. P. Investigation of liquid maldistribution in trickle-bed reactors using porous media concept in CFD. Chem. Eng. Sci. 2007, 62, 70337044. (13) Gunjal, P. R.; Ranade, V. V.; Chaudhari, R. V. Liquid distribution and RTD in trickle bed reactors: Experiments and CFD simulations. Can. J. Chem. Eng. 2003, 81, 821830. (14) Gunjal, P. R.; Kashid, M. N.; Ranade, V. V.; Chaudhari, R. V. Hydrodynamics of trickle-bed reactors: experiments and CFD modeling. Ind. Eng. Chem. Res. 2005, 44, 62786294. (15) Jakobsen, H. A.; Lindborg, H.; Handeland, V. A numerical study of the interactions between viscous flow, transport and kinetics in fixed bed reactors. Comput. Chem. Eng. 2002, 26, 333. (16) Dixon, A. G.; Nijemeisland, M.; Stitt, E. H. Packed tubular reactor modeling and catalyst design using computational fluid dynamics. Adv. Chem. Eng. 2006, 31, 307389.
dx.doi.org/10.1021/ie302028s | Ind. Eng. Chem. Res. 2013, 52, 1204112058

Industrial & Engineering Chemistry Research

(17) Nijemeisland, M.; Dixon, A. G.; Stitt, E. H. Catalyst design by CFD for heat transfer and reaction in steam reforming. Chem. Eng. Sci. 2004, 59, 51855191. (18) Nijemeisland, M.; Dixon, A. G. Comparison of CFD simulations to experiment for convective heat transfer in a gas-solid fixed bed. Chem. Eng. J. 2001, 82, 231246. (19) Nijemeisland, M.; Dixon, A. G. CFD study of fluid flow and wall heat transfer in a fixed bed of spheres. Am. Inst. Chem. Eng. J. 2004, 50, 906921. (20) Taskin, M. E.; Dixon, A. G.; Stitt, E. H. CFD study of fluid flow and heat transfer in a fixed bed of cylinders. Numer. Heat Transfer 2007, A 52, 203218. (21) Theuerkauf, J.; Witt, P.; Schwesig, D. Analysis of particle porosity distribution in fixed beds using the discrete element method. Powder Technol. 2006, 165, 9097. (22) Bai, H.; Theuerkauf, J.; Gillis, P. A.; Witt, P. M. A coupled DEM and CFD simulation of flow field and pressure drop in fixed bed reactor with randomly packed catalyst particles. Ind. Eng. Chem. Res. 2009, 48, 40604074. (23) Eppinger, T.; Seidler, K.; Kraume, M.. DEM-CFD simulations of fixed bed reactors with small tube to particle diameter ratios. Chem. Eng. J. 2011, 166, 324331. (24) Guardo, A.; Coussirat, M.; Angels Larrayoz, M.; Recasens, F.; Egusquiza, E. CFD flow and heat transfer in nonregular packings for fixed bed equipment design. Ind. Eng. Chem. Res. 2004, 43, 7049 7056. (25) Itasca Consulting Group, Inc. PFC3D (Particle Flow Code in 3 Dimensions); Version 4.0, ICG, Minneapolis, 2006. (26) Cundall, P. A.; Strack, O. D. L. A discrete numerical model for granular assemblies. Geotechnique 1979, 29, 4765. (27) Morsi, S. A.; Alexander, A. J. An investigation of particle trajectories in two-phase flow systems. J. Fluid Mech. 1972, 55, 193 208. (28) Ookawara, S.; Kuroki, M.; Street, D.; Ogawa, K. High-delity DEM-CFD modeling of packed bed reactors for process intensication. Proceedings of European Congress of Chemical Engineering (ECCE6); Copenhagen, 1620 September, 2007. (29) Yang, W.; Skjetne, P. Modelling of gas-solid ows in packed bed. 8th International Conference on Computational Fluid Dynamicsin the Oil and Gas; Metallurgical and Process Industries. Trondheim, 2123 June 2011. (30) Atmakidis, T.; Kenig, E. Y. CFD-based analysis of the wall effect on the pressure drop in packed beds with moderate tube/particle diameter ratios in the laminar flow regime. Chem. Eng. J. 2009, 155, 404410. (31) Dalla Valle, J. M. Micromeritics; Pitman: London, 1948. (32) Dixon, A. Correlations for wall and particle shape effects on fixed bed bulk voidage. Can. J. Chem. Eng. 1988, 66, 705708. (33) Giese, M.; Rottschafer, K.; Vortmeyer, D. Measured and Mmodeled superficial flow profiles in packed beds with liquid flow. AICHE J. 1998, 44, 484490. (34) Zhang, W.; Karsten, E.; Thompson, A.; Reedb, H.; Beenken, L. Relationship between packing structure and porosity in fixed beds of equilateral cylindrical particle. Chem. Eng. Sci. 2006, 61, 80608074. (35) Dixon, A. G.; Labua, L. A. Wall-to-fluid coefficients for fixed bed heat and mass transfer. Int. J. Heat Mass Transfer 1985, 28, 879881. (36) Colledge, R. A.; Paterson, W. R. Heat transfer at the wall of a packed bed: A j-factor analogy established. Collected Papers; 11th Annual Research Meeting; Institution of Chemical Engineers: Bath, 1984; 6 pages. (37) Wakao, N.; Kaguei, S.; Funazkri, T. Effect of fluid dispersion coefficients on particle-to-fluid heat transfer coefficients in packed beds: Correlation of nusselt numbers. Chem. Eng. Sci. 1979, 34, 325 336. (38) Ranz, W. E. Friction and transfer coefficients for single particles and packed beds. Chem. Eng. Prog. 1952, 48, 24753.

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