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Powder Technology 184 (2008) 177 188 www.elsevier.com/locate/powtec

Fully-3D DEM simulation of fluidised bed spray granulation using an exploratory surface energy-based spray zone concept
D.K. Kafui , C. Thornton
School of Engineering, The University of Birmingham, Edgbaston B15 2TT, UK Available online 3 December 2007

Abstract An exploratory spray-zone modelling concept which uses energy of adhesion at the contact of particles has been incorporated in a fully-3D Discrete Element Method (DEM)-based granular dynamics fluidised bed model and applied to fluidised bed spray granulation. In this proof-ofconcept spray model, simple functional relationships are used to notionally model surface energy pick-up by particles traversing the spray zone and an increase in energy of adhesion at drying interparticle bonds. The formation and breakage of interparticle bonds is thus governed by theoretical contact mechanics. Early-stage granulation simulation results provide qualitatively realistic granule size evolution trends. 2007 Elsevier B.V. All rights reserved.
Keywords: Granulation; Spray zone; Discrete element method; Fluidised bed

1. Introduction Granulation is an important size enlargement process in which fine powdery materials are agglomerated into larger granules by the addition of a liquid binder. Different processing equipment such as fluidised beds, high shear mixers, rotating drums and pans are utilised for granulation in such diverse industries as pharmaceuticals, mineral processing, food technology, detergents, iron and steel, agricultural products, specialty chemicals and biotechnology [1,2]. Although the physical mechanisms underlying granulation in the various process vessels may be similar, the process variables can have significantly different effects on the granulation process. In fluidised bed spray granulation, liquid binder is introduced into the bed from the top, bottom or side as a fine spray of liquid droplets using an atomizer. Particles traversing the spray zone are coated with liquid binder droplets and subsequent collisions with other particles may lead to granule nucleation and growth. The granulation process is an extremely complex one involving several mechanisms. Iveson et al. [3] have proposed a description of granulation based on three sets of rate processes: (i) wetting and nucleation (ii) consolidation
Corresponding author. E-mail address: kafuidk@bham.ac.uk (D.K. Kafui). 0032-5910/$ - see front matter 2007 Elsevier B.V. All rights reserved. doi:10.1016/j.powtec.2007.11.038

and growth (iii) attrition and breakage. Controlled wetting and nucleation is seen as one of the key requirements for obtaining product granules with the required attributes. Population balance is frequently employed in modelling particulate processes such as comminution, crystallization and polymerization. The complexity of fluidised bed granulation probably accounts for the paucity of models which incorporate detailed physical mechanisms for the constituent rate processes and resort to population balance modelling in which various empirical or semi-empirical models of coalescence and breakage are used to calculate the extent and rate of granulation whilst ensuring a balance in the particle population. Ramkrishna [4] provides an extensive review of the application of population balance modelling to particulate systems. An increasing number of particulate system properties are being employed in multidimensional population balance models in order to describe particulate processes to the level of detail required for optimisation and control. Vemury et al. [5] used particle volume and particle charge to describe coagulation in aerosols and Iveson [6] used granule size, porosity, binder content and composition for a granulation model. Recently, Tan et al. [7] employed granule size and tracer mass for a population balance modelling of fluidised bed melt granulation. Verkoeijen et al. [8] have argued that three intrinsic properties of particle systems: the volume of each solid component, the volume of liquid and the

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volume of air are the fundamental properties required in a threeproperty population balance model. As multi-dimensional population balance variants replace the basic one-dimensional formulation in the attempt to more accurately model the inherently complex, often multiphase, particulate processes, the relationship between the coefficients in these solutions and the underlying physics and chemistry driving the processes become more tenuous [8]. A fundamental weakness of population balance modelling is that there is no procedure for choosing the form of the kernels and the empirically fitted parameters are limited to the range of conditions in which they were fitted [6]. Most population balance models assume well mixed systems for batch processes and spatial uniformity with regard to flow in continuous processes, conditions which rarely apply. In summarising the limitations of applying population balance modelling to wet granulation processes, Iveson [6] suggests that, perhaps this is an application area for which the methodology is not suited and that discrete element method modelling may be more appropriate for such heterogeneous systems. Heinrich et al. [9] developed a detailed physically based mathematical heat and mass transfer formulation in which spraying, wetting, drop deposition and drying were modelled in a study of the temperature and concentration fields in a liquidsprayed fluidised bed. The process domain is treated as a continuum multicomponent mixture and macroscopic balance equations for heat, mass and momentum used with state equations to model evaporation and drying. Full wetting with constant film thickness is assumed in calculating a wetting efficiency. A conical spray nozzle jet region is assumed and concepts of impingement efficiency, adhesion probability, drop penetration depth and linear liquid drop path and constant liquid drop velocity are employed in modelling the liquid deposition. The simulations suggested that liquid droplet deposition occurred mainly in the spray nozzle region and that equilibrium between spraying, deposition, evaporation, heat transfer and dispersion resulted in a constant average temperature in the bed. The spray nozzle region was found to be characterised by high wetting efficiency. Goldschmidt et al. [10] presented the first known application of the discrete element method to spray granulation. Liquid droplets, which are introduced into the bed in a spray zone according to a predetermined rate and velocity, are modelled as discrete entities in addition to the discrete spherical particles and encounters between these two species leads to coalescence and the formation of a wetted particle. Hard-sphere collision laws govern the interaction between the solid spheres resulting in rebound or agglomeration, with a larger sphere replacing the colliding spheres in the latter case. The main weaknesses of this model are the inability to handle multiple contacts and bond breakage. Nevertheless, this model produced reasonable granule size evolution trends and qualitatively illustrated the effects of process conditions such as fluidisation velocity, spray rate and spray pattern. A discrete particle-based code with realistic contact mechanics and particleparticle bonding formulations is capable of adequately simulating the consolidation and growth as well as the attrition and breakage processes. A discrete model for the wetting and nucleation process is therefore the remaining main

challenge in applying the discrete element method to wet granulation. A spray zone in which liquid droplets are introduced into the bed at predetermined rates and size distributions is an appropriate way to model the region where most of the primary wetting which takes place in the bed occurs. The possibility of modelling the interactions between solid particles and liquid droplets using the discrete particle model when combined with droplet drying models can provide a microscopic tool for simulating droplet deposition and nucleation. A significant limitation with this approach is the computational power required to model anything approaching a laboratory scale system. In this paper, a proof-of-concept exploration of the spray zone modelling ideas discussed above is carried out, not with discrete liquid droplets, but using surface energy based on the theory of Johnson et al. [11] as the binding mechanism. The use of surface energy simplifies the problem by not introducing an additional phase into the system and may be notionally compared to binderless granulation [12]. This approach is taken because the primary objective of this work is to test out the methodology within a fully-3D DEM based Lagrangian Eulerian fluidised bed model. In this context the spray granulation simulation of a Geldart group A particle bed is performed. Conceptual notions of wetting (surface of particle becoming active as a result of picking up surface energy in the spray zone, drying (increase in surface energy or adhesion energy value with time), wet surface energy (surface energy that can still form bonds and has not reached some terminal dried out value) have been used here but are not to claim or imply any equivalence to liquid binders. 2. Modelling technique Details of the discrete particle-continuum fluid model have been given by Kafui et al. [13] and only a very brief summary is presented here. The spray model and the basis of the assumptions made are detailed here as is the procedure adopted for the granulation simulation. 2.1. Fluidised bed model For the particulate phase, the translational and rotational motions of each particle i of mass mi and moment of inertia Ii are calculated using the equations mi dvi fci ffpi mi g dt 1

Ii

dxi Ti dt

where fci is the out-of-balance force of the particle due to the solid particleparticle contact force, ffpi is the fluidparticle interaction force, mig is the weight of the particle, Ti is the torque due to the tangential components of the contact forces, and vi and i are the linear and angular velocities respectively of the particle. The frictional solid particleparticle interactions are modelled using theoretical contact laws for elastic particles,

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elastoplastic particles, elastic particles with adhesion and elastoplastic particles with adhesion [1417] from which the out-of-balance contact force fci and torque Ti are obtained. In coupling the discrete particle phase and the continuum fluid phase, the fluidparticle interaction force ffpi acting on a particle is the key term which is calculated using ffpi vpi jp vpi j:sf efdi 3

Here p is the fluid pressure, vpi is the volume of particle i, f is the viscous stress tensor which is obtained from a general constitutive equation given by Bird et al. [18] for a Newtonian fluid, is the local void fraction and fdi, the drag force, is computed from the empirical relationship given by Di Felice [19]. The fluid phase is modelled as a continuum for which the continuity and momentum equations respectively are eqf j:eqf u 0 t eqf u j:eqf uu j:p j:sf Ffp eqf g t 4

This is also equivalent to a full coverage arising from the distribution mechanism proposed by Schfer and Mathiesen [22] where fine droplets of binder cover and coalesce on the powder particle surface to form a film. On the basis of the above and in the context of this study, a full and uniform coverage of our notional surface energy binder is a reasonable first assumption to make for the particles which pick up surface energy in the bed. The following assumptions and notions are adopted in formulating a conceptual representation of a surface energy spray zone: a. The spray zone is represented as a conical region with the spray source or nozzle at the apex. (Fig. 1). A notional concept of an ultra-fine mist of adhesive is assumed to be constantly injected into and limited to this region by the nozzle. b. Particles entering the spray zone are assumed to be uniformly wetted as they pick up surface energy at a rate which depends on the time spent in the zone and the distance of the particle from the source. c. Inside the spray zone, surface energy coating on exposed surfaces remains wet but once particles exit the spray zone, the surface energy increases in value as the coating starts to dry. A dry out period is associated with any value of exposed surface energy beyond which the surface becomes inactive outside the spray zone. d. A particleparticle bond starts drying on formation with a consequent increase in surface energy to an asymptotic upper limit and such a bond is not penetrated by wet surface energy in the spray zone. 2.2.1. Surface energy pick-up in the spray zone Based on the preceding assumptions, simple exponential functions have been employed to formulate the spray model. A particle located in the spray zone at a distance sp from the spray

In Eqs. (4) and (5), u and f are the fluid velocity and density respectively, and Ffp, the fluidparticle interaction force per unit volume, is computed by summing up the fluidparticle interaction force acting on all the particles nc in a computational fluid cell and dividing by the volume of the fluid cell, Vc: Pnc ffpi 6 Ffp i1 DVc An explicit finite difference scheme is used to incrementally calculate the motion of the particles while a semi-implicit finite difference scheme based on a staggered grid is used for discretising the fluid hydrodynamic equations. The details of the numerical schemes have been given in [13,20]. 2.2. Spray zone model The spray is one of the primary mechanisms by which binder is introduced into a wet granulation processing environment and is thus a key factor in wetting and nucleation. Iveson et al. [3] define the nucleation zone as the region where the binder and the powder particles first come into contact and form the initial nuclei. This is essentially a region around the spray nozzle, referred to here as the spray zone, where there is a high probability of binder-to-particle encounter. Iveson et al. [3] have argued that the two processes that are important in the nucleation zone are nuclei formation and binder dispersion, the former being a function of wetting thermodynamics and kinetics and the latter controlled by the process variables. Wetting thermodynamics has been described in terms of the contact angle between the solid and binder and the spreading coefficients of the phases over each other. In the extreme case of very low contact angle between solid and binder or a positive binder-to-solid spreading coefficient [21], full wetting will occur resulting in a film of binder covering the powder particle.

Fig. 1. Notional representation of spray zone as a conical region.

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The surface is considered to have dried and lost all its activity when tso, the time since the particle last left a spray zone, exceeds tds and w is set to zero. Using Eqs. (9) and (10), the surface active w values obtained for wmax = 0.5 Jm 2 and tdmax = 10 s is shown in Fig. 3 for various values of wo. 2.2.3. Drying of particleparticle bonds Two adhering surfaces are said to possess energy of adhesion per unit area equal in total to the work done in separating them [23]. The nature of the interacting solids (ionic, metallic or van der Waal's) significantly influences the values of the surface energy or adhesion but in general, although the magnitudes of the adhesive traction are large (~ 0.5 GPa at separation distance of 2 for rubber with = 0.04 Jm 2), their range of action is very small. The JKR theory [11] extends the Hertz theory to include adhesive contact of perfectly elastic solids. The degree of adhesion is highly influenced by the surface roughness and also the degree of ductility of the asperities, factors which are not accounted for in the JKR theory. The strength of the adhesion between elastic bodies depends on the surface energies of the interacting surfaces. According to the JKR theory, for two adhering elastic spheres with surface energies 1and 2, interfacial energy 12 and radii r1 and r2, the force required for separation is 3r/2 where r = r1r2/(r1 + r2) and the energy of adhesion = 1 + 2 12. In the notional drying concept adopted, increasing energy of adhesion d (= 2d) at a drying particleparticle bond is evaluated using gd gw 1 dfac 11 etb 11

Fig. 2. Accumulation of surface energy for fixed and moving particles in spray zone for wmax = 0.5 Jm 2.

source (Fig. 1) accumulates wet surface energy w (wetting) according to gw gwmax es 1 ets Dgw gwmax es ets 1Ds ets Dts 7 8

where wmax is the limiting surface energy of the spray, s (= sp/ sm) is the normalised distance of the particle from the spray source and ts is the time spent in the spray zone. This simple formulation approximately reflects the expectation that particles will pick up less surface energy farther away from the source due to blockage by other particles in the zone and/or a lower concentration of adhesive in the regions farthest from the source and is considered adequate for the objectives of this study. In any future formulation based on discrete liquid binder droplets, the motion of the droplets through voidages between particles/granules in the zone will be better captured by the discrete element formulation for the particles and liquid droplets. Fig. 2 illustrates the accumulation of surface energy for (i) a particle at different fixed distances from the spray source; (ii) a particle which enters the spray zone near to and moves away from the source; (iii) a particle which enters the zone farthest from and moves towards the source. 2.2.2. Drying of surface energy outside the spray zone Exposed wet surface energy dries up rapidly outside the spray zone and the model associates with this an increase in the active wet surface energy w and an active period tds during which the surface can form a bond with another particle. Both w and tds depend on wo, the wet surface energy of the particle when it last left the spray zone and are modelled using the expressions   gw gwo 1 e1tso =tds 9 tds gwo tdmax gwmax 10

In Eq. (11), an average wet surface energy w of the two surfaces (= (w1 + w2)/2) when the bond was first formed is used, tb is the age of the bond and dfac ( 1), the dry-out factor, is used to model a limiting drying-induced increase in adhesive

Fig. 3. Notional drying of wet surface energy outside spray zone for wmax = 0.5 Jm 2 and tdmax = 10 s.

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energy at the bond. The drying process modelled by Eq. (11) is restricted to a bond dry-out period tdb given by tdb gw tdmax gwmax 12

where tdmax is the maximum dry-out time associated with wmax. If the age of the bond exceeds tdb, the bond strength or energy of adhesion d is set to dfacw. The value of dfac is chosen to reflect the final dried-bond value attainable by d. The increase in the energy of adhesion during drying for bonds formed for various values of wet surface energy is shown in Fig. 4 for a dry-out factor dfac = 2.0.

2.3. Simulation procedures A Geldart group A powder bed consisting of five particle sizes 45, 47.5, 50, 52.5 and 55 m was used in the simulations. The particle properties used in the study are: Young's modulus E = 700 MPa; density = 2500 kg m 3; coefficient of friction = 0.30; Poisson's ratio = 0.33. These values are based on glass beads except for the elastic modulus which is reduced by two orders of magnitude from the actual value in order to increase the time step used in the simulations. A yield stress of ~ 1%E (y = 7 MPa) is employed. A total of 50,000 particles with a mean particle diameter of dp = 50 m and size distribution shown in Fig. 5 were used in the powder bed. Initial bed preparation was carried out by randomly generating the particles in a space of 2 mm 2 mm base area and 5 mm height followed by pluvial deposition. This procedure yielded a bed, shown in Fig. 6(a), with an initial height 1.46 mm (~ 29dp) and a void fraction = 0.408. Fluidising gas (atmospheric air at 313 K) at a uniform flow of 57.1 mm/s (~ 20umf), introduced into the bed from the base, was then used to fluidise the bed prior to the introduction of the sprays. For the bed employed in this study, the minimum fluidisation velocity is estimated at ~ 2.9 mm/s using the corFig. 5. Particle size distributions by mass fraction and number fraction.

relation of Baeyens and Geldart [28] and the fluidising gas flow used is of the order of 12.4umb according to Abrahamsen and Geldart [29]. Although much higher gas velocities in the high bubbling to turbulent regimes would normally be used and the gas flow rate increased with granule growth to maintain good fluidisation ([10], [30]), in our set-up with no re-circulation for particles leaving the bed, the judgement was made to stay in the lower end of the bubbling regime for this study. Periodic vertical boundaries were employed for both the fluid and particle systems. Bottom and top horizontal wall boundaries were used for the particle system while prescribed normal gas influx at the base and a prescribed atmospheric outflow pressure at the top were employed for the fluid system. After fluidising the bed for 24 ms, four identical spray zones were located symmetrically in the bed with the base of each conical zone a height of 5dp above the top of the initial deposited bed. The particle configuration and the spray locations at this stage are shown in Fig. 6(b) and (c) respectively. Each spray zone is defined by specifying the coordinates of the source, the height hc and angle c of the spray cone, the maximum wet surface energy wmax, the dry-out factor dfac and the maximum dry-out time tdmax. The values employed for these parameters in the current simulation are: hc = 20dp, c = 28.07o, wmax = 1.0 Jm 2, dfac = 2.0, tdmax = 10 s. The spray zone dimensions and locations were selected such that the circular section of each spray at its fullest extent covered half the linear dimension of the quarter of the bed cross-section. Considerations of the estimated total simulation time achievable (~ 0.5 s) led to the choice of values for wmax, dfac and tdmax after an examination of the surface active w values obtained in Fig. 2. 3. Granulation simulation 3.1. Granulation and bonds Granulation was simulated with the four spray zones described in the preceding section for 525 ms. In Fig. 7, the trends in the number of granules with three or more primary

Fig. 4. Evolution of adhesive energy during bond drying for various initial wet surface energy values.

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Fig. 6. Initial deposited bed (a) fluidised bed prior to introduction of spray (b) location of spray zones (c).
3+ particles ng , the numbers of bonds and active sprayed particles during the simulation are shown. On introduction of the spray zones, the number of bonds increases rapidly to ~ 7000 in the first 100 ms, then increases more slowly in the next 250 ms to ~ 12,000 followed by a period of a fairly constant average number of bonds. The fluctuations which are a feature of the trend are indicative of bond formation and breakage. The number of active sprayed particles exhibits a similar trend but shows a slight drop in the latter stages of the simulation which is due more to the limited definition of active sprayed particles where bonded particles without free active surface energy are not counted. Nevertheless, the fluctuations are illustrative of particles picking up surface energy and then drying with or

without the formation of bonds. Granulation, as measured by 3+ the number of granules with three or more primary particles ng , shows a rapid increase to ~ 75 granules immediately after the introduction of the sprays followed by a slow fluctuating decrease to ~ 45 granules and then a gradual increase to ~ 450 granules when it then fluctuates for about 10 ms. A further slow increase in the number of granules to a peak of ~ 750, leading to a decrease to ~ 550 and an even slower fluctuating increase to ~ 650 in the last stage of the period simulated completes the trend. Overall, the number of granules increases with time at a decreasing rate within the time scale investigated. The consistency in the trends shown by the number of bonds and number of granules is expected since bonds give rise to granules.

Fig. 7. Evolution of the numbers of granules n3+, bonds and active sprayed g particles during granulation.

Fig. 8. Evolution of the number of granules compared to the maximum and mean adhesive bond energies.

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Fig. 8 compares the evolution of the number of granules with the maximum (max) and mean (mean) adhesive bond energy in the granules. The maximum adhesive bond energy exhibits a near-linear increase punctuated with step drops which indicate breakage of maximum-strength bonds resulting in a slightly nonlinear overall increase as the granulation progresses. During this early stage of granulation, the maximum adhesive bond energy max increases according to the bond drying Eq. (11). A steady, initially nonlinear increase followed by a mildly fluctuating linear increase characterises the evolution of the average granule bond strength which reaches a value of ~ 0.076 Jm 2 compared to 0.62 Jm 2 for max at the end of the simulation period. Significantly more simulation time is required to reach average adhesive bond energies of the order of 1.0 Jm 2 which is the value potentially attainable for the maximum wet surface energy value used for the spray zones. 3.2. Granule size evolution Two definitions of granule size have been explored in this work: the number of primary particles in a granule snp (which has been found to give the same trends as the mass of the granule) and the circumscribing radius of the granule srad. These sizes were monitored throughout the simulation and the mean and maximum sizes are shown together with the number of mean granules in Fig. 9(a). The means of these size definitions, snp mean and srad , both exhibit pronounced growth in the first 20 ms at the start of granulation, followed by about 90 ms of granule breakage and coalescence which is evident in the large fluctuations in the mean size. Subsequently, steady mean sizes mean mean of the order of snp ~ 20 and srad ~ 0.09 mm are attained during the rest of the simulation with only small fluctuations. This may be likened to the steady growth behaviour which Iveson and Lister [24] associate with systems with relatively coarse, narrowly sized particle distributions and low viscosity binders leading to weak deformable granules. The maximum max max granule sizes snp and srad also show fast early growth trends but subsequently, extreme variability marked by sharp falls and rises in the maximum granule size becomes the dominant characteristic of the growth profiles. This trend is indicative of the growth and breakage of rather large granules, some of the order of 4500+ primary particles (~ 1.5 mm). No intrinsic direct 3+ relationship between the growth in the number of granules ng and the maximum granule size trends is expected and none is evident in the semi-log plots shown in Fig. 9(a). However, a 3+ closer inspection of the linear-scale plots of the evolution of ng max and snp in Fig. 9(b), where linear approximations have been superimposed to show the trends in different periods, suggests that the general trends in the evolution of the size of the largest granule is mirrored in the evolution of the quantity of granules. max An overall increasing trend in snp between 0.1 s and 0.2 s leads 3+ max to an increasing ng trend which levels off as the snp fluctuations become bigger towards the end of this period. Following that, a predominant breakage period with no overall max 3+ change in snp ensues, resulting in an increasing ng trend from max ~ 0.23 s to 0.30 s. A steeper overall increasing snp trend between ~ 0.30 s and 0.37 s on the other hand, triggers a fall

3+ in ng (suggestive of coalescing granules) while a steep falling max trend followed by a fairly steady trend in snp produces a more max gradual rise in the number of granules. The trend in the srad evolution did not display the same consistent level of correlation 3+ with the ng trend but this may well be due to an inadequacy of the circumscribing radius as a measure of granule size. 3+ The location of granules ng in the bed at three instances, 0.118 s, 0.354 s and 0.525 s during granulation are shown in Fig. 10 in colours according to size snp. Visually, granule sizes in the range snp[2011000] which are formed by 0.12 s subsequently appear to be coalescing and breaking up to form larger granules in the range snp[10012000] and some smaller granules. An increase in the number of granules in the size range snp[1150] for example, is clearly evident in Fig. 10 from 0.118 s to 0.525 s. Granules are seen to be located in all regions of the bed indicating no strong bias attributable to the spray zone locations and a uniform dispersion of coated particles in the bed. The largest granules, however, have not moved significantly away from the vicinity of the spray zones in the duration of the simulation of this study, a feature attributable to the relatively low fluidising gas velocity employed in the simulation.

Fig. 9. (a) Maximum and mean granule size (snp, srad) evolution during granulation, (b) Comparison of approximate trends in the evolution of n3+ and g smax during granulation. np

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Fig. 10. Visualisation of granules at three stages during granulation (snp colour key: cyan[23], yellow[410], green[1150], pink[51100], violet[101200], orange [2011000], brown[10012000], dark drown[2000+]). (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.)

3.3. Granule size distribution The cumulative mass fraction and frequency plots of granule size (snp) are shown in Figs. 11 and 12 respectively at different times during granulation. Both figures, which include doublets, show steady increases in both the mass fraction and frequency up to t = 0.472 s. At t = 0.525 s, the plots are nearly coincident with those at t = 0.472 s especially for cumulative frequency suggesting the approach to some steady state distribution. Each of the cumulative mass fractiongranule size trends is approximately bilinear on a semi-log plot as are the cumulative frequencygranule size plots. The increasing slopes of the straight line approximation to the first leg of these bi-linear plots

as the granulation proceeds is consistent with overall size or more appropriately, mass enlargement occurring, since the size here snp, is a measure of mass rather than a linear dimension. 3.4. Fractal analysis of granules The concept of fractals is used to quantify a variety of scale invariant processes in nature, where the existence of a power law relationship between number and size signifies fractal behaviour. Natural and artificial fragmentation processes have been known to produce fractal objects [25] as did the agglomeration of submicron alumina in 2-D [26]. Although the final product of granulation is not generally fractal,

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Fig. 11. Evolution of cumulative granule size (snp) by mass fraction during granulation (includes doublets).

application of fractal geometry to the analysis of the evolving granules may give some clues about the mechanisms involved in a complex granulation process. An index, the fractal dimension df with a lower limit of 1 and an upper limit equal to the Euclidean dimension, can be useful in this regard since a tenuous granule structure is indicated by a low df while the higher the value of df, the more space-filling the structure. For a granule with Np primary particles in a circumscribing sphere of radius Rg, a fractal dimension may be obtained from [27]  df Rg 13 Np / rp where rp is the mean primary particle radius and is the fraction of the circumscribing sphere volume occupied by solids (except for a straight chain of particles where ~ 1). A computer-generated random spherical granule made up of five primary particle sizes, the mean primary particle size being

Fig. 13. Plot of the fractal Eq. (13) for granules (n3+) at t = 0.118 s (a), t = 0.525 s g (b).

Fig. 12. Evolution of cumulative granule size (snp) by frequency during granulation (includes doublets).

20 m was found to have a calculated circumscribing sphere volume occupancy = 0.596. Applying Eq. (13) yields a fractal dimension of 2.94 for this spherical granule which is close to the Euclidean dimension limit of 3.0 and confirms a more volumefilling and rotund structure. Eq. (13) was applied to granules with three or more particles during the granulation process. Fig. 13 shows the logarithmic plots of Eq. (13) at times t = 0.118 s and 0.525 s with linear fits from which values of and df have been extracted. The lines for df = 2.0, 3.0 using the mean value extracted from the linear fit to the simulation data and the line for df = 1.0 using = 1 have been superimposed along with a line for the random spherical granule referred to earlier. At the times examined, Fig. 13 suggests granule structures range from near-planar (df ~ 2) to near rotund (df ~ 3) especially when the number of primary particles is less than ~ 20. For the larger granules containing more primary particles, the figures suggest a concentration of the granule structures mid-way between planar and rotund, an effect which appears to shift towards the rotund with a consequent increase in df as time increases. The circumscribing spherical volume occupancy and fractal dimension df obtained from Eq. (13) are shown in Fig. 14.

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the visualisation are not adequately reflected in the results of the fractal analysis. The circumscribing radius employed in the analysis is, by definition, the maximum linear dimension of the space occupied by each granule. Any bias towards one dimension and, for the granules with small Np, protrusions of two or three particles sticking out from the bulk granule tend to appreciably increase the circumscribing radius and hence significantly reduce the circumscribing sphere volume occupancy of the granule. It thus appears that the circumscribing sphere radius may not be an appropriate size measure to use for an analysis of the granules obtained in these simulations. 4. Conclusions
Fig. 14. Variation of fractal dimension df and circumscribing sphere volume occupancy of granules during granulation.

Both df and exhibit an increasing trend during the granulation process. A visualisation of the granules enables us to examine the granules and make deductions on the structures and shapes. Such an examination has revealed that although the granules with more primary particles tended to be slightly longer in one dimension and irregular, in general the structure was more space-filling. For granules with primary particles Np ~ 11200, a large majority of the granules were observed to be rotund while a mixture of stringy to rotund shapes were found for Np ranging from 3 to 10. An illustration of the granule shapes obtained is shown in the elevation and plan views of Fig. 15 for Np ranges 1120, 51200, 2011000 and 10002000 at t = 0.525 s. Evidently, the mainly rotund shapes observed from

A surface energy-driven spray zone concept has been presented and applied to a fully-3D DEM-based fluidised bed granulation simulation of a Geldart group A particle bed. The concept uses simple functional relationships to model the pickup of surface energy (wetting) by particles in the spray zone and the granulation simulation employing four symmetrically located spray zones was found to quickly result in uniform dispersion of spray-coated particles in the bed. Sensible trends in net granule formation have been obtained which can be related to trends in bond formation, bond strength and maximum granule mass. Granule formation and breakage are adequately captured as are the evolution of granule mass and linear size showing mass/size enlargement and reduction. The fast growth rate of the largest granules may be due to the surface energy values used for the spray zones and the relatively low fluidising gas velocities used in the simulations. Fractal analysis of the early stage granules confirms that the products are not

Fig. 15. Visualisation of granule shapes/structures for the indicated Np ranges at t = 0.525 s.

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fractal. The modelling concept explored here holds a lot of promise and, with the anticipated future increase in computer processing capacity, the use of pendular liquid bridges in which liquid binder spray droplets are modelled as discrete elements is a viable extension of the methodology. List of symbols df fractal dimension () dfac dry-out factor ( 1) for a drying bond () dp mean particle diameter (m) E elastic modulus (Pa) Ffp fluidparticle interaction force per unit volume of bed (N m 3) (see Eq. (6)) fci sum of contact forces acting on particle i (N) fdi drag force acting on particle i (N) ffpi fluidparticle interaction force for particle i (N) g acceleration due to gravity (m s 2) hc height of conical spray zone (m) Ii moment of inertia of particle i (kg m2) mi mass of particle i (kg) Np number of primary particles in a granule () nc number of particles in a computational fluid cell () 3+ ng number of granules with three or more primary particles () p fluid pressure (Pa) Rg circumscribing radius of a granule (m) r radius of curvature at the contact between two spherical particles (m) r1, r2 radii of two spherical particles in contact (m); used in definition of rp mean particle radius in a granule (m) s (= sp/sm) normalised distance of a particle from spray source () sm maximum distance of a particle from spray source in a spray zone (m) snp granule size defined by the number primary particles in it () sp distance of particle from spray source in spray zone (m) snrad srad normalised by the average primary particle radius () srad granule size defined by the radius of the circumscribing sphere (m) Ti torque acting on particle i due to tangential component of contact forces (N m) t time (s) tb age of a bond (s) tdb bond dry-out period (s) tdmax maximum dry-out period associated with maximum wet surface energy wmax (s) ts time spent by particle in the spray zone (s) tso time since particle last left spray zone (s) u fluid velocity vector (m s 1) umb minimum bubbling gas velocity umf minimum fluidisation gas velocity (m s 1) vi velocity of particle i (m s 1) vpi volume of particle i (m 3)

Vc xs,ys,zs

volume of a computational fluid cell (m 3) coordinates of spray source (m)

Greek d max mean 1,2 12 w wmax wo d c f y f i

local void fraction () fractional solid volume occupancy of the circumscribing sphere of a granule () energy of adhesion per unit area, defined in Section 2.2.3 (J m 2) (= 2d) energy of adhesion at a drying bond (J m 3) maximum adhesive bond strength (Jm 2) mean adhesive bond strength (Jm 2) surface energies of two spherical particles in contact (J m 2) interfacial energy of two surfaces in contact (J m 3) wet surface energy of a particle (J m 2) limiting surface energy from spray source (J m 2) wet surface energy of particle as it leaves the spray zone (J m 3) surface energy of a drying bond (J m 3) coefficient of solid friction () Poisson's ratio () angle of conical spray zone (m) particle density (kg m 3) fluid density (kg m 3) yield stress (Pa) viscous stress tensor (Pa) angular velocity of particle i (rad s 1)

Acknowledgements The work carried out in this paper was funded by EPSRC Grant No GR/R32314. The authors are grateful to Unilever Research Port Sunlight for the support in a previous but related project and to Prof. Kuipers of Twente University of Technology for the help with the fluid hydrodynamics code. References
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