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Chemical Engineering Science 61 (2006) 1528 – 1539

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Effect of particle shape on liquid-fluidized beds of binary (and ternary) solids


mixtures: segregation vs. mixing
R. Escudiéa, b , N. Epsteina,∗ , J.R. Gracea , H.T. Bia
a Department of Chemical & Biological Engineering, University of British Columbia, 2216 Main Mall, Vancouver, B.C., Canada V6T 1Z4
b Laboratoire de Biotechnologie de l’Environnement (LBE), Institut National de la Recherche Agronomique (INRA), Avenue des étangs, 11100 Narbonne, France

Received 1 June 2005; received in revised form 26 July 2005; accepted 21 August 2005
Available online 2 November 2005

Abstract
Experiments were carried out in water-fluidized binary (and ternary) mixtures of teflon spheres, discs and rods. All particles had the same
volume, while the discs and rods had nearly the same sphericity. It is shown that segregation can occur by shape, with similar segregated and
mixed zones as when binary mixtures of different size or density are fluidized. The model of Pruden and Epstein (1964; Stratification by size
in particulate fluidisation and in hindered settling. Chemical Engineering Science 19, 696), in which the degree of segregation depends on the
bulk density difference(s) of the corresponding monocomponent beds at the same liquid velocity, is vindicated qualitatively for each system, but
sphericity is not sufficient as a single shape factor to yield a single quantitative correlation of the transitions between segregation patterns for the
different systems. Segregation by shape of non-isometric particles appears to require higher reduced density differences than sizing of spheres,
probably because of the greater bed instabilities generated by the non-isometric particles. Overall bed voidage is predicted well by the serial
model of Epstein et al. (1981; Liquid fluidisation of binary particle mixture– I.Overall bed expansion. Chemical Engineering Science 36, 1803).
䉷 2005 Elsevier Ltd. All rights reserved.

Keywords: Fluidization; Particle mixing; Segregation; Shape; Hydrodynamics

1. Introduction may segregate or mix, according to the characteristics of the


particles and the liquid, and the operating conditions.
The use of liquid fluidization in the mining industry was In order to better understand classification phenomena and
practised as early as the 19th century in order to separate solids to simplify the problem, previous studies have focused on
of different sizes or densities, and applications of liquid–solid mixing and segregation in binary-solids mixtures, and in a
fluidized beds to a variety of other operations have increased small number of cases ternary-solids mixtures. Much work
markedly during the past century (Epstein, 2003a). In the last has been devoted to investigating the segregation of particles
three decades, fluidized-bed reactors have received much at- by size (sizing) and, to a lesser extent, by density (sorting). As
tention in the biotechnology sector, one of the most common illustrated for the case of binary sizing in Fig. 1, four different
applications being wastewater treatment. In such bioreactors, segregation or mixing patterns have been identified by Gibilaro
the properties of the fluidized carrier particles (size, density, et al. (1985), who labelled them (a) perfect mixing, (b) par-
shape) can change during the process because of their colo- tial segregation 2, (c) partial segregation 1 and (d) complete
nization by a biofilm. In other industrial applications, even if segregation. Other investigators have used other designations,
the particles are uniform at the beginning of the process, their e.g. “complete mixing” for (a), “continuous stratification with
properties may change due to attrition, coalescence or chemi- no interface” for (b), “segregation with transition zone” or
cal reaction. Consequently, the solids in these reactors can vary “. . .fuzzy interface” or “. . .mixed region” or “. . .continuously
in size and/or density and/or shape, with the result that they stratified intermediate layer” for (c), and “clean-cut segre-
gation with a sharp interface” for (d). For simplicity we
adopt the terms: (a) homogeneous mixing, (b) heteroge-
∗ Corresponding author. Tel.: 1 604 822 2815; fax: 1 604 822 6003. neous mixing, (c) incomplete segregation and (d) complete
E-mail address: helsa@chml.ubc.ca (N. Epstein). segregation.
0009-2509/$ - see front matter 䉷 2005 Elsevier Ltd. All rights reserved.
doi:10.1016/j.ces.2005.08.028
R. Escudié et al. / Chemical Engineering Science 61 (2006) 1528 – 1539 1529

distributor played a dominant role in their experiments, partic-


ularly at higher liquid superficial velocities. Also, their results
for every type of particle classification were almost all within
the dense solids voidage range ( ≈ 0.5.0.6), which explains
their conclusion that “particle density had a much stronger ef-
fect on segregation than size and shape”. This conclusion con-
forms to the generalization (Epstein, 2005) that sorting, unlike
sizing, is best performed in the lower voidage range.
The objective of the present work is to study the liquid-
fluidized-bed classification by shape (“shaping”) of particles
having the same volume and the same density but different
shapes. A predictive model, based on differences of bulk density
of each individual monocomponent bed, is first developed for
“shaping”. This model is examined by generating experimental
data for binary and ternary mixtures of particles of equal volume
Fig. 1. Mixing and segregation patterns for liquid fluidization of binary-sized
spheres of equal density, after Gibilaro et al. (1985).
and equal density but different shapes: spheres, discs and rods.

2. Experimental equipment and measurement technique


Two approaches have been developed to describe and predict
these phenomena. Initiated by Kennedy and Bretton (1966), a The experimental set-up is similar to that described by Lee
dispersion–segregation model based on a one-dimensional ver- et al. (2001), where it was used for three-phase fluidization
sion of Fick’s Law was developed on the assumption that at tests (see their Fig. 1). The column is constructed of acrylic,
any level the dispersive flux of species i relative to the random with an inner diameter (D) of 0.127 m and an overall height of
movement of the fluidized particles can be equated to the seg- 2.58 m. Water at 20 ◦ C is fed from a feed tank and is circulated
regation flux of this species: back to the fluidization column via a centrifugal pump. The
tank is equipped with baffles to calm the flow and minimize
−Di jCi /jz = Ci Upi . (1) entrainment of air with the incoming water. The liquid flow rate
is measured by two calibrated rotameters.
The main problems in solving this equation are the estimations The column consists of three sections: a calming entry sec-
of both the dispersion coefficient Di (Di Felice, 1995; Epstein, tion filled with 25-mm plastic spherical Tri-Packs (FABCO) to
2003b) and the segregation velocity Upi of species i. In addi- homogenize the liquid flow before it reaches the liquid distrib-
tion, this method does not provide any criteria for distinguish- utor, the test section separated from the calming section by the
ing between the four mixing-segregation patterns of Fig. 1. A distributor, and a disengagement section. The discharged water
second approach, initiated by Pruden and Epstein (1964), as- returns by gravity to the feed tank. The distributor, designed so
sumes that the driving force for segregation of a binary parti- that its pressure drop is always at least 25% of that across the
cle mixture is the bulk density difference of the corresponding bed of particles, consists of a perforated plate containing 54
monocomponent beds. This approach is adopted in the present holes of 4.8 mm diameter on a square grid, giving a free area
work. ratio of 7.7%.
Although the effects of particle size and density are now well Along the height of the column, 6.3-mm diameter pres-
established, the influence of particle shape is still unknown. sure taps were located, starting at 64 mm above the distributor
Recently, Barghi et al. (2003) reported on the mixing and seg- and then at four 153-mm intervals followed by thirteen 103-
regation in liquid–solid fluidized beds using an electrochemical mm intervals. A differential pressure transducer, Omega model
technique involving the collision frequencies of tracer parti- PX750-30DI, measured the dynamic pressure drops over each
cles on probes with 3.0 wt% aqueous NaCl solution as the liq- interval, the pressure difference being recorded for periods of
uid. In addition to sizing and sorting experiments, aluminium 60 s at 50 Hz. Assuming negligible wall friction and acceler-
tracer particles of cylindrical shape were mixed with 5-mm ational effects, the dynamic pressure gradient, −P /Z, be-
glass spheres, the cylindrical particles having the same volume tween adjacent pressure taps, i.e., the static pressure gradient
and similar density to the spheres and diameter to length ra- corrected for the hydrostatic head, is then given by
tios, Dc /Lc , of either 1 or 2, corresponding to sphericities of
0.874 and 0.825, respectively. Some segregation occurred only −P /Z = (1 − )(s − l )g, (2)
with Dc /Lc = 2, and then only at the lower velocities in the
heterogeneous mixing mode illustrated by Fig. 1b, the elec- where  is the average bed voidage between successive
trodes at the top of the bed registering more collisions from the pressure taps.
cylinders than at lower levels. It should be noted, however, that In order to understand the effect of particle shape in a binary-
since the bed heights employed by Barghi et al. (2003) were solid liquid fluidized bed, three different shapes of particles
very small (typically, a defluidized bed height of 200 mm and were used, all made of polytetrafluoroethylene (PTFE), i.e.,
voidages not exceeding 60%), mixing effects due to the liquid Teflon䉸 , thereby ensuring the same density (s =2160 kg/m3 ).
1530 R. Escudié et al. / Chemical Engineering Science 61 (2006) 1528 – 1539

Table 1 The initial hypothesis is that the degree of segregation depends


Characteristics of the three types of particles on the difference between the bulk densities of the two particle
Dc (mm) Lc (mm) d (mm)  k species when each is fluidized separately in the same column
with the same liquid at the same superficial liquid velocity, U, as
Spheres N.A. N.A. 9.525 1 N.A.
Discs 12.7 3.50 9.461 0.716 1.342
for the binary (Epstein, 2005). For a binary particle mixture of
Rods 4.76 25.4 9.525 0.686 0.500 uniform density s , uniform volume-equivalent diameter d and
different shapes (2 > 1 ), the driving force for segregation is
then given by
The first type of particles was spherical, with a diameter (dp ) B2 − B1 = [2 l + (1 − 2 )s ] − [1 l + (1 − 1 )s ]
of 9.53 mm (3/8 ) and an Archimedes number of = (s − l )(1 − 2 ), (8)

dp3 l (s − l )g where Bi is the bulk density of the monocomponent flu-
Ar = = 9.8 × 106 (3) idized bed of particle species i, and i is the overall voidage of
2
the monocomponent fluidized bed of particle species i at the
assuming water at 20 ◦ C as the liquid. Hence, these particles are given U.
clearly in the Newton regime (Ar > 100, 000) when undergoing The empirical equation of Richardson and Zaki (1954) can
free settling. be applied to each particle species fluidized separately:
In order to isolate the influence of particle shape, the two
U = Ue1 n1 1 = Ue2 n2 2 , (9)
other types of particles were cut from circular cylinders to have
the same volume (Vp ) as the spheres, so that their volume- where Ue is the value of U when a linear plot of log U vs. log 
equivalent diameter was is extrapolated to =1. Assuming as a crude approximation that
 Ue /Ut is the same for all three particle shapes in the Newton
d = 3 6Vp /. (4) region, Eq. (9) can be re-written
 
From Eq. (4), the cylinder diameter (Dc ) and the cylinder length Ut2 n1 /n2
(Lc ) are related by 1 ≈  . (10)
Ut1 2
d 3 = 3Dc2 Lc /2. (5) Substituting Eq. (10) into Eq. (8),
  
The two types of cylinder were chosen to have different shapes, Ut2 1/n1 n2 /n1
but very nearly the same sphericity (), defined as the ratio of B2 − B1 ≈ (s − l ) 2 − 2 . (11)
Ut1
the surface area of the sphere of the same volume to the surface
area of the particle. For cylindrical particles this leads to By analogy to the sizing phenomenon, a reduced bulk density
difference, , can be defined, and it becomes the governing
d2 measure of the degree of particle segregation:
= . (6)
Dc Lc + 0.5Dc2
(B2 − B1 )
= =  1 − 2 (8a)
Defining k as the ratio of cylinder diameter (Dc ) to volume- (s − l )
equivalent diameter (d), Eqs. (5) and (6) reduce to  
Ut2 1/n1 n2 /n1
6k ≈ 2 − 2 . (12)
= . (7) Ut1
4 + 3k 3
The degree of segregation can be estimated from the value of
For k > 0.874, the shape corresponds to a disc (Lc < Dc ) , which clearly depends on the characteristics of the mono-
whereas k < 0.874 denotes a rod (Lc > Dc ). A range of k val- component fluidized bed expansions, and therefore on the val-
ues was considered to find where the same sphericity occurs ues of the Richardson–Zaki parameters. In general, as shown
for both disc and rod. Since the particles are cut from com- by Haider and Levenspiel (1989) for nonspherical particles, the
mercial PTFE circular cylinders, there are practical limitations terminal settling velocity decreases as the particle sphericity
to the values of Dc available. Rods and discs were then cut decreases (Ut2 > Ut1 ). In addition, the particle shape affects the
to volumes virtually identical to that of the spheres, while the expansion index n in the Stokes regime, with n increasing as
sphericities of the rods and discs were similar, as shown in the sphericity decreases (Chong et al., 1979; Dharmarajah and
Table 1. Cleasby, 1986). In the Newton regime, the expansion index has
been reported to be almost constant (Dharmarajah and Cleasby,
3. Theoretical considerations 1986). Consequently, in both regimes: Ut2 /Ut1 > 1, 2 < 1 and
n2 /n1 1. The right-hand side of Eq. (12) is therefore always
In order to predict the classification of liquid fluidized beds positive, so that particles of larger sphericity should tend to seg-
by shape (“shaping”), we adopt an approach similar to that regate towards the bottom of the column. In the Stokes regime,
initiated by Pruden and Epstein (1964) to predict the segrega- the value of the normalized bulk density difference can in-
tion of binary-size uniform-density spherical particle mixtures. crease, decrease or remain unchanged as U (and hence 2 ) is
R. Escudié et al. / Chemical Engineering Science 61 (2006) 1528 – 1539 1531

increased, depending on the values of Ut2 /Ut1 , n1 , n2 /n1 and disengagement zone, whereas it increases with distance below
2 ; thus no qualitative generalization can be drawn about the the surface of the bed. When the surface is stable and the void
expected effect of bed expansion on segregation in this regime. fraction is homogeneous in the bed, the pressure plot is linear,
However, based on the reasonable assumption that the expan- and hence it is possible to extrapolate the curve to obtain the bed
sion index is almost constant in the Newton regime (n1 ≈ n2 ), height. This was the case for the beds containing the spheres
Eq. (13) can be rewritten for this regime (in which Ut2  Ut1 and those containing the discs. For the rods, the curves were
especially for isometric2 vs. non-isometric1 particles) as linear except close to the distributor and the top bed surface,
   and the latter could be estimated by extrapolating the linear
Ut2 1/n1 portion of the curve.
 ≈ 2 −1 (13)
Ut1
4.1.2. Expansion and global hydrodynamics
so that  always increases as the bed expands. Hence more The general bed characteristics differed for each of the three
segregation should occur at higher voidages. Since the three particle species fluidized separately. For the spheres, the bed
species of particles (fluidized by water with d =dp ) in this work appeared visually to be relatively homogeneous compared to
are in the Newton regime, as noted above, Eq. (13) becomes what was later observed for the discs and the rods, and the inter-
central to this study. face was distinct and stable, regardless of the liquid flow, since
the particles were not appreciably entrained into the freeboard.
4. Results and discussion The void fractions based on all three methods are consequently
in very good agreement (Fig. 4a).
4.1. Monocomponent particle systems For the discs, the interface was less distinct, but the bed
height did not fluctuate much. For a high liquid velocity with
The three different species were first fluidized separately to  > 85%, some particles were entrained into the freeboard. The
determine their bed expansion behaviour and thus to estimate maximum liquid superficial velocity used was restricted to
the Richardson–Zaki parameters. This procedure was accom- 0.33 m/s to minimize this entrainment. As shown in Fig. 4b,
panied by observation of the flow patterns for the different par- the three techniques give small differences in the determination
ticle shapes. of the bed void fraction. The average pressure gradient method
gave poor results for the low void fractions because the number
4.1.1. Voidage measurement techniques of data points available to calculate the mean pressure gradient
Three different methods were tested to determine the voidage was too low.
within the fluidized beds of the three monocomponent particle For the rods, the particle motion differed from that of the
systems. The first was to measure the bed height visually. This other two shapes. Very large circulation loops (vortices) were
ideally requires a very clear and stable interface between the generated within the bed, and the interface was unstable and
particle swarm and the freeboard, which was the case only for oscillating. In addition, for lower liquid velocities, the bed ap-
the spheres in the present study. peared to lock periodically, and some preferential pathways
With the aid of measurements of dynamic pressure drops, two of liquid appeared, a channeling phenomenon observed also
alternative techniques were also employed. Figs. 2a–c present by Briens et al. (1997) for “angular” particles. The minimum
typical dynamic pressure gradient profiles for the spheres, discs superficial liquid velocity for the voidage measurements was
and rods, respectively. In the bed of spheres, well above the liq- therefore taken as that corresponding to the collapse of these
uid injection level, the dynamic pressure gradients are constant pathways. The voidages estimated from the visual observa-
and independent of height. The voidage can then be estimated tions and the two dynamic pressure methods differ significantly
from Eq. (2) as (Fig. 4c), undoubtedly because the visual determination is quite
−P /Z subjective due to the instability of the interface.
=1− . (14) As a result of these comparisons, the third method (extrap-
(s − l )g
olation of the linear part of the dynamic pressure curve to de-
This second method requires a large interval over which the termine the bed height) was adopted to determine the average
pressure gradient is constant, which was the case consistently voidage of both monocomponent and the subsequent binary and
for the spheres, only sometimes for the discs and never for the ternary component beds. In order to test this technique, the to-
rods. However, when the bed height and hence void fraction tal mass of solids introduced in the column was compared in all
were low, the pressure drop could only be determined from two runs with that estimated by the equation for dynamic pressure
or three pressure taps. at the bottom of the bed:
The third method was to plot the dynamic pressure (i.e., M (s − l )g
static pressure minus hydrostatic head of liquid) vs. vertical Pbottom = , (15)
s A
position to determine the height of the bed. The dynamic pres-
sures were obtained additively from measured dynamic pres- where M is the total mass of solids and A the cross-sectional area
sure drops between successive pairs of pressure taps. Figs. 3a–c of the column. As the first pressure tap is located 64 mm above
present dynamic pressure profiles along the column. In the free- the distributor, we assume that the pressure gradient between the
board section, the dynamic pressure is zero above the particle bottom of the column and the first tap is the same as between the
1532 R. Escudié et al. / Chemical Engineering Science 61 (2006) 1528 – 1539

Fig. 2. Dynamic pressure gradient profiles for the three particle shapes: (a) Spheres, U = 0.316 m/s, (b) discs, U = 0.251 m/s, (c) rods, U = 0.316 m/s.

Fig. 3. Dynamic pressure profiles for three particle shapes: (a) Spheres, U = 0.316 m/s, (b) discs, U = 0.251 m/s, (c) rods, U = 0.316 m/s.

first and the second tap. Whatever the particle species and void expansion index n is even lower for the discs and rods, with
fraction, the ratio of the mass of solids calculated from Eq. (15) values of 1.95 and 1.84, respectively. Thus, the expansion index
and the actual mass of particles introduced was within 1±0.03. in our experiments was somewhat affected by the shape of the
Therefore, it is fair to assume that there is negligible holdup particles, even in the Newton regime.
of stagnant particles between the distributor holes, and that the Pressure drop fluctuations can be useful in characterizing the
dynamic pressure profiles provide satisfactory measurements degree of instability (or turbulence) within the bed. For each
of bed voidages. bed composition the intensity percentage, Ip , of the pressure
Table 2 reports values of Ue and n obtained by fit- fluctuations at U = 0.251 m/s was determined as
ting the monocomponent expansion measurements with the 
N
i=1 (Pi − P )
Richardson–Zaki equation, 2
Ip = 100 N , (17)
U/Ue = n (16) i=1 Pi

as illustrated in Fig. 5. The index for the spheres is 2.27, close where Pi is the instantaneous pressure drop between the sec-
to results in the literature for the Newton regime (between 2.3 ond and the third pressure taps from the bottom, and N is the
and 2.4). This experimental value is also in good agreement number of data points. Table 2 summarizes the intensity of
with the correlations of Khan and Richardson (1989) and Rowe pressure fluctuations for the three particle species. The results
(1987) that predict n values of 2.41 and 2.37, respectively. The confirm the visual observation that the fluctuations for the rods
R. Escudié et al. / Chemical Engineering Science 61 (2006) 1528 – 1539 1533

Table 2
Characteristics of the monocomponent fluidized beds

Ue (m/s) n Ip (%)

Spheres 0.458 2.27 7.0


Discs 0.335 1.95 16.7
Rods 0.401 1.84 26.4

Fig. 5. Richardson–Zaki type plots based on dynamic pressure profiles: points


are experimental; lines are best fits of Eq. (16).

4.1.3. Binary-mixture segregation model


The reduced bulk density difference, , defined by Eq. (8a),
has been found to be a reasonably good quantitative indi-
cator for distinguishing between the four qualitative segre-
gation or mixing patterns of Fig. 1 (Epstein and Pruden,
1999) in the analogous sizing problem for spheres. In that
case,  < 0.015 ± 0.005 corresponds to homogeneous mixing,
0.015 ± 0.005 <  < 0.045 ± 0.015 to heterogeneous mixing,
0.045 ± 0.015 <  < 0.10 ± 0.005 to incomplete segregation
and  > 0.10 ± 0.005 to complete segregation. Fig. 6a plots
the bulk densities of the three kinds of particles fluidized sep-
arately, both with  obtained directly from the experimental
measurements and, more smoothly but more approximately,
Fig. 4. Expansion of monocomponent fluidized beds: (a) Spheres, (b) discs,
(c) rods. with  determined from the Richardson–Zaki correlation lines
of Fig. 5. Fig. 6b then shows the corresponding reduced bulk
were significantly higher than for the discs, and these in turn density differences, , for the three possible binary mixtures
were higher than for the fluidized spheres. (spheres-discs, spheres-rods and rods-discs), with the sizing
Thus, when each particle species is fluidized separately, limits for spheres of the four segregation patterns also delin-
the characteristics of the respective liquid fluidized beds dif- eated at the right. The latter provides a relatively quiescent
fer, despite the equal particle volumes and densities. For the base case against which the present less quiescent results can
spheres, pressure fluctuations are small, the interface between be compared.
the bed and freeboard is clear and stable, and the value of the
Richardson–Zaki index, n, is close to that reported in the lit- 4.2. Binary particle systems
erature. When the discs were fluidized, the instabilities within
the bed increased and the interface was less well defined. Experiments were next performed to investigate the effect of
Compared to the spheres, the terminal free settling velocity de- particle shape on the segregation in liquid-fluidized beds. The
creased because the drag on the discs was larger. For the rods, sphere ( = 1) − disc ( = 0.716) and sphere ( = 1) − rod
the pressure fluctuations were even greater and the interface  = 0.686) binary systems allow the influence of sphericity to
was most unstable. be determined, whereas the rod ( = 0.686) − disc( = 0.716)
1534 R. Escudié et al. / Chemical Engineering Science 61 (2006) 1528 – 1539

for a pressure drop measurement within the lower layer. The


occurrence of heterogeneous mixing, i.e., continuous stratifica-
tion with no interface from the bottom to the top of the bed,
could not be distinguished visually from homogeneous mixing.
Instead, use was made of the dynamic pressure profile within
the bed, as shown in Fig. 7 for the sphere-disc mixture with
Xs =0.848. In the case of a perfectly linear plot, the solids con-
centration profile along the bed height is taken to be uniform,
consistent with homogeneous particle mixing. Deviation from
linearity in the upper part of the bed is a consequence of par-
tial segregation within the bed, i.e., of continuous stratification
from bottom to top where there is no visible interface, or from
the lower interface to the top when there is a monocomponent
layer below.

4.2.1. Sphere-disc binary mixtures


As predicted by the theory for the Newton regime that as-
sumes n1 ≈ n2 (Eq. 13), as well as by the more general Eq.
(12) using the measured values of the Richardson–Zaki param-
eters, the spheres and discs segregated at high liquid superfi-
cial velocities, with a pure layer of spheres at the bottom of
the column, and a mixed layer on top. As the liquid veloc-
ity increased, the height of the pure layer increased, whereas
the height of the mixed layer decreased, as illustrated by the
changing position of the interface (shown by dotted lines) in
Fig. 7. For lower liquid velocities, separation into two distinct
Fig. 6. Framework of the segregation model: (a) Bulk density variation with
velocity of monocomponent beds, (b) reduced bulk density difference, , vs.
layers disappeared. The critical velocity above which the seg-
velocity for the three possible binaries, with the observed limits of the four regation with a mixed top transition zone (incomplete segrega-
mixing-segregation patterns for sizing of spheres shown at the right based on tion) starts is reported in Table 3 as a function of the bed com-
Epstein and Pruden (1999). position. This table also presents the superficial velocity below
which apparently homogeneous mixing occurs. This velocity
is independent of the bed composition and equal to 0.182 m/s.
binary system facilitates understanding of the shape effect be- The corresponding reduced bulk density  is 0.066 according
yond that characterized by the sphericity of the two species, to Eq. (8a), much higher than the 0.015 ± 0.005 reported in the
since the rod and disc sphericities were nearly equal. For each case of sizing of spheres. The bed composition also affected
binary, different initial compositions of the bed were used to the degree of particle agitation within the bed, as confirmed by
test the composition-dependence of the phenomena. the Ip values in Table 3, where the intensity of the pressure
Table 3 summarizes the experimental conditions and the main fluctuations (Ip ) is seen to have increased from 6.5% to 12%
results. The initial bed compositions Xs , Xd and Xr are defined as the disc concentration increased from Xd = 0.152 to 0.618.
as the ratio of the mass of the spheres, discs and rods, respec- At the same liquid velocity and at the same location, Ip was
tively, to the mass of the total particles. The initial total bed 7.0% and 16.7% for the monocomponent fluidized beds of
mass for each binary was also varied in order to maximize the spheres and discs, respectively. In other words, for the sphere-
number of pressure drop measurements. The sphere-disc binary disc mixture, the values of Ip mainly fell quantitatively between
experiments with an initial bed composition Xs of 0.650 were those of the corresponding monocomponent beds, depending
therefore performed twice with different initial bed masses of on the relative concentrations of the two species.
5.96 and 3.97 kg. Consider now the incomplete segregation pattern. The pres-
Although the three particle shapes were each coloured differ- sure fluctuations can influence the destabilization of the lower
ently, segregation could be observed visually only when a sepa- pure layer. It is, however, not possible to conclude that the
rate layer of one shape (always the spheres) formed below, with velocity above which this pattern occurs depends only on the
a heterogeneously mixed layer (i.e., a developing transition re- initial bed composition, because it varied also when the initial
gion) above; but no separate layer of the other shape at the top, mass of particles was changed with Xs held constant at 0.650.
as in Fig. 1c, was ever observed. Incomplete segregation was In fact, irrespective of velocity, the pure layer disappeared when
nevertheless reported when two layers formed with a region of the interface between the pure layer and the mixed layer was
spheres alone at the bottom. The bed height of this lower mono- close to 200 mm above the distributor: this is the height below
component layer was measured visually since the interface be- which the distributor generated instabilities. Consequently, it
tween the two layers was usually stable but its height too low appears that the distributor affects the transition between the
R. Escudié et al. / Chemical Engineering Science 61 (2006) 1528 – 1539 1535

Table 3
Experimental conditions and results for the binary-component and ternary-component fluidized beds

System Mass (kg) Initial bed composition Incomplete segregation  Homogeneous mixing  Ip (%)

Sphere-disc 4.57 Xs = 0.848 U > 0.182 m/s 0.066 U < 0.182 m/s 0.066 6.5
5.96 Xs = 0.650 U > 0.208 m/s 0.081 8.5
3.97 Xs = 0.650 U > 0.225 m/s 0.085 8.4
3.38 Xs = 0.382 U > 0.247 m/s 0.096 12.0
Sphere-rod 4.57 Xs = 0.848 U > 0.251 m/s 0.012 U < 0.251 m/s 0.012 9.1
5.96 Xs = 0.650 Intermittently U > 0.300 m/s 0.024 8.4
5.40 Xs = 0.382 No 16.2
Rod-disc 4.01 Xr = 0.831 No U < 0.219 m/s 0.095 22.1
4.98 Xr = 0.669 No 24.2
Ternary 5.27 Xs = 0.848 U > 0.229 m/s U < 0.229 m/s
Xr = 0.076
Xd = 0.076
5.27 Xs = 0.736 No All velocities
Xr = 0.132
Xd = 0.132

heterogeneous mixing and the incomplete segregation patterns.


However, the transition liquid velocity of partially mixed to par-
tially segregated beds ranged from 0.182 to 0.247 m/s, corre-
sponding to a reduced bulk density difference, , between 0.066
and 0.096. This transition zone corresponds to higher values of
 than reported in the literature for the case of sizing ( between
0.030 and 0.060 according to Epstein and Pruden, 1999).
Starting from the experimental measurements, it is possible
to estimate the liquid-free composition of the mixed layer when
incomplete segregation occurs. The quantity of spheres in the
bottom pure layer can be estimated based on the interface height
(hI ) above the distributor, assuming that this layer has the same
voidage as the monocomponent fluidized bed at the same liquid
velocity. The average sphere concentration xs within the mixed
layer is then
ms − (1 − (U/Ues )1/ns )hI As
xs = , (18)
ms − (1 − (U/Ues )1/ns )hI As + md
where ms and md are the initial masses of spheres and discs in
the bed, respectively. Fig. 8 reports the sphere composition xs
of the mixed layer for the four experiments. For U < 0.24 m/s,
the composition of the upper layer was independent of the
initial bed mass and composition, whereas xs decreased lin-
early with increasing superficial liquid velocity, indicating that
more segregation occurred for higher liquid velocities. For Fig. 7. Dynamic pressure profiles along bed for sphere-disc binary mixture
U > 0.24 m/s, there are discrepancies in xs estimated from the with Xs = 0.848. Dotted horizontal lines demarcate the segregation interface
different experiments, perhaps in response to the variation of positions.
transition velocity with the initial bed composition. Fig. 8 can
be regarded as a mixing-segregation map, with the line delineat-
ing the interface between the two patterns. Consider a sphere- not take into account the additional mixing provided by the
disc mixture with Xs = 0.4 fluidized with increasing superficial distributor near the bottom of the column. Consequently, the
liquid velocity starting from Umf . If the liquid velocity is less curve in Fig. 8 provides a limiting case to distinguish between
than about 0.24 m/s, it is not possible to have two layers with incomplete segregation and heterogeneous mixing.
a pure sphere layer at the bottom, because the composition, xs , An estimate of the degree of stratification of the incom-
of the hypothetical mixed layer would exceed 0.4. When the pletely mixed upper transition layer when the incomplete seg-
liquid velocity is just to the right of the xs vs. U curve, a pure regation pattern prevails is provided by Fig. 9, which plots both
layer of spheres forms at the bottom of the column, and xs for the measured P and corresponding  against distance above
the mixed layer would be less than 0.4. This interpretation does the distributor for the highest velocity run with Xs = 0.848.
1536 R. Escudié et al. / Chemical Engineering Science 61 (2006) 1528 – 1539

Fig. 8. Composition of mixed layer for sphere-disc binaries: mix-


Fig. 10. Overall bed voidages (points) compared to serial model predictions
ing-segregation map. Open and filled squares for Xs = 0.650 correspond to
(lines) for sphere-disc binaries. Open and filled squares for Xs = 0.650
M = 3.97 and 5.96 kg, respectively.
correspond to M = 3.97 and 5.96 kg, respectively.

the serial model predicts that


1 X1 1 − X1
= + , (19)
1 −  1 − 1 1 − 2
where  is the overall voidage of the binary-species bed, X1 the
fluid-free volume fraction of species 1 in the total bed, 1 and
2 the voidages of species 1 and 2 when they are each fluidized
alone in the same column at the same superficial liquid velocity.
Fig. 10 compares the experimental and the predicted voidages.
The voidage of each individual particle species is calculated
using the Richardson–Zaki parameters reported in Table 2. The
agreement of the serial model with the present binary-mixture
experiments is quite good.
Fig. 9. Dynamic pressure profile for the sphere-disc binary at the highest
velocity with Xs = 0.848, and the corresponding voidage profile.
4.2.2. Sphere-rod binary mixtures
Table 3 presents the transition velocities between the three
The voidage  at any level was obtained by applying Eq. (2) patterns: homogeneous mixing, heterogeneous mixing and
to the P vs. Z plot, with −dP /dZ replacing −P /Z. The incomplete segregation, for the sphere-rod binary mixtures.
figure shows a gradual voidage increase above the interface Incomplete segregation occurred only for superficial liquid
from  = 0.767, the monocomponent sphere voidage for the velocities exceeding 0.251 m/s with Xs = 0.848. When Xs
lower fully segregated layer, to  = 0.857 at the top of the was decreased to 0.650, incomplete segregation was observed
bed. Since the monocomponent disc composition at the same intermittently, but only for U > 0.300 m/s. For Xs = 0.382,
superficial velocity was 0.864, it is apparent that transition to no bottom segregation could be observed for any of the liquid
a fully segregated disc layer at the top was being approached. velocities tested. Given the reduced bulk density difference
The slight rise in voidage towards the bottom of the bed can be plot in Fig. 6b, it is not surprising that segregation was more
attributed to distributor disturbance. restricted for the sphere-rod mixture than for the sphere-disc
The overall bed voidage is plotted in Fig. 10 against the mixture. The sphere concentration within the mixed layer, xs ,
superficial liquid velocity for all binary experiments and the is computed only for Xs = 0.848 (Fig. 11). Its concentration
monocomponents. The overall binary voidages clearly lie be- is between 0.7 and 0.8, much higher than for the sphere-disc
tween those of the two corresponding monocomponent beds. mixtures, demonstrating the smaller extent of segregation for
Experiments with the same bed composition (Xs = 0.650) but the sphere-rod mixtures.
different initial masses are in good agreement. The experimen- The transition between homogeneous and heterogeneous
tal overall voidages can also be compared to the predictions mixing is again independent of the initial bed composition. The
of the “serial model” (Epstein et al., 1981). In this theory, the critical velocity is 0.251 m/s, which corresponds to  = 0.012,
overall bed expands as if each type of particle acts indepen- a value that is comparable to  = 0.015 ± 0.005 for sizing
dently of the other, whatever the degree of segregation. The se- of spheres. The serial model gives accurate predictions of the
rial model does not take into account any possible contraction overall bed voidage at different velocities for the three different
due to mixing of different species. In the case of a binary bed, compositions, as shown in Fig. 12.
R. Escudié et al. / Chemical Engineering Science 61 (2006) 1528 – 1539 1537

Fig. 11. Solids composition of mixed layer for sphere-rod binary with Fig. 13. Overall bed voidages (points) compared to serial model predictions
Xs = 0.848. (lines) for rod-disc binaries.

bulk density difference theory given by Eq. (12), particles of


higher sphericity tend to segregate to the bottom of the bed. In
addition, as expected from the theory, the segregation tendency
increases in the Newton regime (Eq. 13) with increasing su-
perficial liquid velocity. However, even if the sphericity is the
same for two different shapes of particles, aspects of the shape
not uniquely defined by the sphericity can affect segregation.
The rods and the discs have almost the same sphericity (0.686
and 0.716, respectively, Table 1), but the mixing-segregation
phenomena differ for the sphere-rod and sphere-disc binaries.
Particles of the same volume and sphericity (rods and discs)
can also segregate, at least partially (e.g. in the heterogeneous
mixing mode). Thus the sphericity is insufficient to account for
Fig. 12. Overall bed voidages (points) compared to serial model predictions the tendency of differently shaped particles to segregate. Recent
(lines) for sphere-rod binaries. work by Tran-Cong et al. (2004) also indicates that sphericity
is not the most appropriate shape factor for predicting settling
behaviour of non-spherical particles. They demonstrated that a
4.2.3. Rod-disc binary mixtures combination of two shape factors (particle circularity and ra-
For binary mixtures of rods and discs, no segregation was tio of spherical-surface-equivalent to volume-equivalent-sphere
ever observed, in spite of the expectation, considering the range diameter) is required, along with the projected diameter, to de-
of reduced bulk density difference plotted in Fig. 4, that the scribe the effect of particle shape on the hydrodynamic drag
rods and discs might segregate more sharply than the sphere- coefficient.
rod mixtures. Indeed, the index  for the rod-disc binary falls The model based on the reduced bulk density difference is
within the range at which incomplete segregation starts for the helpful to predict whether or not a binary system segregates
sphere-disc binary. The hydrodynamics of the rod-disc mix- or mixes, because only the expansion characteristics of each
ture differed radically from that of the sphere-disc mixture. The monocomponent fluidized bed is required to compute it. How-
pressure fluctuation intensity, Ip , was close to 26.4%, the value ever, it does not take into account the mixing effect that can
for the rod monocomponent bed (see Table 2). This level of be generated by some non-isometric shapes such as the rods.
fluctuations was generated by vigorous circulation within the In the present study, the voidage fluctuations (manifested as
bed that promoted mixing of the particles. The transition be- pressure fluctuations) are important when the concentration of
tween homogeneous and heterogeneous mixing occurred at a rods is high in a binary system. As a consequence, even if the
superficial liquid velocity of 0.219 m/s, which corresponds to reduced bulk density differences are close for the sphere-disc
a reduced bulk density difference  of 0.095, much higher than and rod-disc mixtures, mixing is more efficient for the rod-disc
for sizing of spheres. The serial model again gives good pre- binary because the voidage fluctuations are higher.
diction of the overall voidage, as shown in Fig. 13.
4.3. Ternary particle mixtures
4.2.4. Discussion
We have shown that particle classification by shape can oc- The three kinds of particles were finally mixed to obtain
cur in solid–liquid fluidized beds. As predicted by the reduced a sphere ( = 1)-disc ( = 0.716)-rod ( = 0.686) ternary
1538 R. Escudié et al. / Chemical Engineering Science 61 (2006) 1528 – 1539

Notation

A cross-sectional area of column, m2


Ar Archimedes number defined by Eq. (3),
dimensionless
Ci volumetric concentration of solid species i,
kg m−3
d volume-equivalent sphere diameter, m or mm
dp diameter of spherical particles, m or mm
D inner diameter of column, m
Dc cylinder (disc or rod) diameter, m or mm
Di axial diffusion coefficient of solid species i,
m2 s−1
Fig. 14. Overall bed voidages (points) compared to serial model predictions g gravitational acceleration, m s−2
(lines) for sphere-disc-rod ternaries. hi vertical distance between distributor and
segregation interface, m
Ip intensity of pressure fluctuations, %
system. Two different initial bed compositions were tested: k ratio of cylinder diameter to volume-
Xs =0.848, Xr =Xd =0.076 and Xs =0.736, Xr =Xd =0.132. equivalent sphere diameter, dimensionless
Table 3 summariszes the main results of these experiments. A Lc cylinder (disc or rod) length, m or mm
segregation pattern with a pure layer of spheres at the bottom of ms , md mass of spheres and discs, respectively,
the column and a ternary-component mixed layer at the top was in the bed, kg
observed only for the case where the sphere volume fraction M total mass of particles, kg
in the total bed solids was 0.848, and this segregation occurred n Richardson–Zaki expansion index,
only for U > 0.229 m/s. The liquid-free fraction of spheres in dimensionless
the mixed layer can be estimated to be higher than 0.77, similar N number of data points in Eq. (22),
to that for the sphere-rod binary in Fig. 11. For the ternary, the dimensionless
heterogeneous mixing pattern, characterized by a continuous P dynamic pressure, Pa
stratification from top to bottom, was never observed, and con- Pbottom dynamic pressure at bottom of bed, Pa
sequently only two patterns were noted: homogeneous mixing U superficial liquid velocity, m s−1
and incomplete segregation. The Ue value of U when a linear plot of log U vs.
serial model, Eq. (19) with
the right-hand side changed to 3i=1 Xi /(1 − i ), is once more log  is extrapolated to  = 1, m s−1
able to predict the total void fraction from the bed character- Upi segregation velocity of species i, m s−1
istics of each particle species fluidized separately, as shown Ut terminal free-settling velocity, m s−1
in Fig. 14. VP particle volume, m3
xs volume fraction of solids that are spheres within
the mixed layer, dimensionless
5. Conclusions
Xi liquid-free volume fraction in bed of particle
species i, dimensionless
Particles of different shapes can segregate in fluidized
Z vertical coordinate, m
beds, even when they have the same volume and density.
Sphericity is not adequate for distinguishing the onset or
degree of segregation between different binary systems. Greek letters
Turbulence enhancement over that for the spheres, as mea-
sured by the intensity of the pressure fluctuations, was
greater for the rods than for the discs, despite their similar  reduced bulk density difference
sphericities, so that the segregation tendencies of the three (B2 − B1 )/(s − l ), dimensionless
binaries decreased in the following sequence: sphere-disc, Pi instantaneous pressure drop, Pa
sphere-rod, rod-disc. The method of Pruden and Epstein  overall voidage, dimensionless
(1964), whereby the degree of segregation in a binary mix- i overall voidage of the monocomponent
ture depends on the difference in bulk densities of the fluidized bed of particle species i, dimensionless
two component species, is shown to give good qualita-  viscosity of liquid, kg m−1 s−1
tive predictions for teflon particles of three shapes flu- Bi bulk density of monocomponent fluidized
idized by water within the Newtonian regime. The overall bed of particle species i, kg m−3
bed expansions for binary and ternary mixtures of spheres, l density of liquid, kg m−3
discs and rods are well predicted by the “serial model” s density of solid particles, kg m−3
of Epstein et al. (1981).  sphericity, dimensionless
R. Escudié et al. / Chemical Engineering Science 61 (2006) 1528 – 1539 1539

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