Chemical Engineering Science 56 (2001) 109}119

A fundamental approach to the phenomenology of #uidization of size

segregating binary mixtures of solids
B. Formisani*, G. De Cristofaro, R. Girimonte
Dipartimento di Ingegneria Chimica e dei Materiali, Universita% della Calabria, I 87030 Arcavacata di Rende (Cosenza), Italy
Received 3 June 1999; received in revised form 14 August 2000; accepted 31 August 2000

Abstract

The paper reports an experimental study of the #uidization behaviour of mixtures of two solids di!ering in size at various average
compositions. The segregation phenomena accompanying the onset of the #uidized state are analysed and the relevance of the
composition pro"le of the binary bed to the de"nition of its minimum #uidization velocity is discussed. It is demonstrated that the
recognition of the dependence of bed voidage and particle average diameter on mixture composition is the essential condition for
getting over current empirical approaches to segregating #uidization and for restoring the predictive ability of theoretical equations.
To this purpose, Carman}Kozeny equation is rewritten in a di!erential form suitable for the peculiar characteristics of
two-component systems. The good agreement with experimental data indicates that the extension of the fundamental approach from
monodisperse to binary beds greatly reduces the number of independent variables to be dealt with in the study of segregating
#uidization of dissimilar solids. The evolution of bed composition pro"les from the "xed to the fully #uidized state, where the gas drag
force "rst balances the particulate bed weight, makes clear that full #uidization is constantly associated to the achievement of
practically thorough mixing. It can therefore be assumed that component segregation is not a distinctive property of binary
#uidization, rather it is the sign of its incompleteness.  2001 Elsevier Science Ltd. All rights reserved.

Keywords: Fluidization; Mixing; Segregation; Packed bed; Solid mixtures; Voidage

1. Introduction a steady distribution of mixture components along the

Simultaneous treatment of dissimilar materials is nor-
mally encountered in a fairly large number of industrial
applications of gas}solid #uidization technology
(Nienow & Chiba, 1985). Both in the case of chemical
conversions and of physical operations, the presence of
two or more solids, di!ering in one or more of their
constitutive properties, is often requested by some speci-
"c characteristic of the process; in other situations, hav-
ing to deal with a multicomponent solid charge may
quite be the real reason for resorting to #uidization as the
most e$cient mode for #uid}particle contact.
A well-known feature of #uidized beds of solid mix-
tures is that they usually are strongly a!ected by segrega-
tion phenomena. Whenever an assembly of particles with
more than one density or size (or also, at some extent,
shape) undergoes #uidization, a peculiar mixing/segrega-
tion equilibrium is rapidly reached. This gives rise to
* Corresponding author. Tel.: 39-984-492037; fax: 39-984-492058.
E-mail address: bruno.formisani@unical.it (B. Formisani).
bed height which depends both on constitutive particle
properties and on the whole set of operative and geomet-
ric conditions of the process. From one extreme to an-
other, the system may be formed by a unique well-mixed
phase or by distinct layers of each of the solid species, but
more frequently an intermediate component distribution
is observed. In principle, either limit condition is able to
provide speci"c advantages: a high degree of mixing may
be required for achieving the homogeneity of products or
the easiness of process control, whereas solid separation
can be bene"cial for locating staged chemical or physical
operations in distinct regions of the #uidized bed or for
discharging solids separately at di!erent heights in the
plant.
The ability to predict or regulate the extent of mixing
or strati"cation of a given mixture is, therefore, an impor-
tant concern for industrial operations. Accordingly, and
particularly for the case of size segregating systems which
constitute the subject of this study, a remarkable research
e!ort to achieve a clear picture of their #uidization be-
haviour has been made by many groups in the last two

0009-2509/01/$ - see front matter  2001 Elsevier Science Ltd. All rights reserved.
PII: S 0 0 0 9 - 2 5 0 9 ( 0 0 ) 0 0 4 2 6 - 7
110 B. Formisani et al. / Chemical Engineering Science 56 (2001) 109}119
decades. In spite of that, it must be remarked that al-
though the e!ects of segregation phenomena have been
widely described, their mechanisms are still somewhat
obscure, so that the few prediction tools to date available
(Cheung, Nienow, & Rowe, 1974; Nienow, Rowe,
& Cheung, 1978) are essentially empirical. The apparent
complexity of the problem is attributable to the large
number of factors that are reported to a!ect the mixing
pattern of the system; moreover, it is not clear how and at
what extent the theory of #uidization developed for
monodisperse beds can be adapted to a multicomponent
system. Indeed, the latter aspect of the problem has too
often been neglected, and this may perhaps explain the
lack of generality of many results and relationships so far
proposed.
Moving from these considerations, and out of the
empirical approach generally followed in most of the
available literature, this paper tries to identify and out-
line the role of some of the particle properties and of the
operative variables that have a major in#uence on the
#uidization behaviour of size segregating systems; to this
purpose, it illustrates and discusses experiments per-
formed on equidensity binary mixtures, in each of which
a limited number of parameters is let change. Through
the use of spherical solids, which permits to avoid pos-
sible errors connected to the determination of particle
shape factors, it also attempts to demonstrate that some
of the basic relationships of #uidization fully keep their
validity when the peculiar nature of two-component beds
is correctly accounted for.
2. Experimental equipment, procedure and materials
All the experiments of this study have been performed
in a 10.1 cm ID perspex #uidization column, equipped
with a high-pressure drop porous gas distributor.
Fluidizing air #ow rates were regulated by a set of
rotameters and total pressure drop across the particulate
bed was measured by a pressure tap located just above
the distributor level, connected to an electronic
transducer; occasionally, a U-tube water manometer, in
parallel to the transducer, was used. A vertically sliding
pressure probe was used for measuring the axial pressure
pro"le in the bed.
Bed heights were evaluated by averaging the values
read on three graduated scales put at 1203 around the
column wall, and then used for determining bed void
fractions.
A solenoid valve on the feed line was employed to cut
the air #ux o! instantaneously, thus `freezinga the partic-
ulate bed in the mixing state associated to a given steady
#uid dynamic condition; subsequently, the solid was gen-
tly drawn from the top of the column by means of
a vacuum device, in horizontal layers of particles gener-
ally 2 cm thick (or 1 cm thick, when a higher resolution
was needed). Each of these layers was then sieved to
measure, by weighing, the mass fraction of either solid
component, and its void fraction was also determined.
Both voidage and concentration values were then refer-
red to the average height of the relevant layers and used
to trace the respective pro"les in function of height.
Owing to the absence of free "ne percolation after the
interruption of the gas #ow, the technique employed,
used by many research groups (Nienow et al., 1978;
Geldart, Baeyens, Pope, & Van de Wijer, 1981; Rice
& Brainovich, 1986; Wu & Baeyens, 1998 and many
others) and widely accepted in the "eld, is able to ensure
reliable results.
Three closely sieved samples of glass ballotini having
a density of 2.53 g/cm and an average Sauter diameter,
respectively, of 499, 271 and 172 lm (with size distribu-
tions, respectively, in the range 350}700, 200}375 and
125}225 lm) carefully checked by a Sympatec Helos
laser di!raction analyser, were used to obtain two types
of binary mixtures, hereafter indicated as GB499-GB172
and GB499-GB271. Minimum #uidization velocities of
the three components, determined in preliminary experi-
ments, were, respectively, equal to 21.1, 6.5 and 3.5 cm/s.
For each mixture, three di!erent average compositions,
corresponding to x "0.25, 0.50 and 0.75, were pre-
D
pared, so that the behaviour of six binary systems in all
was studied.
With the exception of the measurements devoted to the
study of the in#uence of bed height on segregation, all the
experiments were carried out with beds of 2 kg of solids,
a mass that corresponds to bed aspect ratios H/D nearly
equal to 1.7.
3. Results and discussion
The analysis of the #uidization properties of a binary
mixture undergoing segregation by size presents, as a "rst
di$culty, the problem of adopting a proper de"nition of
its minimum #uidization velocity. As in the case of mono-
disperse beds, the parameter u not only quantitatively
KD
indicates the amount of drag force needed to attain solid
suspension in the gas phase, but also constitutes a refer-
ence for the evaluation of the intensity of the #uidization
regime at higher velocity levels. Owing to the fact that the
onset of #uidization is always accompanied by that of
segregation phenomena, the de"nition of the minimum
#uidization velocity of a binary mixture is not obvious,
and has to be discussed in the light of the speci"c charac-
teristics of the system.
In particulate systems formed by two narrow cuts of
spheres of the same material, percolation of the "ne
component through the packed bed of the coarse one
cannot have place if the diameter ratio d /d is higher
D A
than a limiting value that depends on the degree
of looseness of the coarse packing. Simple geometric
 B. Formisani et al. / Chemical Engineering Science 56 (2001) 109}119
considerations indicate that the theoretical limit for in-
terstitial penetration of "nes is given by d /d "0.41, that
D A
corresponds to the most open, cubic coarse structure
(Rowe, Nienow, & Agbim, 1972); anyway, in all practical
cases the coarse sphere packing is random and conse-
quently the d /d value that "xes the percolation limit is
D A
somewhat lower and has to be determined experi-
mentally. Whenever the "ne-to-coarse size ratio is su$-
ciently high to exclude the possibility of "ne percolation,
the #uidization pattern of the mixture is found to be
strongly a!ected by the axial distribution of either solid,
so that its minimum #uidization velocity cannot be
de"ned on an absolute basis, but only with reference
to a particular state of mixing of the two-component
system.
3.1. The onset of yuidization in segregated and well-mixed
beds
At the beginning of a #uidization experiment, the bi-
nary system can be charged into the column in di!erent
Fig. 1. Pressure drop versus super"cial gas velocity (at increasing gas #ow rate) for initially mixed/segregated mixtures. De"nition of experimental
values of u ,u and u .
KD+ KD1 DD
111
ways: the "xed-bed arrangement may be that of a
well-mixed assembly of particles, of two completely
segregated layers of each component (in either order) or
may represent any other intermediate situation. For
GB499-GB271 and GB499-GB172 mixtures, with the
"ne component initially on the top for the segregated
case, Fig. 1 shows that when the super"cial gas velocity is
gradually increased, quite di!erent patterns of growth of
the total bed pressure drop are obtained.
The separation of the two experimental curves re#ects
the substantial di!erence existing in the way that leads to
the onset of #uidization in a totally segregated system
and in a well-mixed one: in the former case, the voidage
of each of the two-particle layers is practically una!ected
by the presence of the other, so that, as long as the whole
bed is "xed, the total pressure drop is expected to be close
to the sum of those of the two monodisperse beds in
series. By gradually increasing the gas #ow rate, the
underlying coarse layer acts as a passive gas distributor
for the upper "ne bed which "rst reaches incipient #uidiz-
ation and then rapidly enters the bubble regime. Beyond
112 B. Formisani et al. / Chemical Engineering Science 56 (2001) 109}119

Table 1
Characteristic velocities of experimental mixtures

Mixture d /d Experimental Calculated u

D A DD
(dimensionless) (cm/s)
u u u u u u
KD1 KD+ KD KD1 KD+ KD
(cm/s) (cm/s) (cm/s) (cm/s) (cm/s) (cm/s)

GB499-GB172
x "0.25 8.88 4.37 8.09 8.87 5.09 7.95 12.3
D
x "0.50 0.345 4.99 2.90 5.04 5.61 2.76 4.73 9.3
D
x "0.75 3.33 2.43 3.59 4.10 2.38 3.76 8.8
D
GB499-GB271
x "0.25 12.19 10.14 12.81 13.68 10.43 14.19 15.2
D
x "0.50 0.543 9.78 7.49 10.13 11.06 7.73 10.61 14.2
D
x "0.75 7.18 6.68 8.19 8.92 6.64 9.38 13.9
D

this point, which is marked by a clear change of slope of
*p versus u curve, the progressive rise of gas velocity
leads to coarse particle #uidization, which takes place
with the "ne weight already fully balanced by gas drag
and is followed by the gradual mixing of the two solid
species. Finally, when full #uidization velocity, u , is
DD
reached, total pressure drop no longer grows and the bed
is well mixed and vigorously bubbling. Experimental
values of u are given in Table 1.
DD
Following what is commonly done for any monodis-
perse bed of particles, the experimental minimum
#uidization velocity is normally assumed as the u value
corresponding to the intersection of the "xed-bed pres-
sure drop line with the horizontal line representing the
#uidized state (Chiba, Chiba, Nienow, & Kobayashi,
1979; Thonglimp, Hiquily, & Laguerie, 1984; Noda,
Uchida, Makino, & Kamo, 1986). Thus, for any given
mixture of equidensity solids, the segregated bed case
provides, as shown by Fig. 1, the upper limit of the range
of variation of minimum #uidization velocity, indicated
in this paper as u . On the other hand, the case of the
KD1
well-mixed bed is the one that "xes the lower boundary
of the minimum #uidization velocity "eld, here indicated
as u . Whatever its average composition, when the
KD+
mixture is charged as a homogeneous assembly of par-
ticles, its "xed bed voidage as well as its minimum #uidiz-
ation voidage is lower than that of each of its single
components (Yu & Standish, 1987). For this kind of
systems, the onset of the #uidized state is gradual: a front
of #uidization is observed which travels from the top to
the bottom of the particulate bed, starting at a velocity
always intermediate to u values of its single compo-
KD
nents. At any gas velocity higher than u , an increas-
KD+
ingly smaller part of the bed, located at its bottom, is left
mixed bed not yet touched by the #uidization front. The
presence of such a de#uidized layer acts as a temporary
obstacle to the progress of #uidization, which is therefore
stopped until the gas #ow rate is furtherly increased;
because of that, the *p versus u curve of a well-mixed
binary system often exhibits a characteristic
`saw-tootheda shape. Once that super"cial gas velocity
eventually equals u , the whole particulate mass is sup-
DD
ported by the #owing gas and bubbling takes place
throughout its height.
3.2. The prediction of u and u by modixed forms of
KD1 KD+
Carman}Kozeny equation
Both for the case of segregated and of well-mixed
binary mixtures, graphs of Fig. 1 clearly show that none
of the six systems under examination can be considered
as fully suspended in the gas stream when the super"cial
gas velocity is equal to u . As a matter of fact, it is only
KD
at a higher value of u, that corresponds to the full #uidiz-
ation velocity u , that the total pressure drop really
DD
equals the buoyant weight of the whole bed, so that it can
well be said that both u and u are but "ctitious
KD1 KD+
values of the incipient #uidization velocity. Notwith-
standing that, the problem of predicting such character-
istic velocities is of some importance, as it illustrates how
classical equations of #uidization can be modi"ed to
account for the binary nature of the system.
Similar to what was done by Chiba et al. (1979), when-
ever the #uidization process takes place in the viscous
regime, as in the case of all of the mixtures of this study,
Carman}Kozeny equation can be written, for an initially
segregated mixture, in the form

 
in the "xed state, and #uidization of the "ne component (1!e ) H (1!e ) H
180k u AKD A# DKD D
located in the upper portion is accompanied by compon- E KD1 e d e d
ent segregation; thus, a layer rich in de#uidized coarse AKD A DKD D
particles is normally found between the "ne bubbling (m #m )g
" A D (1)
layer in the superior zone and that part of the originally A
 B. Formisani et al. / Chemical Engineering Science 56 (2001) 109}119 113

and be used for predicting u . For all the mixtures

KD1
investigated, the comparison between experimental and
calculated values of u is presented in Table 1.
KD1
For u(u , lines obtained by equating *p to the
KD1
left-hand side of Eq. (1) are reported in Fig. 1: as long as
mixtures keep their fully segregated arrangement, the
agreement with experimental data is rather good, al-
though a certain tendency to underestimate the pressure
drop is observed. Such deviations can be explained if one
considers that Eq. (1) merely adds up the contributions of
the two beds, calculated separately, to the total pressure
drop, without accounting for the existence of an interface
between them; actually, in the region of the contact plane,
"ne particles tend to "ll the coarse interparticle voids, Fig. 3. Voidage of the well-mixed mixture (poured or fastly de-
with a strong reduction of local voidage that gives rise to #uidizated) versus "ne-component average fraction.
a perceptible increase of pressure drop. Such an e!ect can
be demonstrated by plotting in function of u, as done in mixed binary mass yields voidages lower than those
Fig. 2, a series of experimental lines of *p, relevant to obtained by abruptly stopping full #uidization by means
"xed beds made of 2, 4 and 6 alternate layers, i.e. with 1, of the solenoid valve. Accordingly, the interpretation
2 and 3 "ne-on-coarse interfaces: a gradual increase of *p given below of #uidization experiments which start from
versus u slope is observed, from the base line relevant to the poured bed state, utilizes the curves determined with
the sum of the *p's measured for each layer in separate the former procedure.
experiments, up to the maximum slope characteristic of Given the homogeneous nature of the particle assem-
the mixed bed. bly, the prediction of u can be obtained by writing
KD+
As regards well-mixed mixtures, since it is practically Carman}Kozeny equation in the form (Formisani, 1991)
impossible to measure their height right at their min- k (1!e ) (m #m )g
imum #uidization point, where they begin to undergo 180 E u KD+ " A D , (2)
d KD+ e A
size segregation accompanied by some bubbling, the ex-  KD+
perimental dependence of e on x has been assumed in which the average particle diameter, de"ned in such
KD+ D
to be the same of that of e . As in the case of monodis- a way as to provide the same drag surface for the #uidiz-
+
perse beds of particles belonging to Geldart's B group, ing gas, is given, as the solid component density is the
this approximation introduces a negligible error in calcu- same, by the relationship
lations, since no signi"cant expansion occurs in the 1 x 1!x
transition from the packed to the incipiently #uidized " D # D (3)
d d d
state.  D A
Both for GB499-GB172 and GB499-GB271 mixtures, and e is read from the lower couple of curves of
KD+
Fig. 3 reports two distinct sets of experimental values Fig. 3; similar to what was done for u , experimental
KD1
of e at varying x , because these curves are, and calculated values of u are reported in Table 1.
+ D KD+
albeit repeatable, sensitive to the experimental method Reverting to Fig. 1, it can be seen again that rather
followed; actually, carefully pouring into the column the accurate predictions of *p are obtained from Eq. (2) as
long as the arrangement of the mixed bed is not de-
stroyed by the onset of segregation.

3.3. Dexnition of a repeatable minimum yuidization velo-

city

Although useful for individuating the limits of vari-

Fig. 2. Pressure drop versus super"cial gas velocity (at increasing
gas #ow rate) for segregated "xed beds with various "ne-on-coarse
interfaces.
ation of u , both the de"nitions of minimum #uidization
KD
velocity so far examined are referred to extreme initial
states of mixing, quite di!erent from those spontaneously
assumed by the mixture under the action of the #uidizing
gas. Similarly, any intermediate initial state of mixing
gives rise to a peculiar *p versus u curve, so that it can be
said that in experiments conducted at increasing gas #ow
rate any binary system of given average composition
x exhibits as many values of its minimum #uidization
D
114 B. Formisani et al. / Chemical Engineering Science 56 (2001) 109}119
Fig. 4. Pressure drop versus super"cial gas velocity at decreasing gas
velocity for various average compositions. Mixture: GB499-GB172.
Fig. 5. Pressure drop versus super"cial gas velocity at decreasing gas
velocity for various average compositions. Mixture: GB499-GB271.
velocity as it has packed bed composition pro"les, also if
all pressure drop curves eventually converge to the same
point at full #uidization velocity u . Although this e!ect
DD
is not clearly visible in diagrams of Fig. 1, for any couple
of solids, u is found to decrease when the average
DD
fraction of "nes x is increased.
D
When, instead, the determination of u is made at
KD
decreasing gas #ow rate starting from the fully #uidized
regime, as generally advised also for monodisperse beds,
any mixture gradually reverts to the "xed state along
a repeatable pressure drop path which is characteristic of
its average composition x . Such curves are reported in
D
Figs. 4 and 5, respectively, for GB499-GB172 and
GB499-GB271 systems. Once that the mixture has reach-
ed its state of repose, any subsequent #uidization}de#ui-
dization cycle follows this very pressure drop locus, so
that its u remains, since then on, unvaried.
KD
Given the close connection between total bed pressure
drop and component distribution in the binary bed, the
existence of a characteristic dependence of *p on u im-
plies that also the axial composition pro"le of x ob-
D 180k u
tained at the end of a slow de#uidization process starting
Fig. 6. Fine-component fraction versus height in the "xed bed at the
end of a slow de#uidization process for various average compositions.
Mixture: GB499-GB172.
Fig. 7. Fine-component fraction versus height in the "xed bed at the
end of a slow de#uidization process for various average compositions.
Mixture: GB499-GB271.
from u has to be repeatable as well. That is con"rmed
DD
by experiments, and curves of x in function of h, given in
D
Figs. 6 and 7 for the two systems investigated, really
prove repeatable and dependent only on mixture com-
position x .
D
Understanding the mechanism through which de#ui-
dization spontaneously gives rise to these sigmoidal mix-
ing pro"les is not easy, and a better description of it will
be given later on in this paper. Anyway, once that the
x versus h curve in the packed bed has been determined
D
experimentally, it is possible to predict the value of the
minimum #uidization velocity it repeatably corresponds
to. Bearing in mind that any change of x along the
D
vertical axis implies a consequent variation both in local
voidage, according to the higher couple of curves of
Fig. 3 (relevant to the procedure of sudden de#uidiz-
ation), and in local average particle diameter, to be cal-
culated by Eq. (3), Carman}Kozeny equation can be
written in the form

''(1!e ) (m #m )g
KD+ dh" A D (4)
E KD d e A
  KD+
 B. Formisani et al. / Chemical Engineering Science 56 (2001) 109}119 115

Fig. 8. Pressure drop versus height in the "xed bed. Mixture: GB499- Fig. 9. Fine-component fraction versus height at full #uidization for
GB172. x "0.25; u"1.4 cm/s. various average compositions. Mixture: GB499-GB172.
D

in which e and d are functions of height h, and

KD+ 
solved numerically to determine u . As done in the
KD
other cases, calculated values of u are reported in
KD
Table 1 and compared with the relevant experimental
results. The agreement between lines of *p obtained from
the left-hand side of Eq. (4) and experimental data of
Figs. 4 and 5 is good for all of the six mixtures investi-
gated. The same equation, written for the "xed bed as


F (1!e )
*p"180k u + dh (5)
E d e
  +
with e and d functions of height h, can be integrated
+ 
at varying h in order to obtain the pressure pro"le in
the packed binary bed. An example of that is given in
Fig. 8 for the GB499-GB172 mixture with x "0.25; the
D
small experimental di!erence between the total pressure
drop at h"H and bed weight per unit section causes
a small error (about 8%) which does not exceed, anyway,
that ordinarily found also for monosize particle systems.
3.4. Full yuidization state and minimum bed aspect ratio
Whenever the velocity of the gaseous stream is equal
or higher than u , as individuated by the equality be-
DD
tween bed pressure drop and buoyant weight of the
whole particulate mass, the #uidization regime provides,
as a distinctive feature, practically homogeneous mixing
of the two solid components throughout the bed. With
the exception of two small regions, one located just above
the gas distributor, the other at the top of the bed, where
a certain predominance, respectively, of coarse and of
"ne particles is normally found, component distribution
along the bed height keeps constantly close to its average
value.
Pro"les of x , plotted in Figs. 9 and 10, respectively,
D
for GB499-GB172 and GB499-GB271 mixtures, are
stable to any further increase of gas velocity over the full
#uidization treshold, which just promotes the growth of
bubble #ow. The existence of the two aforementioned
regions is probably due to the fact that close to the
Fig. 10. Fine-component fraction versus height at full #uidization for
various average compositions. Mixture: GB499-GB271.
distributor plane "nes are more easily swept away by
local peaks of gas velocity, whereas at the top of the bed
the mechanism of capture of "ne particles in the interstiti-
ces of coarse sphere bulk is not as e!ective as elsewhere,
so that a thin layer of almost pure "nes is always found.
It has to be remarked, anyway, that even at full #uidiz-
ation velocity the condition of homogeneous mixing is
achieved only if the #uidized bed is not too shallow, i.e.
only over a certain value of the bed aspect ratio H/D. To
this purpose, Figs. 11 and 12, referred to mixtures with
x "0.5, report axial pro"les of "ne-component frac-
D
tion at various H/D; it can be observed that the height of
the region above the distributor dominated by the tend-
ency to segregation does not vary, so that its relative
importance rapidly decreases as the bed aspect ratio
becomes increasingly higher. At the same time, the thick-
ness of the "ne layer in the superior zone of the bed is
practically negligible.
3.5. The transition from the full yuidization regime to the
xxed bed state
Accurate experiments on each of the mixtures
of this study have been devoted to achieve a better
116 B. Formisani et al. / Chemical Engineering Science 56 (2001) 109}119
Fig. 11. Fine-component fraction versus height at full #uidization for
various bed aspect ratios. Mixture: GB499-GB172. x "0.50.
D
Fig. 12. Fine-component fraction versus height at full #uidization for
various bed aspect ratios. Mixture: GB499-GB271. x "0.50.
D
understanding of the mechanism of segregation. At pro-
gressively decreasing gas #ow rate, along the transition
from the fully #uidized regime back to the packed state,
the x pro"le measured in the particulate mass with the
D
`freezinga technique illustrated in Section 2 gradually
changes, reverting from the state of thorough mixing to
the characteristic composition curves already shown in
Figs. 6 and 7. Two series of curves of x versus h,
D
respectively, relevant to GB499-GB172 with x "0.25
D
and to GB499-GB271 with x "0.50, are reported in
D
Figs. 13 and 14. These plots, in which values of u repres-
ent #uidization velocities at the moment of air #ux inter-
ruption, show that for each binary system the decrease of
gas velocity is accompanied by the progressive de#uidiz-
ation of the coarse component, which sinks together
with a certain amount of "nes; that causes the gradual
reduction of the well-mixed region of the bed, which
becomes increasingly richer in the "ne component.
As gas velocity is gradually reduced, a de#uidization
front travels from the bottom to the top of the column
and the "xed bed builds up at the column base by
a mechanism of addition of de#uidized layers richer and
Fig. 13. Fine-component fraction versus height at various super"cial
gas velocities (slow de#uidization and `freezinga of the bed). Mixture:
GB499-GB172. x "0.25.
D
Fig. 14. Fine-component fraction versus height at various super"cial
gas velocities (slow de#uidization and `freezinga of the bed). Mixture:
GB499-GB271. x "0.50.
D
richer in "nes; in this way an increasingly larger portion
of the bed composition pro"le assumes the ultimate as-
pect of the x versus h curves of the "xed bed, already
D
shown in Figs. 6 and 7. Such a mechanism is consistent
with the reverse one observed during the opposite
process of #uidization, whose front starts from the top
and travels downwards, up to the deepest region of the
particle assembly.
4. Further remarks
Individuation of design and operation criteria suitable
for excluding or promoting particle strati"cation in
#uidized bed processes that employ multiparticle beds
requires an understanding of segregation dynamics much
deeper than that attained to date. To this purpose, a fun-
damental step is that of identifying, among the many
parameters that are reported to play a role in the de"ni-
tion of the mixing/segregation state of such systems, the
ones constituting the more restricted set of independent
variables.
 B. Formisani et al. / Chemical Engineering Science 56 (2001) 109}119
4.1. The identixcation of independent variables in the anal-
ysis of size segregating yuidization
Results of this study clearly demonstrate that min-
imum #uidization velocities of single components are
parameters that have practically no reference meaning in
the de"nition of the #uidization behaviour of their mix-
tures. Indeed, whereas both particle density and diameter
do not change when a solid is mixed, in any proportion,
with another, the same is not true for its interparticle
voidage. Thus, for the case of size segregating solids,
e and e , as well as their respective functions
AKD DKD
u and u , cannot be subjected to averaging
AKD DKD
methods meant to calculate e and u of the binary
KD
system. Accordingly, mixture classi"cation criteria based
on component u (Rowe et al., 1972; Nienow et al.,
KD
1978), which is not a primary parameter even for mono-
disperse solids, are not endowed with an absolute valid-
ity. For the same reason, any possible de"nition of
mixture u should not be referred to minimum #uidiz-
KD
ation velocities of its pure components (Formisani, 1991).
In the absence of reliable models for its prediction, and
given also its great sensitivity to the actual measurement
conditions, two-component bed voidage must necessarily
be evaluated in the speci"c experimental context it refers
to. The dependence of e on both particle diameter ratio
d /d and mixture composition x , comprehensively il-
D A D KD
lustrated by Yu and Standish (1987) out of the "eld of
particle #uidization and veri"ed in previous work (For-
misani, 1991) as well as in this study (see again curves of
Fig. 3), is by far the key-feature of gas}particle interaction
inside the binary bed, whose recognition proves essential
to the interpretation of two-component segregating #ui-
dization. Therefore, d and d (both on their own and
A D
through their ratio) and x (as average value x or,
D D
more generally, as a function of h within the bed) are
surely in the limited number of independent variables
a!ecting mixture #uidization and segregation patterns.
Accounting for the axial variability of voidage and of
particle average diameter with mixture composition
proves to be, through the reduction of the number of
variables of the problem, the crucial condition for a
theoretical approach to size segregating #uidization.
As previously demonstrated with regard to the possible
de"nitions of u , the predicting ability of a classical
KD
equation such as Carman}Kozeny's is fully restored if
this is written in modi"ed forms able to adhere to the
speci"c mixing condition of the "xed bed. The revalida-
tion of Carman}Kozeny equation leads to the de"nition
of minimum #uidization velocity given with Eq. (4) that
has, in comparison with others, a higher degree of gener-
ality as it is fully independent of the initial state of mixing
of the mixture. Moreover, it also establishes, through Eq.
(5), a relationship between axial pro"les of composition
and pressure which furtherly reduces the number of inde-
pendent variables to be taken into consideration.
117
4.2. Operative velocity and mixing/segregation equilibrium
The possibility of devising easy modes of control and
regulation of particle strati"cation in a #uidized bed of
more than one solid lies in that of identifying reliable
relationships between the independent variables of the
process and the internal composition pro"le of the bed.
In this regard, the most important operative parameter
is, no doubt, operative velocity.
The results of this study have shown that segregation
takes place in a well-de"ned velocity range: in experi-
ments conducted at increasing gas #ow rate, its inferior
limit depends, for any value of x , on the initial state of
D
mixing of the mixture, whereas the upper limit is inva-
riably "xed by its u . At decreasing gas #ow rate, in-
DD
stead, both velocities are functions only of x . Although,
D
as discussed above, u can be related, through Eq. (4), to
KD
the internal pro"les of x and e, an equally predictive
D
relationship for u , capable of providing the upper velo-
DD
city bound of segregation in function of mixture average
composition, is not easy to elaborate, and constitutes one
of the objectives of future work.
Finally, also if a quantitative description of segregation
dynamics is out of the scope of this paper, the following
points seem however worthy of remark.
The circumstance that between the two limits of velo-
city "xed by u and u the bed weight is not yet
DD
balanced by gas drag allows stating that the tendency to
segregation must not be considered a characteristic of
binary #uidization but, on the contrary, a consequence of
the incompleteness of system #uidization. The import-
ance of this argument, which will certainly deserve
a closer analysis, lies in the fact that it is in contrast with
current interpretations of particle mixing in two-com-
ponent #uidized beds, according to which this is caused
solely by bubbles (see, for instance, Nienow & Chiba,
1985).
The rather complex nature and the repeatability of
curves of Figs. 13 and 14, which correspond to a sequence
of "xed, transitional and well mixed portions within
the partially #uidized bed, can hardly be encompassed,
as ordinarily done in most of the literature (Nienow et al.,
1978; Nienow & Chiba, 1985), in a unique mixing
index referred to the whole bed mass. As for the predic-
tion of u , accounting for the composition pro"le
KD
along the bed height is perhaps the essential condition
for a deeper understanding of the mixing/segregation
equilibrium.
5. Conclusions
The interpretation of the #uidization behaviour of size
segregating binary mixtures of solids can hardly be
achieved on a merely empirical ground. On the contrary,
some of its essential features can successfully be subjected
118 B. Formisani et al. / Chemical Engineering Science 56 (2001) 109}119

to a theoretical analysis that accounts for the peculiar u mixture minimum #uidization velocity from Eq.
KD
nature of the two-component system. Based on this ap- (4) or
proach, the experimental investigation of this paper leads minimum #uidization velocity (in general), cm/s
to conclusions that can be summarized as follows: u minimum #uidization velocity of the coarse
AKD
(a) the #uidization behaviour of a binary mixture of component, cm/s
solids of the same density is strongly in#uenced by the u minimum #uidization velocity of the "ne com-
DKD
internal composition pro"le of its "xed bed, which is ponent, cm/s
associated to the axial variation of average particle dia- u minimum #uidization velocity of the well-mixed
KD+
meter and of bed voidage; these, in turn, considerably mixture, cm/s
a!ect the onset of #uidization and of component segrega- u minimum #uidization velocity of the segregated
KD1
tion; mixture, cm/s
(b) whatever the initial state of mixing of its "xed bed, x "ne-component fraction, dimensionless
D
unless it is too shallow, any mixture achieves practically x "ne-component average fraction, dimensionless
D
thorough mixing at a characteristic `full #uidization ve-
locitya u at which the total pressure drop equals bed Greek letters
DD
buoyant weight per unit section; u , which inversely
DD
depends on the average "ne fraction x , is therefore an e bed voidage (in general), dimensionless
D
important parameter of size segregating systems; e bed voidage at minimum #uidization (in gen-
KD
(c) minimum #uidization velocity, however de"ned, eral), dimensionless
can be predicted by rewriting classical equations such as e bed voidage of the well-mixed mixture in the
+
Carman}Kozeny's in modi"ed forms suitable for taking "xed state, dimensionless
into account the axial variability of bed voidage and of e voidage of the coarse component layer at min-
AKD
particle average diameter; the same equation can success- imum #uidization, dimensionless
fully be used for predicting the axial pressure pro"le in e voidage of the "ne component layer at minimum
DKD
the packed bed; this procedure leads to a better identi- #uidization, dimensionless
"cation of independent variables of the problem, whose e bed voidage of the well-mixed mixture at min-
KD+
number is accordingly reduced; imum #uidization, dimensionless
(d) when gradually de#uidized from its full #uidization k gas viscosity, g/cm s
E
velocity, any mixture gives place to a "xed bed having
a repeatable and characteristic axial composition pro"le,
whose progressive build-up is accompanied by the grad- Acknowledgements
ual reduction of the well mixed portion of the bed. Such
a de#uidization pattern de"nes the only repeatable u of This work was partially supported by the Italian Min-
KD
the mixture. Size segregation takes place in a velocity istry of University and Scienti"c Research (MURST),
range not exceeding u , and is due to the incompleteness through the `Co"n '98a program. The authors wish to
DD
of system #uidization. thank Mr. R. Mazzitelli, who carried out the preparation
and the granulometric analysis of solids.

Notation
References
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