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pubs.acs.org/IECR

Effects of Material Properties on Segregation of Binary and Ternary

Powder Mixtures in a Small Scale Cylindrical Silo
Niklas Engblom,†,* Henrik Sax
en,† Ron Zevenhoven,† Henrik Nylander,‡ Gisle G. Enstad,§ and
Matti Murtomaa||
†
Department of Chemical Engineering, Thermal and Flow Engineering Laboratory, Åbo Akademi University, Piispankatu 8, FI-20500,
Turku, Finland,
‡
Saint-Gobain Weber, Kalkkitehtaantie, FI-21600, Parainen, Finland.
§
Tel-Tek, department POSTEC, Kjølnes ring 30, N-3918, Porsgrunn, Norway.
)

Faculty of Mathematics and Natural Sciences, Department of Physics and Astronomy, Laboratory of Industrial Physics,
University of Turku, FI-20014, Turku, Finland.

ABSTRACT: The segregation of binary and ternary particulate mixtures at filling and at discharge of a 0.4 m3 cylindrical silo has
been investigated experimentally. Raw materials used in commercial construction products are utilized and include bulk solids with
different particle size, solid density and shape. Mixtures with varying mass fractions, particle size ratio or size distribution, particle
solid density ratio and flow properties (free-flowing to cohesive) are prepared. Discharge flow patterns are determined either visually
or by using tracer particles. This work gives qualitative information on the influence of material properties on the embedding,
(impact) fluidization and air-current segregation mechanisms, which are relevant for the handling of commercial dry mineral-based
construction materials in silos of industrial scale. The results show that material properties have a significant effect on the distribution
of the powder mixture at silo filling, while the material distribution at filling and the discharge flow pattern determine the
composition at emptying. At filling, mixture composition (component mass fractions) determines the segregation pattern, that is,
whether fines are accumulated in the center or at the silo walls. For the latter, segregation is aggravated by increasing the particle size
ratio between coarse and fine component for a binary mixture or size distribution for a ternary mixture, or by reducing the particle
solid density ratio between fine and coarse component significantly below unity.

1. INTRODUCTION
Segregation is the tendency of particles that differ in some
property, that is, size, shape, density, surface texture, electrostatic
charge, etc., to separate during handling and concentrate in
different places. This demixing of particulate solids causes many
problems including lower quality and unexpected changes in
the flow properties of bulk solids. Segregation can occur
almost anywhere in industrial production processes handling
granular matter and can be very difficult—or sometimes nearly
impossible—to avoid. The consequences of segregation are
usually at least economical and in the worst cases of a disastrous
nature. Several review articles on segregation are available in the
public domain.1 7
1.1. Segregation Mechanisms. Segregation is classified in
various ways by different investigators. A division into forces,
processes, flow regimes and applications was presented by Bates,1
whereas others8 20 limit their discussion to various aspects of
segregation mechanisms in different unit operations or parts
thereof without a subclassification. A multitude of mechanisms
have been identified and were summarized by Mosby,21 includ-
ing percolation, sifting, rolling, embedding, impact, angle of
repose, fluidization, trajectory and air-current segregation, but
attempts to condense this have been proposed.2,3 Sifting or
sieving results in accumulation of fines at the impact point as a
result of fine particles finding their way through the openings in a
matrix of coarse particles, for example, when a bulk solid is
poured onto a heap such as at filling of silos. Rolling of large
particles further away from the filling point because small
particles are more easily captured by irregularities on the heap
surface leads to the same segregation pattern, i.e., concentration
of fines at a heap apex and large particle at the base. Segregation
by the embedding mechanism arises from penetration and lock-
ing of large or dense particles in the upper layers of a bed of
particulate solids during charging of material onto a heap.
Consequently, large or dense particles are concentrated at the
point of impact while small or light particles are found further
away.4 Segregation caused by fluidization of fine components has
been reported to induce vertical segregation at filling of silos by
pneumatic conveying.2 Some authors believe that fluidization
may also be induced by an abrupt change in the flow direction of a
particulate solid, such as at impact with the deposited heap at silo
filling,1 and hence the alternative definition of impact fluidization
may also be used. Some evidence of fluidization leading to
horizontal segregation with accumulation of fines away from
the filling point has also been presented recently.22,23 Air-current
segregation is enforced by entrainment of small or light particles
in gas (air) streams induced by a rapidly moving (falling) solid
phase, transportation of these particles with the air flow and
concentration of entrained particles in specific positions (e.g., at
Received: March 11, 2011
Accepted: August 19, 2011
Revised: August 18, 2011
Published: August 19, 2011

r 2011 American Chemical Society 11097 dx.doi.org/10.1021/ie200490a | Ind. Eng. Chem. Res. 2011, 50, 11097–11108
Industrial & Engineering Chemistry Research
silo walls) as a result of settlement caused by changes in intensity
or direction of the air flow.9 In summary, sifting and rolling lead
to opposite material distributions compared to embedding,
fluidization and air-current segregation at silo filling. However,
while the former have been well documented by many workers
previously, the latter are not as well understood.
1.2. Construction Materials. Dry mineral-based construction
materials are multicomponent and highly heterogeneous mix-
tures of different minerals and other raw materials. Examples of
construction materials are products for tile fixing, renders for the
facades of buildings, floor screeds, and masonry mortars. Com-
mercial construction products typically include sand and lime-
stone as filler, cement and gypsum as binder, and a vast amount of
additives including glue, cellulose derivates and synthetic fibers.
One product can easily contain over ten different raw materials
and the final products therefore include particles of varying
shape, solid density and especially size. Exact specifications for
commercial products are subject to confidentiality, but these
exhibit continuous particle size distributions often reaching over
several orders of magnitude (from less than 1 μm up to several
millimeters) and many include significant amounts of fine
particles (typically 20 80%-wt below 125 μm). Construction
materials may be free-flowing or cohesive depending on their
composition. Each raw material or group of raw materials (fillers,
binders, additives) give the final product specific properties.
Binders are fine powders (with particle sizes below 63 μm) that
react chemically with water and influence the expansion or
contraction shortly after application. Including the right propor-
tion of binders is therefore essential for correct behavior of the
products at construction sites. A typical outcome of using out of
spec products is reduced workability at application or the
formation of cracks during the drying phase, while more serious
problems include reduced strength of the ultimate construction.
1.3. Segregation of Construction Materials. In industrial
production of construction materials, in plant segregation leads
to tedious and costly reprocessing of the final products. Although
the amount of segregated product of the total production is
usually limited to a few percent or less, it still means that many
tons of segregated material must be rejected on a daily basis. This
has a negative impact on the maximum production rate and
sustainability. In addition, segregated products may in theory be
delivered to customers by mistake. Short-term storage of the final
products in silos situated downstream of the mixer and upstream
of packing has been identified as the most critical processing
stage with respect to segregation.22
When commercial construction products are filled centrally
into silos with sufficient free fall distance (i.e., > 1 m), consider-
able segregation occurs with accumulation of large particles at the
filling point and fine particles near the walls. Such segregation has
previously not been reported as extensively as the opposite case,
that is, collection of fines at the filling point and large particles
farther away. When a product silo empties in funnel flow, bulk
solids situated next to the walls in the hopper section and lower
part of the vertical section are discharged last. In such cases, the
fines content of construction products increases substantially
(i.e., above the quality requirement limit) toward the end of
complete silo discharge. The relevant segregation mechanisms
for construction materials handled in silos have been identified in
previous work, and include embedding, (impact) fluidization and
air-current effects.23 These occur during filling and no further
segregation is induced at discharge, that is, percolation or sieving
does not occur. The possibility of investigating segregation of
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commercial construction materials in large silos (with capacity
<100 ton) with a ternary mixture in small scale (0.4 m3) was
reported recently;22,23 the same segregation pattern was observed
despite a considerable difference in silo scale. To the best of the
present authors’ knowledge, segregation of construction materials
has not been extensively investigated and very few contributions
are available in the public domain. Kwade and Ziebell12 con-
sidered the segregation of a multiphase plaster in a large silo
(with capacity ≈ 100 ton) and examined several technical
solutions.
1.4. Purpose of Present Work. Segregation is notorious for
the abundance of influential parameters such as properties of the
handling equipment, process parameters and characteristics of
the particulate solid itself.1 3 Work reported in the present paper
focuses on material properties. It is well-known that increasing
the particle size ratio or particle size distribution aggravates
segregation. The effect of particle solid density and mixture
composition is not always obvious and seems to be more case
specific. The present study was performed in order to clarify the
effects of mixture composition (mass fractions), particle size ratio
or size distribution, and particle solid density ratio on segregation
of binary and ternary powder mixtures consisting of raw materials
used in commercial construction materials. The particles also
differ in shape and exhibit varying electrostatic properties. This
paper is the first of two parts investigating segregation of powder
mixtures in a small scale silo; the influence of silo design (hopper
angle) and process parameters (intermittent filling and dis-
charge, free fall distance and filling rate) will be examined in
the second part.24
2. CHARACTERIZATION
2.1. Methods. The following properties of the raw materials
and mixtures were determined:
• particle size distribution
• particle solid density
• particle shape
• electrostatic charge
• bulk density
• moisture content
• flow properties
Particle size distributions were determined by laser diffraction
and sieving. Measurement of particle size distribution by laser
diffraction was performed with a commercial apparatus (HELOS
from Sympatec GmbH). Dry sieving was employed and different
sieve sets were used depending on how the size distributions
were obtained (from supplier, provided by production plant or
checked separately before the experiments). Particle solid den-
sities were determined with a commercial instrument (Heliumauto-
pycnometer from Micromeritics). Images of the individual particles
were obtained with scanning electron micrography (SEM) and
ordinary microscope. The electrostatic properties, that is, the
affinity of the individual particles of a bulk solid to become
electrostatically charged, were determined by sliding electrically
neutralized samples into a Faraday pail through a grounded
stainless steel pipe (length 500 mm and angle 50° to the
horizontal plane). Charge was recorded using an electrometer
(Keithley 6517A, Keithley Intruments Ltd.). The samples were
also weighed and the results are presented as charge-to-mass ratio.
Measurements of bulk density were performed with equipment
for determination of the Hausner ratio (i.e., ratio between tapped
and poured bulk density). A Hausner ratio exceeding unity implies
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Table 1. Properties of the Raw Materials Used for Preparation of the Mixtures
property sand 1 sand 2 limestone 1 limestone 2 limestone 3 glue cement hydrated lime unit

d10 1.12 0.51 0.20 0.06 0.010 0.025 0.001 0.001 mm

d50 1.71a 0.76a 0.45a 0.19a 0.113b 0.105b 0.010b 0.005b mm
d90 2.99 1.04 0.70 0.41 0.220 0.241 0.035 0.053 mm
particle solid 2760 2762 2779 2600 2796 1210 3103 2336 kg/m3
density
bulk density
poured 1594 1652 1576 1399 1250 488 857 414 kg/m3
tapped 1563 1649 1600 1518 1466 538 1120 549 kg/m3
Hausner ratio 0.98 1.00 1.02 1.09 1.17 1.10 1.31 1.33
moisture 0.31 0.10 0.05 0 0.06 0.80 0.50 0.17c %-wt.
d
charge 0.37886 (0.09996) 1.25463 (0.20722) 1.81679 (0.24207) 20.89096 (2.55945) nC/g
a
Measured by sieving analysis, distribution given on mass basis. b Measured with laser diffraction, distribution given on number basis. c Moisture content
increased during drying. d Average of ten tests performed at 22 °C and 30% relative humidity. The standard deviation of all tests is given in parentheses.

Figure 1. Particle shape for sand 2 (a), limestone 2 (b), glue (c), cement (d), and hydrated lime (e). Images obtained by scanning electron microscope
with the exception of glue for which an ordinary microscope was used.

that the material is cohesive. Moisture content was determined
by the weight loss after drying (12 h, 100 °C) and flow properties
were analyzed with a Jenike shear cell (standard design, Jenike
and Johanson Inc., 1969).
2.2. Raw Material Properties. Eight different raw materials
were utilized for preparation of the mixtures including two sand
fractions, three limestone fractions, a glue, Portland cement and
hydrated lime. Raw material properties are summarized in
Table 1, where the raw materials have been arranged by mean
particle size (decreasing from left to right). Sand 1 is the coarsest
raw material and hydrated lime is the finest. The particle solid
density is highest for cement, similar for all sand and limestone
fractions, slightly lower for hydrated lime, and clearly the lowest
for glue. The bulk density mainly follows particle size and solid
density, that is, bulk density decreases with decreasing size or
solid density. The majority of raw materials include only small
amounts of moisture, but the moisture content of hydrated lime
actually increased during drying as a result of its hygroscopic
nature. The electrostatic properties of sand 2, limestone 2 and
11099
cement are similar (small negative charge), but hydrated lime
behaves entirely differently and obtains a large positive charge. In
Figure 1, images of individual particles are given for some raw
materials. It is evident that sand 2, limestone 2, cement, and
hydrated lime include particles of different nonspherical shape
whereas the glue particles are mainly spherical. Flow properties
for a subset of the raw materials are depicted in Figure 2a together
with classification limits according to the theory by Jenike.25
Based on the results for all raw material characterization tests it
can be assumed that both sand fractions and the two coarsest
limestone fractions are free-flowing, limestone 3 and glue are free
or easy flowing, and the fine powders (cement and hydrated
lime) are either cohesive or very cohesive.
2.3. Mixture Properties. Experiments were performed with
six binary (M1-M6) and three ternary (M7-M9) mixtures. The
mixtures were prepared on mass basis with an industrial mixer at
a construction material producing plant and packed in bags
containing 20 or 25 kg of mixture depending on the bulk density.
Table 2 reports the mixture compositions and Table 3 gives the
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Figure 2. Flow functions for a subset of the raw materials (a) and mixtures (b) together with classification limits according to Jenike.25.

Table 2. Composition (%-wt) and Ratios for Mixtures Used in the Experiments
mixture sand 1 sand 2 limestone 1 limestone 2 limestone 3 glue cement hydrated lime size ratioa density ratiob

M1 90 10 76 1.1
M2 70 30 76 1.1
M3 50 50 76 1.1
M4 50 50 7 1.0
M5 50 50 7 0.4
M6 75 25 7 0.4
M7 33.4 33.3 33.3 76 1.1
M8 33.4 33.3 33.3 171 1.1
M9 33.4 33.3 33.3 342 0.8
a
Ratio of d50 for coarse component and d50 for fine component, that is, d50,coarse/d50,fine. b Ratio of particle solid density between fine and coarse
component, that is, Fsolid,fine/Fsolid,coarse.

Table 3. Cumulative Particle Size Distribution for Mixtures for the mixtures together with classification limits according to
Used in the Experiments Jenike25 (flow properties not determined for M4 and M6). The
flow properties of the mixtures mainly follow those of their
< 0.063 < 0.125 < 0.25 < 0.5 <1 <2 <4
constituents; mixtures with low mass fractions of cohesive raw
mixture mm mm mm mm mm mm mm
materials are free or easy flowing (M1, M2, and M5) whereas
M1 10 10 11 17 90 100 mixtures with high mass fractions of cohesive components
M2 30 30 31 35 92 100 exhibit cohesive properties (M3 and M7 M9).
M3 50 50 51 54 94 100
M4 11 33 50 54 94 100 3. EXPERIMENTAL SECTION
M5 12 30 45 53 94 100
3.1. Setup and Procedures. Experiments were performed
M6 6 15 23 31 91 100
with a 0.4 m3 cylindrical silo, see Figure 3. The vertical section is
M7 37 43 58 69 96 100
constructed of standard steel and the hopper section is manu-
M8 33 35 38 53 67 89 100 factured from stainless steel. A separate hopper equipped with a
M9 33 35 38 53 67 89 100 butterfly valve and placed above the silo is used for filling (not
shown in Figure 3). Two different inlet (dinlet = 100 mm and
cumulative particle size distributions calculated from the size 150 mm) and outlet (doutlet = 100 mm and 200 mm) sizes were
distributions of the raw materials and the mixture compositions used in the experiments. The silo is supported by a steel frame
(mass fractions). Binary mixtures M1 M3 are composed of sand and enclosed by plywood sheets in order to restrain dust from
2 and cement in varying mass fractions, whereas binary mixtures dispersing into the surroundings.
M4 M6 include sand 2 as the coarse component and either The material distribution at filling was determined by sampling
limestone 3 (M4) or glue (M5 and M6) as the fine component. (sample size approximately 100 g) with a scoop from the surface
Mixtures M7 and M8 are composed of sand, limestone and layers of the deposited heap in different circumferential direc-
cement, but the coarse and intermediate components are differ- tions and radial positions, and at several levels (see Figure 4a
ent (coarser for M8). In mixture M9, the fine component of M8 and b). One sample was collected from each position marked C
is changed to hydrated lime. Figure 2b illustrates flow functions (Center) and P (Periphery) in Figure 4a in all experiments, and
11100 dx.doi.org/10.1021/ie200490a |Ind. Eng. Chem. Res. 2011, 50, 11097–11108
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Figure 3. Schematic of silo.
Figure 4. (a) Top view of radial positions and circumferential directions
used for sampling and seeding of tracers, (b) side view of levels used for
sampling and seeding of tracers with material amounts for M1, and (c)
numbered pieces of garden hose (20 mm  20 mm) used as tracer objects.
individual samples were collected at positions marked M
(Middle) in one experiment. The number of sampling levels
varied between experiments. The silo was discharged into bins
holding 80 100 kg of powder mixture and samples (50 150 g)
were collected across the entire discharge stream at regular
intervals with a sampling device built for the purpose. This
device consists of polycarbonate pieces inserted into a ply-
wood sheet put on rails and positioned underneath the silo
outlet. Hollows were cut into the polycarbonate pieces for
collection of samples and the plywood sheet also contains
holes large enough for the entire discharge stream to flow
through. With this setup, the sampling device could be slid
across the silo outlet enabling the entire discharge stream to be
sampled for short periods. Further details of the sampling
procedure and the sampling device used at discharge are given
in previous work.22
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The material distribution at filling and size distribution at
discharge were determined by sieving of the entire samples. For
binary mixtures an appropriate sieve size was chosen for dividing
the samples into a fine and coarse fraction (250 μm for M1 M3
and 300 μm for M4 M6). For the sake of clarity and reasons
explained in the introduction, the mass fraction below 125 μm
(fines content) is used for presentation of the results for ternary
mixtures. The fines content of each sample is normalized with the
mean fines content at discharge in the specific experiment to
eliminate the effect of minor compositional variations in the
mixtures. The mean fines content at discharge in each experi-
ment was quite close (from 0.5 to +3%-wt units) to the fines
content for the mixture as calculated from the raw materials
(cf. Table 3).
Tracer objects have been utilized in earlier work to describe
the discharge flow pattern or zone order discharge of bulk solids
in bins and silos.26 28 In this work, the sampling positions and
levels illustrated in Figure 4a and b are also used for seeding of the
bulk material with numbered tracer objects (Figure 4c) in a
majority of the experiments. One tracer was placed at each
position indicated in Figure 4a, but the Middle-position was
omitted in some experiments and the total number of tracers
included in each experiment also depends on the number of
levels utilized. A wire mesh was placed on top of the discharge bin
to separate and capture tracer objects from the output stream of
powder mixture. The silo was emptied in intervals of 10 or 20 kg
and discharge was stopped for collection of withdrawn tracers
objects. In this way, the mass of powder mixture discharged from
the silo at withdrawal of each tracer could be recorded. The
mean value of mass discharged from the silo for a specific
interval was used as the exit “time” for all tracers withdrawn
during the interval. Because of variations in the discharge flow
rate, this measure gives a more accurate description of the
discharge flow pattern compared to monitoring the actual
time (measured in time units) taken for the tracers to be
withdrawn. For presentation of the data, the exit “time” of
each tracer is normalized by the total mass of powder mixture
used in the experiment (fractional mass discharged) and
fractional mass discharged versus initial tracer position
(radial position and level) is illustrated in order to obtain a
description of the discharge flow pattern.
3.2. Conditions. The experimental conditions are summar-
ized in Table 4. Three experiments were performed under
identical conditions with mixture M1 and M8, respectively, in
order to investigate the reproducibility with free-flowing and
cohesive materials. Single experiments were performed with the
other mixtures. The total mass of material used in each experi-
ment varied for practical reasons; the capacity of the mixer is
approximately 400 kg, but the total amount of packed mixture
varied with the bulk density, and the last bag from the mixer was
always discarded. Either one (20 or 25 kg) or two (40 or 50 kg)
bags were emptied into the filling hopper before charging into the
silo. In each experiment the butterfly valve of the filling hopper
was fully opened, but variations in the instantaneous filling rate
occurred especially with the cohesive mixtures because of arching
and the mean filling rate varied between the mixtures. Filling was
completed before discharge in all experiments. The instanta-
neous discharge rates were more constant compared to the filling
rates, but the mean discharge rate varied between mixtures even
though the butterfly valve at the silo outlet was kept almost fully
open in all experiments. Moisture content was determined for
single samples collected at discharge.
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Table 4. Experimental Conditions (Funnel Flow Discharge in All Tests)

mixture test nr dinlet (mm) doutlet (mm) total mass (kg) chargea (kg) filling rate (kg/s) discharge rate (kg/s) flow pattern determination moisture (%-wt.)

M1 1 100 100 500 50 6.25 ( - c 0.55 ( 0.03 visual 0.20

2 100 100 500 50 6.47 ( 0.12 0.56 ( 0.05 visual c

3 100 100 500 50 6.52 ( 0.20 0.56 ( 0.03 visual c

M2 1 100 100 375 50 2.00 ( 0.26 0.47 ( 0.12 tracers 0.30

M3 1 100 100 500 50 Low b Low b visual 0.30
M4 1 150 100 375 50 3.89 ( 2.52 0.46 ( 0.06 tracers 0.30
M5 1 150 100 320 40 3.33 ( 0.43 0.23 ( 0.04 tracers 0.50
M6 1 150 100 390 50 2.54 ( 0.15 -c tracers 0.40
M7 1 150 200 400 25 0.32 ( 0.25 0.28 ( 0.06 tracers c

M8 1 150 200 400 25 4.36 ( 2.33 0.20 ( 0.03 tracers 0.30

2 150 200 400 25 4.76 ( 1.89 0.19 ( 0.04 tracers c

3 150 200 400 25 5.43 ( 2.58 0.19 ( 0.04 tracers 0.20

M9 1 150 200 380 20 6.06 ( 2.69 0.21 ( 0.01 tracers 0.40
a
Mass of material filled into the silo at a time. b Rate could not be measured accurately because of intermittent flow (due to arching). c Not measured.

to discharge in mass flow according to the theory by Jenike.25 It

Figure 5. Top view of rathole in the silo center at the early stages
of discharge with mixture M3 (approximately 100 kg withdrawn from
the silo).
4. RESULTS
4.1. Discharge Flow Patterns. Flow patterns were observed
visually for mixtures M1 and M3, and determined with tracer
objects for the other tests. Visual observations for M1 and M3
will be described next followed by presentation of tracer data for
some of the other experiments.
For mixture M1, the entire silo contents started moving
downward as discharge commenced and clean walls were
observed as the surface descended. Both findings are typical for
mass flow. However, the material surface quite quickly changed
from a heap to a centric V-shape with avalanching of the bulk
solid toward the center of the silo also taking place, which is
typical for funnel flow. Apparently the hopper walls are not steep
enough to induce mass flow with M1, which requires a (stainless
steel) hopper with angle g70° from the horizontal plane in order
11102
was therefore concluded that funnel flow occurred at discharge in
this experiment.
With M3, a rat-hole29 developed in the central part of the silo
shortly after discharge was started (see Figure 5), which is typical
for funnel flow silos with outlets dimensions smaller than the
critical size as determined by Jenike.25 The critical hopper angle
for M3 (71° from the horizontal plane) implies that funnel flow
should occur and the silo outlet diameter (10 cm) is smaller than
the critical outlet size (18 cm) required for unobstructed flow
with M3.
Tracer data for mixture M4 is depicted by the bar chart in
Figure 6a and illustrated schematically in Figure 7. In Figure 6a,
the mean value and standard deviation for all four tracers seeded
in the Middle and Periphery position, respectively, at each level
are given. The figure shows that tracers placed on the silo axis
(center) discharge in a first-in-first-out pattern during the initial
stage of emptying, which means that a central core was with-
drawn first. Tracers placed in the middle position discharged
after the central tracers and were followed by tracers seeded next
to the silo walls (periphery) from each level. This is typical for
silos discharging in funnel flow. The schematic illustration in
Figure 7a shows that the central core (1 2) was followed by
material from a slightly broader region at the surface (3). During
discharge the surface changed from a heap (inverted-V) to a
V-shape and avalanching of powder mixture from peripheral
regions toward the center of the silo (4) occurred. Figure 7b
shows the situation when approximately 40% of powder
mixture had been withdrawn from the silo. For the remaining
part of discharge, avalanching from peripheral regions toward
the center continued (5 7) and material from the vicinity of
the walls in the transition area between hopper and vertical
section, that is, Level 2, was discharged last (8). Similar results
were obtained for the other tests with binary mixtures where
tracer objects were used (mixtures M2, M5, and M6). With
mixture M2 and M5, the middle position was omitted and
tracers were placed on the silo axis and next to the walls, but
the flow pattern was still clearly identified despite the reduced
number of tracers (a total of 20 tracers used for M2 and M5,
respectively). A description of the overall silo discharge flow
pattern can apparently be obtained with relatively few well
placed tracer objects.
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Industrial & Engineering Chemistry Research
Figure 6. Fractional mass discharged from silo (mi/mtot) at withdrawal of tracer objects seeded in different radial positions (center, middle, and
periphery) and levels (cf. Figure 4) with mixture M4 (a) and first experiment with mixture M8 (b). Mean value (column bar) and standard deviation
(error bars) given for radial positions including four tracers per level (middle and periphery).
Figure 7. Schematic side view of discharge pattern based on tracer data
for mixture M4 with full silo (a) and with approximately 60% of mixture
left in the silo (b). Numbers indicate order of withdrawal.
Figure 6b shows tracer data for the first experiment with
mixture M8, where a greater number of levels were used
compared to the experiment with mixture M4. The results are
similar for both mixtures. With M8, tracers seeded on the silo axis
at Levels 2 3 and Levels 5 7 were withdrawn later than
expected, which was most likely caused by unwanted movement
of these tracers before discharge as a results of additional material
being filled into the silo. Figure 6b shows that material from near
the walls of the entire hopper section and lower part of the
vertical section discharged last (no tracers seeded in the middle
position at Level 1). Similar results were obtained in the other
tests with mixture M8 and for the rest of the ternary mixtures
(M7 and M9).
In summary, funnel flow discharge occurred in all of the
experiments included in this work.
4.2. Sampling. The fines content of multiple samples col-
lected in the same radial position (i.e., positions marked M and P,
respectively, in Figure 4a) at filling are averaged for each
sampling level used in the experiment. Results are presented in
bar charts, where columns denote the average fines content and
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error bars depict the standard deviation. No error bars can be
given for the silo axis (C in Figure 4a) as this position includes
only one sample per level.
4.2.1. Binary Mixtures of Sand and Cement. Results for
mixture M1 are shown in Figure 8, where data for three experi-
ments have been averaged. At filling (Figure 8a), no clear
segregation was visible at the first two levels (Level 2 and 4),
but more fines were found in the center of the silo at Levels 6, 8,
and 10 as a result of sifting and rolling. The composition of the
mixture was constant for the major part of discharge (see
Figure 8b), but a depletion of fines occurred at the end of
complete emptying. The error bars for discharge indicate that the
reproducibility is quite good. For M2 (results not given) no clear
segregation occurred at filling, and the composition at discharge
was constant excluding some fluctuations and a minor increase of
the fines content at the end.
Figure 9 depicts results for the experiment with mixture M3. At
filling (Figure 9a), a surplus of fines was found near the silo walls
at the first four sampling levels (Levels 2, 4, 6, and 8) as a result of
embedding, fluidization and air-current segregation, and no segrega-
tion occurred at the last level (Level 10). At discharge (Figure 9b),
the fines content was below average in the beginning, then rose to
the mean value and increased significantly toward the end.
Comparison of the results for mixtures M1-M3 makes it
possible to draw some interesting qualitative conclusions. Mixture
composition clearly affects the segregation pattern at filling; a
mixture with low fines content (M1) segregates by accumulating
fine particles at the filling point whereas a mixture with high fines
content (M3) segregates oppositely and fine particles are con-
centrated at the silo walls. Similar findings have been presented for
die filling.15 Apparently, mixture composition determines which
segregation mechanisms, out of a number of possible mechan-
isms present at silo filling, that are activated and this decides the
material distribution. Based on visual observation with the naked
eye, M1 can be described as a coarse continuous and M3 as a fines
continuous mixture according to Arteaga and T€uz€un.30,31 For all
binary mixtures of sand and cement, the distribution at filling and
the discharge flow pattern govern the composition of the mixture
at silo emptying.
4.2.2. Binary Mixtures of Sand and Limestone or Glue. Results
for mixture M4 exhibit a homogeneous distribution at filling
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Industrial & Engineering Chemistry Research ARTICLE

Figure 8. Results for mixture M1 at filling (a) and at discharge (b). Mean values and standard deviations for three experiments. Fines content of samples
normalized with mean fines content at discharge in each experiment. Fractional mass discharged = mi/mtot.

Figure 9. Results for mixture M3 at filling (a) and at discharge (b). Fines content of samples normalized with mean fines content at discharge. Fractional
mass discharged = mi/mtot.

Figure 10. Results for mixture M4 at filling (a) and at discharge (b). Fines content of samples normalized with mean fines content at discharge.
Fractional mass discharged = mi/mtot.

(Figure 10a) and some fluctuations, but no segregation, occur- evident when the results for mixture M3 and M4 are compared;
ring at discharge (Figure 10b). The effect of particle size ratio is reducing the size ratio between large and small component while
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Industrial & Engineering Chemistry Research ARTICLE

Figure 11. Results for mixture M5 at filling (a) and at discharge (b). Fines content of samples normalized with mean fines content at discharge.
Fractional mass discharged = mi/mtot.

Figure 12. Results for mixture M7 at filling (a) and at discharge (b). Fines content of samples normalized with mean fines content at discharge.
Fractional mass discharged = mi/mtot.

keeping the mass fractions of a binary mixture constant reduces
or eliminates segregation.
Figure 11 illustrates the results for mixture M5. At filling
(Figure 11a), the mixture was segregated considerably at all levels
with concentration of fine particles (with low solid density) next
to the walls, which suggests that the embedding, fluidization and
air-current segregation mechanisms are activated by decreasing
the solid density for the small sized particles. At discharge
(Figure 11b), the fines content exhibited an increasing trend
and some quite large fluctuations, but no steep increase of the
fines content toward the end was visible (such as for M3).
Comparison of the results (especially at silo filling) for M4
(limestone) and M5 (glue) shows the marked effect of fine
particle solid density on segregation.
The results for mixture M6 (not given) were similar to M5, but
less segregation occurred at silo filling. Interestingly, the fines
content for mixture M6 (25%-wt) is large enough to induce
segregation with accumulation of fines at the silo walls whereas
mixture M2 (with 30%-wt fines) did not segregate, which implies
that this type of segregation is affected by both particle size
and solid density ratio. Results for binary mixtures M4-M6 also
11105
demonstrate that the composition at silo emptying is determined
by the material distribution at filling in combination with the
discharge flow pattern.
4.2.3. Ternary Mixtures. At filling of the ternary mixture M7
(Figure 12a), some accumulation of fines at the silo walls was
observed at Levels 2 and 4. This is in agreement with the results
for M2 (no segregation) and M3 (strong segregation) as the fines
content for M7 (43%-wt) is between these two mixtures (30%-wt
and 50%-wt for M2 and M3, respectively). No segregation was
observed at Levels 6 and 8, which suggests that segregation
depends on the free fall distance. The fines content was fairly
constant during most of the discharge and increased toward the
end of complete emptying (Figure 12b).
Results for mixture M8 are illustrated in Figure 13, where data
for three experiments have been averaged. At filling (Figure 13a)
a surplus of fines was found near the walls at the first two levels
(Levels 2 and 4) while no segregation occurred at the last two
levels (Levels 6 and 8), which again implies a correlation between
segregation and free fall distance. Comparison of the results for
M7 and M8 at filling shows the influence of particle size distri-
bution on segregation; the magnitude of segregation is clearly
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Industrial & Engineering Chemistry Research ARTICLE

Figure 13. Results for mixture M8 at filling (a) and at discharge (b). Mean values and standard deviations for three experiments. Fines content of
samples normalized with mean fines content at discharge in each experiment. Fractional mass discharged = mi/mtot.

Figure 14. Results for mixture M9 at filling (a) and at discharge (b). Fines content of samples normalized with mean fines content at discharge.
Fractional mass discharged = mi/mtot.

higher at Level 2 and somewhat higher at Level 4 for M8, which
has a wider particle size distribution. At discharge of M8
(Figure 13b), the composition was relatively constant until the
fines content increased substantially toward the end. The error
bars for discharge indicate that the results are fairly reproducible.
Compared to mixture M7, the magnitude of segregation at the
end of emptying was higher with M8, which can be ascribed to
stronger segregation at Level 2 during filling.
As for mixture M9 at filling (see Figure 14a), a considerable
accumulation of fines in the vicinity of the silo walls was observed
at all sampling levels. Compared to mixture M8, the segregation
was much stronger as a result of lower solid density and smaller
size of the hydrated lime particles (fine component of M9)
compared to cement (fine component of M8). For M9 the fines
content of the outflow was below average and fluctuated for the
first two-thirds, but increased substantially during the last third of
discharge (Figure 14b). The fines content started increasing
earlier, the increase was not as sharp as for mixture M8, and the
magnitude of segregation at the very end of discharge was con-
siderably greater for M9.
In summary, all ternary mixtures segregated at silo filling as a
result of the embedding, fluidization and air-current mechanism,
11106
and the results confirm the combined effect of the material
distribution observed at silo filling and the discharge flow pattern
on the size distribution for the outflow.
5. DISCUSSION
The effect of mixture composition on segregation is clearly
shown by the results for binary mixtures of sand and cement
(M1-M3); the segregation pattern is completely different for a
mixture with low fines content (M1) compared to a mixture with
high fines content (M3). Addition of a third intermediate size
component (mixture M7) has the same effect as increasing the
fines content of a binary mixture. Based on visual inspection, M1
can be described as fine particles dispersed in a matrix of coarse
particles, whereas the mixtures M3 and M5 M9 clearly consist
of large particles dispersed in a bed of fine particles. This finding
is reminiscent of previous work,30,31 where the critical fines fraction
for percolation with binary and ternary mixtures was examined. It
was concluded that percolation ceases to occur when the surface
area of the large particles is covered by the fine particles or, stated
in another way, when the mixture is transformed from “coarse
continuous” to “fines continuous”. Other investigators21 report
dx.doi.org/10.1021/ie200490a |Ind. Eng. Chem. Res. 2011, 50, 11097–11108
Industrial & Engineering Chemistry Research
that percolation can no longer occur when the void space
between the large particles is completely filled by the small
particles. Although different segregation mechanisms were
investigated in this work, it can be speculated upon that similar
geometrical arguments may determine the segregation pattern at
filling of silos with free fall. Segregation with concentration of
fines away from the filling point seems to occur with fines
continuous mixtures whereas fine particles are collected at the
filling point with coarse continuous mixtures. Similar findings
have been reported for segregation of lead and iron particles
during die filling.15
Particle size ratio or particle size distribution influences
segregation to a great extent. The effect of this parameter is most
clearly seen when the results for binary mixtures M3 and M4 and
ternary mixtures M7 and M8 are compared. Segregation is
aggravated by increasing the particle size ratio of binary mixtures
or particle size distribution for ternary mixtures, which agrees
with the findings of many previous investigations.3,15,21
Comparison of the results for mixture M4 and M5 shows the
influence of the solid density ratio on segregation, and there are
several possible explanations for this. During filling lighter
particles are trapped in air currents induced by the falling
solid phase and carried away from the filling point more easily
compared to heavier particles. Furthermore, when particulate
solids are mixed on mass basis, the particle solid density
influences the number of particles included in the mixture.
The volume occupied by the fine component can be very
different for two mixtures with equal mass based composi-
tions, but with different solid density for the fine particles.
Penetration of larger or denser particles in the surface layers of
the deposited powder bed at the point of impact may be
facilitated in a mixture with light small particles. To some
extent the effect of this parameter is also shown by a compar-
ison of the results for M8 and M9, although the mean particle
size for the fine component in these two mixtures is not
identical but slightly smaller for M9.
The effect of particle shape was not rigorously studied in this
work. Comparison of the results for mixture M4 and M5
(limestone and glue, respectively, as fine component) indicates
that the effect of this parameter be less important compared to
other material properties. If particle shape were the determining
factor, mixture M4 should have segregated more than M5
because the effect of air drag is stronger for cubic particles
(limestone) compared to spherical particles (glue) of the same
size. Accordingly, limestone particles should have been carried
away from the filling point more easily than glue particles by air
currents directed toward the silo walls. However, the effect of
shape is likely to be more important for very nonspherical
particles, such as needles or flakes.
The effect of particle charge on segregation also seems
of lesser importance based on the results presented here.
Hydrated lime will charge positively in contact with other
particles or surfaces, while the particles of all other raw
materials are expected to obtain a negative charge. Segregation
should in principle be reduced by agglomeration for mixture
M9 (hydrated lime) since opposite polarities attract each
other. However, no such effect could be seen for M9 and
segregation was, in fact, stronger than for M8 (cement). This
implies that electrostatic charging of particles is of minor
importance compared to other material properties such as
mixture composition, particle size ratio or distribution and
particle solid density ratio.
11107
ARTICLE
6. CONCLUSIONS
Segregation of binary and ternary powder mixtures at filling
and discharge in a 0.4 m3 silo has been investigated experimen-
tally. The results of this work confirm our earlier findings, at
widely varying scales, on the combined effect of the material
distribution at filling and the discharge flow pattern on mixture
composition at complete emptying of silos. Useful qualitative
information has been obtained that deepens the understanding
of segregation in industrial production of commercial construc-
tion products, where segregation is a major problem and has not
been extensively investigated to date. In particular, the findings of
this work give insights into the material properties that influence
the embedding, (impact) fluidization and air-current segrega-
tion mechanism, which are relevant for construction materials
handled in larger silos. Key material parameters include mixture
composition (mass fractions), particle size ratio or particle size
distribution, and particle solid density ratio. Mixture composition
clearly determines the segregation pattern at silo filling. A
mixture with low mass fraction of fines induces a common type
of heap segregation with accumulation of fines at the heap apex
(e.g., silo axis) and large particles farther away (silo walls) as a
result of sifting and rolling segregation. Mixtures with high fines
content segregate in the opposite way, that is, large particles are
accumulated on the silo axis (for centrally filled silos) and fines
are concentrated to the silo walls, as a consequence of embed-
ding, fluidization and air-current effects. This segregation pattern
is unconventional and has not been extensively reported by
others. Findings of other investigators on the effect of particle
size ratio on segregation are confirmed; increasing the size ratio
between the coarse and fine component of a binary mixture or
size distribution for a ternary mixture aggravates segregation.
Reducing the solid density of the fine component significantly
below the solid density of the large particles induces or increases
segregation. Further work has been performed in small scale to
investigate the effects of other relevant parameters, such as silo
design and process conditions, on segregation and will be presented
in a separate paper.24
’ AUTHOR INFORMATION
Corresponding Author
*Phone: +358 2 215 4549; fax +358 2 215 4792.
’ ACKNOWLEDGMENT
Saint-Gobain Weber is gratefully acknowledged for financial
support of this work.
’ REFERENCES
(1) Bates, L. User guide to segregation; Hayes, G., Ed.; British
Materials Handling Board: Marlow, U. K., 1997.
(2) Carson, J. W.; Royal, T. A.; Goodwill, D. J. Understanding and
eliminating particle segregation problems. Bulk Solids Handl. 1986,
6, 139.
(3) Tang, P.; Puri, V. M. Methods for minimizing segregation: A
review. Part. Sci. Technol. 2004, 22, 321.
(4) Brown, R. L. The fundamental principles of segregation. J. Inst.
Fuel 1939, 13, 15.
(5) Williams, J. C. The segregation of particulate materials. A review.
Powder Technol. 1976, 15, 245.
(6) Johanson, J. R. Particle segregation and what to do about it.
Chem. Eng. 1978, 8, 183.
dx.doi.org/10.1021/ie200490a |Ind. Eng. Chem. Res. 2011, 50, 11097–11108
Industrial & Engineering Chemistry Research ARTICLE

(7) Carson, J. W. Preventing particle segregation. Chem. Eng. 2004, (31) T€uz€un, U.; Arteaga, P. A microstructural model of flowing
111, 29. ternary mixtures of equal-density granules in hoppers. Chem. Eng. Sci.
(8) Salter, G. F. Investigations into the Segregation of Heaps of 1992, 47, 1619.
Particulate Materials with Particulate reference to the Effect of Particle
Size, Dr. Phil. Thesis, University of Greenwich, 1999.
(9) Zigan, S.; Thorpe, R. B.; Tuzun, U.; Enstad, G. G.; Battistin, F.
Theoretical and experimental testing of a scaling rule for air current
segregation of alumina powder in cylindrical silos. Powder Technol. 2008,
183, 133.
(10) Jochem, K.; Schwedes, J.; Vidal, J.-L. Entmischung bin€arer
Sch€uttgutmischungen in einem Versuchssilo. Sch€uttgut 1998, 4, 31.
(11) Shinohara, K.; Golman, B.; Nakata, T. Size segregation of
multicomponent particles during the filling of a hopper. Adv. Powder
Technol. 2001, 12, 33.
(12) Kwade, A.; Ziebell, O. Reducing the segregation of multi-phase
plaster by selective alteration of the silo geometry. ZKG International
2001, 54, 680.
(13) Drahun, J. A.; Bridgwater, J. The mechanisms of free surface
segregation. Powder Technol. 1983, 36, 39.
(14) Matth
ee, H. Segregation phenomena relating to bunkering of
bulk materials: Theoretical considerations and experimental investiga-
tions. Powder Technol. 1968, 1, 265.
(15) Lawrence, L. R.; Beddow, J. K. Powder segregation during die
filling. Powder Technol. 1969, 2, 253.
(16) Shinohara, K.; Shoji, K.; Tanaka, T. Mechanism of segregation
and blending of particles flowing out of mass-flow hoppers. Ind. Eng.
Chem. Process Des. Dev. 1970, 9, 174.
(17) Shinohara, K.; Shoji, K.; Tanaka, T. Mechanism of size segrega-
tion of particles in filling a hopper. Ind. Eng. Chem. Process Des. Dev. 1972,
11, 369.
(18) Shinohara, K.; Miyata, S. Mechanism of density segregation of
particles in filling vessels. Ind. Eng. Chem. Process Des. Dev. 1984, 23, 423.
(19) Tanaka, T. Segregation models of solid mixtures composed of
different densities and particle sizes. Ind. Eng. Chem. Process Des. Dev.
1971, 10, 332.
(20) Harris, J. F. G.; Hildon, A. M. Reducing segregation in binary
powder mixtures with particular reference to oxygenated washing
powders. Ind. Eng. Chem. Process Des. Dev. 1970, 9, 363.
(21) Mosby, J. Investigations of the Segregation of Particulate Solids
with Emphasis on the Use of Segregation Testers; Dr. Ing. Thesis,
NTNU/Telemark University College, 1996.
(22) Engblom, N.; Sax
en, H.; Zevenhoven, R.; Nylander, H.; Enstad,
G. G. Segregation of premixed construction materials in silos. Part 1:
Experimental findings on different scales. Part. Sci. Technol. 2011, DOI
10.1080/02726351.2011.553880.
(23) Engblom, N.; Sax
en, H.; Zevenhoven, R.; Nylander, H.; Enstad,
G. G. Segregation of construction materials in silos. Part 2: Identification
of relevant segregation mechanisms. Part. Sci. Technol. 2011, DOI
10.1080/02726351.2011.552097.
(24) Engblom, N.; Sax
en, H.; Zevenhoven, R.; Nylander, H.; Enstad,
G. G. Effect of process parameters and hopper angle on segregation of
cohesive ternary powder mixtures in a small scale cylindrical silo. Adv.
Powder Technol. 2011, DOI 10.1016/j.apt.2011.06.003.
(25) Jenike, A. W. Storage and Flow of Solids; Bulletin No 123;
Engineering Experiment Station, University of Utah: Salt Lake City, UT,
1964.
(26) Graham, D. P.; Tait, A. R.; Wadmore, R. S. Measurement and
predicition of flow patterns of granular solids in cylindrical vessels.
Powder Technol. 1987, 50, 65.
(27) Ooi, J. Y.; Chen, J. F.; Rotter, J. M. Measurement of solids flow
patterns in a gypsum silo. Powder Technol. 1998, 99, 272.
(28) Ooi, J. Y.; Rotter, J. M. Flow visualization. In Silos: Fundamentals of
Theory, Behavior and Design; Taylor & Francis: Abingdon, 1998.
(29) Schulze, D. Powders and Bulk Solids: Behavior, Characterization,
Storage and Flow; Springer: Berlin-Heidelberg, 2008.
(30) Arteaga, P.; T€uz€un, U. Flow of binary mixtures of equal-density
granules in hoppers—Size segregation, flowing density and discharge
rates. Chem. Eng. Sci. 1990, 45, 205.

11108 dx.doi.org/10.1021/ie200490a |Ind. Eng. Chem. Res. 2011, 50, 11097–11108