School of Chemical Engineering

Particulate Processes

Topic 4

Particle Size Enlargement

Part 2
Granulation rate processes
Granulation equipment

Life Impact | The University of Adelaide

Overview
Particle Size Enlargement
Part 1
• Introduction
• Objectives of size enlargement
• Methods of size enlargement
• Agglomeration processes
• Agglomerate bonding mechanisms
Part 2
• Granulation
G l ti rate
t processes
• Granulation equipment
2
Agitative Agglomeration - Granulation
Rate Processes of Granulation
1. Wetting and Nucleation
Liquid
q drop
p
Nucleus granule

Particles

2. Consolidation and Growth

Nucleus Granule
granules
l

3 Breakage and Attrition

3.

3
Growth and Consolidation
Evolution of granule size & size
y several
distribution is controlled by
competing mechanisms:
• Nucleation of p
particles to form initial
primary granules;
• Coalescence of existing granules and
layering of particles onto previously
formed nuclei or granules.
• Granules may simultaneously be
p
compacted byy consolidation and
reduced in size by breakage

• Dominant mechanisms are dictated by relationship between

critical particle properties & operating variables as well as by
mixing,
i i size
i didistribution,
t ib ti and
d th
the choice
h i off processing.
i
4
Growth and Consolidation
Growth Physics and Contact Mechanics
• for two colliding
gggranules to coalesce rather
than break up, the collisional kinetic energy
must first be dissipated to prevent rebound.
• The strength of the bond must also resist
any subsequent breakup forces due to bed
agitation intensity.
intensity

• The ability of the granules to deform during processing increases the

bonding
b di or contact
t t area thereby
th b dissipating
di i ti bbreakup
k fforces and
dhhas a
large effect on growth rate.
• A critical granule size (dc) exists above which coalescence becomes
impossible.
 dc increases with the deformability (K) of the granule
• It is thus possible for the collision of two large granules to be
unsuccessful, their average size exceeding dc, whereas the collision of a
unsuccessful
large and small granule may lead to successful coalescence.
5
Growth and Consolidation
Granule Consolidation
• Granules
G l are compactedt d as they
th collide
llid d
due tto b
bed
d agitation
it ti iintensity.
t it
• This process expels pore fluid to the granule surface, thereby increasing
local liquid saturation in the contact area of colliding granules
granules.
• This surface fluid increases tensile strength of the liquid bond (σT),
and granule deformability (K).
(K)
 In low-deformability systems, growth is largely controlled by the extent
of this fluid layer
layer.
 For high-deformability systems, the combined effect of these
increases is more complex.
• Deformability K is related to both the yield strength of the material (σy),
i.e. the abilityy of the material to resist stress,, and the abilityy of the surface
to be strained without rupture of the granule, indicated by the maximum
allowable critical deformation strain (ec).
• In general, high deformability K requires low σy and high ec.
6
Growth and Consolidation

ec
e
Effect of liquid saturation S on
granule deformability
IIncrease in
i granulel deformability
d f bilit
Dicalcium phosphate with a 15%
with moisture increases granule size
binder solution of PVP/PVA
y g
Granulation of calcium hydrogen
phosphate with aqueous binder solutions
in a high-shear mixer. 7
Growth and Consolidation
Growth
• Two types of growth behaviour
depending on granule deformation:
Steady growth (High
(High-deformation)
deformation)
• Granule size increases proportionally
with granulation time
time, ii.e.
e a plot of
granule size versus time is linear.

Induction growth (Low-deformation)

• Granules form and consolidate, but do
not grow until porosity is reduced
enough to squeeze liquid to the surface.
• this excess free liquid on the granules
causes sudden coalescence of
granules and a rapid increase in size.
8
Growth and Consolidation
Effect of Equipment Mechanical Variables
• The
Th importance
i t off deformability
d f bilit tto th
the growth
th process d
depends
d on
bed agitation intensity in comparison to the strength of the
formed granules.
granules
• Agitation intensity controls the relative collisional velocities of
granules
l and dhhence growth,
th bbreakage,
k consolidation,
lid ti and
d fifinal-
l
product density.
• Low agitation intensity processes include fluidized bed, drum,
and pan granulators.
• High agitation intensity processes include pin and plow shear-
type mixers, and high-shear mixers involving choppers.
• Bed agitation intensity and compaction pressure are controlled by
mechanical variables of the process such as excess gas velocity
in fluidized bed or mixer-impeller speed.
9
Low-Agitation Intensity Growth
• Consolidation of granules occurs at much slower rate than growth,
and g
granule deformation can be ignored.
g
• Model growth process by collision of two rigid granules each
y a liquid
coated by q layer
y of thickness h. The p probability
y of
successful coalescence is governed by a Stokes number (St)
Collisional Kinetic Energy 4ρGudG
St = =
Viscous Dissipation Energy 9μ
u = relative collisional velocity of the granules; ρG = granule density
dG = average granule diameter; μ = viscosity of solution phase binder.

• Successful growth by coalescence or layering requires

St* = (1 + 1 er ) ln (h ha )
St < St * where St

St* = critical Stokes No representing the energy required for rebound

er = the coefficient of restitution of the granules
ha = measure of surface roughness. 10
Low-Agitation Intensity Growth
1. Non-inertial Regime of Granule growth: St < St*
• For small granules or high binder viscosity: all granule collisions result in
successful growth provided binder is present.
• Growth rate independent of collision energy
energy, particle size,
size binder viscosity
• Rate of wetting of binding fluid thus controls growth.
2 Inertial
2. I ti l Regime:
R i local
l l St > St*
• As granules grow in size, their collisional momentum increases, leading
t localized
to l li d regions
i iin th
the process where
h St > St*
St*.
• Granule size, binder viscosity, and collision velocity determine the
proportion of the bed in which granule rebound is possible.
possible
3. Coating Regime: spatial average St > St*
• Growth balanced by granule breakage
• Growth continues only by coating of primary particles onto existing
granules (growth by layering).
11
High-Agitation Intensity Growth
• For processes involving high-shear mixing, granule deformability and
plastic deformation are significant.
Two stages of growth are evident:
1 Initial non-equilibrium
1. non equilibrium growth
• In early stage of growth, freshly formed, uncompacted granules are
easily deformed. This stage is controlled by granule deformability.
• Increase in St due to lower viscosity or higher impeller speed
increases ggrowth rate since the system
y becomes more deformable and
easier to knead into larger-granule structures .
• Growth continues until disruptive and growth forces are balanced.
2. Final equilibrium growth
• as growth proceeds and consolidation occurs
occurs, granules will surface
harden and become more resistant to deformation.
• dissipation and collisional kinetic energy is balanced
balanced, where increasing St
decreases final granule size, as expected from the Stokes analysis.
12
 High-Agitation Intensity Growth

(a) (b)
Influence of deformability on granule growth for high-shear mixer granulation
(a) Granulation of lactose with liquid loading of 15 wt % binder and impeller speed of
1400 rpm for two different viscosity grades of polyethylene glycol binders
(b) Granulation of dicalcium phosphate with 15 wt % binder solution of PVP/PVA for
varying impeller speed.
Ref: Schaefer et al., Pharm. Ind., 52(9), 1147 (1990) 13
Consolidation
• Consolidation determines granule porosity, hence granule density.
• Granules may consolidate over time and achieve high densities if
there is no simultaneous drying to stop the consolidation process.
• The extent and rate of consolidation are determined by balance
between collision energy and granule resistance to deformation.
• Decreasing feed
feed-particle
particle size decreases consolidation rate due to
high specific surface area and low permeability of fine powders.
• Effects
Eff t off binder
bi d viscosity
i it and
d liquid
li id content
t t are complex
l and
d
interrelated:
 L
Low viscosity
i it bi
binders:
d consolidation
lid ti iincreases with
ith liliq. content
t t
 High viscosity binders: consolidation decreases with increasing
liquid content
• Increasing agitation intensity increases the degree of consolidation
by increasing the energy of collision and compaction.
14
Controlling Growth and Consolidation
• Granule growth & consolidation can be maximised by making
g in formulation ((material)) and p
changes processing
g ((operating
p g
variables).
• Growth & consolidation strongly
g y influenced by
y Stokes number ((St).
)
• Increasing St increases energy dissipation during deformation of
granules. Hence, rates of growth & granule consolidation generally
increases with St for deformable systems.
• St may be increased by decreasing binder viscosity or increasing
agitation intensity.
• Changes in binder viscosity may be accomplished by formulation
changes (e.g. type or concentration of binder) or by operating
p
temperature changes
g ((e.g.
g with drying).
y g)
• Increasing particle size increases rate of consolidation, and this
can be modified
ca od ed by upst
upstream
ea milling
goor ccrystallization
ysta at o co conditions.
dto s

15
Breakage
Mechanisms of Breakage
• Determined
D t i db by size
i off process zone relative
l ti tto
granule size
• Agglomerates with small process zones
compared to granule size break by brittle
fracture into smaller fragments
g
(fragmentation or fracture).
• Agglomerates with process zones of the order
of their size, break by wear, erosion, or
attrition – due to insufficient agglomerate
volume to concentrate enough elastic energy
to propagate gross fracture during a collision.
• Agglomerates formed with very weak bonds
may shatter into small fragments or primary
particles.

16
Controlling Breakage
• Both fracture toughness and hardness are strongly influenced by
p
the compatibilityy of the binder with the p
primaryyp
particles,, as well
as the elastic/plastic properties of the binder.
• Hardness and toughness increase with decreasing granule
porosity, and influenced by previous consolidation of granules.
• Increasing gas velocity and bed height increases breakage of
dried granules, but reduces the breakage rate of wet granules due
to increased consolidation and density (lower porosity).
• Granule structure also influences breakage rate, e.g. a layered
structure is less prone to breakage than a raspberry-shaped
agglomerate.
• Measurements of fracture properties help define expected
breakage rates for a product and aid product development of
formulations.
formulations
17
Granulation Equipment
• Three main types of granulators in common use:
Tumbling granulators
 Disc drum
Disc,
Mixer granulators
 Continuous, batch high shear
Fluidised bed granulators
 B bbli
Bubbling, spouted
t dbbeds
d

18
Granulation Equipment
Granulation Product Granule Scale/ Comments Typical
Method granule density throughput applications
size
(mm)
Tumbling 1 - 20 Moderate 0.5
0 5 - 800 t/h Very Fertilizers, Iron
Fertilizers
disc, drum spherical ore, Agricultural
granules chemicals
Mixer 0.1 - 2 Handles Chemicals,
continuous Low < 50 t/h cohesive Detergents,
& batch high High < 500 kg materials Pharmaceuticals
Pharmaceuticals,
shear batch well Ceramics
0.1 - 2 Low < 50 t/h Good for Continuous
Fluidised (agglome coating, (Fertilizers,
bubbling, -rated) Easy to Detergents)
p
spouted High
g 100 - 500 scale up,
p, Batch
beds (layered) kg batch Not for (Agricultural
cohesive chemicals,
powders Pharmaceuticals)

19
Granulation Equipment
Tumbling granulators
• tumbling motion is imparted to the
particles in an inclined cylinder (drum
granulator) or pan (disc granulator).
granulator)
• operate in continuous feed mode and
able to deal with large throughputs
throughputs.
• can produce spherical granules in
sizes 1-1 20 mm.
• inherent size classification action in
disc granulators results in products with
narrow size distributions.
• drums up p to 4 m dia and discs to 10 m,, Disc Granulator
with throughputs up to 100 t/hr
• widely y used in industryy ((minerals,,
fertilizers, agricultural chemicals).
20
Tumbling Granulators

Mars Mi
M Minerall Pelletizer
P ll ti with
ith deep
d
pan design and rear feed.
(Mars Mineral Corporation)
Pelletizing disc with re-roll ring.
ring
(Dravo Corporation)
21
Granulation Equipment
Mixer Granulators
• have agitator to mix particles and liquid to
cause granulation.
• rotation speeds from 50 rpm in horizontal
mixers used for fertilizer granulation, to
> 3000 rpm in vertical Schugi high shear
granulator for detergents & agri. chemicals. Horizontal axis Mixer Granulator
• for vertical axis mixers used in pharma.
pharma
industry, impeller speeds range from 500 -
1500 rpm for mixers less than 30 cm in
diam., to 50-200 rpm for mixers > 1 m.
• can produce small (< 2 mm) high-density
granules by controlling amount of liquid
and intensity & duration of mixing
• can process plastic, sticky materials Vertical axis Mixer Granulator

22
Mixer Granulator – High Shear

Schematic of a
bottom-driven
bottom driven high
shear granulator
(Glatt/Germany)
Horizontal axis Mixer Granulator

Technical
T h i l ffeatures
t off high
hi h shear
h
granulators - patented Z-rotor
and chopper (Glatt/Germany) Vertical axis Mixer Granulator

23
Granulation Equipment
Fluidised bed granulators
• b
bubbling
bbli or spouted
t dbbed.
d
• batch or continuous
• liquid binder and wetting agents
are sprayed in atomized form
above or within the bed.
• produce high-porosity granules
by agglomeration or high-strength
layered granules by coating
• good heat & mass transfer, mechanical simplicity, ability to
combine drying with granulation and to produce small granules
f
from powder
d feeds.
f d
• High running costs & attrition rates cf. other granulators
• Applications: chemicals, agri-chemicals, pharmaceuticals.
24
Fluidised bed granulators

Horizontal fluidized bed for

Batch fluidised-bed unit with continuous processing
exchangeable material
container
t i (Glatt/Germany)
(Gl tt/G )
25
References for Further Study

R. Holdich,
R Holdich Fundamentals of Particle Technology
Technology, Midland
Midland,
2002.
R H Perry and D
R.H. D.W.
W Green
Green, Perry's Chemical Engineers'
Handbook, 7ed., McGraw-Hill, 1998.
M Rhodes,
M. Rh d IIntroduction
t d ti tto P Particle
ti l TTechnology,
h l 2
2ed.,
d Wil
Wiley,
2008.
K.P. Hapgood, et al., ‘Granule rate processes’ in Granulation,
Handbook of Powder Technology, Vol. 11, A.D. Salman et al.
( d ) Elsevier,
(eds), El i L London,
d 2007
2007, p. 933
933.

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