Powder

Technology.

44 (1985)

227

227

- 237

Mechanical Properties of Moist Agglomerates in Relation

Mechanisms
Part I. Deformability
of Moist, Densified Agglomerate8
H. C. KRISTENSEN.
Deportment

E. HOLII

of Phornroccuticc,

to Granulation

nnd T. SCHAEFER
Royal Danish School

of Pharmacy.

2 UkvcrsirctsParherS

DK-2100

Copcnhagcn

(Denmark)

(Received Fcbruan 5. 1985)

-SUAIMARY

The mechanical properties of moist samples

of fine. potydisporsa
powders
are inuestigated
by measuring
the tensile strength by a diametrical compression
test and the stress
strain relationship of .samples exposed
to
uniaxial comprcsvion.
The strengths dctermined by the two methods correlate well.
The strength of moist samples compressed
to porosities comparable to the level of intragranular porosltics
achieved by granulation
in high-speed mixers is shown to bc infiusnced significantly
by particle interactions
in
addition to mobile liquid bondings. For a
particular material the strength is controlled
mainly by porosity
and liquid saturation.
It is shown that the effect of a growing liquid
saturation is to reduce particle interactions
and thus to facilitate densification
during
granulation.
The deformability
of moist
samples, which is dependent
on strength and
deformation
behauiour, is assessed for lactose
and dicalcium phosphate.

INTRODUCTION
In a recent work on granulalion in a highspeed mixer [ 1, 21, it was shown that power
consumption
and granule growth rate were
correlated with the liquid saturation of the
moist granules, i.e. the dcgrce of filling intragranular voids with binder solution. Evaluation of the deformation
behaviour of moist
samples of the starting materials revealed that
the samples changed from brittleness at
lower liquid satur-tlons into L state charactcrixed by plastic deformation
at higher liquid
saturations. The change from brittleness into
0 032-5910185/$3.30

-_-._-

-~.--

plastic bchav;our occurred in the same range

of liquid saturations where power consumption and granule growth increased rapidly
against a slight increase of the saturation.
It was suggested that the power consumptivn to agitate the mass is dependent on the
strain behaviour
of moist, agglomcntes
esposed to external stresses due to agitating.
tumbling, rolling, etc. The strain behaviour
also influences the granule grolvth by coalescence according to the generally accepted
model
for granlllation
mechanisms
[3].
The
demonstrated
correlation
between
power consumption
and granule growth can
therefore be explained.
It means that the
deformability
of moist agglomerates
must
be one? of the principal factors that govern
granulation mechanisms and granule growth,
cc also Kapur [ 4 1.
The deformabllity
of a moist agglomerate
comprises its strength as well as its ability
to be strained without degradation.
The
preliminary study on stress-strain relationships of moist samples [l] showed that the
strength was reduced as the liquid saturation
was increased at a fixed sample porosity.
If this is valid in general for the dense
aggglomcrutes produced in a high-speed miser.
it means that a growing liquid saturation
on the one hand facilitates densification
of
the moist agglomerates due to the reduction
of the strength, and on the other hand improves the deformability
and, hence. rhc
granule growth rate due to its cffcct upon the
strain behaviour.
The results of a study on the tensile
strength and stress-strain
relationship
of
moist snmplcs of the starting materials used
previously for the granulation experiments
[I, 21 arc reported below. Since the high0 Elsevier

Sequoia/Printed

in The

Ncthnrlends

22s

speed mixer densifies the granules to porosities well below 40%, emphasis was placed on
investigating the strength and strain behaviour of moist samples with porosities in the
same range. The effects of the particle size
distribution
on the stress-strain
behaviour
and the granule growth rate are dealt with in
Part II of thus paper [ 5]_

STRENGTH

OF MOIST

AGGLOMERATES

Rumpf
[6] claimed that moist agglomerates are brittle with the exception
of the
most moist. When a brittle agglomerate is
strained, the particle packing undergoes
rearrangements
so that tensile stresses leadmg to fracture occur_ The tensile strength is
therefore of particular interest m connection
with the strength of moist aggIomerates
against strain induced
by compression,
impact, shear, bending and abrasion
It is
usually accepted that the strength of moist
agglomerates
IS controlled
by mobile liquid
bondmgs according to the theoretical model
developed
by Rumpf and his co-workers
161. The theory is presented in major monographs on granulation techniques
[3, 4, i] _
Principles for measuring the tensile strength
are reviewed by Schubert [ 8]_
Rumpfs model for mobile liquid bonding
strength presupposes
that the particles are
monosized spheres. In normal practice, however, the constituent
particles exhibit a size
dispersion and the content of fines plays a
dominant
role m determining
the strength
[-Cl - Further, theoretical
studies of tensile
strength do not account for irregularly shaped
particles, nor for the large changes of tensile
strength with porosity of the particle packing
that have been observed [ 91 unless adhesion
strengthenmg due to effects of compressional
forces are taken into consideration
[lo] _
A few experimental
studies on tensile
strength of moist samples of polydisperse
powders
are reported_ Eaves and Jones
[ll
- 131, who used the traction table
method.
showed that the tensile strength
of fine, cohesive powders of sodium chloride and potassium chloride increased significantly when a small amount of water was
added. Further addition produced decreasing
tensile strength values. In the case of calcium
phosphate,
the tensile strength remained

constant until the mass was saturated with

water. The studies concern samples with porosities above 60%_ Tensile strength of moist
samples of calcium carbonate with porositres
below 50% was measured by Takenaka et al.
[ 141, who used a diametrical compression
test. They reported that the tensile strength
had a maximum
at liquid saturations of 20
to 30%
Beyond that, the tensile strength
was reduced against increasing liquid saturations_ The tensile strength values were significantly larger than the strength to be expected
from Rumpfs model on mobile liquid bondings. Mitsui 1151 showed an effect of water
content on breaking strength of calcium carbonate samples which was very similar to the
effects observed by Takenaka et al. [14] _
Finally, in our preliminary
study on stressstrain relationships
of moist samples of
lactose and dicalcium phosphate exposed to
one-dimensional
compressive
stresses, it was
shown that the strength had a maximum
at
liquid saturations of 15 to 25%, and that the
strength was reduced as the liquid saturation
was further increased_
It is apparent that experimental
findings
on the strength of moist samples of polydisperse powders are not consistent
with
theoretical
models
on effects of mobile
liquid bondings. The tensile strength is higher
than expected,
and the effect of moisture
IS a reduction of the strength, in contrast to
the models which claim an increasing strength
with Increasing liquid saturation_

EXPERIMENTAL

For pratical reasons it IS not possible to

measure the strength and deformation
behaviour of moist agglomerates
produced
in a
high-speed mixer. The maximum agglomerate
size achieved is usually below about 5 mm.
The measurements
have therefore to be made
upon moist samples compressed
to the
required porosity , which is below 40%.
For the present study it was decided to
compress moistened powders in a cylindrical
die using a very low punch speed, allowing
the particles to adjust to the dense packing.
An attempt to measure the tensile strength
by the wall adhesion test [S] failed because
residual tensions in the sample gave rise to
very low tensile strength values. The com-

229

TABLE

Starting materials for the investigation

b
sgn-

Material

Lactose
Dicalcium phosphate
Glass spheres

56
14
68

1.8
2.2
1.2

Specific
surface area=
(ma lg)

Particle
densi
y
(g/cm
)

0.30
-

1.51
2.34
2.39

0.04e

=Geometric mean weight diameter

nGeometric standard deviation determined as the ratio of the 50Y0 to the 15.87%
=Determined by a Strijhlein@Area Meter
dDetermined by a Beckman@Air Comparison Pycnometer
rCalculated from particle size distribution

pressed samples were therefore removed

from the die and submitted to a diametrical
compression
test or a uniaxial compression
test.
Objections
may be raised to direct comparison between the strength of moist agglomerates produced in the granulating equipment
and that of moist samples prepared
by
compression
in a die, because the final
packing configurations
may well be differe&,.
This is valid especially when the moisture content or liquid saturation is low_ Therefore,
measurements
on samples prepared
with
liquid saturations below about 20% were
omitted.
Materials
The starting materials used were lactose,
dicalcium
phosphate
(calcium
hydrogen
phosphate)
and glass spheres, the two first
mentioned
of Ph. Eur. grade. The materials
are described in Table 1. For the preparation
of moist samples, the materials were moistened with purified water or an aqueous solution
of a PVP-PVA
copolymer
(Kollidona
VA
64?). The concentration
of the binder solution was 10% for lactose and 15% for dicalcium phosphate and glass spheres in accordance with the granulation experiments
[ 1,2] _
Table 2 gives the surface tensions of the
liquids and their contact angles to the starting materials_ For glass spheres, the contact
angles could not be measured, but they are
assumed to be close to zero. For lactose, the
*Supplier: DMV (The Netherlands)
**Supplier:
*Supplier:

Albright & Wilson (U.K.)

BASF (F.R.G.)

TABLE

size of the distribution

Contact angles of lactose and dicalcium phosphate

and surface tension of the moistening liquids (25 C)
Contact

Moistening
liquid

;Fo:e

Surface
tendon b
(mN r-n- )

CS

72

39

47

45

Lactose

Water
Kollidon@
lOwt.%
Kollidori9
15wt.s

anglea

Material

VA 64
in water
VA 64
in water

aDetermined
bDetermined

by the Kossen -Heertjes method

by the drop-weight method

[21]

contact angles were measured using liquids

saturated with lactose.
The material to be tested was wetted with
purified water or the binder solution. It was
then sieved and allowed to equilibrate
by
storage of the moist mass for 24 h in a closed
container_ A cylindrical sample was prepared
by compression
of the moist mass in a die
with a punch speed of 100 ,um/min. The mass
of the sample and its moisture content were
chosen so that cylinders with specified dimensions and with predetermined
porosity
(on
the dry basis) and liquid saturation could
be prepared. Before the test, the dimensions
of the sample were controlled by a dial gauge.
The moisture content was determined
by
drying and weighing. Knowing the mass of
the sample, its dimensions, the moisture content and the particle density, the sample
porosity and liquid saturation could be calculated.

The moist samples of lactose could be compressed to porosities between 13 and 30%.
Further compression gave rise to formation
of a hard shell at the die wall and a nonuniform liquid distribution in the sample. For
the same reason, moist samples of dicalcium
phosphate could be compressed to porositics
between 50 and 37%.
Tensile

strength

For the tensile strength measurements,

cylindrical samples with diameter 11.3 mm
and length 5.6 mm were prepared. The
measurement
was performed
by applying
a load across the diameter of the sample.
At a critical load, the sample fractures along
the diameter parallel to the load. Provided
that the sample is brittle up to the limiting
load and that there is an exact line loading,
the tensile strength is given by [ 81
2P
Crt= _-oI,

010
3.[

Fig. 1. Tensile strength of moist ~1as.s sphcrcs. E =

0, Wetted with water; l . wetted with a 15%
aqueous solution of Kollidon@ VA fX; I. hizhcst and
lowest me;auremcnt3 uf four.
42%.

CL)

IS the diameter and L the length of the

sample. P is the limiting load causing fracture.

The sample was loaded between twc flatfaced punches driven hydraulically at a constant rate of 100 pm/min.
The load was
measured by an electric load transducer
Kistlcr Type 9203
or a strain gauge system
using a Philips PR9307
carrying a
frequency
bridge. _4n LVDT displacement
transducer Type 1315
was used for the strain
measurement. The record was obtained by an
X-Y
n-corder.
Preliminary experiments showed that moist
samples with low and moderate liquid saturation were brittle and behaved during loading
as described above. At high liquid saturations,
however. some samples could he strained
without being fractured. This means that with
the present technique there was an upper
limit beyond which the tensile strength could
not be measured.
Figure 1 shows the correlation
between
tensile strength and liquid saturation for
moist samples of glass spheres.
Both graphs

*Manufacturer.
Kistler
Instrument
AG. CH-8408
\Vmterthur (Swrtzerland)
++iCIanufacturcr: Philips, Eindhoven (The Netherlands)
Pfanufacturer:
Penny & Giles Potentiometers Ltd.,
Christchurch, Dorset (U.K.)

refer to samples with 42% porosity. Due to

the method of preparing the samples, the
porosity could not be varied more than a
few per cent :rom 42%. The vertical bars
give the variat :on between highest and lowest
measurement
of four. It appears that the
variation was high at the highest liquid saturation utilized. This is due to plasticity of
the samples, which gives rise to uncertainties.
The range of tensile strengths presented in
the graphs as well as the effect of the bquid
saturation agree well with Rumpfs
model
for the effect of mobile liquid bondings, cfi
Schubert [ 81. The tensile strength of samples
moistened with the binder solution is slightly
less than the strength of samples moistcncd
with water. This is in agreement with the
expected effect of the surface tension of the
two liquids, see Table 1.

UNIAXIAL

COMPRESSION

TEST

Records of the stress-strain relationship

were obtained by loading the cylindrical
sample on the flat face with a constant
strain rate of 100 I.tm/min using the same
equipment
as described
for the tensile
strength measurement.
Preliminary experiments
showed that the
stress-strain record was influcnccd
by the
length of the cylindrical sample. A length

231

Fig. 2. Stre.ss+.train relationship with cyclic unloading and loading for dicalcium phosphate.
Sample
porosity 4590, liquid saturation 57%.

I
0

20

40
l.iquld

so

so

saturation

Fig. 3. Tensile abrength of moist samples of lactose

wetted with water. 0, E = 43%; A, E = 37%; x , f =
30%.

to diameter ratio value of 1 was chosen

for
the measurements
according to gmdelines
given for testing moist soil materials by the
triaxial compression
test [17]_
Figure 2 shows a stress-&ram record with
cyclic loading and unloading for a dicalcium
phosphate
sample with porosity
45% and
liquid saturation of 57%. According to tensile
strength measurements,
the sample behaved
like a brittle mater&.
The record demonstrates, however, that the strain is far from
that of an ideal elastic-brittle
body.
The
strain at stresses well below the maximum
stress is partially plastic.
Schubert et al [16] have demonstrated
a similar strain behaviour of moist limestone samples exposed to tensile stresses.
They claimed that the plastic part of the
deformation
is characteristic
for agglomerates with different
bonding mechanisms.
For the present sample, Fig. 2, the plastic
deformation
is likely to be due to effects
of particle interactions,
mechanical
interlockings and mobile liquid bondings. Additional experiments
showed that the plastic
deformation
took place to some extent at
all liquid saturations and porosities.
Preliminary
results for the strain behaviour of moist samples of lactose and dicalcium phosphate
were reported previously
[l] . It was shown that the strain required
to fracture the moist sample increases as the
liquid saturation is increased. At a limitmg
liquid saturation depending on the porosity,
the deformation
became purely plastic.

Fig. 4. Tensile strength of moist -pies

of lactose
wetted with a lOwt.% aqueous solution of Kolhdon@
VA 64. 0, E = 43%; A, E = 37%; X, E = 30%.

TENSILE

STRENGTH

OF MOIST

SAMPLES

Figures 3 to 6 show tensile strength against

the liquid saturation of samples of lactose and
dicalcium phosphate_ Each point in the graphs
represents the mean of two measurements.
In general a measurement
could be reproduced with a standard deviation of about 7%.
The drawn lines in the graphs are regression
lines, the calculation
of which is mentioned
below.
The figures demonstrate
that the sample
porosity has a pronounced
effect upon the

232

ular, the tensile strength of dicalcium phosphate samples is very high.

Figure 3 to 6 demonstrate
that the tensile
strength is influenced by the moistening
liquid in addition to the effects of porosity

Fig. 5. Tensile strength of dicalcium phosphate

wetted with water. +, E = 50%; o, E = 43%; A, E = 37%.

and liquid saturation_ The strength of samples

moistened
with the binder solution is less
than the strength of samples moistened with
water, but the difference
between the two
liquids diminishes as the liquid saturation is
increasedThe results of the investigation
demonstrate that the tensile strength of moist
samples of the present fine, polydisperse
powders
is significantly
higher than the
strength caused by liquid bondings.
Thus,
particle-particle
interactions
must be active
in addition to liquid bridges and capillary
pressures_ Due to the effect of the sample
porosity on tensile strength, the results bear
resemblance
to the tensile strength of dry
powder compacts.
Chan et al. [19] have recently presented
a theory of the tensile strength of single
powders and binary mixtures. The following
equation
was derived and verified experimentally :

(2)
(Y is a material

20

40

SO

so

Fig. 6. Ten&e strength of dicalcium phosphate wetted with a 15 wt.% aqueous solution of Kollidon@
VA 64. +. E = 50%; o, E = 43%;a, E = 37%

tensile stength. Graphs of the tensile strength

on a log-scale against porosity
produced
straight-line
relationships
for fixed liquid
saturation_ This means that the effect of porosity is the same as its effect upon the tensile
strength of dry powder
compacts
[18] _
Further, the figures show that the effect of
liquid saturation is a reduction
of tensile
strength as the saturation is increased_ Comparing the observed tensile strength values
with theoretical
models for mobile liquid
bondings,
the present vahres appear to be
higher than the strength caused by liquid
bridges and capillary pressures. In particu-

characteristic
describing the
intnnsic interaction between like particles in
a pair. m, k and g are universal constants.
t expresses the distance of separation between
two particles. E is the porosity of the particle
packing. ;i, Sand V are the mean effective
diameter, surface area and volume, respectively, of the particles.
For a particular powder, eqn. (2) can be
simplified:
o,=A

l--E
--

o!
t

(3)

where A is a material characteristic_

For
reason of srmplicity, the constant m of eqn.
(2) has been given the value 1 which IS close
to the experimental
value of 0.975 estimated
by Char-r et al. [19].
It was investigated whether the tensile
strength values presented in Figs_ 3 to 6
could be interpreted on the basis of eqn.
(3). If so, the distance parameter t must take
a constant value at a particular porosity,
independent
of the liquid saturation and the

233
TABLE

Estimated

.
of parameters A, 01and f of eqn. (3) derived from tensile strength measurements

Parameter

Lactose

Sample porosrty
t Wn)

(a)

Liqmd saturation (%)

a(N-m/cm)
(water)
a(N-/&n/cm*)
(Kollidon@
1Owt.Z in water)

VA 64

Parameter
Sample porosity
f Wm)

Liquid saturation (%)

cr(N-m/cm*)
(water)
cu(N-m/cm*)
(Kollidon@
lOwt.70 in water)

in Figs. 3 - 6
A = 0.951

43
4.9

37
3.1

30
1.3

15
1.23

25
1.10

35
0.96

45
0.81

0.79

0.71

0.62

0.52

Dicalcium
(%)

presented

phosphate

A = 1.03

SO
2.25

43
1.40

37
0.70

30
9.02

50
7.23

70
4.78

90
2.72

6.74

5.44

3.63

2.38

VA 64

moistening
liquid
used.
CY, which
expresses
the interaction between particles in a pair,
was assumed to take a constant value at a
particular liquid saturation_ a! is expected
to depend on the moistening liquid.
Estimates of A, a and t were obtained
by the trial-and-error
method described by
Chan et al. [ 19]_ The estimates are given in
Table 3. It is noted that estimates of t for
each material are common for samples moistened with water and the binder solution_
The lines drawn in Figs. 3 to 6 are calculated
by inserting the estimates of A, CY and t (Table
3) in eqn. (3).
The figures demonstrate
an acceptable
agreement between the experimental
tensile
strength values and eqn. (3). The deviations
of the points from the drawn lines are of the
same magnitude as the deviation between two
repeated measurements.
The tensile strength
measurements
can therefore
be interpreted
on the basis of eqn. (3).
Figures 7 and 8 show the relation between
liquid saturation and the estimates of CY_
According
to eqn. (3), LYhas the dimension
of work. It expresses the work required to
fracture samples in a standard state with
unit mean distance between particles. The
two graphs demonstrate
that the effect of
an increasing liquid saturation is a reduction
of the work required to separate the particles_ The reduction is proportional
to an
increase in the liquid saturation. The effect

Fig 7. Intrmsic interaction parameter CYfor lactose

wetted with water (0) and a lOwt.% aqueous solution
of Kollidon@ VA 64 (e)_

of the moistening
liquid may be compared
to the effect of a lubricant which reduces
particle interactions.
The correlation
between (Y and the liquid
saturation is dependent
on the liquid- The
effect of dissolving the binder in water is
a reduction of Q, and hence a reduction of the
particie interactions_ The binder solution,
therefore, facilitates compaction
of the morst
agglomerates
dunng granulation,
which in
turn gain strength due to the effect of the

234

which shows that the effect of particle interactions diminishes at high liquid saturations,
so that the strength is controlled
by liquid
bondings.
The interpretation
of the tensile strength
measurements
on the basis of cqn. (3)
involves an estimation
of the distance of
separation f between particles in the sample.
The estimates of L (Table 3) show that t is
dependent
on porosity.
t depends also on the
particle size of the material, but further inferences about the distance parameter cannot bc
made from the present results.
UNIAXIAL
SAMPLES
Fig. 8. Intrinsic interaction p.w:kmetcr Q for dicalcium phosphate wetted with water (0) and B 15wt.X
aqueous solution of Kollido#
VA 64 (0).

porosity
upon the tc.lsile strength of the
moist agglomcrat.
F;gure 7 she .JS that an extrapolation
of the
correlation
to 100% saturation reduces 01 to
zero. Ihls means that the strength of lactose
samples which arc nearly saturated is indepcndent of particle interactions
and depends
only on mobile liquid bondings.
In the case
of dicalcium phosphate,
Fig. 8. the extrapolation to 100% saturation
shows that there
remains a significant particle interaction.
For
this material the tensile strength of the saturated samples is considerably
higher than the
strength caused by capillary pressures.
A previous study [ 11 on the granulation
of dicalcium phosphate
showed that a rapid
gr-nule growth by coalescence did not occur
until the agglomerates
were almost saturated
with binder solution.
Degradation
of the
saturated agglomerates
was not detected. The
saturated agglomerates
must therefore possess
sufficient strength to withstand the agitation
ir. the high-speed
mixer. This agrees with
Fig. 8, showing that a certain strength remains
in the saturated sample. This may be due to
the surface roughness of the particles. On
eanulating
the present quality of lactose,
which consists of particles with a fairly
smooth surface, the moist mass had the
appearance
of an ovenvetted
mass at liquid
saturations
vf about
70Y0. At. higher
saturations, the granular structure of the mass
disappeared.
This is in agreement with Fig. 7,

COMPRESSION

TEST

ON MOIST

The typical record of the stress-train

relationship obtained by the uniaxial compression
test has been demonstrated
carlicr, set Fig. 8
in [l] . The record shows an approximately
linear increase in the stress required to maintain the constant strain rate. At a certain
strain, referred to hereafter
as thct critical
strain, the stress reaches a maximum
which
is called the critical stress. A brittle sample is
crushed when the critical stress is reached or
immediately
after the maximum is passed,
while a perfect plastic sample maintains the
masirnum or critical stress at continuing
strain.
The critical stress of the present qualities
of lactose and dicalcium phosphate moistcncd
with an aqueous solution of KollidonO
VA
64 is shown in Figs. 9 and 10. The moist
samples were prepared
with the same poroskies as utilized for the tcnsllc strength
measurements.
In the two graphs, each point
represents the mean of two measurements.
The standard deviation
of a measurement
was about 7%. as for the tensile strength
measurement.
A comparison
between tensile strength and
critical stress of the moist samples revealed
that they were proportional.
This is shown
by the lines drawn in Figs. 9 and 10. The
lines were calculated according
to the relation
UC, = co,

(4)

u cr denotes the critical stress and u, the

tensile strength derived from eqn. (3) using
the estimate
given in Table 3. C is a proportionality constant. The value of C used for

235

9. Critical stress of lactose samp+

moistened
with a lOwt.70 soIution of KollidonW VA 64. 0,
Porosity 43%; 0, porosity 37%; 0, porosity 30%.

Figs. 9 and 10 is considered acceptable,

taking the standard deviation of the measurements into account.
Hence, the strength
of moist samples of a particular material may
be investigated using the uniaxial compression
test as well as the tensile strength measurement. The correlation
between
the two
strength measurements
must rely upon the
intrinsic interaction parameter c~ of eqn. (3).
In the uniaxial compression
test, the work
required to separate the particles and thus
to deform the sample is Car times the work
required for separation by tensile stresses.
In the uniaxial compression test, the load
applied to the sample induces shear and
tensile stresses leading to deformation
of the
sample. A high value of constant C indicates
a high ratio of shear to tensile strength, and
that the sample is primarily brittle according
to Rumpf [ZO] _ The brittleness of the samples
is therefore expected to decline in the order:
dicalcium phosphate,
lactose, glass spheres.
This has in fact been confirmed by the previously reported effect of liquid saturation
upon the critical stram of moist samples of
the three materials [l] _ It was shown that
moist samples of lactose became perfectly
plastic at liquid saturations above about 25%,
depending on the sample porosity.
When
the porosity
is reduced, the change from
brittleness to plastic deformation
requires
an increasing liquid saturation. For dicalcium
phosphate of the present quality, the moist
samples with porosities below about 40%
remained primarily
brittle until complete
saturation with liquid.

CONCLUSIONS
Fig. 10. Critical stress of dicalcium phosphate samples
moistened with a 15wt.% solution of KoIIidon@ VA
64 o, Porosity 50%; @, porosity 43%; 0, porosity
37%.

the calculation
was 9.98 for lactose and 19.7
for dicalcium phosphate_ It was found that
C is independent of the liquid used for wetting the powder. It is therefore dependent
only on the properties of the solid particles.
For glass spheres, the comparison between
tensile strength and critical stress showed
that they were proportional with C = 5.00.
The

agreement

between

the

measurements

of the critical stress and the lines drawn in

It 1s shown that the tensile strength of

moist samples determined by a diametrical
compression test is correlated with the critical
stress determined
by uniaxial compression.
For a particular material, the two stremgth
values are shown to be proportional.
The
proportionahty
constant C, defined by eqn.
(4), is dependent
on the shear to tensile
strength ratio of the sample_ A high value
indicates that the material forms moist
samples that are primarily brittle, while a low
value indicates that samples with plastic
deformation
are formed. For the purpose of
studying the effect of liquid saturation and

236

porosity
on the stressstrain
behaviour
of
a particular material, the simple uniaxial
compression
test may be applied as well as
the diametrical compression
test.
The investigation of two fine, polydisperse
powders compressed
to moist samples with
porosities on a level comparable
to the range
of intragranular porosities appearing in highspeed mixers demonstrates
that the strength
of the moist samples is affected by particle
interactions
in addition
to the effects of
mobile liquid bondings. It means that the
strength
is intermediate
between
the
strength of dry compacts
and the strength
due to mobile liquid bondings. The effect of
particle interactions
diminishes as the liquid
saturation of the sample is increased. The
strength
of the moist samples increases
rapidly with a reduction of the sample porosity_
Applying the model for tensile strength of
dry powders proposed by Chan ef aZ_ [19],
it
is shown that the particle interactions
are
reduced proportionally
to an increase in the
liquid saturation.
For lactose which consists
of rounded particles with a smootll surface,
the contribution
of particle interactions
to
the strength becomes
insignificant
at high
liquid saturations.
At the same time, the
moist samples exhibit plastic deformation.
For dicalcium phosphate
with irregular particles of rough surface, there remains a certain strength at complete
saturation. At the
same time the moist samples remain brittle
until saturation. These effects compare well
with the results obtained by granulation of
the two materials m a high-speed
mixer
[1, 2]_ It supports the assumption
that
the deformability
of moist agglomerates
is essential to granule growth by coalescence.
Inferences about the strength and deformation
behaviour
of moist
agglomerates
produced in a high-speed mixer from the
present results may be questioned_ Compression of the moist mass in a die may well give
rise to a packing configuration
of the particles
which differs from that in the moist agglomerate. Another
aspect is that the liquid
distribution
in the agglomerate
is likely to
be non-uniform
due to capillary effects. It
is striking, however, that there is an agreement between the effect of the liquid saturation upon the stress-strain
behaviour of the

moist samples and the granule gro-&h pattern in the high-speed mixer.
Assuming that the results of the present
study are applicable
to the stressstrain
behaviour
of moist agglomerates
produced
in a high-speed mixer, it is concluded
that
the major effect of the binder liquid is to
facilitate
the densification
of the agglomerates. The liquid acts as a lubricant because
it reduces particle interactions.
In that respect
the aqueous solution of Kollidon@ VA 64 IS
more efficient than purified water. Due to
densification,
the agglomerates
gain strength
during the granulation
process. According
to the assumption
that growth by coalescence is facilitated
by a large deformability,
the densification
of the agglomerates
is
expected
to counteract
the granule growth.
This aspect of granulation
theory is dealt
with in Part II of this paper [5] -

ACKNOWLEDGEMENTS

The work was supported financially by the

Damsh Council for Scientific
and Industrial
Research.

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