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Ind. Eng. Chem. Res. 1999, 38, 1911-1916 1911

A Model for the Bulk Crushing Strength of Spherical Catalysts

Yongdan Li,*,† Dongfang Wu,† Liu Chang,† Yahua Shi,‡ Dihua Wu,§ and
Zhiping Fang§
Department of Catalysis Science and Technology and State Key Lab on C1 Chemical Technology, School of
Chemical Engineering, Tianjin University, Tianjin 300072, China, Research Institute of Petroleum Processing,
Beijing 100083, China, and SINOPEC Technology Company, China Petrochemical Corporation, A-6 Huixin
Dongjie, Chaoyang District, Beijing 100029, China

Statistics and experiments reveal that the mechanical failure of a spherical catalyst under single-
particle crushing strength and bulk crushing strength tests are both brittle fracture and the
fact that the single particle strength data follow a Weibull distribution. A model is proposed for
the packing of spherical particles, which assumes tetrahedral contact and force transmission
between the spheres. A deduction from this packing is that the broken percentage of spheres
during bulk strength measurement follows the relationship of the Weibull equation. Experimental
results confirm this conclusion, which relates the single particle property and the bulk behavior
of the packed bed of catalytic materials.

1. Introduction presents BCS data as the curves of the percentage of

The mechanical strength of solid catalyst is one of the
most important factors for the reliable and efficient
performance of a fixed-bed reactor.1,2 Its measurement
was discussed in a small committee of AIChE in 19743-6
and was written as one of the most important charac-
terization techniques in the textbooks of catalysis.7,8
Single-particle crushing strength (SPCS) and bulk
crushing strength (BCS) of a small bed have been
proposed as the two most important methods. The SPCS
method has been accepted as the standard in many
countries,9-11 while the BCS method and data are often
found in the literature.7 Nevertheless, up to now, the
scientific basis for both the SPCS and BCS measure-
ments and the relationships between the SPCS and BCS
data of one single sample are still not clear.
A probabilistic method has been used in publications
from this group in the description of the scattering
property of the SPCS data of cylindrical tablets.12-17 It
has been proposed that the solid catalysts are typical
brittle materials and their strength failure is due to
brittle fracture.12 The Weibull equation has been proved
to be successful in the description of the scattering
properties of the SPCS data of tablets.12-17
Solid catalysts have a wide spectrum of shapes. They
are normally in the state of mixed oxides, though in less
common cases a prereduced form is available, which is
a mixed oxides supported highly dispersed metal; in
these cases the matrix which offers the strength is
mixed oxides. These are all brittle materials. Their
behaviors before strength failure can be assumed to obey
the laws of elasticity. Among their different shapes,
spherical and cylindrical shapes are the ones with which
the analytical solution of elastic equations is possible.
The BCS data of solid catalysts have been recom-
mended to be more reliable than those of SPCS. BCS
has a closer meaning to packed beds and is supposed to
be applicable to catalysts of all shapes.7 The literature
* Corresponding author. E-mail: ydli@tju.edu.cn.
† Tianjin University.
‡ Research Institute of Petroleum Processing.
§ China Petrochemical Corp.
fines and displacement versus the pressure applied.4,7
A major difficulty encountered in the modeling and
correlation of the data to the particle properties exists
mainly due to the unclearness of the packing and
contact laws of various shaped particles in a packed bed.
Recently, a number of papers studied the packing
density and coordination number by computer simu-
lation;18-22 some others presented idealized mechanical
models of heaped granular materials.23,24 Kanda et al.25
investigated the energy consumption of compressive
crushing of large particles to small ones. Ouwerkert26
simulated the bulk crushing strength of spherical
particles by a distinct element method. However, there
is still a lack of literature on the relationship between
the percentage of failure and applied force and the
dependence of BCS on the properties of the particles.
In the present work, the relationship between BCS
and SPCS of ideal shaped spherical catalysts is dis-
cussed. Simplified models for the packing and the
correlation between BCS and SPCS are proposed. A
quite good fit of the experimental data is obtained.
2. Theoretical Section
2.1. Weibull Statistics for SPCS of Spherical
Catalysts. Because of the brittleness of catalytic ma-
terials and the tensile fracture nature of its strength
failure,12 the SPCS data of catalysts scatter in rather
large ranges. In our previous work, the Weibull distri-
bution has been used in the calculation of the mechan-
ical reliability of tablets. Here again, the SPCS data are
described by the Weibull distribution27
F(σ) ) 1 - exp(-β′σm) (1)
Hiramatsu and Oka28 gave an analytical solution of
the elastic equations for the two-point pressing of an
elastic sphere. They found that the tensile stress
induced has a maximum value at around the axis
passing the two contact points. They proposed that this
stress leads to the fracture and has a relation to the
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1912 Ind. Eng. Chem. Res., Vol. 38, No. 5, 1999

Figure 1. Tetrahedral packing of spheres (top view).

force as follows:
F forces F2 equals force F1. Therefore, every layer of
σ ) 2.8 (2)
πdp2
If the failure initiates on the surface, the tensile stress
leading to fracture should be calculated by29,30
F coordination number of 12. Any interior sphere contacts
σ ) 1.6 (3)
πdp2
It is reasonable to assume that the tensile stress
leading to fracture is proportional to the total load for
spheres with an identical diameter, no matter how the
fracture initiates. Combining eqs 1-3, we get
F(F) ) 1 - exp(-βFm) (4)
2.2. An Idealized Three-Dimensional Crushing
Model. In the BCS test, particles of catalyst are
randomly packed in a cylindrical container. An axial
pressure P, applied on catalyst particles via a piston, is
transmitted from one particle to another through con-
tacts. The effect of the weight of the particles in this
case is ignored.
A three-dimensional ideal pack of equal spheres has
been presented by Li and Bagster23 and can be shown
as in Figure 1. It has tetrahedral packing, which can
be approached by setting a distance between the par-
ticles within each layer of spheres of hexagonal dense
packing. Set the distance between the surfaces of any
two adjacent spheres in the same layer as 2δ; then each
sphere receives three supports and three contacts on its
top. In this case the coordination number of any interior
sphere is 6. A tetrahedral force transmission system of
the packing can be shown as in Figure 2.
When a pressure P is applied on the top layer of the
packing, each sphere of the top layer is subjected to force
F1.
Figure 2. Force transmission system of four spheres with three
contacts.
For the interior sphere, the resultant force of three
spheres has the same forced condition as the top layer
ones; that is, in the tetrahedral packing, all of the
interior spheres are each subjected to six contact forces
given by eq 6. In the case of δ ) 0, the tetrahedral
packing becomes dense rhombohedral packing with a
with another six spheres in the same layer. The spheres
inside are subject to six contact forces as in the above
model and another six contact forces to the other
spheres in the same layer, which results from the
limitation effect of these spheres to the deformation of
itself. However, the dense packing cannot be reached;
the real packing of the spheres is between the model
proposed above and the dense packing. It can be
convincing to do the analysis on the cases of δ > 0.
As mentioned by Ouwerkert,26 the force and stress
relation for the SPCS needs to be generalized to the
compression of a particle with a number of contacts.
According to eqs 2 and 3, the stress may be expressed
as proportional to F/dp2 for multipoint contacts. It is
reasonable to assume that the crushing strength of
spherical catalysts under six contact forces F2 also
follows a Weibull distribution.
F(σ) ) 1 - exp(-β0σm0) (7)
In eq 7, the tensile stress σ leading to fracture within
each sphere is supposed to be proportional to F2, i.e.
σ ) φF2 (8)
Substituting eqs 5, 6, and 8 into 7, we obtain
F(P) ) 1 - exp(-BPM) (9)
where
M ) m0 (10)

F1 )
x3
2 (
Pdp2 1 +
2δ
dp) 2
(5)
B ) β0 [x2
4
φdp2 f
δ
dp ( )]
m0
(11)

( ) ( )( )
The force F1 from each of the three adjacent top layer δ 2δ 2
2δ2 2δ 1/2
spheres, in turn, applies force F2 at three contacts of a f ) 1+ 1- - (12)
second layer sphere. dp dp dp2 dp

F1
( 2δ2 2δ
) Equation 9 gives the relationship between the applied
1/2
F2 ) 1- - (6) pressure and fracture probability of each sphere in the
x6 dp2 dp packing. Consequently, the broken percentage (i.e.,
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Ind. Eng. Chem. Res., Vol. 38, No. 5, 1999 1913

Table 1. Geometric Size and Textural Properties of the Catalyst Samples

ratio of pore volume in a
skeletal density particle density porosity surface area mean pore specific diameter range (%)
sample diameter (mm) (g/cm3) (g/cm3) (mL/g) (m2/g) diameter (µm) >50 nm >20 nm
A 4.43 ( 0.14 2.594 1.190 0.4548 168.3 0.0119 36.9 42.5
B 6.02 ( 0.14 2.149 1.371 0.2640 24.35 0.1971 75.2 87.1
C 5.75 ( 0.17 2.041 1.364 0.2434 25.69 0.1870 75.4 83.9

BCS Measurement. About 125 mL of spheres,

selected beforehand to eliminate broken and defected
ones, was charged. An increasing piston pressure was
applied to the top of the packed bed by a hydraulic
system oiled at a uniform rate. After pressure applica-
tion, the bed was removed and the broken spheres
including fines were chosen by hand. The spheres
broken or cracked with visible defects were taken as
failed ones. The weight percentage of broken spheres
and the ultimate piston pressure were recorded.
It should be mentioned that before all tests the
samples were heated in air at 200 °C for 4 h.
3.4. Data Treating. SPCS. Equation 4 can be put
into the form

ln ln ( 1
1 - F(F) )
) m ln F + ln β (14)

The maximum load F can be measured; F(F) can be

estimated by listing the SPCS data from the minimum
to the maximum value, i.e.

F1 e F2 e ... e Fi e ... e Fn-1 e Fn

Figure 3. Apparatus for the bulk crushing strength measure-
ment. Then the probability is estimated by31-33

relative amount of breakage) in the packing can be i - 0.5

Fi(F) ) (15)
obtained n
The Weibull parameters m and β can be obtained by
dm/m ) 1 - exp(-BPM) (13) linear least-squares regression between ln F and ln
ln(1/(1 - F(F))).
where the broken percentage dm/m is the mass ratio BCS. Equation 13 can be written as
of broken spheres.
1
3. Experimental Section
ln ln (1 - dm/m) ) M ln P + ln B (16)

3.1. Samples Used. Three spherical samples were
used in this work. One is γ-alumina (denoted as sample
A); the other two are 3A zeolite with different physical
properties (denoted as samples B and C). Their geomet-
ric size and texture properties are listed in Table 1.
Their texture properties and the pore size distribution
were obtained by an Autopore 9220 II porosimeter.
3.2. Apparatus. A scale permitting one to measure
two decimals after millimeters was used to get the
diameters of the spheres. SPCS measurements were
carried out with a ZQJ-II strength tester made in
Dalian, China. A balance used for the determination of
the weight has one decimal of precision after grams. The
BCS tests were performed using a typical device de-
signed by Beaver.3,4 The schematic diagram of the
apparatus is shown in Figure 3. The cylindrical sample
container is 54.26 mm in diameter and about 100 mm
in depth. The piston diameter is nearly equal to the
inside diameter of the container. The piston and con-
tainer are both made of stainless steel.
3.3. Experimental Method. SPCS Measurement.
The particle was loaded diametrically until failure
between the two anvils of the strength tester. The load
at which fracture of the sample occurred was recorded.
The total pressure P and percentage broken dm/m can
be measured. The parameters M and B can also be
obtained by linear least-squares regression.
4. Results and Discussion
4.1. SPCS. In the SPCS test, brittle fracture hap-
pened suddenly and completely, with the sphere break-
ing into several fragments. In some cases, the fragments
were nearly hemispherical, while fracturing to many
segment-shaped pieces was more frequent. The surface
of the section was not smooth but rather irregular and
has the features of typical brittle fracture, similar to
that of cylindrical tablets after the same measure-
ment.12,17
Table 2 lists the results of the SPCS tests on the three
samples. It can be seen that the SPCS data have a large
scattering range, which is the inevitable result of the
brittle fracture. For catalysts, they are porous and full
of defects, dislocations, and discontinuations in the bulk
phase; these are in the same range of size and nature
as the microcracks defined by fracture mechanics, which
are the origins of the stress concentration and lead to
the scattering of the data.
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1914 Ind. Eng. Chem. Res., Vol. 38, No. 5, 1999

Table 2. Results of the SPCS Tests of the Three Samples

SPCS (N)
sample mean standard minimum maximum Weibull Weibull size
sample size value deviation value value modulus parameter
A 53 56.2 19.6 22 99 3.02 3.83 × 10-6
B 88 36.3 11.1 11 66 3.56 1.81 × 10-6
C 86 43.9 17.9 10 90 2.87 1.40 × 10-5

in turn provides the possibility of reliability prediction.

Figure 4. Correlation of single-particle crushing strength with
a Weibull distribution funciton: ], sample A; 4, sample B; O,
sample C.
Figure 4 gives the quality of the fit of the SPCS data
with eq 4. These data are fit quite well. This is an
indirect evidence for the brittle fracture nature of the
strength failure and provides a possibility of the calcu-
lation of the probability of strength failure under specific
loading or stress conditions for these catalysts, which
The description of catalyst strength failure by prob-
ability should be more advanced than the method
described in the national standards.9-11
4.2. Bulk Crushing Strength. Many differently
shaped fragments were found after the BCS test. Figure
5 shows photographs of several typical fragments. These
cases can be divided into two categories. One is as
illustrated by parts a-c; these have the same features
as that after the SPCS test. The fragments are either
approximately hemispherical (parts a and b), or seg-
ment-shaped (part c). The other one does not appear in
the SPCS test. Part d shows that fracture happens at
the same time on two sides of the sample, while in part
e a local peeling feature is seen on a large part of the
fractured sphere. These sections all present the typical
features of brittle fracture. This is evidence for the
tensile stress to be the reason of fracture. It should be
mentioned that an amount of fines was also generated
when the applied pressure was high.
In Figure 6, the broken percentage in the packed bed
is plotted as a function of piston pressure, where the
curves are drawn by eq 13 and the points are the
measured values. The parameters in the equation are

Figure 5. Photographs of the typical fragments after the BCS measurements.

中国科技论文在线
Figure 6. Correlation of the percentage of particles broken after
the BCS measurement with the total pressure applied: ], sample
A; 4, sample B; O, sample C.
Table 3. BCS Distribution Parameters of the Samples
sample M B
A 3.02 0.0266
B 3.18 0.0918
C 2.80 0.119
given in Table 3. It is noticed that the measured and
calculated values deviate when the pressure applied
exceeds some critical value. In Figure 6, the broken
percentages of samples B and C for point P ) 1.8 MPa
are less than the calculated values. One explanation is
that when the pressure is sufficiently high, a large
amount of fines is generated and fills the voids between
the particles, which scatters the contact force and
reduces the fracture probability. Another less important
reason might be that the wall effect for relatively large
particles is enhanced when pressure exceeds a critical
value. Therefore, it is likely that the breakage curve
obeys the Weibull equation only in the low loading
range. However, the model is of practical significance
because the breakage nature and the broken percentage
in the low loading range are the most interesting for
the industrial practice. The amount of sample loaded
has an effect on the experimental result because of the
statistical nature of the fracture. In this work, we
adopted the recommendation of Dart:3,5 the initial bed
height L and the diameter D is in a ratio of about 1:1.
The results show it is fairly good. The wall of the
container also influences the geometrical arrangements
of the particles in space. However, it can be neglected
if the diameter of the particles is much smaller than
the inside diameter of the container.
The applicability of a Weibull equation to the descrip-
tion of the relationship between the percentage of
broken particles in a packed bed and the total force
applied along the axial direction of the bed is reasonable.
The BCS data represent the failure of spheres in the
packed bed as group behavior. This correlation provides
a possibility for the reliability prediction of a fixed-bed
converter. There are also possibilities of doing experi-
ments at high pressure and temperature with the
configuration of the present apparatus, and there is
strong reasoning for the applicability of eq 13 to the data
of high pressure and temperature cases.
4.3. Relationship between SPCS and BCS. From
eq 10, M is predicted to be equal to m0, while m and m0
should be identical for the same sample because they
relate only to the defect distribution. The results
presented in Tables 2 and 3 show that these values are
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Ind. Eng. Chem. Res., Vol. 38, No. 5, 1999 1915
not exactly the same; however, the sequence of M in
Table 3 for different samples is the same as that of m
in Table 2. This deviation may come from two origins.
First, it can come from the statistical nature of the SPCS
and BCS data and the comparatively small number of
points measured in the experiments. Second, it is
noticed that the deviation between the two values
increases with an increase of the diameter of the
spheres, i.e., the smaller D/dp is, the larger the devia-
tion is. For the SPCS data, the Weibull modulus
describes the scattering property of the data. The larger
m is, the smaller the scattering range is. For BCS, the
larger M is, the higher the slope of rising of the curve
is. It seems very reasonable that the curves of SPCS
and BCS should have some similarities, as the features
of both have nearly the same physical meaning. Another
deduction is that when m is same, a higher mean value
of SPCS leads to a shift of the BCS curve to higher
range.
SPCS is simple and informative if a probabilistic
method is introduced to the interpretation of the data,
while the BCS method is closer to the meaning of the
fixed bed. The two methods give an identical Weibull
parameter for the same sample, in the case that the
sample size is large enough; however, in the SPCS case
the modulus has a meaning different from that of the
parameter in BCS. BCS gives a more direct feeling of
the strength reliability. For instance, in Figure 4, it is
difficult to determine which of samples B and C has a
higher strength, while in Figure 6, it is very clear.
However, BCS measurement is much more complex
than that of SPCS; it needs more complex equipment
and patience.
5. Concluding Remarks
The strength failure of a spherical catalyst under both
SPCS and BCS testing conditions is the case of brittle
fracture. As a consequence, the SPCS data scatter in a
rather large range and can be fit quite well by the
Weibull distribution. This provides a method for the
calculation of the probability of strength failure under
specific loading conditions.
The real packing of spheres is between the one
extreme as described by the model and the other which
is the dense packing; i.e., the number of contact points
is between 6 and 12. Under a multipoint contact
situation, the origin of failure is still tensile stress brittle
fracture. This is consistent with the elastic theory. A
deduction is that the crushing strength of individual
particles within the bed follows the Weibull distribution.
This results directly in the conclusion that the percent-
age of breakage and the total pressure applied in BCS
measurement can be related by a Weibull equation,
which now does not represent a concept of data distri-
bution but a definite law for the behavior of a packed
bed.
It is assumed that the Weibull modulus m of the
SPCS data and the factor M in the BCS correlation have
an identical value. This was found to be really true for
one of the samples, while for the samples with larger
diameters, the deviation between the two values in-
creases with an increase of the sphere diameter. This
indicates the size effect of the cylinder in the BCS
equipment.
The model presented here has several theoretical
gaps. First, it needs a more clear description of the
packing of the spheres in a bed. Second, it needs an
中国科技论文在线
1916 Ind. Eng. Chem. Res., Vol. 38, No. 5, 1999
exact solution of the elastic equations for the multipoint
pressed configuration of a sphere. The experimental
results confirm the final relationship between the
percentage of failure and the total pressure applied and
the deduced conclusions from the model. This model has
a rather important practical significance, as it relates
directly the percentage of failed particles in a bed under
a specific loading condition, which has a close meaning
as the reliability of a fixed-bed converter. The model also
relates the property of a single particle to the bulk
performance of catalytic materials.
Acknowledgment
The financial support for the catalyst mechanical
strength issues from the NSF of China, Ministry of
Education, and SINOPEC Technology Co. is gratefully
acknowledged.
Nomenclature
B ) parameter in the model
BCS ) bulk crushing strength
D ) sample container diameter, mm
dm/m ) percentage of broken particles, wt %
dp ) spherical particle diameter, mm
F ) total load at fracture in the SPCS test, N
Fi ) individual crushing strength data of a sample
F1 ) force applied on each sphere of the top layer, N
F2 ) contact force between particles, N
F(σ), F(F), F(P) ) fracture probability
i ) sequential number of the SPCS data
L ) initial bed height, mm
m, m0 ) Weibull modulus
M ) parameter in the model
n ) number of SPCS data measured for a sample
P ) axial piston pressure, MPa
SPCS ) single-particle crushing strength
Greek Letters
σ ) maximum tensile stress leading to fracture, MPa
β, β′, β0 ) Weibull size parameter
φ ) constant in eq 8, mm-2
δ ) distance between the surfaces of any two adjacent
spheres in the same layer, mm
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Received for review June 8, 1998
Revised manuscript received January 22, 1999
Accepted February 3, 1999
IE980360J