Advanced Powder Technol., Vol. 17, No. 2, pp.

219 228 (2006)

VSP and Society of Powder Technology, Japan 2006.
Also available online - www.vsppub.com

Original paper
Structure of strength-limiting aws in alumina ceramics
made by the powder granule compaction process
KAZUYOSHI SATO 1, , HIROYA ABE 1 , MAKIO NAITO 1 , TADASHI HOTTA 2
and KEIZO UEMATSU 3
1 Joining

and Welding Research Institute, Osaka University, 11-1 Mihogaoka, Ibaraki,

Osaka 567-0047, Japan
2 Japan Fine Ceramics Center, 2-4-1 Mutsuno, Atsuta, Nagoya 456-8587, Japan
3 Department of Chemistry, Nagaoka University of Technology, 1603-1 Kamitomioka, Nagaoka,
Niigata 940-2188, Japan
Received 22 June 2005; accepted 3 August 2005
AbstractAlumina ceramics were made by the powder granule compaction process and the structure
of strength-limiting aws was examined. Optically projected images obtained by transmission optical
microscopy for a thin alumina specimen revealed that there were many round-shape large aws of
several tens of microns. The cross-sectional views of the large aws observed after polishing the
thinned specimen clearly showed that their structure was a crack-like pore rather than a spherical one.
The fractography indicated that the fracture of the alumina ceramics originated at the crack-like pore
which was a part of the corresponding large aws located near the tensile surface of the specimen.
The internal structure of the compact before ring was examined by the liquid immersion method.
It was clearly shown that the large aws resulted from non-uniform powder packing associated with
granule deformation during compaction.
Keywords: Alumina; strength-limiting aws; granule; powder compaction.

1. INTRODUCTION

The powder compaction process is widely used for producing a variety of ceramic
parts. The powder granules used in this process tend to form large strength-limiting
aws [1, 2]. The authors have examined the formation of the aws over the
entire processing stages with optical microscopy operating in the transmission mode
[2 6]. Incomplete joining at the granule interfaces was found to be responsible
for the formation of aws in the compact. They survive the subsequent sintering
process, forming large aws, and one of them limits the strength of resultant
To

whom correspondence should be addressed. E-mail: k-sato@jwri.osaka-u.ac.jp

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ceramics. The exural strength and its variation were successfully explained in
terms of the equivalent diameter of aws measured on the optical micrographs for
alumina ceramics [6].
Although the optical method is very powerful for detecting large aws, it shows
only their shadow as black circular dots. It does not show the detailed characteristics
of them. Recently, a new approach was proposed to examine the detailed structure
of aws in a sintered alumina [7, 8]. It consists of two steps. First, the location of a
large aw in the bulk ceramic is identied with transmission optical microscopy
operating at low magnication. Then, the characteristics of the large aw are
examined in detail, after being exposed to the external surface by controlled
polishing. This method is very effective for examining the structure of large aws,
since the most difcult part in their examination is the identication of their exact
location in the bulk. Once their location is known, it is rather easy to examine the
detailed structure of the aw. The examination showed that most of the large aws
are pores of an apparently round shape. However, a subsequent detailed examination
which involved controlled polishing to expose large aws at the surface showed that
their shapes are far different from round. This new approach will provide accurate
knowledge on their structure and formation mechanism, and lead to remarkable
progress in powder compaction processing.
In this study, the formation mechanism of strength-limiting aws is studied in
detail through a new characterization method of the aws in alumina ceramics
prepared by the powder compaction process.

2. EXPERIMENTAL PROCEDURE

A commercial alumina powder (AL160-SG4; Showa Denko, Japan) was chosen as

the starting material. It has an average particle size 0.4 m and a slightly elongated
particle shape. Aqueous slurry with a solid content of 35 vol% was prepared by
ball milling for 24 h with an acrylic dispersant (Ceruna D305; Chukyoyushi, Japan)
and distilled water. The amount of dispersant added to the slurry was 0.4 mass%
on the basis of the weight of alumina powder. Abnormally large particles in the
slurry were removed by passing it through a 32-m sieve. After a binder and a
wax were added and stirred, the slurry was spray-dried to prepare the granules.
The operating conditions of the spray drier were: inlet and outlet temperatures of
air = 150 and 100 C, respectively, feed rate of the slurry = 6 l/h, and rotation
speed of the atomizer = 8000 r.p.m. Abnormally large granules were removed by a
150-m sieve before compaction.
Granules obtained were poured into a hardened steel die, uniaxially pressed at
20 MPa and then isostatically pressed at 176 MPa. The green compact was sintered
at 1550 C for 2 h in air. The ceramic obtained was machined into specimens with
dimensions 4340 mm3 for mechanical testing. The tensile surfaces of specimens
were carefully polished with ne diamond abrasives to remove aws induced by
machining. A thin specimen with a thickness around 50 m was prepared from

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221

the ceramics to characterize the process-related aws. Thin alumina ceramic is

transparent when both surfaces are mirror polished and its internal structure can be
examined with an optical microscope in the transmission mode.
The morphology of the granule was evaluated with by scanning electron microscopy (SEM). The internal structure of the green compact was characterized by
the liquid immersion method [2 5]. The method is based on the reduced reection
of transmitting light at particle/surrounding medium interfaces by substituting the
space between particles by an immersion liquid which has a refractive index close
to that of the particle. The reectance R at a particle/medium interface is described
as:
R=

(n 1)2
,
(n + 1)2

where n is the relative refractive index given by the ratio of refractive index of
particles (n1 ) and that of the surrounding medium (n2 ). For alumina, the refractive
index n1 is 1.76 [5]. For a clear image of the structure, adequate transparency
and optical contrast are needed, and an immersion liquid with a refractive index
slightly different from that of the particle must be selected. 1-Bromonaphthalene
(n2 = 1.65) was used as the immersion liquid in this study [5].
The internal structure of the sintered body was observed with an optical microscope in the transmission mode. Once a large aw was found, its location (the
distance from the surface) was determined by considering the refractive index of
the matrix, i.e. the true location was determined by multiplying the apparent depth
by the refractive index of alumina. The apparent depth corresponded to the distance
from the surface of the specimen for focusing the aw. Then, the specimen was polished down to the aw to expose it on the external surface. The three-dimensional
structure of the aw could be observed through repeated polishing and observation.
Fractography was also applied to specimens after strength measurement to
examine the detailed structure of the fracture origin.

3. RESULTS

Figure 1 shows a granule prepared in this study. The granule has dimples, which is
typical for those obtained from a well-dispersed slurry [9]. Flocculated slurry tends
to form solid granules.
Figure 2 shows the internal structure of a green compact observed with the
liquid immersion method. The direction of observation was perpendicular to the
direction of the uni-axial compaction. Many round objects were observed in the
photomicrograph. They were clearly traces of granules that survived the compaction
process. Crow foot cracks were observed at the multiple granules junctions. Poor
joining of granules was clearly responsible for their formation. Crescent-like aws
located at the center of granule traces were also noted. They are formed from the
dimples of the granules shown in Fig. 1. These structures indicate that the granules

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Figure 1. SEM micrograph of an alumina granule.

Figure 2. Internal structure of a green compact observed with the liquid immersion method.

were just deformed and not destroyed even after cold isostatic pressing at 176 MPa.
These aws in the green compact may survive the sintering process and persist as
strength-limiting aws in the nal parts.

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223

Figure 3. Internal structure of a sintered specimen observed with an optical microscope in the
transmission mode.

Figure 3 shows the typical internal structure of a sintered specimen observed with
an optical microscope in the transmission mode. Black dots in the photomicrograph
correspond to aws. Note that the sintered density of the specimen is high, i.e.
approximately 99% of theoretical. Specic aws, especially large ones in the green
compact, grow and are emphasized after sintering, although the number of granule
traces appears to decrease.
Figure 4 shows detailed views of the aw shown in Fig. 3, which were observed
in the transmission and reection mode with an optical microscope. These
photomicrographs were taken before and after lowering the specimen surface by
13 and 20 m by polishing, respectively. The large aw at the center of the
photomicrographs clearly originated from the granule traces. The aw appeared to
be a semispherical pore in the transmission photomicrographs. The thin specimen
also contains many other small aws. A part of the large aw in the transmission
photomicrographs is noted as a white region in the reection photomicrographs.
The apparent difference in the images of the aw is due to the diffused reection
of light at the matrix/aw interfaces in the specimen. After 13 m of polishing,
a part of the upper rim of the large aw was exposed to the surface. Most of the
aw was still under the surface, since 20 m of polishing was needed to expose
the upper rim of the large aw completely to the surface. These photomicrographs
indicate that the structure of the large aw is clearly far from hemispherical and is
crack-like, extending three-dimensionally. It also shows that the dark images in the
transmission photomicrograph are due to the light scattered by the crack-like aws.

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Figure 4. Three-dimensional images of the large aw shown in Fig. 3 observed by optical microscopy:
(a) transmission and (b) reection mode after polishing.

It should be also mentioned that a small aw appeared on the polished surface after
20 m of polishing. The locations of other small aws were clearly not at this depth
of the specimen. The result indicates that large aws are rarely present in ceramics
and their identication is very difcult through conventional observation on a given
cross-section.
Figure 5 shows a SEM micrograph of the large aw shown in Fig. 4 after 20 m
of polishing. It conrms that the aw has a crack-like shape rather than a simple
void.

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Figure 5. SEM micrograph of the large aw shown in Fig. 3 after being exposed on the polished
surface.

Figure 6 shows a cross-sectional view of another large aw exposed to the fracture

surface of a thin specimen. The transmission photomicrograph suggests that a part
of the large round pore is exposed to the fracture surface. The SEM micrograph
shows a large crack (shown by arrows) rather than a simple void on the fractured
surface. The diameter of the aw observed in the transmission photomicrograph
(approximately 30 m) was consistent with the length of the aw in the horizontal
direction in the SEM micrograph.
Figure 7 shows an example of fracture origin in the exural test specimen. A set
of micrographs is important to examine the fracture origin accurately. The concave
structure may suggest that a spherical pore is the fracture origin in the micrograph
of Fig. 7a. A convex region was observed, however, at the corresponding location
on the opposite fracture surface (Fig. 7b). The sizes of the fracture origin were
approximately the same on both fracture surfaces. Clearly the fracture origin is a
crack-like aw rather than a simple pore. Flaws of this type dominated the strength
of ceramics prepared in this study. The exural strength of ceramics is governed by
crack-like aws located near the tensile surface of the exural test specimen.

4. DISCUSSION

Formation of the strength-limiting aws was examined on alumina ceramics prepared through the powder compaction process. Through the accurate observation of
their structure, the most detrimental aws were found to be crack-like rather than

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Figure 6. Structure of a aw observed by (a) optical microscopy in the transmission mode and
(b) SEM on the fractured surface of the thinned specimen.

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Figure 7. Typical fracture origin in a sintered body.

simple pores. This is consistent with the fundamentals of fracture mechanics. It

suggests that a crack is more detrimental to the strength than a spherical pore, since
the stress intensity factor is greater for the former than the latter.
There are two types of large aws which appeared crack-like and round in the alumina ceramics made though the compaction process with the hollow granules [2].
The former type of aw was formed from incompletely joined granules and the later
from the dimple of granules. Crack-like aws are reported to be larger than round
pores [2].
Structural evolution of crack-like aws has to be discussed based on the powder
packing structures in the granules and the green compact. The aw structure of the
green compact is emphasized after sintering, as shown in Fig. 3. It can be explained
as the growth of specic, large aws during sintering due to the non-uniform
densication behavior. It is known that granules prepared with well-dispersed
slurry are hard and brittle due to the dense packing of primary particles [10].
Their complete destruction may be difcult even at very high compaction pressures,
although they have the merit of good owability in the commercial production of
ceramics. As a result, the hard and brittle granules tend to form poorly joined
region between them during compaction. In addition, the rate of densication
must be higher within the granules than the rest of the compact. As a result,
local microlaminations will occur at poorly joined granule interfaces during the
densication, forming crack-like aws [3]. Granules which can plastically deform
should be effective for reducing the size and number of aws, and thus for increasing
the strength of ceramics [11]. They can be prepared from a occulated slurry [9, 10].
The slurry properties must be carefully controlled for improving the properties
of granules as well as the resultant ceramics. Slurry properties govern the packing
structure and the properties of the granules, and thus the formation of strengthlimiting aws.

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5. CONCLUSIONS

Formation of strength-limiting aws was examined for alumina ceramics made

through powder granule compaction process. The aws observed as black circle
dots in transmission optical microscopy were found to be cracks rather than pores.
The aws are formed due to incompletely joined granules during compaction. These
aws located near the tensile surface actually governed the strength of the specimen.
The results indicate that the packing structure of granules in the green compact is
critical for formation of the strength-limiting aws and must be carefully controlled
for better ceramics.

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