Pull-out During Grinding of Ceramics

Containing an Amorphous Phase

F. Jorge Lino*
DEMEGI/SMPT
Faculdade de Engenharia da Universidade do Porto
Porto, Portugal

When grinding and polishing ceramics,

specific problems are encountered which
are related to the high hardness and brittle
behaviour of this class of materials. Pullouts are frequently observed during the
grinding of alumina (Al2O3), c-zirconia (cubic ZrO2) and alumina-zirconia (50:50 %
vol.) samples. These pull-outs can result in
an incorrect microstructural analysis, since
it is more difficult to identify pores, measure
grain size, determine particle distribution
and other related problems. Although the
pull-out effect can be reduced by modifying the grinding parameters of the sample
preparation machine, such as time and
pressure, pull-outs are more difficult to reduce or eliminate when the ceramic material has a vitreous (amorphous) phase.
Using previous experience in sample preparation, obtained during an intensive
study into the effect of liquid phase on
coarsening behaviour in single phase and
duplex microstructures, conducted by the
author at Lehigh University (USA), an effec-

tive preparation method for this type of

ceramic materials is proposed.
1. Introduction
Many ceramic materials have a liquid phase
at the sintering temperature, which after
cooling generates an amorphous (vitreous)
phase between the grains. Though the
thickness of this phase (film) changes with
the amount of the liquid phase (glass)
added to the ceramic, its value does not
increase continuously, as suggested by
Clarke1, but instead adopts an equilibrium
thickness. The presence of very thin amorphous (glassy) films at the grain boundaries has a dramatic effect on the electrical2
and mechanical properties3 of polycrystalline materials. These film, located on the
grain boundaries and grain corners is responsible for fast sintering rates (enhances
the rearrangement stage)4 and affects the
grain growth rate5. For instance, in order to
produce dense silicon nitride samples by
pressureless sintering, the presence of a

Grinding

liquid phase at the sintering temperature is

essential6. Although this is often the only
way of producing dense (without porosity)
ceramics, this vitreous phase unfortunately
results in a decrease in the strength of the
ceramic. Effectively, the presence of the
glassy phase in a sample decreases the
cohesion between the grains and, moreover, significantly increases their pull-out
during the grinding stage.
In this article we describe a complete procedure for grinding and polishing ceramics
containing a liquid phase. This procedure
reduces the incidence of pull-outs to levels
where it does not significantly affect the
quality of the microstructural analysis.
2. Experimental Details
Ultra high purity (99.995%) alpha alumina
powder (AKP-HP, Sumitomo Chemical
Company, Japan) with a mean particle size
of 0.45 m, cubic zirconia (8 mol% Y2O3,
Tosoh Corporation, Japan) with a mean

Diamond impregnated metal-bonded disc

30m

Speed (rpm)

300

Force (N)

170

Ph.D., Assistant Professor at Faculty of Engineering,

Mechanical Engineering Department, Oporto, Por-

Time (min.)

Until plane

tugal and INEGI (Institute of Mechanical Engineering

and Industrial Management) technical manager.

Table I Grinding steps

Polishing

DP-Plan

DP-Plan

DP-Plan

DP-Plan

Abrasive

Diamond paste 15 m

Diamond paste 6 m

Diamond paste 1 m

OP-S

Lubricant

Blue

Blue

Blue

Speed (rpm)

150

150

150

150

Force (N)

170

170

250

250

Time (min.)

18

Table II Polishing steps

18

35
Pull-out During Grinding of Ceramics Containing an Amorphous Phase

them in boiling water), and some of them

polished by hand (200 turns) on a felt cloth
using a colloidal suspension of 0.02 m
SiO2. This step is helpful, in particular for
samples with glass, because it promotes
surface relief that helps identify the glass
distribution.
After polishing, samples were washed in
water, cleaned with alcohol and dried
(Drybox-2).
Fig. 1 SEM micrograph of pressureless sintered
alumina with 0.5% vol. of anorthite
(CaO.Al2O3.2SiO2) glass. One region of pull-out
is indicated in the micrograph by the red circle.

Fig. 3 SEM micrograph of sintered c-ZrO2 with

10% vol. of anorthite (CaO.Al2O3.2SiO2) glass.
The lighter regions correspond to the places
where pull-outs occurred. Some regions of pullout are indicated in the micrograph by a red
circle.

Fig. 2 SEM micrograph of sintered alumina with

10% vol. of anorthite (CaO.Al2O3.2SiO2) glass.
The lighter regions correspond to the places
where pull-outs occurred. Some regions of pullout are indicated in the micrograph by a red
circle.

Fig. 4 SEM micrograph of sintered alumina-czirconia (AZ50 - 50:50 alumina:c-zirconia) with

10% vol. of anorthite (CaO.Al2O3.2SiO2) glass.
The lighter regions correspond to a pull-out of a
group of grains. Some regions of pull-out are
indicated in the micrograph by a red circle.

particle size of 0.59 m and anorthite

(CaO.Al2O3.2SiO2, Alcoa Industrial Chemicals, USA) glass were used as starting
powders. Powders were mixed (when necessary), pressed and sintered at 1650C
for 30 minutes to generate the different
types of samples (alumina, alumina with
glass, c-zirconia, c-zirconia with glass,
AZ50 (50:50% vol. alumina: c-zirconia) and
AZ50 with glass. Samples were cut in
quarters (Labotom) and then annealed in
air at 1650C for times ranging from 0 to
54 hours5.

Samples were glued onto an aluminium

stub (small samples were mounted in epoxy resin (Epofix), using thermal wax, which
fits into an aluminium specimen holder,
and then automatically polished (Abrapol)
using diamond impregnated discs and
diamond paste on cloth. The successive
preparation steps are indicated in tables I
and II.
After polishing, the samples were thermally
removed from the aluminium holders (or
from the epoxy mounts, by immersing

3. Results
Figures 1 and 2 are SEM micrographs
which show the microstructures of pressureless sintered alumina samples with 0.5
and 10% vol. of anorthite glass, respectively. Both pictures show pores inside the
grains. This is a result of not doping the
alumina with MgO5. Glass is located at the
grain boundaries with the largest amounts
of the glass located at the grain corners.
Figure 2 shows intensive pull-out (see red
circles in figure) which is the result of the
presence of 10% vol. of glass. Some
grains were removed during the grinding
step, which leaves a hole (white regions)
on the surface of the sample. The number
of pull-outs increased with the volume
fraction of anorthite glass, due to a decrease in the strength between the grains
and an increase in brittleness of the ceramic. Figure 3 shows the same problem in
porous c-ZrO2 samples with glass.
Comparing this microstructure with the
one in figure 2, it can be said that alumina
grains are faceted and c-ZrO2 are rounded.
The different grain morphologies do not
seem to affect the pull-out of the grains,
since it occurred at the same rate in both
materials. Figure 4 shows pull-out in the
two phase material (AZ50) with 10% vol. of
glass. The dark phase is alumina and the
grey phase cubic zirconia.
Analysing the pictures, it can be concluded
that pull-outs frequently occur in samples
containing a liquid phase, increasing with
the volume fraction of glass, and does not
significantly depend on the specific type of
ceramic material analysed.
During the grinding stage, due to the brittle
behaviour of ceramics, most of the grains
were removed from the surface of the

19

sample. Although different combinations of

forces and times were tried during the
grinding and polishing stages, it seems
that only a small reduction in the incidence
of this effect was obtained. The initial step
on a diamond metal impregnated disc proved to be too aggressive for this type of
ceramic material. Substituting this disc for
SiC paper reduces the amount of pull-out,
however the SiC paper suffers a rapid
wear, which means that longer times and a
large number of SiC papers need to be
used until the samples are plane. Obviously, this is not a good solution.
A new grinding disc (MD-Allegro- a combined lapping-grinding disc), developed
recently (1995) by Struers (and used later
in our research5), when impregnated with
15 m diamond paste and a force of
170 N, proved to significantly reduce pullouts. This new disc eliminates the grinding
step in the 30 m diamond impregnated
metal-bonded disc which caused most of
the pull-out.
4. Conclusions
The preparation of ceramic samples for
microstructural analysis presents specific
problems which need to be considered.
The high hardness and brittleness of this
class of materials often promote pull-outs
during the grinding stage. This effect is
even more pronounced in ceramic materials containing a vitreous phase. Although
longer polishing times and lower applied
forces lead to a small improvement in the
quality of the polished samples, the pullout problem is not solved. In the course of
an extensive study into the effect of liquid
phase on coarsening behaviour in single
phase and duplex microstructures, conducted by the author, it was found that the
pull-out is significantly reduced when an
MD-Allegro disc impregnated with 15 m
diamond paste and a force of 170 N is
used during the grinding stage.

20

References
[1] D. R. Clarke, On the Equilibrium
Thickness of Intergranular Glass
Phases in Ceramic Materials, J. Am.
Ceram. Soc., 70 [1] 15-22 (1987).
[2] Q. Zou and Z. Meng, Microstructure
and Grain Boundary Structure of Na+Diffused (Sr, Ca)TiO3 CapacitorVaristor Ceramics, J. Am. Ceram.
Soc., 78 [1] 58-64 (1995).
[3] N. P. Padture and H. M. Chan, On the
Constrained Crystallization of Synthetic
Anorthite (CaO.Al2O3.2SiO2), J.
Mater. Res., 7 [1] 170-77 (1992).
[4] R. M. German, Liquid Phase
Sintering, Plenum Press, NY (1985).
[5] F. J. Lino Alves, Effect of Liquid Phase
on Coarsening Behavior in Porous
Single-Phase and Duplex Microstructures, Ph.D. Thesis, Lehigh University,
Bethlehem (USA), August (1997)
[6] M. Cinibulk, H.-J. Kleebe, and M.
Ruhle, Quantitative Comparison of
TEM Techniques for Determining
Amorphous Intergranular Film Thickness, J. Am. Ceram. Soc., 76 [2] 42632 (1993).