Tribdogy

Ceramic

tribology

Inrernafional

Vol. 28. No. 1, pp. 1-6, 1995

Elsevier Science Ltd
Printed in Great Britain
0301-679X/95/$10.0
+O.OO

in Japan

Yuji Enomoto

This paper reviews recent fundamental

work in Japan on the
tribology
of engineering
ceramics.
These ceramics
show a
characteristic
tribological
response
depending
on the materials
and
environmental
species in a vacuum,
in various gases, in oils, in
water and in low-viscosity
fluids and at elevated
temperatures.
The
unique tribological
interactions,
in some cases, significantly
affect
both the friction
and the wear behaviour
of ceramics.
Keywords:

ceramics,

friction,

wear,

tribochemistry,

solid lubricant

Introduction
During the last decade, especially since the National
R&D programme on Fine ceramics was initiated in
Japan in 1981 to promote basic studies on the practical
application of ceramics, engineering ceramics have
attracted the attention of many researchers as promising
tribomaterials
for mechanical components operating
under severe or hostile environments. Practical applications, however, have been slow to materialize in
comparison with initial expectations. Nevertheless,
silicon nitride ball bearings have now been in use since
1986, and mechanical parts for car engines, such as
valves, turbocharger rotors and rocker-arms made of
silicon nitride. have followed.

generated in a plastically deformed zone act as

luminescent centres. Observation of cross-sections of
MgO crystals scratched by a diamond hemisphere
shows that the zone deformed by sliding contact
consists of three characteristic zones whose structure
depends on a/R, which is a measure of the contact
strain*. CL observation of alumina sliding surfaces
also reveals fatigue-type subsurface cracking, because
lateral cracks suppress the penetration of the electron
beam and/or the escape of luminescence, thus reducing
the CL intensity2. The load (W) dependence of the
friction coefficient (p) could be explained, provided
that all the fractional work was expended in the CL
zone.

The subsequent national project on the Ceramics gas

turbine engine has been underway since 1990 to
develop engines for 300 kW power plants. Further
R&D in the car industry is working on the development
of a ceramic turbocompound
engine and an alcoholfuelled two-cycle ceramic engine. Further research
work is still needed to understand the friction and
wear behaviour of engineering ceramics especially
under hostile conditions, and many presentations on
related topics were made at the recent JAST Tribology
Conference. This paper reviews recent research work
in Japan on the fundamental tribological responses of
ceramics.

Observation of the wearing surface of S&N4 using an

SEM reveals that cracks, initiated at preferential sites
of subsurface defects, cause the removal of fragments,
which are dragged along the sliding surface while
being crushed to create two-dimensional
plastically
deformed grooves. There is a geometrical resemblance
between this microtopography
and that often found
on metallic sliding surfaces in a steady state3.

Deformation

and fracture

in sliding

contact

Although ceramics are typically brittle solids, ductile

deformation
can occur when a contact stress is
concentrated on the real-contact area of the sliding
surfaces. This deformed zone of oxide ceramics can
be seen using the cathodoluminescence
(CL) mode of
a scanning electron microscope, because point defects
Mechanical
305, Japan

Engineering

Laboratory,

Namiki

I-2,

Tsukuba,

Ibaraki

Tribology

The brittle behaviour of ceramics under a concentrated

sliding contact has been analysed based on fracture
mechanics. Kimura and Shima employed a longitudinal
contact-point model to evaluate stress intensity factors
at wear cracks by three-dimensional
finite element
analysis. They showed that the amplitude of the mode
II stress-intensity factor at an L-shaped crack reaches
as high as 2.8 MPaml*,
which exceeds the threshold
value for crack extension, as shown in Fig 1. This
suggests that horizontal parts of L-shaped cracks may
grow in the direction of sliding.
On the other hand, Hokkirigawa et a1.5J employed a
transverse contact model, and analysed the crack
extension conditions of a vertical crack at the rear of the
contact zone. Using the crack propagation conditions as
a basis they deduced the dimensionless parameter S
(or S*), which is a function of contact stress or

International

Volume 28 Number 1 February

1995

Ceramic

tribology

in Japan:

longitudinal

contact

Y. Enomoto

Silicon nitride ball bearings with a solid lubricant film

were developed by Ogawa et aL9 for high-vacuum,
high-temperature,
high-speed application.
All S&N4
bearings with an MoS, film and hybrid bearings (S&N4
ball + steel races) with a Pb or an MoS2 film
have good durability if lamellar solid/metal composite
retainers are used.

model

L-shaped

crack

To develop a dust-free bearing system, Ito et a1.l

recently conducted experiments in a vacuum to count
the number of particles emitted from a bearing system.
Of the various bearings, including soft metal-coated
steel bearings, hard-coated steel bearings and ceramics,
they found that the best combination for a dust-free
system is a ZrOz ball with a steel inner and outer race
and a PTFE retainer.

Tribochemistry
environments

Fig 1 Stress intensity factor KI1 of S&N, at the subsurface

craclp

hardness, the fracture toughness, friction coefficient

and crack size. These parameters accurately describe
the transition behaviour from severe wear due to
microfracture to mild wear resulting from ploughing.

Friction and wear of ceramics in a vacuum

The friction and wear of various engineering ceramics
on themselves in a vacuum were investigated in a
vacuum by Sasaki. The friction coefficients k of
A1203, PSZ and SIC were relatively high at /.~=0.4-0.8.
Although the friction coefficient of S&N4 showed
~=0.3 in a vacuum, the coefficient was p=O.7 at
atmospheric pressure. The wear behaviour of ceramics
depends on the nature of the materials and the
surrounding gas. The wear of Sic on itself is minimum
at pressures of 10-l Pa to 1 Pa.
Recently, Hiratsuka et a1.8 found that when a ceramic
pin is slid in a vacuum against a metal disk, which
has the lower absolute standard heat of formation,
both friction and wear were low. Figure 2 shows the
friction coefficient of A1203, ZrOz and Si02 rubbed
against various metals. The friction coefficient of an
A1203 pin rubbed against a platinum disk was as low
as 0.005, whereas in oxygen it was 0.45.

Standard

of ceramics in gaseous

It is well established that tribochemical

interactions
between ceramic surfaces and environmental
species
have an important effect on both friction and wear.
A notable technique has been employed by Mori et
al.ll to determine
the dynamic behaviour of the
adsorption of gas species on wearing surfaces using a
scratch tester in a vacuum chamber equipped with a
Q-mass spectrometer. They evaluated the adsorption
rate and adsorption activity of molecules on nascent
ceramic surfaces and found that?
1.
2.

Even chemically stable saturated hydrocarbons

chemisorb on nascent ceramic surfaces, and
Polar compounds, such as water, amines and
carboxylic acids that are barely chemisorbed on
nascent metal surfaces, are chemisorbed well on
nascent ceramic ones. As shown in Fig 3, the
absorption activity of the polar compounds propyl
amine and propionic acid rises as the ionic character
of the ceramic bond increases12. This indicates
that such polar compounds are adsorbed onto the
ceramic surfaces by electrostatic interaction.

In experiments by Sasaki, ceramics were slid against

themselves in nitrogen (carrier gas) + organic gases
saturated at 2oC, ethanol, acetic acid, acetone,
hexane, benzene and water. As shown in the results
for Zr02 and S&N4 in Fig 4, both friction and wear
are strongly affected by the environmental
species.
The marked bars in Fig 4 indicate that a grease-like
reaction product (the so-called friction polymer) was

tt tt

-1000
t
Mg St Fe
heat of oxide

-2000

TlAl

fromation

(kJ/mol)
Amount

Fig 2 Friction coeficient of Alz03, ZrOz and SiO,

rubbed against various metals in a vacuum as a function
of standard heat of oxide formations
2

Tribology

International

Volume

28 Number

of ionic

character,

Fig 3 Adsorption
activity of non-oxide
function of ionic character
1 February

1995

4b

ceramics

as a

Ceramic

GZiSG3

Friction

CoeffiCient

0.2

a)

0.4

specific

0.6

0.8

,o

1.0

H2a
C&OH

rate

mm2lN
10-7 ,0-s
7

Nz

wear

,OO ,0-v 104

I
H

CHJCOOl

l-l

(CH312CO

C&4
C&6

b)

I*

m
Y

NZ
H20

C&OH

tally 0.1250.6,
0.1420.2, 0.08?0.3 and 0.11?0.4,
respectively. To further improve the lubricity of
ceramics, some additives are needed. Tsuya et all3
showed that engineering ceramics and ceramic coatings
are very sensitive to the base oils with and without
SP-type additives. Ceramic coatings such as Ti02,
Cr203 and ZrO, showed better tribological responses
in the oils at elevated temperatures of around 300C.

Lubrication

u
I*

II

(CH3)2CO

m*

.i

I*

c6b

Y. Enomoto

l-4

CHjCOOH

C6H14

in Japan:

Imazumi and Hatal showed that a kind of phosphate

and alkyl-type phosphite additive in paraffin oil reduced
the wear of a S&N4 block in combination with a steel
ring, whereas an aryl-type phosphite did not, as shown
in Fig 5. Formation of FeP04, FeSi03 and a friction
polymer acts as a wear inhibitor.

I+

tribology

Fig 4 Friction and wear of (a) A&O, and (b) Si,N,

in an organic compound
+ nitrogen vapour7. *A
grease-like friction polymer was visible by eye on the
sliding surface

a)
.,
35,

in low-viscosity

fluids

Since the pioneering work on water lubrication

of
S&N4 by Tomizawa and Fischeris, the lubrication of
ceramics in various low-viscosity process fluids has
been studied in detail. According to their work, when
S&N4 is slid in water hydrodynamic lubrication exists
above a certain critical speed. Further studyi showed
that this behaviour strongly depends on the sintering
additives in the materials. For a lower sintering
additive content in Si,N4, the critical velocity at which
hydrodynamic lubrication sets in is reduced. However,
at velocities below the critical value, both the friction
and wear of S&N4 are relatively high. To improve this
behaviour, the effect of an aqueous solution of additive
fluids, such as fatty acids, silane coupling agents, acids,
etc. was examined7J6..
Hibi and Enomoto showed
that an aqueous solution of a silane coupling agent
with an amino group greatly reduced both friction and
weari, as shown in Fig 6. This is due to the fact that
a polysiloxane film forms on oxyhydrated S&N4 and
acts as a lubricant.
Sliding tests of S&N, in a diluted aqueous solution of
different pH values by Mizuhara and Hsu* showed
that both friction and wear increase with increasing
pH, and fall to a minimum in a pH = 3 solution. The

TEP. 1BP,mP, 1DS/70.2,

1

AlkYl

LYP

.I[.

1Y

type

Fig 5 Wear of SI,N, in oils containing

and (b) phosphate compound additivesI

(a) phosphite

visible by eye on the surface after sliding. In this case,

both friction and wear were relatively low.
W

Lubrication

x iU8m&kg~mm

in oils

Ceramics may also be used for the mechanical sliding

parts of high-precision
machine tools, etc. where
lubrication with oil is needed. The friction coefficients
of Si3N4, Sic, ZrO,, A1203 under boundary lubrication
in poly-phenylether
found by Kawamural* were typiTribology

silane

3 aq.

0.001
0.01
0.1

mol/l
molll
molll
5

I
10

15

2b

Fig 6 (a) Friction and (b) wear of S&N, in an aqueous

solution of 3-aminopropyltriethoxysilane
(silane 3)16
International

Volume

28 Number

1 February

1995

Ceramic

tribology

in Japan:

Y. Enomoto

hydrophilic
silicic acid film, formed on the sliding
surface, easily dissolves in a solution of higher pH
values. On the other hand, dissolving of the film is
suppressed in a solution of a lower pH value, and
thus a thin, tight film forms on the sliding surfaces,
helping to reduce the friction coefficient.
Lubrication
tests of S&N4 with water and water
dissolved in oil by Kimura and Okada19 showed that
the friction of S&N4 in water and water + polyalkylene
glycol was high in the low Hersey number region, and
transition to very low friction took place at a threshold
value, forming Stribeck-like curves in some cases, but
no such transition was found with the emulsion with
a paraffinic base oil. The presence of water considerably
increased the amount of wear.
Kitaoka et al.*O investigated the tribological characteristics of a-alumina and S&N4 in a high-temperature
water vapour up to 300C. They showed that the wear
of these ceramics significantly increases at elevated
temperatures. The wear of alumina is attributed to
the solution of intergranular impurities and corrosion
cracking*, whereas the tribochemical dissolution into
water in the following reaction scheme is the predominant wear mechanism for Si3N4*l:
Si3N4 + 6H2O + 3Si0,

+ 4NH3

Hibi and Enomoto22,23 found that, as shown in Fig 7,

purified n-alcohols effectively reduce the friction and
wear of Si3N4 even at a lower sliding velocity; i.e. the
coefficient of friction is 0.1 for lower alcohols and
0.07 for higher ones. As the carbon number ZV, in
lower n-alcohols increases, wear decreases. Hibi and
Enomoto showed that silica, amines and polymeric
compounds are formed due to tribochemical interaction
between Si3N4 and lower n-alcohols according to the
following reaction scheme24:
a-Si3N4 + R*OH+Si02
R*:
H,
CH3,
where R **: H,
H,CH,

+ R**NH,
C2H5,

C3H7,

H,

H,

+ Polymer
C4J&

Hisakado et a1.25 showed that the friction and wear of

Si3N4, Sic and Zr02, Al2O3, lubricated in ethanol,
decrease as the mean depth of fine roughness of the
ceramic surfaces increases.
Triboelectronic
The sliding
Furthermore,

lead to the emission of charged particles, the socalled tribo-emission or fracto-emission. Although this
behaviour has been known since ancient times, the
relationship
between tribo-electrification
and triboinduced physiochemistry is not yet fully understood.
The effect of environmental
gas pressure of triboelectrification of various ceramics under sliding contact
was measured using a vibrating-reed type electrostatic
voltmeter26. As seen in Fig 8, the surface electrostatic
potential in a Zr02 pin on a ZrO,, disk configuration
reached as high as 3 kV at a N2 pressure of less than
10 Pa, and decreased quickly to the level of 0.5 kV
around the N2 pressure range of 0.1-l Pa. Although
the wear of Zr02 was so small that it could not be
measured, it is interesting to note that the wear of
Sic was minimum at a similar pressure range. Further
detailed investigation is needed to clarify the mechanism responsible for the correlation between triboelectrification and the friction and wear behaviour of
ceramics.
Intense fracto- or tribo-emission of charged particles
from fracturing brittle solids has been successfully
measured under atmospheric conditions using a newly
developed fast operating charge amplifier.
It was
suggested that the fracto-emission of electrons is caused
by the separation of charges on the fracturing surfaces,
which leads to the formation
of an electric field
and the liberation of exo-electrons28. Recently this
technique has been used to investigate the electrical
activity of fracturing rocks for studying the source
mechanism of seismic electromagnetic
signals29 and
the role of charged particles under boundary lubrication
conditions30.
High-temperature

solid

lubrication

There is an increasing need to lubricate mechanical

components in advanced applications such as ceramic
gas-turbine engines and combined jet engines for
hypersonic transportation
to show operation in air
over a wider temperature
range, say from room
temperature up to 1000C. Conventional solid lubricants such as MoS2, graphite, etc. however, do not

phenomena
of ceramics causes triboelectrification.
the sliding and fracture of ceramics also
aI
'G
5

7!!!2i

----\
.

0.6-

.-a

ew

.\

E
c 0.4.-0
z

Fig 7 Friction and wear map of S&N, and Sic in water

and n-alcoholti2.
m; S&N,, 0; Sic
4

Tribology

International

Volume

- 1 t
z

10-4

,jL,
100

N2 pressure

Coefficient

28 Number

z
9

0e

/
-2a

0.2-

lk

Friction

/'.
','

1
3 5

lo4

(Pa)

Fig 8 Electrostatic
potential of Sic due to frictional
electrification as a function of N2 pressure26
1 February

1995

Ceramic

have a stable friction coefficient over such wide

temperatures due to oxidation degradation.
Yamamoto and Ura31 showed that when a Sic surface
was oxidized by heating to 1000C in air, it exhibited
excellent friction and wear characteristics in argon,
but not in air.
Metallic thin films such as Mn, Fe, Co and Ti on
ceramics effectively reduce both friction and wear up
to 1000C as long as the film lasts long enough3,33.
These results are shown in Fig 9. The metallic films

1.0
Co fflm(0.2

T I film

(1 vam)/AlzO3~

T I fllm(0.2

pm)/AlzO3

NaZrO3

t
8

pm)lA12Og

+ 23.3%CrzO3/Al~O3

500

Temperature,

1000

Fig 9 Friction coefficient of metal-coated ceramics and

oxide lubricants as a function of temperature in air
Table 1 (a) Effect of metal film on wear reduction
surfaces
after tests at 1000C by X-ray analysis
(a)

S&N,

SIC
40s
30,

tribology

in Japan:

Y. Enomoto

were subjected to oxidation during sliding and served

to prevent adhesion between the ceramics. Shimura
and MizutanP3 found that the first transition metals
having a high oxidation number show better lubrication
properties, as seen in Table l(a). Their results indicate
that films which effectively prevent adhesion have a
form of complex oxides rather than a stoichiometric
oxide, as indicated in Table 1(b).
In general, oxide substances are naturally stable under
oxidizing environments, even at higher temperatures.
Solid oxide lubricants have been investigated among
double, tertiary and quaternary oxides and their
mixtures3j. As a result of a series of experiments,
Na*ZrO, + 28.8 wt% Crz03 shows good lubrication
properties from room temperature up to lOOOC, as
illustrated in Fig 9. Since the complex oxide, however,
is a deliquescent substance, we need further research
into more stable solid oxide lubricants. Recently, a
solid oxide lubricant, in which the Na in the above
solid oxide lubricant was replaced by Ba or Ca, showed
greater chemical stability and stable lubrication of p
= 0.3-0.4 up to 1oOOc-5.
Takebayashi et al. 36 confirmed that S&N4 bearings
with self-lubricating
retainers made of a graphiteboron-chromium
composite perform better at 500C
in air and at a rotational speed of 15 000 rpm.

of ceramics.

(b) Metallic

oxides

as detected

on sliding

Cr

Mn

Fe

co

Ni

cu

&I

Ni-Cr

C
A
A
B

A
A
A
C

A
A
A
C

A
A
A
C

A
B
B
C

C
C
A
A

C
C
A
C

A
A
C
B

A: fair W, i 3 x lo-
mgim,
very little damage
B: good
W, < 3 x 10m6 mg/m,
slight damage
C: no good W, > 3 x 10ee mg/m,
substantial
damage
lb)

Cr

Mn

Fe

co

cu

Ag

Ni-Cr

Si,N,

CrAL

MM3
Mn304

cu-Fe,O,

Co,SiO,
cowo,

&I
SiO,

SIC

CrA

MnJL
MM,

cu-Fe,O,
SiO,

Co,SiO,
SiO,

cue
SiO,
cue
cu,o
SiO,

NiO
NiCr,O,
NiO
CrA
NiCr,O,
Ni,Si

ZrO,

Cr203

wFe203
wFe,O,
(Fe,AI 1203
FeAI,O,
cy-Fe,O,

co304
co3Ql
CoAI,O,
coo
co,o*

cue
cue
CuAIO,
CuAI,O,
cue
cu,o

Ag

40,

(700C -+I
Mn,O,
MnAI,O,
CrJL

Tribology

International

MM,

Volume

(Ag)
SiO,

Ag
Ag

28 Number

NiO
NiCr,O,
NiAI,O,
NiO
NiCr,O,

1 February

1995

Ceramic

tribology

in Japan:

Y. Enomoto

Conclusions
Recent studies on the tribological behaviour of engineering ceramics have demonstrated that unique tribological interactions with environmental
species often
significantly affect the friction and wear characteristics
of engineering ceramics. These findings suggest that
such characteristics of engineering ceramics may be
utilized for tribomaterials
under certain special conditions.
Newly developed micro-analytical
tools are expected
to reveal the nature of tribo-induced physiochemical
interactions at the atomic and molecular level, thus
increasing the reliability of tribomaterial
design.

16.

17.

18.

19.

20.

Ceram.

Acknowledgments
The author wishes to thank Professor Y. Kimura
the opportunity to present this review paper.

for

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Y. Sliding damage of
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K. and I&u S.M. Tribochemistry of silicon-based
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Volume 28 Number 1 February 1995