ISSN 1995-0780, Nanotechnologies in Russia, 2015, Vol. 10, Nos. 3–4, pp. 261–267. © Pleiades Publishing, Ltd., 2015.

Original Russian Text © M. Tokita, 2015, published in Rossiiskie Nanotekhnologii, 2015, Vol. 10, Nos. 3–4.

Recent and Future Progress on Advanced Ceramics Sintering

by Spark Plasma Sintering
M. Tokita
Lobachevsky State University of Nizhniy Novgorod, pr. Gagarina 23, Nizhni Novgorod, 603950 Russia
e-mail: kseniayashina@mail.ru
Received August 20, 2014

Abstract—This article describes recent trends in Spark Plasma Sintering (SPS) technology. The SPS method
is widely recognized as a useful sintering technique to develop various kinds of attractive ceramics, metals,
and composite materials due to its excellent features of rapid heating, electromagnetic field effect, and a well-
controlled microstructure.

DOI: 10.1134/S1995078015020202

INTRODUCTION nanofibers, hard materials, electronic materials, ther-

Spark plasma sintering (SPS) is a method of sinter-
ing under the effect of an electric current developed by
the Japanese company JAPAX and based on the con-
cept of applying a current pulse to cosnolidate powder
materials that appeared in early 1960s [1]. In 1968 the
method was transferred to the Lockheed Missile Cor-
poration (United States) as a patented export technol-
ogy and started to be used in as a technology for the
rapid sintering of beryllium and titanium alloys. How-
ever, at that stage the method showed problems with
repeatability and application in mass production and,
even though the SPS method continued to be used for
the sintering of some metal and magnetic materials,
scientific publications on achievements in the field of
SPS almost disappeared by the early 1980s.
The SPS method in the modern form was devel-
oped by Sumitomo Coal Mining Со, Ltd. in 1989 and
it has, together with the concept of simultaneous
application of high pulse current and high mechanical
pressure and due to improved hard and software,
become a new phase in powder technology.
The major peculiarity of the SPS method is sinter-
ing in a conducting mold with the simultaneous appli-
cation of mechanical pressure and DC pulses, which
makes processes of densification and sintering run
simultaneously.
Recently, the method has transformed into a new
technology of producing powder materials whose
advantages include energy efficiency, little effect on
the environment, and high production capacity.
The SPS method showed high efficiency in the
consolidation of ceramic and metal nanomaterials,
composite materials, functionally gradient materials,
composite materials based on carbon nanotubes and
mal electric materials, and biomaterials [2–7].
The SPS method was seen to be applicable when
used for the consolidation of nanomaterials [8–12].
For example, dense ceramics with a grain size of 10–
15 nm were produced from nanopowder CeO2 with a
grain size of 6–7 nm [13].
This paper includes a brief description of the SPS
method and recent successes and prospects for this
technology.
PECULIARITIES AND PRINCIPLES
OF THE CONSOLIDARION
OF POWDERS BY SPS
Compared to traditional technologies of sintering,
SPS has some features offering wide possibilities for
the development of new materials:
1. Rapid sintering (heating rate up to 2000°C/min).
2. Reliable control of sintering process parameters
and, as a result, control of material microstructure.
3. Generation of temperature gradient during sin-
tering providing the sintering of functionally gradient
materials.
4. Solid phase sintering (sintering of SiC and WC
up to high density without additional binders).
5. Low-temperature sintering (sintering of amor-
phous materials and magnetic materials below Curie
temperature).
6. Possibility of affecting sintered material with
electromagnetic field energy.
7. Possibility of combining sintering methods:
SPS–HP, SPS sintering in a magnetic field, SPS–
SHF (microwave) sintering, etc.

261
262 TOKITA

1
8

2 4
3
5 9
10
6
7
11

Fig. 1. Principle scheme of SPS plan: (1) upper electrode, (2) water-cooled vacuum chamber, (3) powder, (4) upper piston,
(5) mold, (6) lower piston, (7) lower electrode, (8) supply source (pulse generator), (9) hydraulic system, (10) sintering parame-
ters control system, and (11) sintering proess control system.

SPS usually implies the use of a graphite mold
filled with powder feedstock. Mechanical pressure
(20–100 МPа) and electric pulse current of low volt-
age (approximately 4–20 V) and high power (0.5–
40 kA) are applied to the mold along the vertical axis.
Molds for sintering can be made of steel, hard
alloys, ceramics, etc. The value of applied pressure can
reach 1GPa. The heating rate is usually 20–
200 K/min, though super rapid heating is possible at
rates of 500–1000 K/min.
For samples with small diameters (20–30 mm), the
heating and dwell time at a preset temperature take
approximately 20 min; for samples with large diame-
ters it might take up to 2 h, which nevertheless is a
quite rapid cycle that makes it possible to obtain high-
quality products with high density.
The basic scheme of an SPS plant is shown in Fig. 1.
A photograph of a standard single-chamber SPS
plant of moderate size is shown in Fig. 2. In addition
to this construction, there are plants with a built-in
glove box for sintering nanopowders and fully auto-
matic industrial plants.
The SPS process is based on the thermal, mechan-
ical, and electromagnetic effect on powder.
Using SPS results in a decrease in sintering tem-
perature by 100–200 K when compared to traditional
sintering methods. The basic mechanism controlling
the process of SPS is surficial diffusion stimulated by
rapid heating and the presence of electric field.

EXAMPLES OF USING SPS FOR CERAMICS

Fig. 2. SPS test plant (Sinter Land Co., Ltd., Japan).
(Maximum pressure 150 KN; maximum pulse current
force 7500 А).
PRODUCTION
High-temperature SPS offers the potential for
developing new characteristics of materials that will be
higher than characteristics of materials obtained by
hot pressing (HP) and hot isostatic pressing (HIP).
SPS makes it possible to obtain ceramics based on
oxides (Al2O3, ZrO2, TiO2, SiO2, MgO, CeO), cor-
bides (WC, SiC, B4C, TaC, TiC), borides (TiB2,
HfB2), and nitrides (Si3N4, TiN, AlN).
Figure 3 shows samples of various ceramics
obtained by SPS indicating sintering conditions.

NANOTECHNOLOGIES IN RUSSIA Vol. 10 Nos. 3–4 2015

 RECENT AND FUTURE PROGRESS ON ADVANCED CERAMICS SINTERING 263

Samples obtained by SPS

1 AbO3 40MPa 10 min −1300°C−2 min

1
2 PSZ 40 MPa 10 min −1300°C−2 min
1
3 SbN4 40MPa 13 min −1650°C−2 min
1
4 SiC 40 MPa 15 min −1900°C−2 min
1
5
1
B4C
40MPa 15 min −1900°C−2 min
6 TiBa
40 MPa 15 min −1900°C−2 min

ceramics
0.5 μm

Fig. 3. Ceramic samples produced by SPS.

The possibility of carrying out solid phase sintering

is a significant advantage of SPS when compared to
traditional sintering technologies. SPS makes it possi-
ble to obtain high-density materials with a structure
featuring high mechanical properties. Nanosized par-
ticles obtained due to rapid heating rates make it pos-
sible to improve the electric properties of ceramics
applied in electronics industry. In addition, if we pro-
vide the conditions under which diffusion occurs only
in surface layers of powder particles while inside parti-
cles changes are minimum and carry out sintering to
avoid the appearance of new phases on the surface of
sintering and concentration of impurities, then a sig-
nificant improvement of properties of sintered materi-
als can be achieved. Examples of Al2O3 and SiC
ceramic production by SPS are presented and their
characteristics are described.
Al2O3 BASED CERAMICS
Many papers are devoted to studies of the SPS of
ceramics based on oxides (Al2O3, ZrO2, TiO2, SiO2,
MgO, СеО, etc.). The most commonly used additives
are Y2O3, c-BN, TiN, SiC, ZrB2, TiO2, CaSiO3, car-
bon nanotubes (CNTs), hydroxyapatite (HAP), etc.
SPS makes it possible to minimize grain growth and
obtain high-density ceramics with grain sizes close to
the particle size of the initial powder.
Figure 4 shows micrographs of a fracture surface of
ceramics obtained by SPS from a α-Al2O3 powder of
high purity. The particle size of the initial powder was
100 nm. The heating rate was within a range of 50–
100 K/min. As the figure shows, sintering under a
temperature of 1423 K and pressure 100 МPа makes it
0.5 μm
Fig. 4. Raster electronic image of fracture surface of Al2O3
samples produced by SPS at (а) 1423 K, 100 MPa, and
(b) 1473 K, 30 MPa.
possible to obtain ceramics with a grain size of 200–
300 nm while the density of ceramics is 99.18% of the
theoretical value. The increased temperature of 1473 K
and decreased pressure of 30 МPа resulted in an
increase in grain size up to 400–500 nm, while the
density of the sample was 98.3%.
Thus SPS makes it possible to select parameters of
sintering to obtain desired physical properties of mate-
rial by controlling the microstructure and makes it
possible to control the process of consolidation, com-
bining restrained grain growth and higher material
density.
SiC BASED CERAMICS
In [10], the kinetics of densification and physical
and mechanical properties of silicon carbide obtained
by SPS and HP methods were compared. Under inves-
tigation was β-SiC powder (particle size of 0.28 μm).
5 wt. % Al2O3 and 3 wt. % Yb2O3 were added as sinter-
ing aids to β-SiC. The heating rate was 100 K/min for
SPS and 70 K/min for HP. The value of applied pres-
sure in both cases was 30 МPа.

NANOTECHNOLOGIES IN RUSSIA Vol. 10 Nos. 3–4 2015

264 TOKITA

Relative density, % 100

90

80

SPS
70
HP

(a) 1 nm
60
1800 1900 2000 2100 2200 2300 2400
Sintering temperature, K

Fig. 5. Dependence of density on the sintering temperature

of SiC samples produced by HP and SPS.

800
Bending strength, MPa

600 (b) 1 nm

Fig. 7. Raster electronic image of etched surface of SiC

samples produced by (а) SPS (2073 K, 30 MPa) and
400 (b) HP (2273 K, 30 MPa).

hardness of 23.5 GPа and fracture strength coefficient

200 SPS
HP
0 the grain size of ceramics obtained by SPS is larger
1800 1900 2000 2100 2200 2300 2400
Sintering temperature, K
Fig. 6. Dependence of bending strength on sintering tem-
perature of SiC samples produced by HP and SPS.
Figures 5–6 show the dependences of ceramics
density and bending strength on sintering temperature
under conditions of SPS and HP.
As Fig. 5 shows, in the case of SPS, a maximum
density of 98% is reached at the temperature of 2023 K,
while HP requires a temperature of 2173 K.
The bending strength (Fig. 6) of silicon carbide
obtained by SPS at a temperature of 2073 K is 720 МPа
with a hardness of 25 GPа and fracture strength coef-
ficient of 4 МPа m1/2. The sample obtained by HP at a
temperature of 2273 K has a density of 640 МPа at a
of 3.5 МPа m1/2.
Thus, the physical and mechanical properties of
silicon carbide obtained by HP are lower, though the
(Fig. 7).
X-Ray diffraction analysis (Fig. 8) showed that,
compared to HP, SPS does not result in the formation
of amorphous phases during sintering. The absence of
an amorphous phase is the reason for higher density of
SiC ceramics sintered by SPS [10].
SPS makes it possible to control phase transforma-
tions in materials, making it possible to create materi-
als with high functional properties.
WEAR RESISTANT CERAMICS BASED
ON Si3N4–Al2O3
Figure 9 shows items of thin technical ceramics
based on Si3N4–Al2O3 industrially produced by SPS.
These items are used as wear resistant elements in
homogenizers.

NANOTECHNOLOGIES IN RUSSIA Vol. 10 Nos. 3–4 2015

 RECENT AND FUTURE PROGRESS ON ADVANCED CERAMICS SINTERING 265

4H(004)

3C(220),4H(004)
YbAG(420), 4H(100)

3C(200),YbAG(521)

3C(400),4H(008)
3C(311),4H(114)
YbAG(721)(552)
YbAG(611)(533)
YbAG(321)

YbAG(640)
YbAG(444)

YbAG(642)
YbAG(422)
HP

4H(101)

4H(102)

4H(104)
4H(103)

4H(105)

4H(106)

4H(202)
Intensity

SPS

3C(111)

3C(200)
4H(102)

3C(220)

3C(311)

3C(400)
Powder

20 30 40 50 60 70 80
2θ, deg
Fig. 8. X-ray diffraction graph of SiC samples produced by HP and SPS.

As was mentioned earlier, one of the peculiarities of in a water jet and sand-blasting processing plants. In
the SPS method is the possibility for high-rate sinter- these plants, particles of alumina (Al2O3) or other
ing, providing the absence of grain growth of the initial ceramic material are added into water or another fluid
powder and the absence of micropores and structure as abrasive media. This mixture is jet sprayed under
inhomogeneities, which at a relative density of 99– certain pressure from a ceramic nozzle made of mate-
100% makes it possible to obtain hardness above
20 GPa. rial featuring high wear resistance and strength.
With molds of different designs (in the form of a SPS allows one to produce nozzles of materials
ring, cylinder, convex, etc.), nearly net-shaped items based on Al2O3 or В4С using a 3D net shape that
may be produced with allowance for machining of makes it possible to achieve a relative density of mate-
only 0.2–0.3 mm. rial of 100% and reduce following turning and grind-
SPS makes it possible to reduce the costs of produc- ing. The sample obtained by SPS has precise dimen-
tion due to the simplification of operations of the fol- sions of inner and outer diameter of the nozzle within
lowing processing of thin ceramics of high hardness.
a tolerance value of ±0.1 to ±0.2 mm. The hardness of
samples obtained by this method is approximately
WEAR RESISTANT CERAMICS BASED 29 GPа for В4С and 20 GPа for Al2O3. It should be
ON Al2O3–B4C noticed that the resistance of these items is ten times
Figure 10 shows the example of a nozzle made of higher than the resistance of nozzles available at the
Al2O3–В4С produced by SPS. These nozzles are used market at present.

Fig. 9. Ceramic parts produced on the basis of a composite Fig. 10. Nozzles for sand blasting cutting produced on the
system Si3N4–Al2O3 by SPS. basis of Al2O3 by SPS.

NANOTECHNOLOGIES IN RUSSIA Vol. 10 Nos. 3–4 2015

266
Fig. 11. Molds for nonspherical lenses produced of pure
WC by SPS.
Fig. 12. Functionally gradient samples of ZrO2 (3Y) (6 lay-
ers (on the left); 21 layers (on the right)) produced by SPS.
Fig. 13. Al2O3 sample with a diameter of 300 mm pro-
duced by SPS (relative density 98–99%).
NANOTECHNOLOGIES IN RUSSIA
TOKITA
STRONG PURE WC CERAMICS
Recently, pure tungsten carbide has been used for
molds for stamping nonspherical glass lenses used in
digital cameras and mobile phones [13].
The ceramics of pure WC is a product of the reac-
tive sintering of free carbon with WC powder with a
particle size less than 200 nm; it does not contain
inhibitors of grain growth and, compared to non-
bonded carbide available on the market, has a high
resistance to oxidation and high hardness (26 GPa)
and features a low thermal extension coefficient.
With the WC microstructure characterized by grain
growth of several hundreds of nanometers, the surface
roughness is not more than 10 nm while the absence of
binders in a form of Co or Ni makes it resistant to high
temperatures, wear, and thermal extension.
A photograph of WC mold is shown in Fig. 11.
FUCTIONALLY GRADIENT MATERIALS
SPS makes it possible to create a gradient inside the
sintered material, providing the possibility for sinter-
ing various multilayer samples. This method is quite
effective for the production of functionally gradient
materials [7, 12].
Figure 12 shows functionally gradient material
based on ZrO2 (3Y) ceramics and stainless steel
(SUS410L). This material, super resistant to any tem-
peratures, features a stepped concentration of compo-
nents. One side of the sample contains 100% of ZrO2
(3Y) and another is 100% metal, while in the middle it
contains metal–ceramic layers.
Various powder functionally gradient materials
with nonstepped gradient property based on the sub-
stances and combinations mentioned below were suc-
cessfully obtained: ZrO2/steel, ZrO2/TiAl, ZrO2/Ni,
Al2O3/steel, Al2O3/Ti, TiB2/Ti, Al2O3/Ti-6Al-4V,
WC/Co, WC/steel, WC/Ni, Cu/steel, SiO2/steel, apa-
tite/Ti, polyamide resin/Al, polyamide resin/Cu, phe-
nol resin/Cu, and composite materials based on Si3N4.
LARGE CERAMICS
Due to its rapid heating and short sintering time,
the use of SPS is related to problems of scaling, i.e.,
increasing sizes of blanks of sintered materials. These
problems are not as important for samples with diam-
eters smaller than 15–50 mm, for which it is easy to
achieve uniform heating of material. However, if the
sample diameter is 100–300 mm, a significant tem-
perature gradient inside of the sintered material may
occur which results in nonuniform densification.
A combination of fast and uniform heating is com-
plicated due to the nonuniform heat distribution
affected by such factors as the difference between ther-
mal conductivity of sintered material and molds, the
transfer of powder particles during sintering, the non-
uniform distribution of stresses in and blank during
pressing, etc.
Vol. 10 Nos. 3–4 2015
 RECENT AND FUTURE PROGRESS ON ADVANCED CERAMICS SINTERING
This problem is revealed most strongly during the
SPS of large ceramic parts under high temperatures
(1400–2700 K).
For the practical use of SPS, it is very important to
accumulate information on the proper preparation of
material and sintering furniture, as well as heating and
cooling conditions. In addition, the development of
specialized nonstandard equipment for SPS depend-
ing on the final purpose of products, including the
design of molds of various geometries and shapes, the
use of multiaxial and multistage pressing machines,
etc., is desired.
At present, SPS makes it possible to obtain ceramic
samples of Al2O3 with a maximum diameter of
300 mm and density of more than 98% (Fig. 13).
CONCLUSIONS
This paper covers a brief description of SPS and
examples of its applications.
The most important aspect for implementing SPS
in industrial production is parallel scientific studies
that would provide a “trinity” of hard ware, produc-
tion process, and the selection of powder materials as
part of a single approach.
ACKNOWLWDGMENTS
We would like to thank the Ministry of Education
and Science of the Russian Federation support
(Agreement no. 02.В.49.21.0003 dated August 27,
2013, between the Ministry of Education and Sci-
ence and Lobachevsky State University of Nizhni
Novgorod).
REFERENCES
1. K. Inoue, U.S. Patent No. 3241956.
NANOTECHNOLOGIES IN RUSSIA Vol. 10 Nos. 3–4
267
2. M. Tokita, “Trends in advanced SPS Spark Plasma
Sintering systems and technology,” J. Soc. Powder
Technol. Jpn. 30, 790–804 (1993).
3. M. Tokita, “Development of hardware and software for
Spark Plasma Sintering (SPS) technology,” J. High
Temp. Soc. Jpn. 31 (4), 215–224 (2005).
4. M. Tokita, “Development of advanced Spark Plasma
Sintering (SPS) systems and its applications,” Ceram.
Trans. 194, 51–60 (2006).
5. Z. A. Munir, U. Anselmi-Tamburini, and M. Ohyan-
agi, “The effect of electric plasma sintering method,”
J. Mater. Sci. 41, 763–777 (2006).
6. S. Grasso, Y. Sakka, and G. Maizza, “Electric current
activated/assisted sintering (ECAS): a review of patents
1906–2008,” Sci. Techn. Adv. Mater. 10, 053001 (2009).
7. M. Tokita, “The potential of Spark Plasma Sintering
(SPS) method for the fabrication on an industrial scale
of functionally graded materials,” Adv. Sci. Technol.
63, 322–331 (2010).
8. T. Takeuchi, M. Tabuchi, Y. Suyama, and H. Kageyama,
“Preparation of dense BaTiO3 ceramics with submi-
crometer grains by spark plasma sintering,” J. Am.
Ceram. Soc. 82, 939–943 (1999).
9. Z. Shen, M. Johnsson, Z. Zhao, and M. Nygren,
“Spark plasma sintering of alumina,” J. Am. Ceram.
Soc. 85, 1921–1927 (2002).
10. M. Tokita, N. Tamari, T. Takeuchi, and Y. Makino,
“Consolidation behavior and mechanical properties of
SiC with Al2O3 and Yb2O3 consolidated by SPS,” J. Jpn.
Soc. Powder Powder Metall. 56, 788–795 (2009).
11. Y. Makino, K. Mizuuchi, M. Tokita, Y. Agari, et al.,
Mater. Sci. Forum, 638–642, 2091-2096 (2010).
12. M. Tokita, “Spark Plasma Sintering (SPS) method,
systems, and applications,” in Handbook of Advanced
Ceramics, 2nd Ed. (2013), Chapter 11.2.3, pp. 1149–1177.
13. M. Tokita, Jpn. Patent No. 3935029.
Translated by S. Saveleva
2015