Applied Surface Science 442 (2018) 12–19

Contents lists available at ScienceDirect

Applied Surface Science

journal homepage: www.elsevier.com/locate/apsusc

Full Length Article

Preparation and flash sintering of MgTiO3 nanopowders obtained

by the polyacrylamide gel method
Xinghua Su ⇑, Ge Bai, Jing Zhang, Jie Zhou, Yongjie Jia
School of Materials Science and Engineering, Chang’an University, Xi’an 710061, China

a r t i c l e i n f o a b s t r a c t

Article history: Using a polyacrylamide gel method, phase pure and well-dispersed MgTiO3 nanopowders were prepared
Received 23 November 2017 at 800 °C for 2 h. It was found that a high mole ratio of monomers to precursors resulted in low formation
Revised 23 January 2018 temperature of MgTiO3, due to the highly mixing homogeneity and smaller particle sizes of precursors.
Accepted 31 January 2018
Sintering behaviors of MgTiO3 nanopowders under DC electric field from 500 to 800 V/cm were investi-
Available online 6 February 2018
gated. Nearly full dense MgTiO3 ceramics can be prepared in 30 s. An abrupt and simultaneous increase in
current density and power dissipation were observed in sintering process, which are characteristics of
Keywords:
flash sintering. The power dissipation for the flash sintering was found to be 82 mW/mm3. The densities
Magnesium titanate
Nanopowders
and average grain sizes of samples increase with the increase of the electrical field strength. It was sug-
Polyacrylamide gel method gested that Joule heating was the main mechanism of flash sintering of MgTiO3 ceramics. Our work pro-
Flash sintering vides a useful route for the fabrication of dense MgTiO3 ceramics at low temperature in short time.
Ó 2018 Elsevier B.V. All rights reserved.

1. Introduction
Magnesium titanate (MgTiO3) ceramic is a well-known dielec-
tric material applicable to microwave devices and systems due to
its excellent dielectric properties [1–3]. Several approaches for
the synthesis of MgTiO3 powders have been developed, such as
solid-state reaction method [4,5], sol-gel method [6–8], auto-
igniting combustion technique [9], solar physical vapor deposition
[10,11] and electrodeposition [12]. Solid-state reaction method is a
simple and cost-effective approach to prepare MgTiO3 powders.
However, a metastable phase MgTi2O5 usually appears in the final
products. MgTi2O5 as a secondary phase can worsen the dielectric
properties of the MgTiO3 ceramics [13], so MgTi2O5 should be
avoided using the solid-state reaction method. Other methods,
such as sol-gel method, auto-igniting combustion technique, solar
physical vapor deposition and electrodeposition, are complicated
and not suitable for large-scale production. Therefore, a facile syn-
thetic method to prepare pure MgTiO3 powders is needed to be
developed. In addition, the sintering temperature of MgTiO3 is high
to above 1400 °C, which is high energy consuming. In order to
lower the densification temperature, sintering aids are usually
used [14,15]. However, the unexpected secondary phase is formed
during the sintering process, which deteriorates the dielectric
properties of the MgTiO3. Very recently, Apostol et al. obtained
MgTiO3 geikielite major phase by solar sintering mixture of MgO
⇑ Corresponding author.
E-mail address: suxinghua@chd.edu.cn (X. Su).
and TiO2 powders at 1100 °C in air [16]. However, there is still
secondary phase existed in the prepared sample. Therefore, it is
important to prevent the formation of MgTi2O5 during the syn-
thetic process, and at the same time to lower the sintering temper-
ature for the fabrication of high quality MgTiO3 ceramics.
In the last several years, a novel sintering technology called
flash sintering has attracted worldwide attentions, because of its
low sintering temperature and high densification rate [17–20].
Flash sintering gives us an opportunity to fabricate dense MgTiO3
ceramics at low sintering temperature in short time.
In this work, a polyacrylamide gel method combined with the
flashing sintering is used for the fabrication of MgTiO3 ceramics
at low temperature. The polyacrylamide gel method is employed
to prepare high pure and well-dispersed MgTiO3 nanopowders.
The preparation conditions including the mole ratio of acrylamide
to precursor and the calcination temperature have been systemat-
ically investigated. In addition, the sintering behaviors of
as-obtained MgTiO3 nanopowders under a DC electrical field are
studied. Finally, the flash sintering mechanism is discussed and
an interpretation with Joule heating is proposed.
2. Experimental procedure
2.1. Preparation of MgTiO3 nanopowders
Titanium sulfate (Ti(SO4)2), magnesium nitrate (Mg(NO3)2
6H2O),
acrylamide (AM), N,N’-methylene-bis-acrylamide (MBAM), and
ammonium persulfate ((NH4)2S2O8) were used as raw materials.

https://doi.org/10.1016/j.apsusc.2018.01.316
0169-4332/Ó 2018 Elsevier B.V. All rights reserved.
 X. Su et al. / Applied Surface Science 442 (2018) 12–19 13

In a typical procedure, a aqueous solution containing 0.01 mol/L

Ti4+ and 0.01 mol/L Mg2+ was prepared by dissolving Ti(SO4)2 and
Mg(NO3)2
6H2O in deionized water. Then the monomers, AM and
MBAM were added to the solution. The concentration of AM was
adjusted to 0.3, 0.6, and 1.2 mol/L, respectively. After the mono-
mers were completely dissolved, (NH4)2S2O8 was added to the
solution. In all experiments, the mole ratio of AM/MBAM/(NH4)2S2O8
was kept as 24/2/1. The mixed solution was kept stirring until a
clear solution was obtained. Then the solution was heated at 80 °C
to form a white gel. The white gel was dried at 80 °C in oven to
obtain xerogel, which was then calcined at different temperatures
(600, 800 and 1000 °C) for 2 h in air at a heating rate of 5 °C/min.

2.2. Flash sintering process

The as-prepared MgTiO3 nanopowders were mixed with 5 wt% Fig. 1. DTA-TGA curves for the xerogel with an acrylamide to MgTiO3 mole ratio of
PVA binder in aqueous solution. Then the mixed nanopowders 120.
were grounded and uniaxially pressed into dog bone-shaped green
compacts at a pressure of 300 MPa. The green compact had a rect- on the TGA curve, revealing complete removal of the organic
angular gauge section with a length of 20 mm, width of 3 mm, and species.
thickness of 0.90 ± 0.05 mm. These green compacts were pre- XRD patterns of the samples prepared by calcining the xerogel
sintered at 700 °C for 1 h to burn out the PVA binder and to allow with A:MT mole ratio of 30 at different temperatures are shown
easier handling for successive flash sintering experiments. Then in Fig. 2. At 600 °C, there are only some weak and broaden diffrac-
the green compact was suspended with platinum wires and plat-
inum paste was used to ensure good electrical contact. Flash sin-
tering experiments were performed in a tubular furnace by
applying different DC electrical field strengths (500, 600, 700,
and 800 V/cm) with a heating rate of 10 °C/min; the power control
switched from constant voltage mode to constant current mode
when the current reached a preset maximum value of 100 mA;
samples were hold for 30 s at the constant current mode. The volt-
age was applied using HPS 0614 power supply (Lanyi, China); the
current through the circuit was measured using DMM 4040 digital
multimeter (Tektronix, USA).

2.3. Characterization

The thermal behaviors of the xerogel were investigated by a

DTA-TGA analyzer (SDT Q600, TA Instruments, USA). The crys-
talline structure evolution of the sample was studied by an X-ray
diffractometer (XRD, Bruker D8 Davinci, Germany). The morphol-
ogy of the MgTiO3 nanopowder and surface morphology of bulk
obtained from flash sintering were examined by a field emission Fig. 2. XRD patterns of powders obtained by calcining the xerogel with an A:MT
mole ratio of 30 at different temperatures.
scanning electron microscopy (SEM, Hitachi S-4800, Japan). Sin-
tered bulk density was measured by the standard Archimedes
method and the relative density was determined with respect to
the theoretical density of MgTiO3 (3.894 g/cm3). The average grain
size of the sample was calculated by linear intercept method from
the SEM image of the thermally etched surface. Thermal etching for
the bulk was carried out in air at 1000 °C for 10 min.

3. Results and discussion

Fig. 1 shows the DTA-TGA curves of the xerogel with the

acrylamide (AM) to MgTiO3 (abbreviated as A:MT) mole ratio of
120. The broad endothermic peak from room temperature to 220 °C
corresponding to a mass loss of 11.7% is attributed to the loss of
physically and chemically adsorbed water. The endothermic peak
around 265 °C corresponding to a mass loss of 23.5% is assigned
to the decomposition of Mg(NO3)2 [21]. The third endothermic
peak around 308 °C with a mass loss of 11.8% is considered to be
the decomposition of Ti(SO4)2 [22]. The exothermic peak centered
at 546 °C is due to the decomposition of polyacrylamide [23]. At Fig. 3. XRD patterns of powders obtained by calcining the xerogel with an A:MT
temperatures higher than 610 °C, there is no further weight loss mole ratio of 60 at different temperatures.
14 X. Su et al. / Applied Surface Science 442 (2018) 12–19
Fig. 4. XRD patterns of powders obtained by calcining the xerogel with an A:MT
mole ratio of 120 at different temperatures.
tion peaks can be observed, implying the poor crystallization of
sample. The crystalline structures cannot be determined. At 800 °C,
the XRD pattern shows obvious diffraction peaks that can be
assigned to MgTiO3 (PCPDF#06-0494) and TiO2 (PCPDF#78-
2485), respectively. At 1000 °C, diffraction peaks of TiO2 are
completely disappeared and the XRD pattern shows the strong
diffraction peaks of MgTiO3. Meanwhile, the weak diffraction peaks
of MgTi2O5 (PCPDF# 79-0832) appear in this pattern. From the XRD
results, it can be concluded that the sample prepared at 1000 °C
consists of the major MgTiO3 phase and the minor MgTi2O5 phase.
Fig. 3 shows the XRD patterns of samples prepared by calcining
the xerogel with A:MT mole ratio of 60 at different temperatures.
At 600 °C, diffraction peaks of both MgTiO3 and MgTi2O5 coexist
in the XRD pattern. At 800 °C, the diffraction peak intensities of
MgTiO3 increase obviously and diffraction peak intensities of
Fig. 5. SEM images and particle size distributions of the MgTiO3 nanopowders obtained by calcining the xerogel with an A:MT mole ratio of 60 (a, c), and 120 (b, d) at 800 °C.
Fig. 6. Schematic diagram illustrating the preparation of MgTiO3 nanopowders.
MgTi2O5 decrease, indicating the expense of MgTi2O5 as the calci-
nation temperature increases. When the calcination temperature
increases to 1000 °C, there are only the diffraction peaks of MgTiO3
can be observed, implying the complete formation of MgTiO3.
Based on above XRD results, it is found that the mole ratio of A:
MT has great effect on the formation temperature of single-phase
MgTiO3. We further increased the A:MT mole ratio to 120 and cal-
cined the xerogel at 600, 800 and 1000 °C, respectively. The XRD
results are shown in Fig. 4. At 600 °C, the XRD pattern contains
the strong diffraction peaks of MgTiO3, together with some weak
diffraction peaks of MgTi2O5. After calcination at 800 °C, only
 X. Su et al. / Applied Surface Science 442 (2018) 12–19 15

strong diffraction peaks of MgTiO3 can be observed, indicating the

Fig. 7. Relationship between current density and furnace temperature in flash
sintering of MgTiO3 nanopowders under different electrical field strengths.
single-phase MgTiO3 is obtained. When calcination temperature
increases to 1000 °C, the diffraction peaks of MgTiO3 become
stronger and sharper, resulting from the further crystallization of
MgTiO3. Obviously, increasing the A:MT mole ratio can lower the
formation temperature of single-phase MgTiO3. In the present
study, pure MgTiO3 can be prepared at 800 °C when A: MT mole
ratio increases to 120.
The morphologies of the as-prepared MgTiO3 nanopowders are
observed by SEM. Fig. 5 shows the SEM images of the MgTiO3
nanopowders prepared by calcining the xerogel with different A:
MT mole ratios at 800 °C. As shown in Fig. 5(a) and (c), the MgTiO3
nanoparticles prepared with A:MT mole ratio of 60 are well-
dispersed, showing uniform polyhedral morphology, and having
an average particle size of about 92 nm. Increasing the A:MT mole

Fig. 8. SEM surface and cross section images of the samples sintered at different electrical fields: (a, b) 500 V/cm, (c, d) 600 V/cm, (e, f) 700 V/cm, (g, h) 800 V/cm.
16 X. Su et al. / Applied Surface Science 442 (2018) 12–19

ratio to 120, the obtained MgTiO3 nanoparticles are still well-

dispersed, showing similar polyhedral morphology. However, the
average particle size decreases to about 66 nm (Fig. 5(b and d)).
According to the SEM results, it can be concluded that the average
particle size of MgTiO3 nanopowder decreases with increasing the
mole ratio of A:MT.
In general, the preparation of MgTiO3 by traditional solid-state
reaction method is unavoidably accompanied by the formation of
secondary phase of MgTi2O5 due to the low solidus limit of the
MgTiO3 system [14]. To prepare pure MgTiO3, it is necessary to
improve the mixing homogeneity of the precursors. Bernard et al.
synthesized the pure MgTiO3 powder at 1000 °C by optimizing
mixing/grinding condition of MgO and TiO2 powders [4]. They
claimed that the mixture of precursors MgO and TiO2 should be
extremely mixed, so the element diffusion distances during the
solid-state reaction were shortened and pure MgTiO3 can be pre-
pared at lower temperatures. In this work, the AM and MBAM Fig. 9. Relative density and average grain size of MgTiO3 bulks as a function of DC
electrical field.
monomers polymerize to form a three-dimensional polymer net-
work which helps the distribution of the precursors in the solution.
It ensures the homogeneous mixing of the precursors, and also
Table 1
prevents the aggregation of the MgTiO3 nanoparticles during the
Relative densities and average grain sizes of samples sintered at various applied
calcination process. As a result, pure and well-dispersed MgTiO3 electrical fields.
nanopowders can be prepared at relatively low temperature.
Electrical field (V/cm) Average grain size (nm) Relative density (%)
Fig. 6 illustrates the formation of MgTiO3 nanopowder by polyacry-
lamide gel method. 500 68 84.5
600 980 89.2
The sintering behaviors of as-prepared MgTiO3 nanopowders
700 1230 94.7
with an average particle size of 66 nm under the DC electrical field 800 1242 97.6
are investigated. Fig. 7 shows the relationship between the current
density of sample and the furnace temperature under the different
electrical field strengths. It can be seen that the current density
increases sharply when the furnace temperature rises to a particu-
lar value, which is a characteristic of flash sintering [24–26]. The
onset temperatures of flash sintering under the electrical field
strengths of 500, 600, 700 and 800 V/cm are 1241, 1228, 1154
and 1128 °C, respectively. Obviously, the onset temperature
decreases with the increase of the electrical field strength.
Fig. 8 shows the SEM images of the samples obtained by flash
sintering at various electrical field strengths. The MgTiO3 sintered
at 500 V/cm exhibits a fine grain size of about 68 nm and some
amount of pores are existed, as shown in Fig. 8(a). The cross section
image shows that the sample mainly consists of particle aggregates
(Fig. 8(b)), indicating the low density of MgTiO3 ceramic. This is
also confirmed by the density measurement. At 600 V/cm, the
average grain size of the sintered sample increases rapidly to
Fig. 10. SEM image of the sample sintered at 1400 °C for 30 s under the
980 nm, and the SEM images show a dense structure with only a conventional sintering condition.
few pores, as shown in Fig. 8(c and d). When the sample sintered
at 700 V/cm, the average grain size increases to 1230 nm, and a
more dense structure can be observed from the SEM images
(Fig. 8(e and f)). At 800 V/cm, the SEM images show that MgTiO3
ceramic is nearly full dense and only several pores can be observed,
as shown in Fig. 8(g) and (h). The relative densities and average
grain sizes of the sintered MgTiO3 ceramics at various applied elec-
trical fields are summarized in Table 1 and Fig. 9. It can be seen that
both the relative density and grain size increase with increasing
the electrical field strength. The average grain size increases
rapidly from 68 nm at 500 V/cm to 980 nm at 600 V/cm, while
slowly increases to 1230 nm at 700 V/cm. When the electrical field
increases to 800 V/cm, the average grain size is only slightly
increased. Researchers have reported the retardation of grain
growth during the flash sintering [27–29]. However, in this work,
the retardation of grain growth does not be observed. It is interest-
ing that the grain size increases rapidly at relatively low electrical
fields and increases slowly at high electrical fields. How this hap-
pens need to be further studied. It should be noted that the flash
sintering is an effective method to prepare dense MgTiO3 ceramics Fig. 11. Power dissipation during flash sintering of MgTiO3 nanopowders (current
in short time at low temperature. For comparison, the MgTiO3 limit = 100 mA). The dashed line indicates the two different sintering behaviors.
 X. Su et al. / Applied Surface Science 442 (2018) 12–19
nanopowder with an average particle size of 66 nm is sintered at
high temperature of 1400 °C without an electrical field for 30 s.
The surface morphology of the sample is shown in Fig. 10. It can
be seen that the sample has a porous structure with a relative den-
sity is 82%, lower than that obtained by flash sintering.
The specific power dissipation as a function of the furnace tem-
perature at various electrical fields is shown in Fig. 11. The curves
can be categorized into two different regions: in the region of the
power dissipation lower than 82 mW/mm3, the curves show a lin-
early Arrhenius profile, which is a conventional sintering behavior
under the electrical field; in the region of the power dissipation
higher than 82 mW/mm3, the curves show a line vertical to the
axis, which is consistent with the results of previous reports [30–
32]. It is well known that flash sintering is characterized by an
onset of the power-surge, and an abrupt increase of the electrical
conductivity, as indicated in Fig. 7. It is therefore concluded that
the flash sintering of MgTiO3 nanopowders occurs when the power
dissipation is approximately 82 mW/mm3. According to the previ-
ous reports, for electrically conducting, semiconducting and dielec-
tric materials, the flash sintering occurs when the power
dissipation is in the range of 10–50 mW/mm3 [33–38]. It is recog-
nized that effects of electrical field to the flash sintering can vary
significantly for different materials systems [39]. Since MgTiO3 is
an insulating material, it may lead to a higher onset of the
power-surge for flash sintering.
Fig. 12 illustrates the power dissipation against time curves for
a holding duration of 30 s after the occurrence of flash sintering
under different electrical fields with a current limit of 100 mA.
Obviously, the power dissipation rises abruptly to a limited maxi-
mum value. Nearly instantaneously, the power supply switches
from voltage control to current control. Then the power dissipation
Fig. 12. Power dissipation against time curve for a duration of 30 s after the occurrence of flash sintering under a DC electrical field of 500 (a), 600 (b), 700 (c), and 800 V/cm
(d), with a current limit of 100 mA.
17
declines sharply to a steady state. A spike with a width of about 2 s
is observed. At the steady state, the power dissipations are about
35, 58, 88 and 102 W for the electrical fields of 500, 600, 700 and
800 V/cm, respectively. Clearly, the power dissipation at the steady
state increases with increasing the electrical field.
Joule heating is an important effect that accompanies the flash
sintering. Due to the Joule heating, the actual sample temperature
increases with the dissipation of electrical power energy. The
increase of the temperature is calculated using a black body radia-
tion model. The calculation is based on the following equation
[40]:
 1=4
W
T ¼ T 40 þ ð1Þ
Ar
where T is the actual sample temperature, and T 0 is the furnace
temperature, A is the surface area of sample, which is
1:614  104 m2 in this experiment, r is the black body radiation
constant, which equals to 5:67  108 W=m2
K4 , W is the electrical
power dissipation at steady state during the flash sintering. Using
the Eq. (1), the actual sample temperature of MgTiO3 is estimated
and reported in Table 2 and Fig. 13. In our experiments, the power
dissipation increases with increasing the electrical field strength.
Consequently, although the furnace temperature at the onset of
the flash sintering decreases when the electrical field strength is
increased, the actual sample temperature increases. The function
of the electrical field and estimated temperature (actual sample
temperature) reveals a linear relationship, as shown in Fig. 13.
When the electrical field is 500, 600, 700, and 800 V/cm, the esti-
mated sample temperature is 1463, 1565, 1653, and 1695 °C,
respectively, which are high enough to sinter MgTiO3 ceramics.
18 X. Su et al. / Applied Surface Science 442 (2018) 12–19

Table 2 Science Foundation under grant No. 2015M582584, the Postdoc-

Electrical field, power dissipation, furnace temperature for onset of flash sintering, toral Research Project of Shaanxi Province under grant No.
and sample temperature calculated from a black body radiation model.
2016BSHEDZZ06, the Special Fund for Basic Scientific Research of
Electrical Power Furnace temperature for Sample Central Colleges, Chang’an University under grant No.
field dissipation onset of flash temperature 310831171011, the International Science & Technology Coopera-
(V/cm) (W) sintering (°C) (°C)
tion and Exchanges Plan in Shaanxi Province of China under grant
500 35 1241 1463 No. 2016KW-044, and the Special Fund for Basic Research Support
600 58 1228 1565
700 88 1154 1653
Programs of Chang’an University.
800 102 1128 1695

References

[1] R.J. Cava, Dielectric materials for applications in microwave communications, J.

Fig. 13. Estimated temperature and furnace temperature as a function of applied
electrical field strength.
Higher electrical field leads to the increased power dissipation at
the steady state (Fig. 12), resulting in the higher sample tempera-
ture. It should be noted that the estimated temperature refers to
the sample at steady condition, and the actual sample temperature
at the initial transient condition of flash sintering is even be higher
than those calculated values [41]. Therefore, it is suggested that the
diffusional mass transport is enhanced by the rapid increase of tem-
perature due to the Joule heating under applied electrical fields,
resulting in the rapid densification of MgTiO3.
4. Conclusions
Phase pure and well-dispersed MgTiO3 nanopowders with uni-
form particle size have been successfully prepared using the poly-
acrylamide gel method. High mole ratio of monomer (AM) to the
precursors leads to a low formation temperature of MgTiO3, due
to the high homogeneity and smaller particle sizes of the precur-
sors. As a result, MgTiO3 nanopowders with an average particle
size of 66 nm are prepared at 800 °C for 2 h.
During the flash sintering of MgTiO3 nanopowders, the current
density through the sample rises sharply when the furnace tem-
perature increases to a certain value. The power dissipation for
the onset of the flash sintering is about 82 mW/mm3. SEM analysis
shows that the grain size increases rapidly at relatively low electri-
cal fields and increases slowly at high electrical fields. Joule heating
is suggested to be responsible for the flash sintering of MgTiO3.
This work provides a potentially useful technique for the fabrica-
tion of phase pure and dense MgTiO3 ceramics at low furnace tem-
perature in short time.
Acknowledgements
This work was supported by the National Natural Science Foun-
dation of China under grant No. 51102022, the China Postdoctoral
Mater. Chem. 11 (2001) 54–62.
[2] J. Zhang, Z. Yue, X. Zhang, L. Li, Low-temperature sintering and microwave
dielectric properties of CaF2-doped MgTiO3 ceramics, Ceram. Int. 41 (2015)
S515–S519.
[3] J. Bernard, D. Houivet, J.E. Fellah, J.M. Haussonne, MgTiO3 for Cu base metal
multilayer ceramic capacitors, J. Eur. Ceram. Soc. 24 (2004) 1877–1881.
[4] J. Bernard, F. Belnou, D. Houivet, J.M. Haussonne, Synthesis of pure MgTiO3 by
optimizing mixing/grinding condition of MgO+TiO2 powders, J. Mater. Process.
Technol. 199 (2008) 150–155.
[5] K. Sreedhar, N.R. Pavaskar, Synthesis of MgTiO3 and Mg4Nb2O9 using
stoichiometrically excess MgO, Mater. Lett. 53 (2003) 452–455.
[6] H. Wang, Q. Yang, D. Li, L. Huang, S. Zhao, S. Xu, Sintering behavior and
microwave dielectric properties of MgTiO3 ceramics doped with B2O3 by sol-
gel method, J. Mater. Sci. Technol. 28 (2012) 751–755.
[7] R.R. Kanna, N.R. Dhineshbabu, P. Paramasivam, V. Rajendran, R. Yuvakkumar,
Synthesis of geikielite (MgTiO3) nanoparticles via sol-gel method and studies
on their structural and optical properties, J. Nanosci. Nanotechno. 16 (2016)
7635–7641.
[8] Y.-M. Miao, Q.-L. Zhang, H. Yang, H.-P. Wang, Low-temperature synthesis of
nano-crystalline magnesium titanate materials by the sol-gel method, Mater.
Sci. Eng. B 128 (2006) 103–106.
[9] M.K. Suresh, J.K. Thomas, H. Sreemoolanadhan, C.N. George, A. John, S.
Solomon, P.R.S. Wariar, J. Koshy, Synthesis of nanocrystalline magnesium
titanate by an auto-igniting combustion technique and its structural,
spectroscopic and dielectric properties, Mater. Res. Bull. 45 (2010) 761–765.
[10] I. Apostol, K.V. Saravanan, C.J.A. Monty, P.M. Vilarinho, Solar physical vapor
deposition: A new approach for preparing magnesium titanate nanopowders,
Appl. Surf. Sci. 285P (2013) 49–55.
[11] I. Apostol, A. Mahajan, C.J.A. Monty, K.V. Saravanan, Nanostructured MgTiO3
thick films obtained by electrophoretic deposition from nanopowders
prepared by solar PVD, Appl. Surf. Sci. 358 (2015) 641–646.
[12] N. Hashimoto, S. Hatakeyama, N. Doki, M. Yokota, K. Shimizu, Novel
reproducible fabrication of MgTiO3 nanoparticles by electrodeposition,
Chem. Lett. 37 (2008) 364–365.
[13] E.S. Kim, S.N. Seo, Evaluation of microwave dielectric properties of MgO-TiO2
system by dielectric mixing rules, J. Kor. Ceram. Soc. 47 (2010) 163–168.
[14] F. Belnou, J. Bernard, D. Houivet, J.M. Haussonne, Low temperature sintering of
MgTiO3 with bismuth oxides based additions, J. Eur. Ceram. Soc. 25 (2005)
2785–2789.
[15] Q.L. Zhang, H. Yang, Low-temperature sintering and microwave dielectric
properties of MgTiO3 ceramics, J. Mater. Sci: Mater. Electron. 18 (2007) 967–
971.
[16] I. Apostol, J. Rodríguez, I. Cañadas, J. Galindo, S.L. Mendez, P.L.A. Martinsc, L.
Cunha, K.V. Saravanan, Concentrated solar energy used for sintering
magnesium titanates for electronic applications, Appl. Surf. Sci. 10.1016/j.
apsusc.2017.09.224.
[17] M. Cologna, B. Rashkova, R. Raj, Flash sintering of nanograin zirconia in <5 s at
850 °C, J. Am. Ceram. Soc. 93 (2010) 3556–3559.
[18] C. Schmerbauch, J. Gonzalez-Julian, R. Röder, C. Ronning, O. Guillon, Flash
sintering of nanocrystalline zinc oxide and its influence on microstructure and
defect formation, J. Am. Ceram. Soc. 97 (2014) 1728–1735.
[19] A.L.G. Prette, M. Cologna, V. Sglavo, R. Raj, Flash-sintering of Co2MnO4 spinel
for solid oxide fuel cell applications, J. Power Sources 196 (2011) 2061–2065.
[20] X. Hao, Y. Liu, Z. Wang, J. Qiao, K. Sun, A novel sintering method to obtain fully
dense gadolinia doped ceria by applying a direct current, J. Power Sources 210
(2012) 86–91.
[21] F. Paulik, J. Paulik, M. Arnold, R. Naumann, Investigation on the thermal
behaviour of Mg(NO3)2 6H2O I. The decomposition behavior, J. Therm. Anal.
Calorim. 34 (1988) 627–635.
[22] J.R. Sohn, S.H. Lee, P.W. Cheon, H.W. Kim, Acidic properties and catalytic
activity of titanium sulfate supported on TiO2, Bull. Korean Chem. Soc. 25
(2004) 657–664.
[23] M. Mardali, R. Sarraf-Mamoory, B. Sadeghi, B. Safarbali, Acrylamide route for
the co-synthesis of tungsten carbide-cobalt nanopowders with additives,
Ceram. Int. 42 (2016) 9382–9386.
[24] E. Bichaud, J.M. Chaix, C. Carry, M. Kleitz, M.C. Steil, Flash sintering incubation
in Al2O3/TZP composites, J. Eur. Ceram. Soc. 35 (2015) 2587–2592.
[25] K. Sun, J. Zhang, T. Jiang, J. Qiao, W. Sun, D. Rooney, Z. Wang, Flash-sintering
and characterization of La0.8Sr0.2Ga0.8Mg0.2O3-d electrolytes for solid oxide fuel
cells, Electrochim. Acta 196 (2016) 487–495.
 X. Su et al. / Applied Surface Science 442 (2018) 12–19
[26] E. Zapata-Solvas, S. Bonilla, P.R. Wilshaw, R.I. Todd, Preliminary investigation
of flash sintering of SiC, J. Eur. Ceram. Soc. 33 (2013) 2811–2816.
[27] Y. Liu, X. Hao, Z. Wang, J. Wang, J. Qiao, Y. Yan, K. Sun, A newly-developed
effective direct current assisted sintering technique for electrolyte film
densification of anode-supported solid oxide fuel cells, J. Power Sources 215
(2012) 296–300.
[28] D. Yang, R. Raj, H. Conrad, Enhanced sintering rate of zirconia (3Y-TZP) through
the effect of a weak DC electric field on grain growth, J. Am. Ceram. Soc. 93
(2010) 2935–2937.
[29] S. Ghosh, A.H. Chokshi, P. Lee, R. Raj, A huge effect of weak dc electrical
fields on grain growth in zirconia, J. Am. Ceram. Soc. 92 (2009) 1856–
1859.
[30] M. Biesuz, V.M. Sglavo, Flash sintering of alumina: Effect of different operating
conditions on densification, J. Eur. Ceram. Soc. 36 (2016) 2535–2542.
[31] J.S.C. Francis, R. Raj, Flash-sinterforging of nanograin zirconia: field assisted
sintering and superplasticity, J. Am. Ceram. Soc. 95 (2012) 138–146.
[32] K.S. Naik, V.M. Sglavo, R. Raj, Field assisted sintering of ceramic constituted by
alumina and yttria stabilized zirconia, J. Eur. Ceram. Soc. 34 (2014) 2435–
2442.
[33] J.A. Downs, V.M. Sglavo, Electric field assisted sintering of cubic zirconia at 390
°C, J. Am. Ceram. Soc. 96 (2011) 1342–1344.
19
[34] M. Cologna, J.S.C. Francis, R. Raj, Field assisted and flash sintering of alumina
and its relationship to conductivity and MgO-doping, J. Eur. Ceram. Soc. 31
(2011) 2827–2837.
[35] A. Karakuscu, M. Cologna, D. Yarotski, J. Won, J.S.C. Francis, R. Raj, B.P.
Uberuaga, Defect structure of flash-sintered strontium titanate, J. Am. Ceram.
Soc. 95 (2012) 2531–2536.
[36] S.K. Jha, R. Raj, The effect of electric field on sintering and electrical
conductivity of titania, J. Am. Ceram. Soc. 97 (2014) 527–534.
[37] H. Yoshida, Y. Sakka, T. Yamamoto, J.-M. Lebrun, R. Raj, Densification behavior
and microstructural development in undoped yttria prepared by flash-
sintering, J. Eur. Ceram. Soc. 34 (2014) 991–1000.
[38] J.-C. M’Peko, J.S.C. Francis, R. Raj, Field-assisted sintering of undoped BaTiO3:
microstructure evolution and dielectric permittivity, J. Eur. Ceram. Soc. 34
(2014) 3655–13600.
[39] Y. Zhang, J. Nie, J.M. Chan, J. Luo, Probing the densification mechanisms during
flash sintering of ZnO, Acta Mater. 125 (2017) 465–475.
[40] R. Raj, Joule heating during flash-sintering, J. Eur. Ceram. Soc. 32 (2012) 2293–
2301.
[41] T. Jiang, Y. Liu, Z. Wang, W. Sun, J. Qiao, K. Sun, An improved direct current
sintering technique for proton conductor-BaZr0.1Ce0.7Y0.1Yb0.1O3: The effect of
direct current on sintering process, J. Power Sources 248 (2014) 70–76.