04-Ilmenite-type structure and pervoskite structure mix-phase ceramics at microwave frequency

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Ilmenite-type structure and pervoskite structure
mix-phase ceramics at microwave frequency
Yuan-Bin Chen
To cite this article: Yuan-Bin Chen (2024) Ilmenite-type structure and pervoskite structure mix-
phase ceramics at microwave frequency, Journal of Asian Ceramic Societies, 12:1, 79-85, DOI:
10.1080/21870764.2023.2301238
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RESEARCH ARTICLE
Ilmenite-type structure and pervoskite structure mix-phase ceramics at 
microwave frequency
Yuan-Bin Chen
School of Electronics and Electrical Engineering, Zhaoqing University, Guangdong, PR China
ABSTRACT
The impact of CuB2O4 additive used as a sintering aid on the microstructures and microwave 
dielectric characteristics of mixed phase (Mg0.95Zn0.05)Co0.05TiO3-Ca0.6(La0.9Y0.1)0.2667TiO3 cera-
mics was investigated. CuB2O4 additives can effectively lower the densification temperature of 
(Mg0.95Zn0.05)Co0.05TiO3-Ca0.6(La0.9Y0.1)0.2667TiO3 from 1450°C to the range of 1050°C ~ 1175°C. 
Doping CuB2O4 (0.25 ~ 2 wt%) in 0.875(Mg0.95Zn0.05)Co0.05TiO3-0.125Ca0.6(La0.9Y0.1)0.2667TiO3 
ceramics can substantially enhance their microwave dielectric properties and density. With 
the addition of 1% and 0.25% CuB2O4, Q × f values of 43,000 GHz and 7700 GHz were obtained 
at 1050–1175°C, respectively. Different additions of CuB2O4 have a significant effect on the Q × 
f value. Temperature coefficient of resonant frequency of 0.875(Mg0.95Zn0.05)Co0.05 
TiO3-0.125Ca0.6(La0.9Y0.1)0.2667TiO3 (0.875MZCT–0.125CLYT) varied from 16 to 30.9 ppm/°C 
when adding different CuB2O4 (0.25 ~ 2 wt%).
ARTICLE HISTORY 
Received 6 September 2023 
Accepted 28 December 2023 
KEYWORDS 
Microwave; ceramics; 
dielectric
1. Introduction
As mobile communication technology enters the (5th 
generation mobile networks) 5 G era, the development 
of massive multi-input multi-output (MIMO) technol-
ogy, coupled with the increasingly stringent require-
ments brought by base station integration, puts 
forward higher requirements for filters [1,2]. 
Microwave ceramic filter element media, which has 
received a lot of interest in the field of next- 
generation filters [2,3], has a comprehensive 
advantage of light weight and good temperature 
drift resistance under the premise of achieving the 
core performance requirements [4–8].
The manufacture of powder raw materials and the 
improvement of ceramic properties of microwave 
dielectric are now the most challenging technical 
issues to overcome in order to better fulfill the devel-
opment needs of ceramic filters. Permittivity(εr), quality 
factor (Q × f), and temperature coefficient of resonant 
frequency are the three main characteristics of micro-
wave dielectrics. A low εr can shorten the signal trans-
mission time, a high Q × f can increase the selectivity 
and longevity of microwave components, and 
a temperature coefficient of resonant frequency close 
to zero can allow electronic devices to operate reliably 
in a range of temperature environments [9–18].
MgTiO3-based microwave dielectrics have been 
intensively studied for years with low dielectric loss. 
MgTiO3-CaTiO3 ceramics made of a mixture of 
modified magnesium titanate and perovskite struc-
tured calcium titanate have been applied in dielectric 
resonators and patch antennas. With a ratio of Mg:Ca 
= 95:5, 0.95 MgTiO3-0.05CaTiO3 mixed phase ceramic 
has an εr ~21, a Q×f ~ 56,000 (at 7 GHz), and a zero τf 
value [19]. With the partial replacement (Mg0.7Zn0.3) 
by Co, (Mg0.7Zn0.3)0.95Co0.05TiO3 had excellent dielec-
tric properties with an εr ~20, Q×f ~ 163,560 GHz, and 
a τf ~ −65 ppm/oC. To produce a temperature-stable 
material, Ca0.6(La0.9Y0.1)0.2667TiO3 which has a large 
positive τf value of +380 ppm/ oC, was added to 
(Mg0.7Zn0.3)0.95Co0.05TiO3.
There are three approaches to reducing the sintering 
temperature of microwave dielectric ceramics: low melt-
ing sintering aids addition [20–22], chemical processing, 
and the use of smaller particles as the starting materials. 
Of these three, sintering aids addition is the most effec-
tive and least expensive. However, no liquid-phase sinter-
ing of xMZCT-(1-x)CLYT with sintering aids addition has 
been reported yet. Previously, CuB2O4 was researched 
and found to have good dielectric properties [23].
In this paper, CuB2O4 was used as a sintering aid for 
reducing the sintering temperature of xMZCT-(1-x)CLYT 
ceramics. The effects of CB content on the densification, 
phase development and dielectric properties of 
0.875MZCT–0.125CLYT ceramics are investigated. The 
analysis focused on the crystal phase, microstructure, 
and microwave dielectric properties of 0.875MZCT– 
0.125CLYT ceramics intermixed with CuB2O4.
CONTACT Yuan-Bin Chen n2890103@outlook.com School of Electronics and Electrical Engineering, Zhaoqing University, Guangdong 526061, PR 
China
JOURNAL OF ASIAN CERAMIC SOCIETIES 
2024, VOL. 12, NO. 1, 79–85 
https://doi.org/10.1080/21870764.2023.2301238
© 2024 The Author(s). Published by Informa UK Limited, trading as Taylor & Francis Group on behalf of The Korean Ceramic Society and The Ceramic Society of Japan. 
This is an Open Access article distributed under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/4.0/), which permits 
unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. The terms on which this article has been published allow the posting 
of the Accepted Manuscript in a repository by the author(s) or with their consent.
http://www.tandfonline.com
https://crossmark.crossref.org/dialog/?doi=10.1080/21870764.2023.2301238&domain=pdf&date_stamp=2024-02-24
2. Experimental
Samples for the 0.875MZCT–0.125CLYT were created 
using traditional solid-state techniques. The initial 
components are combined in accordance with the 
stoichiometric ratio. For CuB2O4 powder, high-purity 
powders of CuO and H3BO3 were weighed, mixed and 
calcined at 850°C for 3 h. As a sintering aid, a trace 
amount of CuB2O4 (0.25%– 2% weight) was used. The 
(Mg0.95Zn0.05)Co0.05TiO3 were synthesized using 
a solid-state mixed oxide route with starting materials 
of high-purity oxide powders (>99.9%): MgO, ZnO, 
CoO and TiO2. Because MgO is hygroscopic, it was 
first fired at 600°C to avoid moisture contain. The 
weighed raw materials were mixed by ball milling 
with agate media in distilled water for 24 h, and the 
mixtures were dried and calcined at 1100°C for 4 h. 
Samples of Ca0.6(La0.9Y0.1)0.2667TiO3 ceramics were pro-
cessed using a conventional solid-state reaction from 
high-purity oxide powders (CaCO3, La2O3, Y2O3,and 
TiO2). After mixing, milling for 24 h, drying, and grind-
ing, the mixtures were calcined at 1000 ◦C for 2 h.
The powder comprising (Mg0.95Zn0.05)Co0.05TiO3 
(MZCT) and Ca0.6(La0.9Y0.1)0.2667TiO3 (CLYT) is weighed, 
and then ground with ZrO2 balls in distilled water for 
12 h before being dried.
The powder calcination at different temperatures, 
then mix with massage fraction 0.875MZCT– 
0.125CLYT. The calcined powder was mixed with vary-
ing quantities of CuB2O4 additives serving as sintering 
aids to achieve the desired composition of 
0.875MZCT–0.125CLYT. It was subsequently reground 
with Polyvinyl alcohol (PVA) solution as a binder for 5 
h. Uniaxial pressing is used to press particles having 
a 1.1 cm diameter and 0.5 cm thickness. At 120 MPA, all 
samples were compressed. These particles are sintered 
in air for hours at a temperature between 1050 and 
1175°C after being degreased.
X-ray diffraction (XRD) with CuKα1 radiation (XRD- 
7000, Shimadzu, Kyoto, Japan) was used to examine 
the phase purity and crystal structure of 0.875MZCT– 
0.125CLYT ceramics. The Archimedes method was 
used to calculate the bulk densities.
Using a scanning electron microscope (FE-SEM, 
Model S4800; Hitachi, Japan), microstructure images 
were taken. The Agilent E8362B network analyzer was 
used to measure the permittivity and quality factor 
values in the TE011 mode, following the Hakki– 
Coleman method [24,25]. The temperature coefficient 
of resonant frequency (τf) was measured for 
a temperature range of 25–85°C to determine the tem-
perature coefficient of resonant frequency. The follow-
ing equation was used to determine the value of τf: 
Where f1 denotes the resonant frequency at T1 and 
f2 denotes the resonant frequency at T2.
3. Results and discussion
Figure 1 shows the XRD patterns of the 0.875MZCT– 
0.125CLYT ceramic sintered at various temperatures for 
4 h. The XRD patterns showed that peaks indicating the 
presence of (Mg0.95Zn0.05)Co0.05TiO3 (MZCT)(ICDD-PDF 
#01-073-7752) as the main crystalline phase, in associa-
tion with Ca0.6(La0.9Y0.1)0.2667TiO3 (CLYT) (ICDD-PDF #22– 
0153) as minor phases. It is understood that crystal struc-
tures of (Mg0.95Zn0.050)Co0.05TiO3 and 
Ca0.6(La0.9Y0.1)0.2667TiO3 are trigonal crystal structures and 
orthorhombic crystal structures, respectively and the fact 
Figure 1. X-ray diffraction patterns of 0.875MZCT–0.125CLYT ceramics with 1 wt% CuB2O4 additives sintered at:(a) 1050°C, 
(b) 1075°C, (c) 1100°C, (d) 1125°C, (e) 1150°C, and (f) 1175°C for 4 h. (✧ : MZCT, +: CLYT, ✰: MgTi2O5).
80 Y.-B. CHEN
that the average ion radii of Ca2+, La3+, and Y3+ were 
bigger than those of Mg2+(72 pm) the solid solution 
could not be produced. MgTi2O5 usually formed as an 
intermediate phase. According to the XRD patterns, the 
(Mg0.95Zn0.05)Co0.05TiO3 phase exists in these specimens. 
X-ray diffraction patterns of 0.875MZCT–0.125CLYT cera-
mics system have not been changed significantly with 
sintering temperatures in the range 1050–1175°C. The 
XRD patterns show peaks indicating the presence of 
(Mg0.95Zn0.05)Co0.05TiO3 as the main crystalline phase, 
a minor phase of Ca0.6(La0.9Y0.1)0.2667TiO3. Figure 2 dis-
plays sintered at various temperatures for 4 h. Four SEM 
images of 0.875MZCT–0.125CLYT ceramics that include 
CuB2O4 additions of 1 weight percent. As the sintering 
temperature increased, it was evident that the grain size 
also increased for the 0.875MZCT–0.125CLYT ceramics. 
However,when 1 wt% CuB2O4 was added, the ceramics 
did not achieve high density and no grain growth was 
observed at 1050°C, as indicated by SEM results for differ-
ent temperatures. As shown in Figure 2, the liquid-phase 
effect caused an increase in grain size as the sintering 
temperature. CuB2O4 impact on the liquid phase could be 
significant. At 1100°C, significant grain development was 
seen, and for specimens sintered at 1125°C, the holes 
were virtually completely obliterated.
Figure 3 depicts the densities of 0.875MZCT– 
0.125CLYT ceramics doped with varying quantities of 
CuB2O4 throughout a 4-h period at varied sintering tem-
peratures. As shown in the figure, due to the increase in 
grain size, the density increases to 1 wt% with the 
increase of sintering temperature and the increase of 
CuB2O4 additives. The rise in bulk density with a higher 
sintering temperature may be attributed to the reduction 
in pore numbers, as depicted in Figure 2, whereas the 
reduction in bulk density could arise from a typical grain 
growth. Even with so much CuB2O4 doping, it seems like 
the bulk density has reached saturation at 1100°C. The 
maximum density of 0.875MZCT–0.125CLYT with 1 wt% 
CuB2O4 is 4.3 g/cm [3] sintered at 1100°C for 4 h. 
Therefore, the inclusion of CuB2O4 additives can signifi-
cantly lower the sintering temperature required for 
0.875MZCT–0.125CLYT ceramics sintering temperature 
Figure 2. SEM images were taken of 0.875MZCT–0.125CLYT ceramics containing 1 wt% CuB2O4, sintered at different temperatures 
for a duration of four hours, including (a) 1050°C, (b) 1075°C, (c) 1100°C, (d) 1125°C, (e) 1150°C, and (f) 1175°C.
JOURNAL OF ASIAN CERAMIC SOCIETIES 81
in the CuB2O4-doped 0.875MZCT–0.125CLYT ceramic. 
Excessive will reduce the density because CB is a glass 
phase and the CB density is lower than 0.875MZCT– 
0.125CLYT, and excessive CB addition over 2 wt.% will 
reduce the density.
When the sintering temperature rises, the energy 
rises meaning that the grain boundary moves better 
and it is easy for the small grains to dissolve, so that the 
grain growth is more uniform and the pores decrease 
with the increase in the sintering temperature, and 
densification occurs. In addition, when various addi-
tives are added to the 0.875MZCT–0.125CLYT ceramics 
to form liquid-phase sintering, this is more conducive 
to small-grain dissolution, an increase in the wetting 
boundary movement rate, and grain rearrangement to 
achieve densification. This can be compared with the 
SEM in Figure 2 for the 0.875MZCT–0.125CLYT cera-
mics with multiple sintering aids CB that were sintered 
at 1050°C for 4 h, where the grains were smaller, more 
pores appeared, and the density was lower; when the 
sintering temperature rose to 1100°C, the grain size 
was consistent, there were fewer pores, and the den-
sity was higher. It can be concluded that liquid-phase 
sintering occurs when using different additives, and 
when the additive exceeds 2 wt%, it will cause 
a slight decrease in the density. Generally, in cases of 
liquid-phase sintering, using appropriate amounts of 
sintering aids can effectively improve the phase- 
forming capacity and reduce the sintering tempera-
ture. However, when the sintering aid content is exces-
sive, the grains grow excessively, and with a larger 
particle size, the rearrangement will be subject to 
greater resistance and there will be a small number 
of pores in the boundary, meaning it is not easy to 
discharge and other factors will affect the change in 
the density and radio-frequency dielectric 
performances.
The dielectric constant marginally rises as the sinter-
ing temperature rises. Additionally, larger CuB2O4 con-
centration raises the density value, which translates to 
higher εr as shown in Figure 4.
Lichterecker [26] proposed an intermediate form 
between the serial and parallel mixing rules form 
called logarithmic mixing rule (in the case where 
α → 0) [26]: 
where εhand εlare the relative dielectric constants of 
the high-dielectric phase and low-dielectric phase, 
respectively, Vh and Vl the volume fractions of the high 
dielectric phase and low-dielectric phase (Vh+Vl = 1), 
εmthe effective dielectric constant of the composite, 
and α a parameter that determines the type of mixing 
rule.
The addition of 1 wt% CuB2O4 to the 0.875MZCT– 
0.125CLYT ceramic, accompanied by a rise in sintering 
temperature from 1050°C to 1100°C, resulted in an 
increase of εr value from 26.73 to 28.9. Microwave 
dielectric loss is influenced byvarious factors, which 
can be classified into intrinsic and extrinsic losses. The 
lattice vibration mode is the primary cause of intrinsic 
loss, whereas second phase, oxygen vacancy, grain 
size, and densification or porosity are the main con-
tributors to extrinsic loss [27]. It is believed that porous 
materials are significantly influenced by interfacial 
polarization [28].
The quality factor (Q × f) value of 0.875MZCT– 
0.125CLYT ceramics that incorporate different CuB2O4 
additives at varying sintering temperatures is pre-
sented in Figure 5.
Internal factors, such as lattice vibration mode, 
impact the Q × f value of microwave loss. The presence 
of cation ordering can often result in an increase in Q × 
f, thus its absence may frequently lead to a decrease in 
Q × f [29].
The decrease of Q × f in mixed systems has been 
associated by some with the loss of cation ordering in 
ordered cation compounds [30].
However, it should be noted that the reduction of the 
Q × f value can be due to either intrinsic (i.e. attice 
3
3.2
3.4
3.6
3.8
4
4.2
4.4
1000 1025 1050 1075 1100 1125 1150 1175 1200B
ul
k 
de
ns
ity
 (g
/c
m
3 )
Sintering temperature (oC)
0.25 wt%
0.5 wt%
1 wt%
2 wt%
Figure 3. Bulk density curves were generated for 0.875MZCT– 
0.125CLYT ceramics with varying amounts of CuB2O4 additives 
sintered at different temperatures for four hours.
23
25
27
29
31
1000 1025 1050 1075 1100 1125 1150 1175 1200D
ie
le
ct
ri
c 
co
ns
ta
nt
Sintering temperature (oC)
0.25
wt%
0.5 wt%
1 wt%
Figure 4. The dielectric constant curves for 0.875MZCT– 
0.125CLYT ceramics with different amounts of CuB2O4 addi-
tives at various sintering temperatures were recorded over 
a period of four hours.
0
10000
20000
30000
40000
50000
1000 1025 1050 1075 1100 1125 1150 1175 1200
Q
xf
(G
H
z)
Sintering temperature (oC)
0.25 wt%
0.5 wt%
1 wt%
2 wt%
Figure 5. The quality factor values were measured for 
0.875MZCT–0.125CLYT systems with varying amounts of 
CuB2O4 additives, sintered at different temperatures for four 
hours.
82 Y.-B. CHEN
related) or extrinsic mechanisms. At microwave frequen-
cies, the unloaded quality factor is said to be dependent 
on extrinsic factors like secondary phases, density, and 
oxygen vacancies. The Q × f value increases to its max-
imum value and subsequently decreases as the sintering 
temperature rises. At 1100°C, the maximum Q × f value 
of 0.875MZCT–0.125CLYT ceramic containing 1 wt% 
CuB2O4 additive is 43,000 GHz. Abnormal grain growth 
at higher sintering temperatures is responsible for the 
degradation of the Q × f value, as demonstrated. 
Conversely, due to the enhancement in densification 
of the specimen by the liquid phase, CuB2O4-doped 
0.875MZCT–0.125CLYT exhibits a single maximum Q × 
f value at lower sintering temperatures. Dielectric losses 
in microwave materials are primarily due to lattice vibra-
tion patterns, as well as pores, impurities, second 
phases, or lattice defects. The controlling role of relative 
density in these losses has been demonstrated in other 
types of microwave dielectric materials as well [31,32].
Due to the addition of sintering aids, the Q × f 
values of the samples in this work are approximately 
half of those of the samples sintered at 1450°C. 
However, adding sintering aids can reduce the sinter-
ing temperature.
Ceramics containing 0.5 wt%of CuB2O4 additive in 
0.875MZCT–0.125CLYT were found to lower the sinter-
ing temperature compared to pure 0.875MZCT– 
0.125CLYT ceramics sintered at 1450°C (Q × f ~90000 
at 8 GHz).
Figure 6 displays the temperature coefficients of 
resonant frequency (τf) for 0.875MZCT–0.125CLYT 
ceramics with different CuB2O4 additives and sintering 
temperatures. The relationship between the tempera-
ture coefficient of resonant frequency (TCF) and the 
temperature coefficient of dielectric constant (TCK) as 
well as the thermal expansion coefficient (a) is stated in 
Equation 4 [33] 
The linear thermal expansion coefficient, denoted 
as L, is a constant in ceramics and directly affects the 
temperature coefficient of capacitance (TCF) through 
its relationship with TCK. The temperature 
dependence of the dielectric constant (TCK) can be 
expressed as three terms(A, B, and C) in Equation 
(4) [34]:
Where and V denote the polariz ability and volume, 
respectively. The term A (commonly negative) represents 
the direct dependence of the polarizability on tempera-
ture. B and C represent the increase of the polarizability 
and the decrease of the number of polarizable ions in the 
unit-cell, respectively; the unit cell volume increased with 
an increase in temperature. The B and C terms are nor-
mally the largest ones but have similar value with oppo-
site signs. Hence, (B+C) has a small positive value. TCK is 
increased by an increase of the tilting of oxygen octahe-
dra in the perovskite structure, which correspond to 
a decrease of TCF by Equation (4).
The temperature coefficient of the resonant frequency 
(τf) is typically determined by the composition and phase 
within the ceramic, while demonstrating insensitivity 
across all sintering temperature ranges. With the increase 
of CuB2O4 additives, the τf value becomes more positive. 
As the sintering temperature varies, the CuB2O4 additive 
increases from 0.25 wt% to 2 wt% resulting in a variation 
of 17.5 to 30.9 ppm/oC. Increasing the amount of CLYT 
can result in achieving zero τf, as the τf values for (Mg0.95 
Zn0.05)Co0.05TiO3 and CLYT are −50 and + 310 ppm/oC, 
respectively.
The temperature coefficient of resonant frequency 
(τf) for ceramics was related to composition and exist-
ing phases. Regardless of sintering temperature range, 
τf was not affected. When CuB2O4 additives were 
increased, the τf value became more positive and ran-
ged from 17.5 to 30.9 ppm/oC. Increasing CLYT con-
tent could achieve zero τf since (Mg0.95 
Zn0.05)Co0.05TiO3 and CLYT had different τf values of 
−50 and +310 ppm/oC, respectively.
4. Conclusion
The study focused on the dielectric properties of 
0.875MZCT–0.125CLYT ceramics containing CuB2O4. 
Secondary phases such as MgTi2O5 were mixed with 
0.875MZCT–0.125CLYT ceramics, with MgTi2O5 serving 
as the primary phase. The addition of CuB2O4 in 
0.875MZCT–0.125CLYT ceramics not only lowers the sin-
tering temperature effectively but also enhances its 
microwave dielectric properties. At a temperature of 
1100°C, ceramics with a composition of 0.875MZCT– 
0.125CLYT and an addition of 1 wt% CuB2O4 exhibit 
exceptional microwave dielectric characteristics including 
εr of approximately 28.9, Q × f value of approximately 
43,000 (at 8 GHz), and τf value of approximately 27.6 
ppm/oC.
10
15
20
25
30
35
1000 1050 1100 1150 1200
 tneiciffeoc erutarep
me
T of
 re
so
ne
nt
 fr
eq
ue
nc
y 
(p
pm
/o C
)
Sintering temperature (oC)
0.25 wt%
0.5 wt%
1 wt%
2 wt%
Figure 6. The resonant frequency values of 0.875MZCT– 
0.125CLYT system, with various CuB2O4 additives sintered for 
four hours at different temperatures, were analyzed for their 
temperature coefficients.
JOURNAL OF ASIAN CERAMIC SOCIETIES 83
Disclosure statement
No potential conflict of interest was reported by the 
author(s).
Data availability statement
The data that support the findings of this study are openly 
available to the reviewers.
Author contributions
Yuan-Bin Chen: Preparation of materials, methodology, and 
software. Preparation of materials. Data curation and writ-
ing – original draft preparation. Writing – reviewing and 
editing. Software, theoretical calculation, and validation.
Declarations
Conflict of interest: The authors declare that they have no 
known competing financial interests or personal relation-
ships that could have appeared to influence the work 
reported in this paper.
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	Abstract
	1. Introduction
	2. Experimental
	3. Results and discussion
	4. Conclusion
	Disclosure statement
	Data availability statement
	Author contributions
	Declarations
	References