Microstructures and dielectric properties of Ba
0.5
Sr
0.5
TiO
3
–Zn
2
TiO
4
composite
ceramics with low sintering temperature for tunable device applications
Xiujian Chou
a,
*
, Zhenyu Zhao
a
, Wendong Zhang
a
, Jiwei Zhai
b
a
Key Laboratory of Instrumentation Science and Dynamic Measurement (North University of China), Ministry of Education,
National Key Laboratory of Science and Technology on Electronic Test and Measurement, Xueyuan Road 3, Taiyuan, Shanxi Province 030051, China
b
Functional Materials Research Laboratory, Tongji University, Siping Road 1239, Shanghai 200092, China
article info
Article history:
Received 20 January 2010
Accepted 4 March 2010
Available online 7 March 2010
Keywords:
A. Composites
E. Electrical
F. Microstructure
abstract
Ba
0.5
Sr
0.5
TiO
3
–Zn
2
TiO
4
composite ceramics with low dielectric constant and high tunability are fabricated
at a relatively low sintering temperature of 1200 °C via the conventional solid-state reaction route.
Zn
2
TiO
4
and Ba
0.5
Sr
0.5
TiO
3
can be friendly coexistent in the composite material system. The dielectric con-
stant is tailored from 2500 to 83 by manipulating the addition of Zn
2
TiO
4
content from 0 wt.% to 80 wt.%
weight ratio. The dielectric loss still keeps around 0.002 and the tunability is 10.3% under a DC-applied
electric field of 30 kV/cm at 10 kHz for the 80 wt.% Zn
2
TiO
4
added Ba
0.5
Sr
0.5
TiO
3
composite ceramics.
These composite ceramics are promising candidates for multilayer low-temperature co-fired ceramics
(LTCC) and potential tunable devices applications.
Ó 2010 Elsevier Ltd. All rights reserved.
1. Introduction
Recently, ceramics multilayer structures with a low sintering
temperature for tunable microwave devices applications attract
considerable attention due to the potential for substantial minia-
turization of microwave components and integration with micro-
electronic circuits [1–3]. Barium strontium titanate (BST)
ferroelectrics with high dielectric non-linearity and low dissipation
factor have become one of the most promising materials to realize
tunable microwave device applications, such as tunable capacitors,
delay lines, filters, resonators and phase shifters [4,5]. However,
pure Ba
0.5
Sr
0.5
TiO
3
ferroelectric ceramics with high dielectric per-
mittivity have difficultly satisfying the requirements of impedance
matching and high power. Meanwhile, they are not suitable for
multilayer structure ceramics co-firing with cheaper base metal
electrodes because of high sintering temperature (>1350 °C or even
higher). Therefore, moderate dielectric permittivity ceramics with
high tunability, low dissipation factor and low sintering tempera-
ture are desired for multilayer structures tunable microwave de-
vice applications [6].
It has been intuitively believed that the dielectric and sintering
performance of BST ferroelectrics can be further manipulated and
improved by mixing them with low sintering temperature dielec-
trics. Zn
2
TiO
4
ceramics are the attractive dielectric properties ow-
ing to low dielectric permittivity (between 15 and 20), and
relatively low sintering temperature (below 1200 °C) [7–9]. In this
paper, Zn
2
TiO
4
non-ferroelectric materials, employed as the sec-
ondary phase, are introduced in Ba
0.5
Sr
0.5
TiO
3
ceramics to reduce
the sintering temperature and improve the dielectric properties.
The phase structures and dielectric non-linear characteristics of
Ba
0.5
Sr
0.5
TiO
3
–Zn
2
TiO
4
composite ceramics have been investigated.
The purpose of the present study are to find a Ba
0.5
Sr
0.5
TiO
3
-based
composite material system with moderate dielectric permittivity,
low dissipation factor, high tunability and relatively low sintering
temperature for tunable microwave device applications.
2. Experimental procedure
Pure Ba
0.5
Sr
0.5
TiO
3
and Zn
2
TiO
4
powders were synthesized via
the conventional solid-state reaction, respectively, from BaTiO
3
(99.9%), SrTiO
3
(99.9%) and ZnO (99.0%), TiO
2
(99.9%) powders at
1100 °C for 4 h. Then, various amounts of Zn
2
TiO
4
(50, 60, 70,
and 80 wt.%) were added into the Ba
0.5
Sr
0.5
TiO
3
powder and mixed
using alcohol and zirconia balls milling media for 24 h. After dry-
ing, the obtained powder mix were pulverized with 8 wt.% polyvi-
nyl alcohol (PVA) binder and pressed into disk-shaped pellets
under 100 MPa. The green pellets of composite ceramics with 50,
60, 70, and 80 wt.% Zn
2
TiO
4
(termed as samples B–E) were sintered
at 1200 °C for 4 h in air and pure Ba
0.5
Sr
0.5
TiO
3
ceramics (termed as
sample A) were sintered at 1400 °C for 4 h in air.
X-ray diffraction (XRD) (Rigaku, Japan) with Cu K
a
radiation
was employed to characterize the phase structures. Scanning elec-
tron microscope (SEM) (JSM EMP-800) with energy dispersive
spectroscopy (EDS) was used to characterize the microstructure
and chemical component elements. The temperature dependent
0261-3069/$ - see front matter Ó 2010 Elsevier Ltd. All rights reserved.
doi:10.1016/j.matdes.2010.03.006
* Corresponding author. Fax: +86 351 3922131.
E-mail address: chouxiujian@nuc.edu.cn (X. Chou).
Materials and Design 31 (2010) 3703–3707
Contents lists available at ScienceDirect
Materials and Design
journal homepage: www.elsevier.com/locate/matdes