Journal of the European Ceramic Society 27 (2007) 2835–2839
Low sintering BaNd
2
Ti
4
O
12
microwave ceramics prepared by
CuO thin layer coated powder
M.-C. Wu
a
, M.-K. Hsieh
b
, C.-W. Yen
a
, Y.-C. Huang
a
, W.-T. Huang
c
, W.-F. Su
a,d,∗
a
Department of Materials Science and Engineering, National Taiwan University, Taipei, Taiwan
b
Department of Chemical Engineering, National Taiwan University, Taipei, Taiwan
c
Industrial Technology Research Institute, Chutung, Hsinchu, Taiwan
d
Center for Condensed Matter Sciences, National Taiwan University, Taipei, Taiwan
Abstract
Recently, BaO–Nd
2
O
3
–TiO
2
systems are widely studied for microwave applications because of their high dielectric constant and high quality
factor. However, pure BaNd
2
Ti
4
O
12
ceramics without additives have to be sintered above 1300
◦
C to achieve densification. Copper oxide has
been known as a good sintering aid for electronic ceramics and less reactive toward silver. We have introduced the CuO into BaNd
2
Ti
4
O
12
by
modifying the surface of BaNd
2
Ti
4
O
12
by CuO thin layer on the calcined powder instead of mixing CuO directly with BaNd
2
Ti
4
O
12
powder. The
process reduces the amount of sintering aid and minimized the negative impact of sintering aid on dielectric properties such as quality factor. The
CuO precursor solution of Cu(CH
3
COO)
2
, Cu(NO
3
)
2
and CuSO
4
, were used to prepare CuO thin layer. They were investigated individually to
determine their effects on the densification, crystalline structure, microstructure and microwave dielectric properties of BaNd
2
Ti
4
O
12
. The CuSO
4
coated BaNd
2
Ti
4
O
12
sintered at 1150
◦
C has exhibited better dielectric properties than those of CuO doped BaNd
2
Ti
4
O
12
(k, 62.5 versus 61.2;
Q × f, 11,500 GHz versus 10,500 GHz). The thin layer dopant coating process has been found to be a very effective way to lower ceramic sintering
temperature without scarifying its dielectric properties.
© 2006 Elsevier Ltd. All rights reserved.
Keywords: Powders-solid state reaction; Dielectric properties; Microstructure
1. Introduction
Low temperature co-firable ceramics (LTCC) possessing
good microwave dielectric properties have been widely investi-
gated due to the necessity for miniaturization of devices in order
to reduce the size of wireless communication system. Because
of the high sintering temperature, Ag–Pd electrode is the only
choice for multilayer ceramic components (MLCCs). Thus, it is
desirable to replace the poor conductivity and high cost Ag–Pd
electrode with the better properties and lower cost of silver or
copper electrodes.
BaO–Nd
2
O
3
–TiO
2
series materials possess marvelous
microwave dielectric properties such as high dielectric constant
and high quality factor, and were extensively investigated for
the applications in microwave devices.
1–8
Recently, the chemical
∗
Corresponding author at: Department of Materials Science and Engineer-
ing, National Taiwan University, No. 1, Sec. 4, Roosevelt Road, 106-17 Taipei,
Taiwan, ROC. Tel.: +866 2 33664078; fax: +866 2 33664078.
E-mail address: suwf@ntu.edu.tw (W.-F. Su).
composition of BaNd
2
Ti
4
O
12
has emerged as a good microwave
material because it exhibits high dielectric constant (k ∼ 84) and
high quality factor (Q × f ∼ 7800 GHz), but its high sintering
temperature (>1350
◦
C) is difficult for LTCC process.
8
Oxide
dopants (B
2
O
3
, Bi
2
O
3
,V
2
O
5
, etc.) and glasses (low temperature
melting glasses) have been used as sintering aids. However, some
studies have reported that oxide dopants and the glasses exhib-
ited pronounced effects on the microstructure and microwave
dielectric properties of the materials. Large and interconnected
pores were observed due to the agglomeration of dopants during
cofiring process.
9–13
Copper oxide has been known as a good sintering aid and
less reactive toward silver.
14–16
We propose to introduce the CuO
into BaNd
2
Ti
4
O
12
by modifying the surface of BaNd
2
Ti
4
O
12
by
CuO thin layer on the calcined powder instead of mixing CuO
directly with BaNd
2
Ti
4
O
12
powder. The process will reduce
the amount of sintering aid and eliminate the negative impact
of sintering aid on dielectric properties such as quality factor.
The CuO layer was prepared from three kinds of Cu precur-
sors: Cu(CH
3
COO)
2
, Cu(NO
3
)
2
and CuSO
4
, respectively. We
0955-2219/$ – see front matter © 2006 Elsevier Ltd. All rights reserved.
doi:10.1016/j.jeurceramsoc.2006.11.057