Journal of Research Updates in Polymer Science, 2014, 3, 157-169 157
E-ISSN: 1929-5995/14 © 2014 Lifescience Global
Copper Ion Doped Mullite Composite in Poly (vinylidene Fluoride)
Matrix: Effect on Microstructure, Phase Behavior and Electrical
Properties
Kumaresh Halder
1
, Biplab Kumar Paul
1
, Biswajoy Bagchi
2
, Alakananda Bhattacharya
1
and
Sukhen Das
1,*
1
Department of Physics, Jadavpur University, Kolkata- 700 032, India
2
Fuel Cell and Battery Division, Central Glass and Ceramic Research Institute, Kolkata 700032, India
Abstract: Highly crystallized copper ion doped mullite composites have been synthesized at 1100°C and 1400°C via sol-
gel technique with five different strengths of copper ion and was incorporated in poly-vinylidene fluoride (PVDF) to make
doped mullite composite/polymer films. We have studied the effects of this dopant on microstructure, phase
transformation, and electrical properties of the polymer films over a wide range of frequency from 1.0 KHz to 2.0 MHz.
Characterizations were done by various analytical tools at room temperature. Prominent mullite phases were observed
from XRD, FTIR spectroscopy and FESEM characterization of composite polymer. The concentration of the dopant and
the sintering temperature were found to be the two basic factors which affect the phase transition of the polymer. The
composite film showed maximum dielectric constant of 19.96 at 1 KHz for 1.2M concentration of copper ion doped
mullite sintered at 1400°C, compared to 3.09 for the pure polymer. Furthermore, both dielectric constant and electrical
conductivity of the composite were found to be highly frequency and temperature dependent. After doping, the A.C.
conductivity of the composite was found to increase with increasing temperature following Jonscher’s power law and the
electrical resistivity reduced too. Moreover, the results revealed that the phase behaviors and micro structural changes of
the copper ion doped mullite composite/polymer film affected its electrical properties with possible impact on its
applications.
Keywords: Polymer, Mullite, Sol–gel technique, XRD, FTIR, Dielectric properties, FESEM.
INTRODUCTION
Polymorphism is an essential characteristic of Poly
vinylidene fluoride (PVDF). PVDF is a semi-crystalline
polymer having four crystal polymorphs referred to as
, , and phases [1, 2]. Conventional melt and
solution processing usually result in phase which has
trans-gauche-trans-gauche (TGTG) chain conformation
[3, 4]. phase has all trans (TTTT) zigzag chain
conformation; formation of this phase in PVDF is
dependent on stretching of the film as well as the
preparation temperature [5, 6]. phase has
TTTGTTTG' chain conformation which can be achieved
by either casting from dimethyl sulfoxide (DMSO) or
dimethylformamide (DMF) solution regardless of
preparation temperature [7]. High electric field, high
pressure and annealing temperatures are also
responsible for producing phase [8-11].
The main advantage of polymer matrix over ceramic
materials is its mechanical quality and it can also be
synthesized easily. It has been observed that pure
polymer matrix possesses large breakdown strength,
good flexibility and great mechanical strength; it is easy
*Address correspondence to this author at the Department of Physics,
Jadavpur University, Kolkata- 700 032, India; Tel: +91 9433091337;
E-mail: sukhenjudas@gmail.com
to process but has a very low dielectric constant [12-
14]. On the other hand, ceramic composites generally
suffer from brittleness which can be reduced to a
commendable extent by integrating ceramic
composites into the polymer matrix. Micro scale
ceramics of high dielectric constant are used as fillers
in polymer to increase its dielectric constant [15-17].
For such composites, filler loadings should be high
enough for attainment of that range of dielectric
constant that is high enough for industrial applications
purposes. Though the electrical resistivity of polymer is
quite high which makes it suitable to be categorized as
an insulator still its electrical properties could be
enhanced by incorporation of fillers in polymeric matrix
as these fillers interact with the polymer chains. Thus
these composites have the ability to exhibit new
properties that single phase materials do not possess
[18].
Thus, novel composites with comparatively high
capacitance, high-energy storage density, and small
volume can be prepared, which are known to be very
useful materials for varieties of applications in
electronics such as, transducers, hydrophones, piezo-
sensors, high-charge storage capacitors [19], etc.
Roy et al. synthesized highly crystallized mullite
composite at 1000
o
C and 1300
o
C via sol gel technique
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