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ARTICLE
Copyright © 2013 by American Scientific Publishers
All rights reserved.
Printed in the United States of America
Advanced Science,
Engineering and Medicine
Vol. 5, pp. 126–132, 2013
(www.aspbs.com/asem)
Ammonium Dihydrogen Phosphate/PVA Composite
Films with High Dielectric Permittivity and
Enhanced Thermal Stability
Md Jamal Uddin
1
, Md G. Masud
1
, Arijit Ghosh
1
, T. R. Middya
2
, and B. K. Chaudhuri
1, *
1
Solid State Physics Department, Indian Association for the Cultivation of Science, Jadavpur, Kolkata 700032, India
2
Department of Physics, Jadavpur University, Jadavpur, Kolkata 700032, India
Transparent and anhydrous ammonium dihydrogen phosphate (NH
4
H
2
PO
4
or ADP) based polyvinyl alcohol
(PVA) composite films of thickness 100 m have been prepared by solution casting technique. Several tech-
niques like XRD, SEM, DSC, TGA and FTIR were used to characterize the prepared samples. The dielectric
properties of the composites as a function of volume fraction of ADP, temperature, and frequency are studied in
details. The dielectric permittivity decreases slowly with increasing frequency and gradually rises with increas-
ing ADP contents in the composites. As the volume fraction of the ADP approaches percolation threshold, an
abrupt increase in the dielectric permittivity occurs due to the formation of the conductive network in the matrix.
The percolation theory, the microcapacitor model, and the simple concept of polarization in the capacitors are
successfully employed to explain the experimental results. Thermal analysis of the composite films showed
an increase in the glass transition temperature of the percolative polymer composite film, which confirms its
enhanced thermal stability.
KEYWORDS: Composites, Dielectric Properties, Filler, Film, Percolation, Thermal Stability.
1. INTRODUCTION
Polymer-based composites with high dielectric permittiv-
ity are important topics in the field of material science,
and much attention has been paid in the past few years
for various applications.
1–3
Polymers are selected as host
materials for the energy storage applications on account
of their intrinsic properties; such as good flexibility, easy
processing, and cost effectiveness.
4 5
However, the dielec-
tric permittivity () of many of the common polymers like,
polyvinyl alcohol (PVA) is extraordinarily low (< 10).
Thus, enhancement of values of the polymer-based mate-
rials, while maintaining their mechanical performance is
necessary. Several important attempts have been made
on ceramic–polymer composite (C/P) systems that adopt
ceramics as fillers, e.g., BaTiO
3
, CaCuTi
4
O
12
, PZT, and
PMN-PT.
6–10
However, these composites have relatively
low dielectric permittivity (< 100) even at a high loading
of ceramics (> 50 vol.%), and high loading also degrades
the mechanical properties of the composites, such as flexi-
bility and quality of the polymer composites.
11 12
To min-
imize such problems of C/P, much effort has recently
∗
Author to whom correspondence should be addressed.
Email: sspjamal@gmail.com
Received: 14 May 2012
Revised/Accepted: 2 June 2012
been made to prepare inorganic filler/polymer compos-
ite based on the percolation theory.
13
Dielectric permit-
tivity of new polymer composites based on PVA such as
graphene-PVA,
14
KDP-PVA,
15
poly(ethylene oxide)-PVA
16
have already been reported. But, the reported dielectric
permittivity of such composite is moderately low (< 300
at 1 kHz) at room temperature. Recently, several stud-
ies on transparent and solid proton conductor NH
4
H
2
PO
doped PVA
17
and PVA/imidazole/NH
4
H
2
PO
4
.
18
Have been
made for their use in solid electrochromic devices. Study
of dielectric properties and percolative behavior of such
system like NH
4
H
2
PO
4
/PVA composites are also important
which have, however, not been yet reported.
It is well known that ammonium dihydrogen phosphate
(ADP) crystals are low cost and water soluble material.
Therefore, if ADP is dispersed into polymer as a conduc-
tive phase, much more microcapacitors could be formed,
and the percolation would also be expected to appear
at a suitable content of ADP, which subsequently could
induce a high dielectric permittivity of the ADP/polymer
composites.
In this paper, we investigate ADP/PVA composites with
low concentrations of ADP to significantly improve the
dielectric permittivity of polymer matrix composites. This
work focuses on frequency, temperature and concentration
dependent dielectric behavior of the ADP/PVA composites
126 Adv. Sci. Eng. Med. 2013, Vol. 5, No. 2 2164-6627/2013/5/126/007 doi:10.1166/asem.2013.1241