Professional Documents
Culture Documents
Dielectric and
microwave properties
of polyvinyl chloride/
graphite/nickel
composites and its
applications
Abstract
A novel dry phantom nanoconducting composite that can simulate the effect of electromagnetic wave on human tissues composed of graphite/nickel (GN) nanoparticles and
polyvinyl chloride (PVC) was successfully fabricated. The morphology of as-synthesized
graphite nanosheets and PVC/GN composites was investigated by means of scanning
electron microscope. Dielectric parameters such as relative permittivity, imaginary
permittivity, and alternating current conductivity are evaluated in the frequency range
of 0.512 GHz. The results are compared with the in vitro equivalent human tissue data
and good agreement is reported. The absorption and reflection coefficient as a function
of frequency of nanocomposites were also studied. The novel PVC/GN nanocomposites
Department of Physics, Faculty of Science, King Abdulaziz University, Jeddah, Saudi Arabia
Department of Physics, Faculty of Science, University of Tabuk, Tabuk, Saudi Arabia
3
Department of Mathematics, Faculty of Science, University of Tabuk, Tabuk, Saudi Arabia
4
Department of Mathematics, Faculty of Science, King AbdulAziz University, Saudi Arabia
5
Department of Physics, Faculty of Science, King Abdelaziz University, North Campus, Jeddah, Saudi Arabia
6
Department of Polymer Engineering, University of Chemical Technology and Metallurgy, Sofia, Bulgaria
7
Department of Chemistry, Faculty of Science, King Abdulaziz University, Jeddah, Saudi Arabia
8
Department of Physics, Faculty of Science, Suez Canal University, Ismailia, Egypt
2
Corresponding author:
AA Al-Ghamdi, Department of Physics, Faculty of Science, King Abdelaziz University, Jeddah, Saudi Arabia.
Email: aghamdi90@hotmail.com
528
Al-Ghamdi et al.
529
have potential applications for dry phantom and the coupling media in microwave
medical imaging.
Keywords
Nanoconducting composites, dry phantom, microstructure, and electrical properties,
microwave properties
Introduction
Nanoconducting composites have received increasingly more attention for their potential
applications as practical structural and functional materials.15 Today, research and
development are performed with a high-speed and high-capacity communication using
higher frequencies than the frequency band previously used in communications and
broadcasting.610 One example is using ultra-wideband (UWB) technology, which is the
next-generation of communication system. UWB technology mainly focuses on shortrange, high-capacity indoor communications, communicates using pulses with narrow
time widths, and uses a wide frequency bandwidth of 3.110.6 GHz.1115 Conductive
polymer nanocomposites are becoming increasingly useful because of their unique combination of metallic conductivity and polymer properties. These materials are widely
used as microwave absorbing materials, electromagnetic shielding materials, antistatic
materials, and others.15 Graphite is layered minerals composed of weakly bonded large
number of graphene sheets that are held together by van der Walls forces with a large
aspect ratio.9,10 Some of the nanocomposite materials suitable for use in vivo as artificial
organs and tissues have been an intriguing topic of research in recent years.1620 The
human tissues can be classified into two categories: low water content tissues such as fat
and skull and high water content tissues such as brain and muscle.1,2 There are several
types of phantoms that are already in use as tissue substitutes for microwave medical
imaging.1620 These compounds composed of polyethylene and/or agar contain sodium
chloride and water, and the other phantoms from ceramics.6,7 The disadvantage of these
kinds of phantoms material are that they decompose overtime, cannot form hard ceramics easily, variability between repeated dilutions and inhomogeneities from air bubbles
or precipitants, and long setup times.8,9 The phantom material should have the same
dielectric properties such as relative real permittivity and conductivity, shape, and size
similar to human tissues.24 Because the relative real permittivity and conductivity are
material constants depending on a given frequency, it is very important to understand the
dielectric characteristics of the materials in constructing the phantom model. Tell now,
there are no published reports on the fabrication of PVC/GN nanocomposites for phantom materials. In this article, a new dry phantom nanoconducting composite of graphite/
nickel (GN) nanoparticles reinforced polyvinyl chloride (PVC) was fabricated. The
influence of GN content on the microstructure and structure was investigated in terms
of scanning electron microscopy (SEM). The applicability of PVC/GN composites as
a dry phantom and microwave imagining devices were examined in details in the frequency range from 1 to 12 GHz.
529
530
Experimental details
Material description
Natural flake graphite with an average diameter of 500 mm and surface area of 46 m2/g
used for preparing the expanded (exfoliated) graphite is purchased from Shandong
Qingdao Graphite Company (Qingdao, China). Commercial concentrated sulfuric acid
and nitric acid from Egyptian Chemical Company (Cairo, Egypt) was used as chemical
intercalant and oxidizer to prepare exfoliated graphite. The 95% (v/v) alcohol and distilled water were used as solvents for the preparation of foliated (nanosheets) graphite.
PVC was obtained from Tokyo Chemical Industry Co. Ltd (Tokyo, Japan). Nickel
powder was supplied by Wako Chemical Company with particle size 10 mm.
Al-Ghamdi et al.
531
Instruments
The morphology of composites was analyzed using a scanning electron microscopy
(SEM, JSM-5310 LVB, JEOL). The specimens were coated with carbon to avoid charging using a vacuum evaporator (JEOL, GEE 500) and the voltage used was 15 kV. The
microwave dielectric properties of composites were determined by the Hewlett-Packard
waveguide line containing spectroanalyzer, power meter, coefficient of reflection meter,
and coefficient of attenuation meter with an accuracy of 0.1. The measurements were
carried out in the frequency ranges 112 GHz using the cavity perturbation techniques.
The sample dimensions were 20 20 0.5 mm3.
532
80
1.2
Experimental
Lichtenecker Eqn
Smith Eqn
Maxwell Eqn
EMT Eqn
Loss tangent
60
Loss tangent
Relative permittivity
0.8
40
0.4
20
12
GN content (wt%)
Figure 1. Comparison of experimental and theoretical relative permittivity of PVC/GN nanocomposites and loss tangent against GN content.
PVC: polyvinyl chloride; GN: graphite/nickel nanoparticle.
diameter of 10 mm obtained from x-ray analysis. Typical SEM image of GN12 sample is depicted in Figure 2(b). In Figure 2(b), it is clear that PVC chain is effectively
incorporated into the galleries of GN layers. Furthermore, we can clearly observe
that the GN nanoparticles were distributed quite uniformly within the PVC matrix
and no aggregates can be seen in the composite. Because of this special structure,
the interfacial affinity of GN nanoparticles with the PVC matrix increased and led
to an ensured thermal stability and electrical contact that served as the electrically
conductive bridge.1,12
Meanwhile, there are a number of theoretical models to predict the effective real
permittivity of the composites. In this study, the following equations were used to
evaluate the effective relative permittivity of the PVC/GN nanocomposites.
Lichtenecker (logarithmic mixing) model is given by the equation21,22
ln "eff ln "i 1 ln "m
Smiths mode is given by the equation23
532
Al-Ghamdi et al.
533
Figure 2. SEM image of (a) as-prepared graphite nanosheets and (b) SEM image of GN12 sample.
SEM: scanning electron microscopy; GN: graphite/nickel nanoparticle.
"eff
"i "m
3"m
"m 1 "i "i
1 3
2"m
"i 2"m
3"i "m
3"m
1 "i
1
2"m
"i 2"m
where "eff, "I, and "m are the permittivity of the nanocomposites, the GN filler, and the
PVC matrix, respectively, is the volume fraction of the GN fillers, and n is the correction factor to compensate for the shape of the fillers used in polymer composites.
In Figure 1, it is observed that the measured relative permittivity shows a deviation
from the predicted values for Lichtenecker, Smiths, and Maxwell models. This is due to
the fact that the complex permittivity depends on several factors like homogeneity and
dispersion of filler, aspect ratio of filler, polarity of filler and matrix, morphology of
filler, size of filler, interface bonding among filler and matrix, extent of filler reinforcement, and others.2024 The reason is that the Lichtenecker model does not consider the
533
534
40
PVC
GN3
30
GN6
Relative permittivity
GN9
GN12
20
10
0
0
10
12
Frequency (GHz)
filler/matrix interface adhesions, and it is only valid in the case of the filler and matrix
having close value of relative permittivity. But smiths model can not predict the permittivity values of PVC/GN nanocomposites precisely. This can be due to the fact that
the used conducting GN fillers are not spherical but in sheet form.21 The Maxwell Garnet
model also gives a considerably lower estimate for the measured relative permittivity of
PVC/GN naocomposites. This can be due to the various factors, which affect the relative
permittivity of the nanocomposites other than GN filler volume fraction and permittivity
of GN fillers. Among the four models, the experimentally observed relative permittivity
is in excellent agreement with that computed using the effective medium theory. The
obtained value of n for PVC/GN nanocomposites is about 0.67.
Figures 3 and 4 depict room temperature plot of relative permittivity and imaginary
permittivity of PVC/GN nanocomposites as a function of frequencies in the range of
0.512 GHz, respectively. The relative permittivity of green PVC is nearly frequency
independent. Clearly, the relative permittivity and imaginary permittivity increased with
an increase in the GN volume fraction into nanocoposites. It is observed that both the
relative permittivity and imaginary permittivity decrease with increasing frequency. This
534
Al-Ghamdi et al.
535
30
PVC
25
GN3
Imaginary permittivity
GN6
GN9
20
GN12
15
10
0
0
10
12
Frequency (GHz)
result coincides with the studies on dielectric properties of biological tissues.58 The low
dielectric constant of green PVC is attributed to the low polarizability of the molecular
segments of PVC polymer. The decrease in relative permittivity with an increase in the
frequency is attributed to the orientation of the polarization in the microwave field.20 At
relatively low microwave frequencies, the total polarizations by electronic, atomic, and
orientation polarization take place. One the other hand, as the frequency of the applied
field increased, the total polarization decreases into composites. This leads to dielectric
relaxation, which in turn, leads to a decrease in relative permittivity. Furthermore, at
high frequencies due to the rotational displacement of polar groups under the influence
of the electric field, frictional loss increases and it reduces relative permittivity. It is
interesting to mention that, when PVC/GN is mixed in definite proportions, the relative
permittivity and conductivity increases and behaves as an ideal stimulant of low and high
water content biological tissues.
The conductivity can be related to the imaginary part of the complex dielectric
constant
2f "0 "00r
5
535
536
140
GN3
120
GN6
GN9
GN12
100
80
60
40
20
0
0
10
12
Frequency (GHz)
The dependence of the alternating current (AC) conductivity of the PVC/GN nanocomposites on frequency is depicted in Figure 5. The AC conductivity is found to
increase with an increase in frequency. This is due to a large dipole moment of the
nanocomposites with increasing GN nanoparticles. The AC conductivity of dielectric
materials in microwave frequency depends upon the dielectric loss factor. Here, as
frequency increases, the dielectric loss factor also increases. The dielectric loss is a direct
function of the relaxation process, which is due to local motion of polar groups.21,22 At
high frequencies, the friction between molecular chain increases, which leads to
higher dielectric loss. This dielectric loss factor causes the so-called conductivity
relaxations. At this relaxation region, the polarization acquires a component out
of phase with the field and displacement current in phase with the field, resulting
in the thermal dissipation of energy, thus generates dielectric loss and thus AC conductivity increases.
The equivalent phantoms for various low water content biological samples in the
frequency range of 23 GHz are given in Table 1.23,24 Comparison of our results with
different equivalent phantoms is recorded in Table 1, it is noteworthy that the mixing of
graphite nanosheets with nickel nanoparticles in definite proportions with PVC can
simulate phantoms of any of these biological tissues. It can be directly related to its
536
Al-Ghamdi et al.
537
Table 1. Relative real permittivity and electrical conductivity of biological tissues and equivalent
phantom from our work in the frequency range 13 GHz.512
Range of relative
real permittivity
Biological name
Bladder (human)
Breast fat (human)
Bone (calcellous, human)
Bone (cortical, ovine)
Bone (cortical, human)
Bone marrow (infiltrated, ovine)
Bone (marrow)
Human (brain)
Chest (fat)
13.5013.10
10.209.80
12.6012.14
11.7811.30
12.4410.96
13.3114.76
4.205.80
3033
2.843.94
Electrical
Equivalent phantom
conductivity (S/m) (our work)
0.2100.215
0.0520.062
0.1500.170
0.0680.710
0.1750.182
0.2310.241
0.0420.055
0.3460.423
0.0120.018
GN3, GN6
GN3
GN3, GN6
GN3
GN3, GN6
GN3, GN6
GN8
GN6, GN9, GN12
GN3
60
PVC
GN3
50
GN6
GN9
GN12
40
30
20
10
10
12
Frequency (GHz)
higher water content compared with that of green PVC and PVC/GN nanocomposites.
Human chest fat, bone marrow, and brain fall in the same dielectric range as GN3, GN6,
and GN9, respectively (Table 1). These composites are noncorrosive, easy to make, and
537
538
10
GN3
GN6
GN9
GN12
0
1
10
13
Frequency (GHz)
cost effective, and thus can be used as suitable dry phantom for biological tissue in
microwave medical imaging devices.
Al-Ghamdi et al.
539
nanosize-confinement effect, which may also have contribution to the high absorption
coefficient of nanocomposites.13,14
In Figure 7, it is seen that the reflection loss decreases with increasing GN content into
composites. This phenomenon is due to the increase in cross-link density and interfacial
bonding among filler and matrix with increasing GN content into composites.
Conclusion
1.
2.
3.
4.
Authors Note
The present research is a result of an international collaboration program between the
University of Tabuk, Tabuk, Kingdom of Saudi Arabia and the University of Chemical
Technology and Metallurgy, Sofia, Bulgaria.
Funding
This work was supported by the University of Tabuk, Tabuk, Kingdom of Saudi Arabia.
References
1. El-Tantawy F, Abdel Aal N, El-Daly AA, Abdel-Daiem AM, Bakry A and Sung YK. A new
phantom model and attenuation backing from epoxy resin nanosized hydroxyapatite -carbon
black and multifunctional agent composites. Mater Lett 2004; 58(27): 33883394.
2. Moon KS, Choi HD, Lee AK, Cho KY, Yoon HG and Suh KS. Dielectric properties of
epoxy-dielectrics-carbon black composite for phantom materials at radio frequencies. J Appl
Polymer Sci 2000; 77: 12941302.
3. Bindu G, Lonappan A, Thomas V, Aanandan CK and Mathew KT. Dielectric studies of
polyvinyl-acetate-based phantom for applications in microwave medical imaging. J Mater Sci
2006; 41: 74197424.
4. Fan Z, Zheng C, Wei T, Zhang Y and Luo G. Effect of carbon black on electrical property of
graphite nanoplatelets/epoxy resin composites. Polymer Eng Sci 2009; 112: 20412045.
5. Al-Ghamdi AA, El-Tantawy F, Abdel Aal N, El-Mossalamy EH and Mahmoud WE. Stability
of new electrostatic discharge protection and electromagnetic wave shielding effectiveness
from poly(vinyl chloride)/graphite/nickel nanoconducting composites. Polymer Degrad Stabil
2009; 94, 980986.
539
540
6. Kim S, Do I and Drzal LT. Preparation and mechanical properties of waterborne polyurethane/
carbon nanotube composites. Polymer Compos 2009; 3: 15.
7. Takimoto T, Onishi T, Saito K, Takahashi M, Uebayashi S and Ito K. Development and characteristics of a biological tissue-equivalent phantom for microwaves. Electron Commun Jpn
2007; 90: 4855.
8. Kalaitzidou K, Fukushima H and Drzal LT. A new compounding method for exfoliated graphite -polypropylene nanocomposites with enhanced flexural properties and lower percolation
threshold. Compos Sci Tech 2007; 67: 20452051.
9. Gabriel S, Lau RW and Gabriel C. Dielectric properties of human urine at microwave frequences. Phys Med Biol 1996; 41: 22712280.
10. Augustine R, Kalappura UG, Laheurte JM and Mathew KT. Characteristics of biological tissue equivalent phantoms applied to UWB communications. Microw Opt Lett 2009; 51(12):
29232927.
11. Tu H and Ye L. Thermal conductive PS/graphite composites. Polymer Adv Tech 2009; 20:
2127.
12. Mo Z, Shi H, Chen H, Niu G, Zhao Z and Wu Y. Thermal, dielectric, and mechanical properties of SiC particles filled linear low-density polyethylene composites. J Appl Polymer Sci
2009; 112: 573578.
13. Droval G, Feller JF, Salagnac P and Glouannec P. Thermal conductive PS/graphite composites. Polymer Adv Tech 2006; 17: 732745.
14. Saleem A, Frormann L and Iqbal A. High performance thermoplastic composites: Study on
the mechanical, thermal, and electrical resistivity properties of carbon fiber-reinforced polyetheretherketone and polyethersulphone. Polymer Compos 2007; 28: 785796.
15. Yasmin A and Daniel IM. Mechanical and thermal properties of graphite platelet/epoxy composites. Polymer 2004; 45: 82118219.
16. Quan H, Zhang B, Zhao Q, Yuen RKK and Li RKY. Facile preparation and thermal degradation studies of graphite nanoplatelets (GNPs) filled thermoplastic polyurethane (TPU) nanocomposites. Compos A 2009; 40: 15061513.
17. Ito K, Furuya K, Okano Y and Hamada L. Characteristics of biological tissue equivalent phantoms applied to UWB communications. Electron Commun Jpn 2001; 84(4): 6777.
18. Lonappan A, Hamsakkutty V, Bindu G, Jacob J, Thomas V and Mathew KT. A novel method
of detecting malaria using microwaves. Microw Opt Tech Lett 2004; 42: 500504.
19. Yohannan J, Jacob J, Lonappan A and Mathew KT. Biocompatibility study of beta tricalcium
phosphate bioceramics and chitosan biopolymer and their use as phantoms for medical imaging applications. Microw Opt Tech Lett 2003; 39: 112117.
20. Mo Z, Sun Y, Chen H, Zhang P, Zuo D, Liu Y, et al. Preparation and characterization of a
PMMA/Ce(OH)3, Pr2O3/graphite nanosheet composite. Polymer 2005; 46: 1267012676.
21. Subodh G, Deepu V, Mohanan P and Sebastian MT. Microwave absorbing property and complex permittivity and permeability of epoxy composites containing Ni-coated and Ag filled
carbon nanotubes. J Phys D Appl Phys 2009; 42, 225501.
22. Subodh G, Deepu V, Mohanan P and Sebastian MT. Polystyrene/Sr2Ce2Ti5O15 composites
with low dielectric loss for microwave substrate applications. Polymer Eng Sci 2009; 49:
1218.
23. Jayasundere N and Smith V. Dielectric properties of nano ZnO-polyaniline composite in the
microwave frequency range. J Appl Phys 1993; 73: 2462.
24. Xie SH, Zhu BK, Wei XZ, Xu ZK and Xu Y. Polyimide/BaTiO3 composites with controllable
dielectric properties. Compos A 2005; 36: 1152.
540