Composite Interfaces

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Effective interactions and dielectric study

of polymer nanocomposite thin films of
polyvinylidene fluoride and graphene oxide

Feba Anna John, Paulose Thomas, George Jacob & Ajith James Jose

To cite this article: Feba Anna John, Paulose Thomas, George Jacob & Ajith James Jose
(2024) Effective interactions and dielectric study of polymer nanocomposite thin films
of polyvinylidene fluoride and graphene oxide, Composite Interfaces, 31:1, 77-97, DOI:
10.1080/09276440.2023.2232979

To link to this article: https://doi.org/10.1080/09276440.2023.2232979

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COMPOSITE INTERFACES
2024, VOL. 31, NO. 1, 77–97
https://doi.org/10.1080/09276440.2023.2232979

Effective interactions and dielectric study of polymer

nanocomposite thin films of polyvinylidene fluoride and
graphene oxide
Feba Anna Johna, Paulose Thomasb, George Jacobc and Ajith James Josea
a
Post Graduate and Research Department of Chemistry, St. Berchmans College (Autonomous),
Changanassery, India; bDepartment of Physics, Marthoma College for Women, Perumbavoor, India; cCentre
for Nanotechnology Research, Vellore Institute of Technology, Vellore, India

ABSTRACT ARTICLE HISTORY

Polyvinylidene fluoride (PVDF) is a well-known fluoropolymer for its Received 25 March 2023
electronic applications. The present work investigates the influence Accepted 30 June 2023
of Graphene oxide (GO) in various weight percentages over the KEYWORDS
dielectric profile of the PVDF matrix. Field emission scanning elec­ Polymer nanocomposite thin
tron microscopy (FESEM) is used to explain the morphological films; polymorphism;
features of the samples. The thermal stability of the PVDF polymer dielectric properties; energy
with the addition of GO was studied using thermogravimetric gap; interactions
analysis (TGA). X-ray diffraction spectroscopy (XRD), confocal
Raman microscopy (CRM), and Fourier Transform infrared spectro­
scopy (FTIR) were used to interpret the appreciable interfacial
interactions between the matrix and the nanofiller and possible
phase transformations. The presence of polar and non-polar poly­
morphic phases in PVDF was verified with the help of XRD, FTIR, and
CRM analyses. The band gap energy of the samples was determined
using the Tauc-plot method from UV–visible observations. The
variation in the polarity of the matrix with the inclusion of GO is
also noted. The dielectric and AC conductivity measurements were
done at 100 Hz and 2 MHz. All these ascertain the candidacy of
PVDF/GO nanocomposite thin films to be incorporated into elec­
tronic devices of this era.

CONTACT Ajith James Jose [email protected] Post Graduate and Research Department of Chemistry,
Changanassery, Kerala 686101, India
Supplemental data for this article can be accessed online at https://doi.org/10.1080/09276440.2023.2232979.
© 2023 Informa UK Limited, trading as Taylor & Francis Group
78 F. A. JOHN ET AL.

1. Introduction
Polymer-nanocomposites conquered various domains, viz. electronics, optoelectronics,
medicine, communication, food, textiles, etc., with their extraordinary features. The
universe has pieces of evidence to substantiate how the blend of polymer science and
nanoscience creates a significant breakthrough in research.
Polymers with symmetrical structures and true covalent bonds always function as
insulators, whereas polymers with polarized covalent bonds exhibit high permittivity,
thereby a high dielectric constant [1]. Polyvinylidene fluoride (PVDF) is a versatile semi-
crystalline, thermoplastic fluoropolymer with an array of properties such as high chemi­
cal resistance, mechanical strength, piezoelectric and pyroelectric properties, good pro­
cessability, adhesive nature, environment friendly, and so on [2]. The physical and
electrical properties of PVDF depend on several factors, viz., molecular weights, chain
configurations, crystalline form, and defects in the chain.
The semi-crystalline PVDF polymer may exist in five different phases, namely α, β, γ,
δ, and ε of which α is the most stable polymorphic phase [3–5]. These five polymorphs
may exist in different chain conformations as follows: all-trans (TTTT) planar zigzag for
β phase, Trans-Gauche-Trans-Gauche’ (TGTG`) for α and ε phases, Trans-Trans-Trans-
Gauche’ (TTTG) for γ and δ phases [6–10]. Polymorphism is crucial for polymers to
govern their dielectric constant, ferroelectric properties, polarity, and membrane perfor­
mance (fouling and wetting) [11,12]. Among the five polymorphs of PVDF crystals, two
are non-polar (α and ε), and the other three are polar (β, γ, and δ). The β polymorph of
PVDF is the most desirable phase with the highest mechanical property [12].
The fate of dielectric properties of the partially fluorinated PVDF polymer lies mainly
on the carbon backbone chain (C–C bonds) and the additional bonds with fluorine
(C-F and CF2 bonds) and hydrogen (C-H). The β polymorph of PVDF polymer is more
significant for its considerable dipole moment owing to its all-trans conformation [13].
Previous studies suggest that the dielectric properties of PVDF-based nanocomposites
can be intensified by combine them with carbonaceous fillers [13,14].
Graphene oxide (GO) is a derivative of graphene where atoms are arranged two-
dimensionally in a hexagonal lattice. GO is obtained by the process of oxidation in
presence of a suitable oxidizing agent. The functional group -OH is located on the sp2
carbon basal plane. In addition, it is easily dispersible in some other organic solvents and
matrices. The pliability of GO suits it for many fields: biomedicine, electronics, energy
storage materials, composite materials, nanotechnology, etc. [15–18]. The enhancement
of dielectric permittivity of PVA polymer with the inclusion GO polymer was reported
[19]. Mensah e al. [20 explained how the dielectric properties of the blend Acrylonitrile-
Butadiene Rubber/Ethylene-Propylene-Diene-Monome reinforced with GO and r-GO.
GO captivated researchers in various fields and explored a plenty of applications
revealing the exceptional properties emerged after the combination of these two. The
improvisation in the tensile strength, Young’s modulus, and thermal stability of PVDF
with GO nanofiller was reported in previous papers [10,14,21]. The effective nucleation
of β phase and the improved dielectric properties of PVDF/GO nanocomposites are
reported in different studies [10]. Xu et al. [22] synthesized PVDF/r-GO polymer
nanocomposite through solution compounding followed by melt compounding method
and explained the dielectric properties of the composite. Recently, Hang Song et al. [23]
 COMPOSITE INTERFACES 79

synthesised PVDF/GO nanocomposite using electro spun method and examined its
piezoelectric properties. The development of PVDF-based innovative energy storage
materials has been growing rapidly due to its exceptional properties [24,25].
The major works which deals with dielectric properties or charge-carrying applica­
tions of PVDF/GO polymer nanocomposite-adopted conventional melt processing
method assisted by solid state shear milling technology [26], electrospun method [23],
spin coating method [27], high shear solution mixing followed by compression moulding
method [28], melt compounding method [22], phase inversion method [29] and many
more. However, the simple solution casting synthesis route to develop PVDF/GO-based
dielectric material is not much explored [10,23,27,30,31]. Therefore, this work intended
to develop the PVDF/GO nanocomposite thin films by solution casting method. In
addition, the electrical and dielectric properties of PVDF/GO nanocomposites are
described according to the interactions between the polar phases of the matrix and the
nanofiller. Field Emission Scanning Electron Microscopic analysis (FESEM),
Thermogravimetric analysis (TGA), X-Ray diffraction analysis (XRD), Confocal
Raman Microscopy (CRM), Attenuated Total Reflectance-Fourier Transform Infrared
spectroscopy (ATR-FTIR), UV–Visible absorption Spectroscopy, and LCR meter are the
tools used to investigate the morphology, thermal stability, chemical environment,
conductivity, and dielectric properties of the PVDF/GO polymer nanocomposite. The
outcome of this study expectantly leads to the development of low-cost, lightweight, and
flexible dielectric material to compete with the materials in the present scenario.

2. Materials and methods

2.1. Materials
PVDF (99.99% purity) powder was purchased from Tech inc, Chennai, Graphite powder
(99.98% purity) (⁓40 μm) (Sigma Aldrich), Sodium nitrate, N, N’-dimethyl formamide
(DMF), and potassium permanganate (Merck). All the chemicals were used directly
without any additional modification or treatment.

2.2. Sample preparation

Graphene oxide is derived from the conjugated carbon nanomaterial graphene by
modified Hummer’s method [32]. The thin films (The pristine PVDF film and PVDF/
GO nanocomposite films) were obtained by using the solution casting method. The
sample films were prepared by dispersing the appropriate amount of both PVDF and GO
separately in DMF solution. At first, the DMF/PVDF mixture was subjected to mechan­
ical stirring, and the DMF/GO mixture underwent sonication simultaneously for 1 hr.
Then both the mixtures were combined together and subjected to mechanical stirring for
4 hrs. After the mechanical stirring, the colloidal solutions of polymer nanocomposite
were cast onto clean glass plates to get thin films of each sample. It was kept aside to
evaporate the solvent and allowed to dry for 3 days. After 3 days, the thin films were
peeled off from the glass plate and the samples of the required shape, size, and quantity
were sent for various analyses. The PVDF/GO nanocomposites were designated as PG1,
80 F. A. JOHN ET AL.

PG2, PG3, PG4, and PG5, respectively, according to the weight percentages 0.0, 0.05, 0.1,
0.5, and 1 of GO. Figure 1

2.3. Characterization techniques

The surface morphology of the samples was examined using Field Emission Scanning
Electron Microscopy (FESEM, TESCAN BRONO s.r.o. Czech). The thermal analysis of
pure and nanocomposite thin films of PVDF with GO was investigated using Perkin
Elmer Simultaneous Thermal Analyzer (STA 6000) at a heating rate of 20°C/min. The
samples were put through the temperature range of 30°C–700°C and the nitrogen gas
flow rate of 20 mL/min. The X-ray diffraction of the PVDF/GO thin films was produced
using the Rigaku Miniflex 600 instrument with Kα radiation and 5 s per step of 0.01° and
10° speed at 2θ = 5° to 90°. Perkin Elmer’s Fourier Transform Infrared Spectroscopy with
Attenuated Total Reflectance (ATR-FTIR) instrument was operated in the wavenumber
range 650–4000 cm−1 to obtain the characteristic fingerprint region of the nanocompo­
sites and to explore its structure and chemical interactions. The Raman spectrum of the
PVDF/GO nanocomposites was recorded on a confocal Raman Microscope (CRM,
WITEC ALPHA300 RA). A 50X/0.75 Zeiss objective was used for the Raman micro­
scopic analysis, and the studies were set to perform two accumulations with 30-s
integration time at 532 nm laser wavelength. The absorbance of the samples was inves­
tigated using a UV–visible spectrophotometer (Jasco Japan) with a wavelength range
from 190 to 900 nm. The band gap energy has been calculated using the Tauc-plot
method to assess the change in the dielectric property of pristine PVDF with GO. The
AC conductivity and dielectric measurements at room temperature are examined using
LCR Hitester with a frequency range from 100 Hz to 2 MHz.

3. Results and discussions

3.1. The extent of interaction, morphology, and crystalline phase moieties
The Field Emission Scanning Electron Microscopic analytical techniques were
employed to examine the uniform distribution of GO in PVDF matrix as well as
their effective interactions. Figure 2(a) represents platelet structure of the nanofiller

Figure 1. Schematic diagram representing the fabrication of PVDF/GO polymer nanocomposite thin
films through solution casting method.
 COMPOSITE INTERFACES 81

GO [33]. Figure 2(b) displayed the porous structure of pure PVDF film [34]. Figure 2
(c-f) shows that the pores in the pure PVDF decreased with the increase in the
concentration of GO [35]. The oxygen-containing groups of GO might be interacted
with the fluorine atoms of PVDF and encapsulated into the porous polymer matrix
[10,36].
Figure 3 represents the comparative thermogravimetric study of PVDF/GO nano­
composite of different nanofiller concentrations. The maximum weight loss that
occurred within the temperature range of 410°C−500°C [37]. The pure PVDF started
to degrade thermally from 365°C owing to the chain scission of the polymer chain, but
the GO fabricated polymer retained almost 100% by weight at this temperature point.
This implies the downtrend in the degradation rate via the dispersion of GO nanofillers
into the PVDF matrix, and it is supported by the barrier effects associated with the
carbonaceous nanofillers. Substantial degradation of the reinforced PVDF with GO was
detected only after 426°C declared the acquired thermal stability of PVDF with the
nanofiller [31].
Furthermore, a significant depletion in the % weight loss was noticed with the addition
of the filler (GO nanoparticles) in the first-degree thermal degradation itself (Figure 4). It
has also been observed that the final residue of pure PVDF after the thermal degradation
is 17.84 wt.%, and the aggregation is increased by the factor 8.4 and 10.24 for 0.05 wt.%
and 0.1 wt.% of GO, respectively. This indicates that the interaction between the polymer

Figure 2. FESEM images of GO (a), PG1 (b), PG2 (c), PG3 (d), PG4 (e), PG5 (f).
82 F. A. JOHN ET AL.

Figure 3. TGA plot of wt.% Vs T ºC of Pure PVDF (PG1) and PVDF/GO (PG2, PG3, PG4, PG5).

Figure 4. TGA plot weight loss % Vs TºC of Pure PVDF (PG1) and PVDF/GO (PG2, PG3, PG4, PG5).
 COMPOSITE INTERFACES 83

matrix and the nanofiller is probably between the oxygen-containing groups of GO and
the fluorine atoms of PVDF (Figure 11) [38]. It is noticed that after 0.1 wt.% addition, the
trend is detoured, and the aggregation is increased by a factor of 6.93 for the next two
additions of GO (0.5 and 1 wt.%) to the matrix. This might be due to the nanofiller
aggregation and bead formation [14].
Figure 5 shows the X-ray diffractograms of GO, pure PVDF, and the PVDF/GO
nanocomposites. A typical diffractogram corresponding to GO with intense peak at
10.7º is portrayed in the inset of Figure 5 [39]. PG1 gives an intense diffraction peak at
20.7º and a weak peak at 41.2º implying the polar crystalline β-phase of the polymer
[1,29,40]. As the wt.% of GO increased the peaks corresponding to β-phase get enhanced.
The diffractogram for PG4 and PG5 displayed a new peak at 26.6º corresponding to the
α- phase of PVDF [29,40]. The absence of characteristic peaks at ~2θ = 10º corresponds
to graphene oxide in the diffractograms of polymer nanocomposites, pointing to the
interaction between GO and PVDF [41].
Figure 6 illustrated the FTIR spectrum of the nanofiller GO. The peak at 1225 cm−1,
and 1014 cm−1 represented C-O-C stretching vibrations and C-O vibrations, respectively,
[42–44]. The C=O stretching vibrations belongs to carboxyl and carbonyl functional
groups are denoted by the peak at 1718 cm−1. The peaks at 1589 cm−1 and 1385 cm−1
represented the C=C stretching vibrations and the hydroxyl group deformation for GO,
respectively, [22].
Figure 7 represents the ATR-FTIR analysis of the polymer nanocomposite (PVDF/
GO) and the polymer matrix within the wavelength range of 950–1500 cm−1. The bands
at 839 cm−1, 1072 cm−1, and 1404 cm−1 are related to β phase (TTTT), and the bands at
1170 cm−1 and 1234 cm−1 are related to γ phase (TTTG). The significant narrowing at
839 cm−1 and 1234 cm−1, the exclusive bands of β (TTTT), and γ (TTTG) phases,
respectively, by the increase in the concentration of GO nanofiller remarks improvement
in the fraction of polar phases of PVDF [26,29,45–49]. Figure 8

Figure 5. X-ray diffractogram of Pure PVDF (PG1) and PVDF/GO (PG2, PG3, PG4, PG5).
84 F. A. JOHN ET AL.

Figure 6. ATR-FTIR transmittance spectra of GO.

Figure 7. ATR-FTIR transmittance spectra of Pure PVDF (PG1) and PVDF/GO (PG2, PG3, PG4, PG5).

The Raman spectral analysis is backing up the findings of FTIR and XRD analyses.
The typical graphitic G-band and the distorted D-band can be obtained from Figure 9
[50]. The G-band at 1594 cm−1 and the D-band at 1349 cm−1 represent the in-plane
vibrations and the out-of-plane vibrations of the carbonaceous bonds accordingly. Here,
 COMPOSITE INTERFACES 85

Figure 8. Structures of (a) non-polar α-phase (TGTG), (b) polar β-phase (TTTT) and (c) polar γ-phase
(TTTG) of PVDF.

Figure 9. Raman spectra of GO.

86 F. A. JOHN ET AL.

the sp2 hybridized carbons swaps to sp3 hybridized carbons, and lattice distortion
occurred [51]. The distortion happened due to the inversion of foreign adatoms, such
as oxygen, hydroxyl groups, and carboxyl groups by the oxidation of some carbons of the
sp2 network, evidencing the GO [52]. Besides the G-band and D-band, it is important to
consider the 2D bands of graphene-based materials. Here, the Raman spectrum of GO
exhibits two 2D peaks, one at 2682 cm−1 represents monolayer and the other at 2921
cm−1 represents multilayer [53].
Figure 10 depicts the Raman spectra corresponding to PVDF/GO nanocompo­
sites. The pure PVDF polymer matrix displayed mainly three Raman peaks at 840
cm−1, 1430 cm−1, and 2975 cm−1. The peak observed at 840 cm−1 is the out-of-
phase combination of CH2 rocking and CF2 stretching vibrations designated β -
PVDF polymorphism [54]. The scissoring and wagging modes of vibrations of –
CH2 have been indicated by the edge at 1430 cm−1 representing the polar β, and γ
phases [55]. Furthermore, the symmetric vibrational mode of sp 3 hybridized
H-C-H bonds in PVDF is defined by the peak at 2975 cm−1 assigning the β
phase [49,55]. PG2, PG3, PG4, and PG5 manifest the introduction of GO to the
PVDF matrix by displaying the shift of the G-band from 1594 to 1598 and
D-band from 1349 to 1341 [49,56]
The ID/IG ratio values corresponds to PVDF/GO composites were decreased with the
increase in the concentration of GO owing to the effective interaction between the
nanofiller and the polymer matrix [26]. It is observed that the intensity of the peak
associated with β crystalline phase at 2975 cm−1 is improved continuously for the first
two additions of GO (PG2 and PG3) and then depleted for PG4 and PG5 this also
implying the interaction between the matrix and the nanofiller. Again, in PG4 and PG5

Figure 10. Raman spectra of Pure PVDF (PG1) and PVDF/GO (PG2, PG3, PG4, PG5).
 COMPOSITE INTERFACES 87

there obtained a peak around 794 cm−1, which is considered as the typical peak for α
phase [57], this observation concedes the findings of the XRD results mentioned above.
When consolidating all the findings of the above analyses, it is found that the OH
groups of Graphene oxide interact and develop hydrophilic bonds with the electrophilic
fluorine atoms of PVDF (Figure 11), helping to sustain β polymorphism of the matrix
[25,45]. The enhancement in the β phase up to the optimum concentration of the
nanofiller (0.1 wt. % of GO) is demonstrated by the XRD, FTIR, and Raman investiga­
tions. These interactions strain the polar bonds on the matrix and restrict its rotations;
consequently, the polar β bonds remain in all trans-polar phase configurations
[27,46,56]. The polar GO, too, contributed to the polarity of the composites. The
improved polarity of PVDF by the nucleation of GO is advantageous for its dielectric
properties [24,46].

3.2. Energy gap, AC conductivity, and dielectric studies

Figure 12 and 13 represented the UV–visible absorption spectra of pure GO, pure PVDF,
and PVDF/GO polymer nanocomposite in 200–900 nm wavelength. In Figure 12 the
absorbance edge observed at 250 nm depict the π-π* transition due to the conjugative
effects of the sp2 cluster in connection with the C=C bonds of GO. The secondary peak at

Figure 11. Hydrophilic interaction between the C-F bonds of PVDF and hydrogen supplying bonds of GO.
88 F. A. JOHN ET AL.

Figure 12. UV-visible absorption curves of GO.

Figure 13. Comparison of UV-visible absorption curves of Pure PVDF (PG1) and PVDF/GO (PG2, PG3,
PG4, PG5).
 COMPOSITE INTERFACES 89

315 nm indicating n-π* transition assigning the C=O bonds of GO [58]. The absorbance
curves inferthat its intensity rises with the GO nanofiller. This shift in absorbance curves
of PVDF/GO composites indicate the variation in the energy gap [59].
The band gap energy indicates how far the valence band is situated from the
conduction band. Usually, the energy gap of dielectrics lies in 3 eV or more, i.e.,
the valance electrons are restricted to cross the forbidden zone. All the same, the
dielectrics loaded with some nanofillers exhibit desirable conducting proper­
ties [60].
The band gap energy of the solution cast samples is determined using Tauc
relation expressing the dependence of the absorption coefficient (α) on the photon
energy (hυ).

where, ‘h’ Plank’s constant, ‘υ’ the photon’s frequency, ‘Eg ’ band gap energy, ‘B’ is
a constant called band tailing parameter.
The γ factor depends on the nature of the electron transition and is equal to ½ or 2 for
direct and indirect transition band gaps, respectively.
Figure shows the direct band gap energy determination by plotting½αhυ�2 on the
Y-axis and energy ðeVÞ on the X-axis [61–64].
As per the Tauc plot (Figure 14), the energy gap (Eg ) for pure PVDF is 5.12 eV, and it
is depleted in the presence of nanofiller for all the additions of GO, which indicates
a slight improvement in the conducting properties of the PVDF matrix [46]. It is noticed
that the band gap energy corresponding to the higher concentrations (for PG4 and PG5)
are higher than that of the PG3 (0.1 wt.% GO), which indicates deformations in the
polymer matrix.
Figure 15 depicts the variations in the dielectric constant (ɛr) values of the PVDF
matrix with the inclusion of GO at different concentrations. The dielectric constant was
determined using the following relationship;

where ‘C’ is the Capacitance, ‘d’ is the thickness of the film, ‘ε0’ is the permittivity
of free space with a value of 8.854 × 10−12 Fm−1, and ‘A’ is the area of the
sample [65].
It is observed that the dielectric constant for all the samples is higher in lower
frequencies, and it increases with the frequency and becomes constant for higher
frequencies. This phenomenon can be best explained with the MaxwellWagner Sillar
(MWS) theory stating the accumulation of charge at the interfaces of two materials with
different relaxation times or interfacial polarization (IP). At lower frequencies, the
induced and permanent dipoles get enough time to align in proper orientation and
accumulated the charges; therefore, this region shows high dielectric constant. As the
frequency increased, the diploes could not get enough time to align properly and showed
less dielectric constant than previously; this phenomenon is known as polarization
relaxation. For higher frequency ranges, the dielectric constant becomes frequency
90 F. A. JOHN ET AL.

Figure 14. Tauc – plot of Pure PVDF (PG1) and PVDF/GO (PG2, PG3, PG4, PG5).

independent so the values become almost constant at this range, this process is termed
micro-capacitor structure model [41,65].
The dielectric constant for the PVDF/GO polymer nanocomposites in various composi­
tions are higher than that of pure PVDF is due to the increases in the interfacial polariza­
tion, which implies the enhancement of all-trans (TTTT) PVDF β polar polymorphism
[46]. The same trend has been observed in the plot between tangent loss (Tan δ) and log
f (Figure 16). If the dielectric constant expresses the electrical polarization, the tangent loss
 COMPOSITE INTERFACES 91

Figure 15. Plot of dielectric constant Vs Frequency of Pure PVDF (PG1) and PVDF/GO (PG2, PG3, PG4,
PG5).

portrays the energy dissipation of the materials [66]. The tangent loss has been obtained
from the real (ε”) and imaginary (ε’) parts of the dielectric constant using the equation
00
Tanδ ¼ εε0 . . . . (3) [31,65].
The upgradation of AC conductivity of PVDF polymer matrix with the inclusion of
GO nanofiller is demonstrated in Figure 17. It was calculated using the following
relationship;

where ‘ω’ is the angular frequency and ‘f’ is the angular displacement per unit of
time [65].
The conductivity measurements for each film increased initially with the frequency
and stay almost constant on further increase in frequency. The conductivity of the
polymer nanocomposite is increased with the addition of GO, and the maximum con­
ductivity was detected at the PVDF/GO 0.1 wt.% composition. The improved electrical
conductivity of the polymer nanocomposite is the ability of the GO nanofiller to provide
percolative pathways for electron transfer [21,31]. These observations can be related to
the dielectric property demonstrations for the PVDF/GO nanocomposite films.
Abbasipour et al. [14] stated that the improvisation in polarity of PVDF polymer by
instituting GO nanoparticles leads to an appreciable hike in the dielectric properties of PVDF.
92 F. A. JOHN ET AL.

Figure 16. Plot for Tangent loss Vs Frequency of Pure PVDF (PG1) and PVDF/GO (PG2, PG3, PG4, PG5).

Figure 17. Electrical conductivity of Pure PVDF (PG1) and PVDF/GO (PG2, PG3, PG4, PG5).

The hike in the dielectric constant, the tangent loss, and AC conductivity, as well as the
reduction in the band gap energy of the PVDF/GO nanocomposite films confirm the
intercalation of GO into the PVDF matrix due to the interaction between the electrophilic
 COMPOSITE INTERFACES 93

fluorine atom and functional groups of GO. This results in the improvement of the fraction of
polar phases and provides electric pathways in the polymer matrix [31,66].
However, it is observed that the band gap energy, dielectric constant, tangent loss, and
AC conductivity belong to 0.5 and 1 wt.% addition of GO is lower than that of 0.1 wt.%
GO. Here, the highest polarity attained by 0.1 wt.% GO is declined by the higher
concentration of GO; consequently, the accumulation of polar bonds failed. Thus, it is
inferred that some of the β phase portions in PG3 converted to the non-polar α phase, as
evidenced by the Raman shift from 840 cm−1 to ~794 cm−1 reported in this work. These
anomalies corresponding to PG4 and PG5 might be due to the bead formation or the
structural defects within the PVDF polymer chain by incorporating GO above the
optimal concentration of nanofiller [10,14,66].

4. Conclusion and future prospective

The thin films of PVDF/GO nanocomposites prepared through the solution casting method
with different filler contents (0.0, 0.05, 0.1, 0.5, and 1 wt.%) were subjected to various
investigative techniques to figure out the finest composition/s and their aptness in the
application and development of dielectric materials. The zig-zag fashion of GO and β-
PVDF facilitates their effective interactions. XRD, FTIR, and Raman microscopic analyses
help to verify the β-phase enhancement. The hydroxyl and carboxylic acid groups associated
with GO created hydrophilic bonds with PVDF and restricted the rotation or movement of all
trans TTTT (β phase) conformed polar C-F bonds to TGTG conformation (α phase). The
energy gap computed from absorbance data using Tauc – plot method hypothesizes that the
PVDF matrix’s improved conductivity by adding GO within the conductivity limit assigned
for typical dielectric materials. Solution casting is an effective method to obtain polar PVDF
thin films; the introduction and interaction of polar graphene oxide helped the matrix to
retain and improve its polarity. This study reiterated that 0.1 wt.% GO is the optimum
concentration for the effective nucleation of β- phase in the PVDF matrix to fabricate an
ideal dielectric material for electronic applications.

Acknowledgements
This research did not receive any specific grant from funding agencies in the public, commercial,
or not-for-profit sectors. The authors acknowledge DST, SAIF, and MGU, Kottayam, for provid­
ing technical assistance for FESEM and Confocal Raman microscopic analysis.

Disclosure statement
No potential conflict of interest was reported by the author(s).

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