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Graphene nanoplatelets (GNPs): a source to bring

Cite this: RSC Adv., 2023, 13, 34308
change in the properties of Co–Ni–Gd-ferrite/GNP
nanocomposites
Zartashia Latif,a Atta Ur Rehman, a
Nasir Amin,a Muhammad Imran Arshad *abc
and Riadh Marzoukid

The nanocomposites of Co0.5Ni0.5Gd0.03Fe1.97O4/graphene nanoplatelets (CNGF/GNPs) were synthesized

by a cost-effective sol–gel auto combustion (SGAC) route. The X-ray diffraction analysis confirmed the
cubic structure of the as-prepared nanocomposites, and a crystallite size of 32.28 nm was observed for
the 7.5 wt% GNPs. Irregular and unique nanoparticles consisting of short stacks of graphene sheets
having a platelet shape were confirmed by the morphological analysis of the as-prepared
nanocomposites. Raman analysis revealed a spinel crystal structure along with a new vibrational mode
due to the GNPs. The energy bandgap was 3.98 eV for the composite with 7.5 wt% GNP concentration.
It was observed that the percentage temperature coefficient of resistance (TCR%) rapidly decreased with
an increase in temperature both in low- and high-temperature ranges. Dielectric studies carried out in
the frequency range 104–107 Hz confirmed that the graphene-added composites had high values for
Received 30th March 2023
Accepted 7th November 2023
both the real and imaginary parts of permittivity at low frequencies. A decrease in saturation
magnetization with an increase in GNP concentration was observed compared with the pure CNGF
DOI: 10.1039/d3ra02080k
samples. Hence, the as-prepared composites are useful for application in high-frequency devices as well
rsc.li/rsc-advances as spintronics.

promising structural, electrical, optical, magnetic, mechanical,

1. Introduction and thermal properties of graphene have opened new avenues
The incorporation of nano-sized particles into the matrix of for learning materials science.5,6 Compared with other nano-
a standard material results in a nanocomposite, which exhibits materials, so ferrites are less expensive, reliably stable, and
drastic improvement in several properties, such as mechanical easy to prepare. Their high permeability at radio frequencies,
strength and magnetic, optical, electrical, and thermal high Curie temperature, high electrical resistivity, low eddy
conductivities. An excellent example of the nanocomposites is current loss, ne environmental stability, and mechanical
graphene with so ferrites, which show tremendous changes hardness make them suitable for application in many devices,
and enhancement in properties and hence are successfully used such as microwave apparatus, inductors, choke coils, trans-
in various elds, such as wastewater treatment, improvement of formers, and electromagnetic interface (EMI) suppressors. One
broadband absorption in gigahertz frequencies and microwave class of so ferrites is cubic spinel ferrites (SFs) with MFe2O4,
absorption, and energy storage sensors.1–4 The structure of where M is a divalent ion, such as Mn2+, Ni2+, Fe2+, Co2+, or
graphene is capable of modifying the different properties of so Mg2+. A lot of studies and research have been done on cubic
ferrites, such as non-conductivity to conductivity, thereby ferrites and many mixed ferrites. Saqib et al. studied the
intensifying their magnetism and improving the structural and structural, electrical, and magnetic properties of Mg-doped
mechanical parameters. Moreover, it can also improve the ZnFe2O4 ferrites.7 Different ferrites are considered unique for
thermal and dielectric properties of the nanocomposites. These different properties; cobalt ferrite has special magnetic
properties8–10 and outstanding chemical and structural
stability.11–13 The substitution of Fe3+ ions with rare earth metals
a
Department of Physics, Government College University, Faisalabad, Pakistan. E-mail: with larger ionic radii than Fe3+ into the spinel structure alters
miarshadgcuf@gmail.com; Muhammad.arshad@ucl.ac.uk the electromagnetic properties of ferrites. Consequently, the
b
Biophysics Group, Department of Physics and Astronomy, University College London, inconsistent behavior of doped nickel ferrites is observed.14–16
Gower Street, London, WC1E 6BT, UK
c
The preparation techniques used for cubic ferrites with
UCL Healthcare Biomagnetics and Nanomaterials Laboratories, 21 Albemarle Street,
different concentrations and the distribution of different
London W1S 4BS, UK
d
Department of Chemistry, College of Sciences, King khalid University, Abha, 61413,
cations at the tetrahedral (A-) and octahedral (B-) sites of the
Saudi Arabia sample lattice play a vital role in tuning the properties. Thus,

34308 | RSC Adv., 2023, 13, 34308–34321 © 2023 The Author(s). Published by the Royal Society of Chemistry
Paper RSC Advances

any addition and alteration in the distribution and ratio of these 2.2 Synthesis of CNGF sample
cations can change their magnetic behavior. Satalkar et al.
The CHNF sample was prepared by the sol–gel auto-combustion
prepared Zn0.7−xNixMg0.2Cu0.1Fe2O4 (x = 0.0–0.7) ferrites by
(SGAC) method. All chemicals at proper stoichiometric
a sol–gel auto-combustion (SGAC) method. They found that Ni2+
proportions were sonicated individually for 10 min at 353 K to
addition plays a part in determining the magnetic properties
make their homogenous solutions in distilled water. All
and changes the cationic distribution.17 Therefore, the usage of
prepared solutions were mixed again by using a magnetic stirrer
suitable additives plays a vital role in gaining high-performance
for up to 15 minutes until well combined, followed by the
ferrites. addition of the citric acid solution. NH4OH was added dropwise
Tremendous work has been done on the addition of rare to maintain the pH of the solution at 7 and stirring was further
earth metals to so ferrites at varying concentrations by using
continued for 20 minutes. The samples were heated at 523 K
a variety of mechanical and chemical procedures, such as sol–
until a gel was formed, aer which the magnetic stirrer was
gel, hydrothermal, and traditional ceramic technology.
turned off while heating was continued, which further led to
Elements of the lanthanide series, such as gadolinium,
self-combustion, and the solution turned into ash. It was
neodymium, cerium, and yttrium, are added to different ferrites
mechanically ground by using a mortar and pestle to make
due to their special characteristics. These elements are
a ne powder, which was calcined at 1123 K for 5 h. The
frequently used with ferrite combinations at different concen- calcined samples were again ground to obtain their powder
trations in many applications as they enhance optical, struc- form.
tural, magnetic, electrical, and morphological properties. Pawar
et al. reported that Gd3+ substitution in the Co–Zn ferrite
increases the saturation magnetization and coercivity. Conse- 2.3 Synthesis of CNGF/GNP nanocomposites
quently, these Gd3+-substituted materials are appropriate for The sonochemical approach was used to prepare the CNGF/
use in permanent magnets and magnetic recording media.18 GNP nanocomposites by keeping the stoichiometric quantities
The properties of cubic ferrites are enhanced when rare earth of GNP at 2.5 wt%, 5 wt%, and 7.5 wt% of the total metal nitrate
metals with higher ionic radii are substituted for Fe3+. The salts. The required amount of GNP was dissolved in distilled
concentration of rare earth metals plays a pivotal role in water, and the mixture was sonicated for half an hour to get
determining the properties of the cubic ferrites.19 Poudel et al. a homogeneous dispersion. All the metal nitrate salts dissolved
studied that the concentration of Gd3+ in Ni ferrite enriched its in distilled water were separately added in dispersed GNP, and
properties.16 Hossain, M. D., et al. studied the properties each mixture was again sonicated for 20 minutes. A calculated
tailored by Gd3+ substitution at the B sites, replacing the Fe3+ amount of citric acid dissolved in distilled water was added to
ions of the Ni–Zn–Co ferrite. Due to substitution with gadoli- the metal nitrate salts -GNP mixture and sonicated further for
nium, they found changes in the structural properties, as well as 10 minutes. This mixture was placed on a magnetic stirrer for
electrical properties.20 It is worth mentioning that the content of thorough mixing, and this was followed by the SGAC method to
graphene plays an important, leading role in dening the get ash, which was ground into a ne powder and then calcined
dielectric behavior of carbon materials along with their at 1123 K for 5 h. Fig. 1 illustrates the step-by-step fabrication
magnetic anisotropy. This subsequently would impact the process.
microwave weakening behavior.
In this work, we followed the sol–gel auto-combustion route
to prepare Ni-doped cobalt ferrites with a stoichiometric 2.4 Characterization techniques used
formula of Co0.5Ni0.5Gd0.03Fe1.97O4 (CNGF) and loaded them on The structural properties and phase conrmation of the
the surface of graphene nanoplatelets (GNP) using a sono- prepared samples were studied by X-ray diffraction (XRD)
chemical approach. Therefore, this work aims to investigate the analysis using a Bruker D8 Advanced X-ray diffractometer
impact of graphene nanoplatelets (GNPs) on the spectral, elec- (XRD) using Cu-Ka source with a wavelength of 1.54 (Å). To
trical, magnetic, and dielectric properties of the CNGF inspect the surface morphology, scanning electron micro-
composites prepared via the sol–gel auto combustion (SGAC) scopic (SEM) images were captured using a Nova Nano SEM
process. series 450. Raman analysis was used to conrm the lattice
structure of the ferrites along with Gd3+ substitution of and
addition of GNP by using laser excitation at 532 and 780 nm in
2. Materials and methods the range of 200–1800 cm−1. The energy bandgap (Eg) of the as-
prepared samples was determined through UV-visible spec-
2.1 Materials troscopy. Current–voltage (I–V) measurements and hence
The following chemicals were used for the synthesis of the resistivity were calculated by using the two-probe technique on
Co0.5Ni0.5Gd0.03Fe1.97O4 (CNGF) sample and the CNGF/GNP an electric meter KEITHLEY Model 2401. The dielectric
composites. Iron nitrate nonahydrate [(Fe(NO3)2$9H2O), nickel behavior was studied using an LCR Meter (IM3533 series) in
nitrate hexahydrate [(Ni(NO3)2$6H2O), aqueous ammonia the frequency range of 4 Hz to 8 MHz at room temperature.
[(NH4OH), cobalt nitrate hexahydrate [(Co(NO3)2$6H2O), gado- The magnetic properties were investigated by studying the M–
linium nitrate hexahydrate [Gd(NO3)2$6H2O], citric acid H loop at 303 K by using a vibrating sample magnetometer
(C6H8O7), and graphene nanoplatelets (GNP). (VSM-175).

© 2023 The Author(s). Published by the Royal Society of Chemistry RSC Adv., 2023, 13, 34308–34321 | 34309
RSC Advances Paper

Fig. 1 A schematic representation of the synthesis of NCGF/GNP nanocomposites.

3. Results and discussion peaks (as shown in Fig. 2) at a 2q value of 26.38°, which denotes
the (002) crystal plane.21 In addition to that, the CNGF/GNP
3.1 Structural properties nanocomposites revealed diffraction peaks at 2q of 30.2°,
To discuss the effect of GNP on the structure of the CNGF 35.6°, 37.2°, 43.3°, 53.3° and 57.3°, corresponding to the (220),
nanoparticles, XRD analysis and Raman spectroscopy were (311), (222), (400), (422), and (511) planes, respectively.22
used, while the effect of GNP on the surface morphology was Further, using Braggs equation: 2d sin q= nl, the d-spacing for
studied using the micrographs obtained from SEM. pure GNP calculated based on 2q = 26.8° corresponding to the
3.1.1 X-Ray diffraction analysis. XRD spectra were used to (002) plane was 3.38 Å, which is larger than the values of the
understand the structural changes in the CNGF crystals aer CNGF nanoparticles and CNFG/GNP nanocomposites, as shown
the addition of GNP, as shown in Fig. 2. GNP showed diffraction in Table 1. Being a cubic crystal structure, the three lattice

34310 | RSC Adv., 2023, 13, 34308–34321 © 2023 The Author(s). Published by the Royal Society of Chemistry
Paper RSC Advances

the CNGF/GNP nanocomposites to that of the CNGF nano-

particles, along with a deteriorating trend of crystalline size,
suggests their enhanced electrocatalytic activity.23
3.1.2 Scanning electron microscopy analysis. SEM images
were used to analyze the morphology of the CNGF nanoparticles
and CNGF/GNP nanocomposites, as shown in Fig. 3(a–d).
Irregular particle morphology was observed in the nano-
particles, as seen in Fig. 3(a). The reported morphology of GNP
is ake-like; moreover, graphene nanoplatelets are unique
nanoparticles consisting of short stacks of graphene sheets
having a platelet shape.24 The SEM images of the as-prepared
CNGF/GNP nanocomposites in Fig. 3(a–d) indicate that the
GNP was densely covered with the CNGF nanoparticles. This
indicates that the mechanism of electrostatic attraction
between the nanoparticles and graphene25 gives rise to the
agglomeration of nanoparticles in the ake-like structure of
Fig. 2The XRD spectra of the CNGF nanoparticles and CNGF/GNP
GNP due to weak van der Waals, electrostatic, and capillary
nanocomposites.
forces, which are responsible for producing magnetic interac-
tions between the particles. The SEM images showed that
samples with graphene were thicker than CNGF, which is due to
constants are the same a = b = c, and their value was calculated
the presence of different functional groups like carboxyl and
using the formula; a = dhkl[h2 + k2 + l2]1/2, where h, k, and l Miller
carbonyl and some traces of oxygen, while, in the absence of
indices of the high-intensity peak (311)were used to calculate
graphene, the nanoparticles showed scattered behavior (as
the value of the lattice constants as listed in Table 1. The values
shown in Fig. 3(a)).24
of unit cell volume (V = a3) were calculated by using the value of
3.1.3 Raman spectroscopy analysis. Fig. 4 reveals the
the lattice constant. The lattice constant and unit cell volume of
Raman spectra of pure GNP, the CNGF sample, and the CNGF/
the CNGF/GNP nanocomposites did not change signicantly.
GNP composites. Pure GNP showed two vibrational bands
This may be due to the incorporation of GNP in the CNGF
around 1343 cm−1 and 1621 cm−1 corresponding to the D-band
nanoparticle spinel lattice. The crystalline size (D) of the as-
and G-band, respectively. The characteristic peaks at
synthesized nanocomposites was calculated using the Scher-
689.1 cm−1, 545.6 cm−1, 471.6 cm−1, 316.8 cm−1, and
rer equation; D = 0.94l/b cos q, where b is the full width at half
370.1 cm−1 of the SFs corresponded with ve active Raman
maxima (FWHM) of the highest intensity peak of the samples, l
modes A1g (R), 3 T2g (R) and Eg respectively, where A, E, and T
= 1.5406 Å is the wavelength of the used Cu Ka radiation source,
denote one-, two- and three-dimensional display of the SFs,
and” represents the Braggs reection angle. The smaller crys-
respectively, and g denotes symmetry at the center of inver-
tallite size of the CNGF/GNP nanocomposites compared with
sion.26 Raman spectra of the samples containing GNP at
the pure CNGF sample may be due to the incorporation of GNP
concentrations 2.5%, 5%, and 7.5% are shown in Fig. 4,
in the CNGF lattice (as shown in Table 1). The dislocation
showing slight changes in the rst ve active modes: the A1g (1)
density (d = 1/D2) is a measure of the number of dislocations per
mode of vibration at around 689.1 cm−1 changed to 686.6 cm−1
unit volume of a crystalline material and follows the opposite
due to GNP addition due to the symmetric stretching of the
trend to crystallite size i.e. when the crystallite size of the
oxygen atoms between Fe–O and metal ions at the tetrahedral
material is the maximum, the dislocation line density is
(A-) site. T2g (3), which is assigned to the asymmetric bending of
minimum and vice versa. The crystallite size was minimum for
oxygen at the octahedral (B-) site relative to Fe, changed from
the CNGF/2.5wt% GNP nanocomposite and it had the
545.6 to 543.3 cm−1 due to the insertion of GNP. T2g (2), which is
maximum dislocation line density, as shown in Table 1. It is
responsible for the asymmetric stretching of the Fe–O bond at
clear from Table 1 that the packing factor (p) also was smaller
the B-site, was originally found at 471.6 cm−1 but shied to
for the CNGF/GNP nanocomposites compared with the CNGF
467.7 cm−1 due to the addition of GNP. A low-intensity peak at
nanoparticles. The increase in the values of microstrain (3) of
370.2 cm−1 representing the Eg mode, which is responsible for

Table 1 The structural parameters of the CNFG nanoparticles and CNFG/GNP nanocomposites

Samples a (Å) D (nm) V (Å)3 d (Å) d × 10−4 (nm−2) 3 p

CNGF 8.345 40.18 581.21 2.518 6.193 0.00294 159.69

CNGF/2.5wt%GNP 8.335 28.76 579.18 2.515 12.131 0.00411 114.44
CNGF/5wt%GNP 8.343 36.38 580.88 2.459 7.552 0.00325 144.64
CNGF/7.5wt%GNP 8.344 32.80 581.05 2.518 9.292 0.00361 130.38

© 2023 The Author(s). Published by the Royal Society of Chemistry RSC Adv., 2023, 13, 34308–34321 | 34311
RSC Advances Paper

The SEM images of the (a) CNGF nanoparticles, (b) CNGF/2.5wt%GNP nanocomposite, (c) CNGF/5wt%GNP nanocomposite, and (d)
Fig. 3
CNGF/7.5wt%GNP nanocomposite.

Fig. 4 The Raman spectra of GNP (inset), CNGF, and CNGF/GNP composites.

34312 | RSC Adv., 2023, 13, 34308–34321 © 2023 The Author(s). Published by the Royal Society of Chemistry
Paper RSC Advances

Fig. 5 (a–d) The Tauc plots for the CNGF sample and CNGF/GNP composites.

the symmetric bending of the oxygen ions with respect to iron, the curves in Fig. 5(a–d). The Eg values were 4.14 eV, 3.99 eV,
moved to 365.8 cm−1 in the CNGF/GNP composites. The T2g (1) 3.88 eV, and 3.94 eV for CNGF, CNGF/2.5wt%GNP, CNGF/5wt%
peak assigned to the translational motion of the complete GNP, and CNGF/7.5wt%GNP, respectively. The Eg of the CNGF
tetrahedron (Fe–O4) was present at 316.8 cm−1 and moved to sample is the widest due to the interaction between the O2−p
314.5 cm−127,28 and Fe-3d energy states, resulting in orbital overlap, while the
change in energy bandgap is due to the insertion of GNP in the
3.2 Optical studies by UV-vis analysis host CNGF sample.
The optical transition nature and energy bandgap of the as-
prepared CNGF sample and CNGF/GNP composites were 3.3 I–V measurements analysis
measured by using the Tauc plot method. SFs and their The two-probe method was used to determine the DC resistivity
composites have a direct energy bandgap.29 The Tauc plot of the CNFG nanoparticles and CNGF-GNP (2.5%, 5%, and
equation is given as:26 (ahv)2 = K(hv − Eg), where “2” is for direct 7.5%) nanocomposites. The resultant measured resistivity
allowed transitions, the absorption coefficient (a) was deter- values of each given sample are summarized in Table 2. The
mined by employing the following equation:26 a = 2.303 log(A)/l, calculated resistivity of the integrated CNGF nanoparticle was
where A indicates the absorbance, and l is the path length of 2.44 × 109 U cm at room temperature. The general behavior of
light along which absorbance takes place, and the energy ferrite nanoparticles is more insulating, but they can conduct
bandgap (Eg) was calculated by extrapolating the linear part of due to the temperature dependency of the electrons, which

Table 2 The DC electrical resistance and resistivity of the CNFG nanoparticles and CNFG-GNP nanocomposites

Samples CNGF CNGF-GNP (2.5%) CNGF-GNP (5%) CNGF-GNP (7.5%)

Resistance (U) 1.36 × 109 5.85 × 107 1.23 × 108 4.41 × 107
Resistivity (U cm) 2.44 × 109 1.05 × 108 2.21 × 108 7.89 × 107

© 2023 The Author(s). Published by the Royal Society of Chemistry RSC Adv., 2023, 13, 34308–34321 | 34313
RSC Advances Paper

a specic temperature at which the log values show a trans-

formation; this is described as the Curie temperature or the
transition temperature and is denoted as (TC). This process or
mechanism also causes the transformation of magnetic colla-
tion from ferromagnetic to paramagnetic, thus forming two
distinct regions in the plots. It is worth noting here that the
region below TC is called the ferromagnetic region, whilst the
region above the TC is referred to as the paramagnetic region.31
On the contrary, the resistivity of graphene is poor, and
hence it is found to be a good conductor with a pristine surface
containing encapsulated sp2-hybridized carbon atoms inside
the hexagonal lattice with certain constraints. This is because of
the availability of functional groups like ethers, carboxyl, and
hydroxyls, which can react with atmospheric humidity to form
acids and other compounds. It is worth noting here that the
Fig. 6 Arrhenius plots of all the samples.
oxidation level has been shown to directly resist the electrical
properties of graphene nanoplatelets due to the quasi-ID active
bonding between the carbon sheets with a conducting nature
and the defects, according to the variable range hopping
causes the transfer of the electrons between the ferrous (Fe2+)
model.32 The temperature dependency of the resistivity of the
and ferric (Fe3+) ions at the octahedral B-lattice sites and
fabricated samples is shown in Fig. 7(a–c), which reveals that in
transfer of holes between the Ni2+ and Ni3+ ions.30 The log r vs.
the low-temperature range, the resistivity of CNGF increases
1000/T (Arrhenius plots) graphs are shown in Fig. 6 at different
with the increase in temperature, but in the medium- and high-
temperatures ranging from 313 K to 673 K. Based on the vari-
temperature ranges, resistivity increases when temperature
ation in the slope of the curve, the resistivity curve can be split
decreases, conrming the semiconducting nature of the
into two regions, namely the ferromagnetic region and para-
gadolinium-doped ferrites. The same trend is found when GNPs
magnetic region. The change in resistivity is in line with

Fig. 7 The temperature-dependent DC resistivity (rDC) of the CNGF nano particles and CNGF-graphene nanoplatelet composites in the (a) lower
temperature range (b) medium temperature range and (c) elevated temperature range.

34314 | RSC Adv., 2023, 13, 34308–34321 © 2023 The Author(s). Published by the Royal Society of Chemistry
Paper RSC Advances

Fig. 8 (a) Temperature versus the temperature coefficient of resistance percentage for all the samples; (b) T versus TCR% for each sample.

are added to CNGF but with less diversity.20 These reveal that in many applications, such as bolometric devices for microwave
lesser ferrite particles could get into the honeycomb or hexag- measurements, astronomy, and thermal cameras.27
onal structures of GNP, causing a rise in the density of func-
tional groups that act as charge carriers. Therefore, the 3.4 Dielectric studies
conductivity of graphene remains supreme, and the resistivity
The term permittivity or dielectric constant refers to the
of the composites deteriorates with different concentrations of
measure of capacitance observed during the formation of an
GNP, as shown in Fig. 7(a–c). The resistivity of the CNGF-GNP
electric eld.34 The electronic distribution of the synthesized
nanocomposites is less compared with the gadolinium-doped
samples was predicted by measuring their polarizations
cobalt nickel ferrite nanoparticles. It is, therefore, compre-
through dielectric analysis.20 The values of dielectric constant
hended that the CNGF-GNP composites have changed the
(3′) and dielectric constant loss (3′′) were plotted as functions log
resistivity of the ferrite nanoparticles, and they can be used in
of frequency (104 Hz to 107 Hz) at room temperature, as shown
the preparation of supercapacitors.33 TCR% is the percentage of
in Fig. 9(a) and (b), respectively. The dielectric constant and loss
the relative change in resistivity per degree temperature change.
initially decreased due to the reduction in the space charge
TCR is a valuable resistor performance stability indicator.
polarization effect. Then, it remained approximately constant.
TCR% is essential for estimating the relationship of resistivity
On the other hand, a high dielectric constant was observed at
with ambient temperature variations, both at low and high
low frequencies. This is because a potential barrier is created at
operating temperatures. TCR% is calculated from resistivity
the grain boundaries by space charge polarization. Subse-
using the formula:42 TCR (%) = [(1/r) × (dr/dT)] × 100%. The
quently, there is an accumulation of charge at the grain
TCR% values were calculated for all samples from 313 K to 673
boundary, resulting in an increase in the real and imaginary
K and plotted against temperature, as shown in Fig. 8(a). The
parts of the permittivity values. The dielectric dispersion can be
TCR% decreased rapidly with an increase in temperature both
explained by the dominance of the impact of grain boundaries
in the low-temperature range and high-temperature range, as
rather than the grains. Koop's phenomenological theory attri-
shown in Fig. 8(b). The CNGF sample without graphene nano-
butes this to the Maxwell–Wagner kind of interfacial polariza-
platelets showed the maximum value of 3.70 K−1 at a tempera-
tion. Both 3′ and 3′′ show maximum values when the frequency
ture of 313 K, while the composites with graphene nanoplatelets
is low because of interfacial and dipole polarization.35 The
showed lesser values at 313 K due to the carbon in graphene.
CNGF nanoparticles showed lower values of dielectric constant
The peak values of TCR% were −2.43% K−1 at 373 K, −2.62%
and dielectric constant loss, while the CNGF/GNP nano-
K−1 at 368 K, −2.71% K−1 at 341 K, and −2.45% K−1 at 368 K for
composites showed higher values of both at low frequencies,
CNGF, CNGF-GNP 2.5%, CNGF-GNP 5% and CNGF-GNP 7.5%
proving the graphene and ferrite interactions and the presence
respectively. Materials with temperature-dependent electrical
of better polarization due to graphene. Moreover, the CNGF/
resistance can be used as a source of radiant heat and are used
5wt%GNP nanocomposite exhibited higher values of the real

© 2023 The Author(s). Published by the Royal Society of Chemistry RSC Adv., 2023, 13, 34308–34321 | 34315
RSC Advances Paper

Fig. 9 The plots of (a) 3′ versus frequency, (b) 3′′ versus frequency, (c) tan d versus frequency, and (d) s ac versus frequency.

and imaginary parts of the dielectric constant than those of the resonance occurring at the domain wall is described by
CNGF nanoparticles. As the frequency was increased, the values calculating the dielectric loss tangent. The plot of tan d and
of 3′ and 3′' remained constant for all the samples. At higher frequency is shown in Fig. 9(c), indicating its dependency on
frequencies, due to fast variation in the applied eld, the the frequency i.e., at a higher frequency, the dielectric loss
dipoles cannot follow the exact variation speedily, and the tangent has the lowest value.32 One of the characteristics of
response of the permanent dipoles along with the contribution nanocomposites is that, with a change in frequency, the ac
of charge carriers decreases, leading to a decrease in the conductivity changes, as noticed in Fig. 9(d), and this behavior
dielectric constants. Graphene enhances the dielectric constant can be well-explained by Koop's theory, according to which
at lower frequencies, making it a signicant factor in the conductivity shows variation/dispersion in the higher
development of high-temperature ceramic supercapacitors.36 frequency range (>105 Hz). At room temperature, transitions
The values of dielectric constant and dielectric constant loss between Fe2+ to Fe3+ at the B-site increase (a hopping mecha-
increased when graphene nanoparticles were added.37 In CNGF, nism) and lessen the effect of oxygen ions, thus forming well-
the net polarization is due to two types of charges: (1) due to conducting grains and poor-conducting grain boundaries.40
electron transfer at the octahedral site between Fe2+ and Fe3+, Firstly, the presence of multiple interfaces between the gra-
and (2) due to p-type charge carriers, namely Ni3+/Ni2+ and Co3+/ phene nanoplatelets and the modied magnetic materials
Co2+, at the B-site. At higher frequencies, the dielectric constant leads to increased interfacial polarization and the subsequent
is not dependent on the frequency, so polarization remains relaxation process. This phenomenon contributes to the
unchanged at these frequencies; this shows that polarization enhancement of dielectric loss. Moreover, recent research
depends on the variation in the frequency range. Moreover, due ndings indicate that charges can be transferred across the
to the insertion of doped ferrites into graphene nanoplatelets, interface of a graphene-ferrite heterostructure due to the
an interface is produced, and charges accumulate at this distinct physical properties of these materials. Hence, in this
interface with different relaxation times when current is passed study, it is reasonable to expect a charge transfer process to
through the sample, which can be well-described by the take place at the interface between the GNPs and the CNGF
Maxwell–Wagner (MW) effect.38 sample. This would result in the introduction of free carriers
The dielectric loss tangent (tan d = 3′′/3′) illustrates its from ferrite into graphene, leading to electric polarization in
dependence on the energy dissipation frequency.39 Energy the as-prepared composites. This process signicantly
dissipation in the samples due to conduction (electrical) and contributes to the increase in dielectric loss.41

34316 | RSC Adv., 2023, 13, 34308–34321 © 2023 The Author(s). Published by the Royal Society of Chemistry
Paper RSC Advances

The electrical performance of the synthesized sample was

calculated by studying the Q factor as a function of frequency.
As the Q factor reveals the association of stored energy with
waste (thermal) energy, it is useful to describe the efficiency of
the material in terms of storing energy. The Q factor versus
frequency graphs of all samples are shown in Fig. 10, which
clearly demonstrate that the samples with graphene nano-
platelets have lower values of Q-factor than CNGF. The Q factor
values increase as the frequency increases due to the AC
frequency and skin effect.42
The samples were also analyzed by studying complex
impedance, which in turn constitutes a real Z′ and an imaginary
part Z′′ and measures the opposition caused by the material
when current is passed through it. Fig. 11 shows the variation in
Z′ with frequency for all four samples: without (CNGF) and with
graphene (CNGF-GNP 2.5%, 5%, and 7%). All the curves show
high impedance at low frequencies; the values decrease when Fig. 11 The variation of the real part of complex impedance with
frequency.
the frequency is increased up to 107 Hz, and then the imped-
ance remains at a constant value even when the frequency is
increased further. The high value of impedance at low and then reaching stability at high values of frequency; this is in
frequencies is due to high dipole polarization and interfacial agreement with the fact that polarization is compatible at low
polarization, which in turn are due to the grain boundaries frequencies but lags at high frequencies, and thus due to the
present in the crystal structure and electrode contribution, transfer of electrons, conduction is possible at high
respectively. CNGF had the maximum impedance, while the frequencies.
CNGF-graphene nanocomposites showed lesser values, which The physical interpretation of the imaginary part is repre-
reveals that the crystal grain boundary defects are lessened due sented as the energy storage component, and the results
to the addition of graphene. Further, the XRD results prove the revealed that graphene-added composites had higher values for
reduction in crystal size due to graphene, and hence the CNGF- the imaginary part of impedance than the bare spinel ferrite.
GNP nanocomposites have low impedance.43 The relationship between the imaginary parts and real parts of
When the frequency is increased, the effect of dipole polar- impedance was plotted based on the Nyquist theorem. All the
ization and space charge participation reduces due to their curves showed incomplete semi-circles, thus demonstrating
inability to respond at these high frequencies; thus, impedance dependence on one dielectric relaxation (Fig. 13(a–d)).
decreases, leading to a constant value at which conduction
becomes prominent due to the hopping of electrons. The 3.5 Magnetic studies
imaginary part of the impedance is plotted against frequency
Experimental evidence demonstrates that pure CNGF exhibits
for all the prepared samples in Fig. 12, which shows high values
characteristic so ferromagnetic behavior, accompanied by
at low frequencies, a decrease in value as the frequency rises,
a small coercivity.44 To investigate the effect of GNP on the
magnetic properties of the CNGF sample, the magnetization

Fig. 12The variation of the imaginary part of complex impedance with

Fig. 10 Q factor variation versus frequency. frequency.

© 2023 The Author(s). Published by the Royal Society of Chemistry RSC Adv., 2023, 13, 34308–34321 | 34317
RSC Advances Paper

Fig. 13 Nyquist plots showing the variations between the imaginary and real parts of the impedance of the (a) CNGF nanoparticles, (b) CNGF-
GNP 2.5% composites, (c) CNGF-GNP 5% composites, and (d) CNGF-GNP 7.5% composites.

versus applied eld (M–H) loops were recorded at room GNPs nanocomposites are reduced due to the formation of
temperature, as shown in Fig. 14. It is clear from Fig. 14 that the a domain.45 The combined magnetization graphs of the
saturation magnetization (MS) of the CNGF sample was the samples plotted against the applied eld are shown in Fig. 14.
greatest, while it decreased with the insertion of GNP in the The trends of Ms and Mr are shown in Fig. 15. The values of
CNGF sample, indicating that GNP has poor ferromagnetic maximum saturation magnetization, remanence, squareness
properties, while ferrites are good, and their combination ratio, and coercivity are tabulated in Table 3. The Hc values are
results in weak magnetization due to the formation of a single also shown in Table 3, which reveals the maximum value for
domain rather than domain walls. Furthermore, it has also graphene, while the minimum value was recorded for the CNGF
been observed from the XRD analysis that the sizes of CNGF- nanoparticles. Coercivity values depend on anisotropy, and

Fig. 14 The M–H loops for all the as-prepared composites. Fig. 15 Variation in the Hc and SQ ratios versus the samples.

34318 | RSC Adv., 2023, 13, 34308–34321 © 2023 The Author(s). Published by the Royal Society of Chemistry
Paper RSC Advances

Table 3 The magnetic parameters of the CNFG nanoparticles and CNFG-GNP nanocomposites

Parameters CNGF CNGF/2.5wt%GNP CNGF/5wt%GNP CNGF/7.5wt%GNP

MS (emu g−1) 119.8 110.5 110 116.3

Mr (emu g−1) 43.3 60 60 61.3
HC (Oe) 361.1 784 805 657
K (erg cm−3) 45 062 90 241.6 92 239.5 76 409.1
SQ 0.36 0.54 0.55 0.53

hence, the magneto-crystalline anisotropic parameters K were Ni0.5 Fe2−xGdxO4-GnP can be tuned by adjusting the ratio of
calculated by using Ms and Hc and are tabulated in Table 3. The GNPs. Such graphene-based spinel ferrites can be used in
CNGF nanoparticles had the minimum anisotropic constant semiconductor applications, such as spintronics.47
value, while it was increased for the samples with GNPs. The
change in coercivity value is due to the change in magneto- 4. Conclusion
crystalline anisotropy as a consequence of the material added in
the Nickel ferrites to replace the Ni ions at the octahedral sites.45 The structural, dielectric, electrical, optical, and magnetic
The squareness ratio was calculated for each sample, as tabu- properties of CNGF nanoparticles and changes in these prop-
lated in Table 3. Moreover, the squareness ratio and coercivity erties due to graphene nanoplatelets are reported in this study
values of the samples are plotted in Fig. 16. by fabricating CNGF-GNP nanocomposites with varying GNP
The saturation magnetization decreased when GNPs were concentrations via a sol–gel auto-combustion route. It was
added to the spinel ferrites. It was also obvious that an increase observed that crystalline size D decreased from 40.1817 nm to
in the GNP ratio led to an increase in the Ms value of the CNGF- 28.76267 nm due to the addition of the graphene nanoplatelets,
GNP nanocomposites, while the anisotropic constant increased besides providing the conrmation of GNP in the crystal
when GNPs were added. A further change in the weight ratio of structure. The SEM images revealed that samples with graphene
GNPs led to a decrease in K values. Previous studies have were thicker than CNGF. The Raman spectra also showed the
revealed that graphene has a diamagnetic nature, so its substitution of GNPs in the CNGF lattice. The TCR% decreased
momentum is in the opposite direction to the applied external rapidly with an increase in temperature both in the low-
magnetic eld. However, our present ndings show that the temperature range and high-temperature range; moreover, the
CNGF-GNP nanocomposites have different magnetic behavior peak values of TCR% were −2.43% K−1 at 373 K, −2.62% K−1 at
from that of their constituents i.e., spinel ferrites, which are 368 K, −2.71% K−1 at 341 K and −2.45% K−1 at 368 K for CNGF,
ferromagnetic, and graphene, which is diamagnetic. Therefore, CNGF-GNP 2.5%, CNGF-GNP 5wt% and CNGF-GNP 7.5wt%,
it can be hypothesized that in the presence of an applied respectively. With the change in frequency, the variations in
external eld, the exchange coupling phenomenon exists permittivity and conductivity were observed. Moreover, at
between them due to which the synthesized neoteric nano- higher frequencies, the external alternating eld vibrated so
composites have wide and shied hysteresis loops as the rapidly that the dipole of the materials remained stationary
momentums of CNGF and GNPs interact.46 Hence, it can be giving no polarization, while the 3′′ intercept presented a higher
stated that the CNGF nanoparticles attached to the layers of value at low frequencies due to the addition of the graphene
GNPs act as functionalizing agents. Accordingly, it can be nanoplatelets, which provided more ions to jump in the direc-
concluded that the magnetic properties of as-prepared Co0.5 tion of the eld at low frequencies. CNGF had the maximum
impedance, while the CNGF-GNPs nanocomposites showed
lower values. The saturation magnetization (Ms) value of the
CNGF nanoparticles was higher, while it decreased when gra-
phene nanoplatelets were added, reaching the minima when
GNP was at 2.5% and 5%. Meanwhile, the squareness ratio
increased from 0.36 for CNGF to 0.55 for the GNGF-GNP
nanocomposites.

Conflicts of interest
There are no conicts to declare.

Acknowledgements
The authors extend their appreciation to the Deanship of
Scientic Research at King Khalid University, Abha, Saudi Ara-
bia, for funding this work through the Research Groups
Fig. 16 The Ms and Mr trend of the samples. Program, under grant no. RGP.2-259-44.

© 2023 The Author(s). Published by the Royal Society of Chemistry RSC Adv., 2023, 13, 34308–34321 | 34319
RSC Advances Paper

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