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Unique perforated graphene derived from

Cite this: Nanoscale, 2017, 9, 4801
Bougainvillea flowers for high-power
supercapacitors: a green approach†
Rajendra P. Panmand, a Purnima Patil,a Yogesh Sethi,a Sunil R. Kadam,a
Milind V. Kulkarni,a Suresh W. Gosavi,b N. R. Munirathnama and Bharat B. Kale*a

Received 24th January 2017,
Accepted 10th March 2017
DOI: 10.1039/c7nr00583k
rsc.li/nanoscale
Herein, we demonstrated a green approach for the synthesis of high surface area (850 m2 g−1) meso-
porous perforated graphene (PG) from Bougainvillea flower for the first time using a template free single-
step method. The existence of PG was confirmed by XRD, Raman spectroscopy, FESEM, and FETEM.
Surprisingly, FETEM clearly showed 5–10 nm perforation on the graphene sheets. More significantly, these
mesoporous perforated graphene sheets can be produced in large scale using the present green
approach. Considering high surface area and unique perforated graphene architecture, these PGs were
studied for supercapacitor applications in detail without any chemical or physical activation. The nano-
porosity and high conductivity of PG derived from Bougainvillea flower exhibited excellent supercapacitive
performance. According to the supercapacitor study, the synthesized perforated graphene sheets
conferred a very high specific capacitance of 458 F g−1 and an energy density of 63.7 Wh kg−1 at the
power density of around 273.2 Wh kg−1 in aqueous 1 M Na2SO4. Significantly, the areal capacitance of PG
was observed to be very high, i.e. 67.2 mF cm−2. The cyclability study results showed excellent stability of
synthesized perforated graphene sheets up to 10 000 cycles. Note that the specific and areal capacitance
and the energy density of the synthesized PGs are much higher than the earlier reported values. The high
supercapacitive performance may be due to high surface area and mesoporosity of PG. The present
approach has a good potential to produce cheaper and high surface area PG. These PGs are good candi-
dates as an anode material in the lithium-ion battery.

1. Introduction with trace amounts of other elements. If this natural waste is

The waste from natural sources is becoming a critical issue
because of its direct combustion (conventional process) to
hazardous gases. In particular, horticulture and gardening
waste management issues have always been a big problem
worldwide. Typically, in India and in other Asian countries, a
large amount of flowers is used for religious worship
(Nirmalyam) as well as for other special functions. Used
flowers are just dumped in the reservoirs of water, such as
lakes and rivers, or burnt, producing ash and hazardous
gaseous pollution products that ultimately creates environ-
mental problem. This waste is a rich source of carbon along
a
Centre for Materials for Electronics Technology (C-MET), Ministry of Electronics and
Information and Technology (MeitY), Government of India, Panchawati off
Pashanroad, Pune-411008, India. E-mail: bbkale@cmet.gov.in, bbkale1@gmail.com
b
Departments of Physics, Savitribai Phule Pune University, Pune-411 007, India
† Electronic supplementary information (ESI) available. See DOI: 10.1039/
c7nr00583k
used to synthesize functional energy storage materials such as
active carbon, it will be a great achievement for the production
of value-added products using natural waste. The conducting
carbon is a well-known anode material for energy storage
devices. Hence, to curtail the environmental problems, use of
natural gardening waste is the best approach and has been
envisaged in the form of active conducting carbon.
The fabrication of energy storage devices (ESDs) is attract-
ing the attention of investigators due to the environmental
problems and limited availability of fossils fuels as well as the
need of efficient storage of solar and wind energy.1,2 Due to
the up growing demand of electronic devices and hybrid elec-
tric vehicles, there has been great urgency for energy storage
devices of high energy and power densities. Among the various
ESDs, supercapacitors or electrochemical capacitors have been
broadly projected in recent years because of their higher
energy density than commercial capacitors and larger power
density and better chemical stability than batteries after thou-
sands of cycles (>105).3 The present commercial super-

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Paper
capacitors were designed based on electrochemical double-
layered capacitors (EDLCs). The EDLCs store energy through
the adsorption of both anions and cations of the electrolyte at
the interface between the electrode and the electrolyte.
Nowadays, the scientific community is motivated to consider-
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ably improve the energy and power density of supercapacitors
by developing new electrode materials. For the fabrication of
electrodes of EDLCs, carbon materials have been extensively
studied as an electrode material due to its eco-friendly nature,
easy availability, high surface area, and moderate cost.4–7
However, commercially available carbon materials have some
limitations as supercapacitor materials due to their low con-
ductivity, low ion-transport, and insufficient ionic diffusion
within the complex micropores; hence, high energy and power
density cannot be achieved. Presently, activated carbon is pro-
duced using diminishing natural products such as petroleum
coke, pitch, and coal.8,9 Recent studies on carbon-based super-
capacitors concluded that micro and mesoporous nanocarbon
produces excellent supercapacitor results.10,11 Hence, there is
an urgent need to explore novel two and three-dimensional
nanostructured porous carbon materials for high performance
supercapacitors. To improve the properties of carbon-based
electrodes, highly porous morphologies should be developed.
In view of this, as activated carbons,12 templated carbons,13
carbon nanofibers,14 carbon nanotubes,15 carbide-derived
carbon16 and graphene17 have been extensively studied. The
activated carbon and nanoporous carbon has an advantage in
the controllable synthesis and acceptable properties.18
However, the poor conductivity and abundant micropores in
activated carbons are a hurdle for ion and electron transport,
which deteriorate capacitance performance at high current
rates.19 Carbon nanotubes have good electric conductivity and
unique pore channels, alleviating ion diffusion and charge
propagation; however, they have poor surface area that affects
the resulting capacitive performance of the supercapacitor.20
To improve the capacitive performance of the carbon-based
EDLC, the dispute between their specific surface area and elec-
tric conductivity should be balanced. In view of this, graphene
has attracted significant interest as an electrode material for
supercapacitors because of the large surface area and porous
layered structure. This will also confer the good conductivity of
the electrode, which can provide low-resistant pathways for
electron transport.21,22
Herein, natural waste was utilized for the synthesis of active
electrode materials for supercapacitors. Activated carbons can
be typically prepared by the carbonization of easily available
natural biomass wastes.23,24 The synthesis of porous carbon
from natural waste has received wide attention. Waste
materials such as waste coffee grounds,25 cow dung,26 human
hair,27 a tea-leaf,28 peat moss,29 and fruit shells and seeds30,31
have been extensively employed as raw materials for carboniz-
ation to synthesize porous carbons as active electrode
materials in supercapacitors. Nitrogen and oxygen-activated
carbon materials were also synthesized via carbonization of
these natural raw materials. The supercapacitance for carbon
as an electrode material derived from the horticulture waste
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has been achieved up to 400 F g−1 at 0.5 A g−1 in 1 M aqueous
H2SO4 as an electrolyte,4 whereas the supercapacitance for
carbon as an electrode material derived from the animal waste
has been achieved up to 349 F g−1 at 1 A g−1 in 1 M aqueous
H2SO4 as an electrolyte.32 Beside natural waste, scientists have
also focused their attention on the manmade waste manage-
ment through the production of value-added products.
Activated carbon has also been synthesized using carboniz-
ation of the scraped tires, plastic etc. This carbon material
exhibits a super capacitance of 100 F g−1 at 10 A g−1 in 6 M
KOH aqueous solution.33,34 Considering the demand for
energy storage devices, there is enormous scope to increase
the efficiency of these devices by developing new carbon
materials with a high surface area as well as to investigate new
sources of activated carbon via waste management. Carbon
materials such as graphene has a high theoretical surface area,
substantially higher than the more common electrode active
material, activated carbon, thus potentially allowing the
storage of more electrostatic charge.35,36 However, it is very
difficult to synthesize these 2D graphene materials with a con-
trolled morphology, structure, and property. It is urgent task to
identify a method to develop these 2D graphene-like materials
for supercapacitor applications. Graphene has been produced
by the reduction of graphene oxide (GO) prepared by the
Hummers and Offeman method37 and other modified
methods.38 Graphene materials have been extensively used for
EDLC supercapacitors; however, the maximum capacitance
was observed to be 250 F g−1.39 Very few reports are available
on the synthesis of perforated graphene from biomass.
Perforated graphene has been synthesized using cost-effective
routes from renewable biomass waste such as waste food
items, dead insects, etc.40 Today, the economics of super-
capacitor is totally dependent on the cost of carbon. It is
possible to achieve high porous perforated graphene using
natural waste (free source) at lower cost, which ultimately
reduces the cost of supercapacitors. Hence, we demonstrated
the preparation of mesoporous perforated graphene using
dead waste Bougainvillea flowers for supercapacitors for the
first time.
In the present investigation, perforated graphene was syn-
thesized by the one-step carbonization of dead Bougainvillea
flower (natural waste) without any chemical or physical acti-
vation. Further, their supercapacitive performance was tested.
A detailed study of the synthesis of mesoporous perforated gra-
phene materials derived from dead flowers of boganvel
(Bougainvillea) was performed. To the best of our knowledge,
there are no reports on the synthesis of high surface area
mesoporous perforated graphene from waste dead flowers.
Using mesoporous perforated graphene derived from the dead
flowers, we achieved a specific capacitance of 458 F g−1 and a
very high energy density of 63.7 Wh kg−1 at the current density
of 2.28 A g−1. These superior properties may be due to the
high surface area and high conductivity of the carbon material.
These properties are superior to those of the commercially
available material as well as other materials reported in the
literature.
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2. Experimental
2.1. Materials
Boganvel (Bougainvillea) dead flowers (waste) from farms
and gardens were used. AR grade sodium sulfate (Na2SO4),
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N-methyl-2-pyrrolidone (NMP), and PVDF ( polyvinylidene
fluoride) were purchased from a reputed source.
2.2. Synthesis of perforated graphene (PG) driven from
dead flowers
The dead boganvel flowers were obtained in large quantity,
thoroughly washed, and dried at 80 °C in an oven. The dried
flowers were crushed to a fine powder. For the synthesis of per-
forated graphene, 10 g boganvel flower powder was pyrolyzed
in a quartz crucible at 600 °C and 800 °C for 5 hours in an
argon atmosphere at the heating rate of 10 °C min−1 and the
samples were marked as RC-A and RC-B, respectively. Fig. 1
shows the process algorithm used for the synthesis of perfo-
rated graphene from dead flower powder and subsequent
supercapacitor measurements.
2.3. Characterization
Perforated graphene synthesized from the abovementioned
dead flowers was characterized by X-ray Powder Diffraction
(XRD) using a Bruker Advanced D8 diffractometer. Raman
spectroscopy using a LabRAM HR800 from JY Horiba and high-
resolution transmission electron microscopy (HRTEM) were
carried out (IFEI, Tecnai F30, FEG with 200 kV). The surface
area of the samples was determined using the Brunauer–
Emmett–Teller (BET) adsorption method (Quantachrome
NovaWin ©1994–2012). Cyclic voltammetry measurements
were performed by Auto Lab (model PGSTAT 30, eco-chemie).
2.4. Electrochemical measurements
The electrodes for electrochemical analysis were prepared on
carbon paper. Two carbon paper substrates with a similar area
Fig. 1 Methodology for the synthesis of perforated graphene from
dead flowers.
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were used for each measurement. Perforated graphene was
loaded on the substrate using the following procedure. Herein,
80 wt% boganvel flower-derived perforated graphene (PG) was
mixed with 10 wt% conducting carbon (acetylene black) and
10 wt% PVDF binder. To the abovementioned mixture, 5–8
drops of NMP were added and thoroughly ground to make a
viscous slurry. This slurry was coated on the carbon paper sub-
strate area. The loaded electrodes were dried at 100 °C for
6 hours. Electrochemical cyclic voltammetry was performed
in an aqueous 1 M Na2SO4 solution in the potential range of
0–1 V at various scan rates.
2.5. Electrochemical impedance spectroscopy measurements
Electrochemical impedance spectroscopy (EIS) was performed
for a symmetrical supercapacitor cell consisting of the bogan-
vel (Bougainvillea) flower-derived PG-PG electrodes in aqueous
1 M Na2SO4 electrolytes. The frequency range used for the
study was from 10 kHz to 10 mHz and an AC amplitude of
10 mV without an external DC applied voltage was utilized.
3. Results and discussion
Generally, the dry or dead flowers consist of flavonoids, gluco-
sides, sugar esters, terpenoids, sterides, and anthraquinones
enwrapped in the thin petal of the flower and these are a rich
source of carbon.41 A pyrolysis treatment can convert these
organic components into carbon. The formation of PG from
flower is given in Scheme 1. In addition to these organic com-
ponents, traces of Ca and Mg are also present, which have
already been reported as porogens to create pores in activated
carbon.4 After carbonization, thin petals of the flower were
directly converted into graphene and elements such as Ca and
Mg were helpful for the generation of porosity after leaching.
Indeed, PG has been prepared without any graphitic catalyst or
activation agent, as reported earlier.42,43
The TGA results are shown in Fig. S1 (see ESI-I†). In the
TGA curve, the weight loss (2.23%) from room temperature to
200 °C was attributed to dehydration/water loss from the
surface and pores of the powder of dead flowers. From 200 to
450 °C, 48% weight loss was observed, which was attributed to
the degradation of cellulose. Further, there is the possibility of
degradation of lignin between 450 and 800 °C by further
extending the temperature, giving a total weight loss ∼60%.
The as-synthesized PG (RC-A and RC-B) was characterized
by XRD. Fig. 2a shows the XRD pattern of the samples RC-A
Scheme 1 Schematic for the formation of PG.
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Fig. 2 XRD pattern (a) and Raman spectra (b) of RC-A and RC-B.

and RC-B. The presence of the characteristic graphitic peaks at

around 26 and 43.8° in the XRD pattern confirms the existence
of graphene sheets. These two diffractions peaks correspond Fig. 3 XPS spectra of C 1s RC-B.
to the (2 0 0) and (1 0 0) planes, which show a turbostratic
structure after pyrolysis. The XRD pattern of the prepared per-
forated graphene matches the recently reported XRD pattern of Physical nature of the nanoporous material was analysed by
reduced graphene.44 The broad peaks indicate the presence of FESEM and FETEM. The FESEM and FETEM images of RC-B
a few layers of graphene. Further confirmation of the gra- are shown in Fig. 4. The FE-SEM images of perforated gra-
phene-like structure was achieved by Raman spectroscopy. phene derived from dead flowers are shown in Fig. 4a. It can
Raman spectroscopy is a unique tool to analyse PG. Raman be clearly seen that the sheets are very thin (few nm in thick-
spectra for the samples RC-A and RC-B are shown in Fig. 2b. ness) and quite comparable in the case of reported chemically
Fig. 2b shows peaks at 1320 cm−1 and 1590 cm−1, corres- reduced graphene oxides.54,55 The sheets have fairly large
ponding to the characteristic D and G bands of graphene, areas and are quite separated like the reported sheets. FETEM
respectively. The defect or disorder-induced band (D: images (Fig. 4b and c) show an ultrathin sheet-like morphology
1320 cm−1) appeared due to the breathing mode of the k-point with an areal size in the range of few hundreds of square nano-
phonons of A1g symmetry and the graphitic band (G: metres, whereas Fig. 4d clearly shows the perforated nature of
1580 cm−1) is attributed to graphite in-plane vibrations of sp2 the PG sheets with 5–10 nm perforation. Fig. S2 in the ESI†
carbon atoms with E2g symmetry.45,46 The very weak 2D band shows the graphitic character (d spacing equal to 0.38 nm).
observed at ∼2700 cm−1 in the case of both samples is broader This perforated nature may assist in enhancing the supercapa-
as compared to that of the standard graphite 2D band, which citive performance.
matches the results of recently reported reduced graphene
oxide.47,48 XRD and Raman spectroscopy showed that prepared
materials are perforated graphene.
It has been reported that the intensity ratio of these two
bands (D band: G band) partially depends on the order of gra-
phitization. The ratio of ID/IG for RC-B is about 1.66, which is
higher than that of RC-A (1.50). The increased intensity ratio
with the pyrolysis temperature suggests that PG is significantly
disordered due to the presence of an imperfect or turbostratic
carbon structure.49 The turbostratic crystallite structure is the
more porous intermediate stage between amorphous carbon
and graphene.
X-ray photoelectron spectroscopy (XPS) was used to charac-
terize the elemental composition of PG. As shown in Fig. 3,
deconvolution of the XPS spectrum of PG shows a sharp C 1s
peak at 284.54 eV, which is mainly due to the sp2 carbon of
graphene. There is a weak shoulder peak from around 286 to
288 eV in the PG C 1s spectrum, indicating that there are still
oxygen-containing groups on PG in the form of typically
epoxide, hydroxyl, and carboxyl groups.50,51 The XPS results
obtained herein are in good agreement with those of previous
reports, which justifies the formation of graphene.52,53 Fig. 4 FE-SEM (a) and FE-TEM (b–d) images of the RC-B.

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Nitrogen physisorption was performed to analyze the poro-
sity of perforated graphene derived from dead flowers (RC-A
and RC-B). Fig. 5a and b show the BET nitrogen adsorption–
desorption isotherm of the CDDF material at 77.4 K. The nitro-
gen physisorption data exhibits the characteristic of type-IV
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isotherms with a distinct hysteresis loop of type H2 in the P/P0
range of 0.4–1.0. This result implies the presence of relatively
large cavities that are not well interconnected in the frame-
works (Fig. 5a and b). The BET surface area for RC-A and RC-B
is around 598 and 850 m2 g−1, respectively. The pore size dis-
tribution indicates the hierarchical pore structure of both RC-A
and RC-B with both nano (1–2 nm) and mesopores (5–10 nm).
The high surface area compounded with a bimodal size distri-
bution comprisingmicropores and mesopores is interesting in
a supercapacitor application point of view, which has been
discussed.
The conductivity of the sample is also an important para-
meter for supercapacitor devices. The conductivity of RC-A and
RC-B was estimated using a cell, as shown in the inset of
Fig. 6. All the conductivity measurements were carried out
under an applied fixed and measured pressure (70.1 kg cm−2).
The schematic of the measurement process is depicted in
Fig. S3,† where 1 g of perforated graphene powder was placed
in a cell and a constant pressure was applied. Under the con-
stant pressure, the resistance was measured and the resistivity
was calculated, as shown in Fig. 6. From Fig. 6, it was observed
that resistivity rapidly decreases with the increasing pyrolysis
temperature. The resistivity of samples RC-A and RC-B were
19.03 and 13.92 Ω cm, respectively. From the measurements, it
is clear that graphene synthesized at 800 °C (RC-B) is highly
conducting in nature.
The electrochemical properties of RC-A and RC-B were
measured to evaluate the performance of the synthesized
materials in the perspective of a supercapacitor device in
aqueous media (1 M Na2SO4 solution as an electrolyte) and the
Fig. 5 N2 adsorption-desorption isotherm for a: RC-B and b: RC-A.
Inset shows the corresponding pore size distribution.
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Fig. 6 Resistivity of RC-A and RC-B.
corresponding results are summarized in Fig. 7. As shown in
Fig. 7a and b, a nearly perfect rectangular-shaped loop was
obtained at the sweep rates of 10, 25, 50, and 100 mV s−1 and
in the potential range from 0 to 1 V without any redox peaks.
The CV loops of RC-A and RC-B exhibited almost a rectangular
shape at different scan rates, indicating a typical double-layer
capacitor formation. From Fig. 7a and b, it can be observed
that all the CV curves are symmetric and rectangular in shape
even at the scan rate of 100 mV s−1, which indicates that the
PG-based electrodes have ideal charge propagation and low
internal resistance.56,57 The specific capacitance of the electro-
des was calculated from the galvanostatic charge–discharge
values using the following formula:
2I
Csp ¼ ð1Þ
dv
m
dt
where Csp is the specific capacitance of a single electrode in F
g−1, I is the discharge current in A, m is the mass of the active
materials in g, and dv/dt is the slope obtained from the dis-
charge curve. The typical galvanostatic charge–discharge
curves were obtained at 2.28, 3.33, 4.66, and 5.82 A g−1 current
densities (Fig. 7c and d). The RC-A and RC-B samples reveal
the charge–discharge curves with nearly isosceles triangular
shapes with a slight IR drop at low current densities, which
indicates the ideal EDLC nature of the device.
The specific capacitance was calculated at different current
densities ranging from 2.28 to 5.82 A g−1, as shown in Fig. 7c
and d (Table 1). At the current density of 2.28 A g−1, highest
specific capacitance i.e. 316 and 458 F g−1, was obtained for
RC-A and RC-B, respectively. The specific capacitance
decreased with the increasing current density, which is due to
the limited diffusion of ions on the electrode surface because
of fast charging. Hence, a relatively low capacitance was
obtained at a high current density than at a low current
density.
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notably high areal capacitance i.e. 67 mF cm2 (Table 1) as com-

pared to those of other natural waste-driven carbon-based elec-
trode materials used for supercapacitor.
There are few reports on the supercapacitor performance of
microporous carbon and graphene58,59 derived from natural
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waste with and without any activation. The comparative data

has been presented in Table 2 and Table S1 of the ESI.† Both
the Table 2 and Table S1† undoubtedly show excellent super-
capacitor performance of the boganvel flower-derived carbon
than those of other natural waste material-derived carbon. The
stable performance of the electrode material was confirmed by
repeating the charge–discharge study up to 10 000 cycles at
5.81 A g−1 (Fig. 8). The cyclic performance of RC-B (Fig. 8) indi-
cates stable specific capacitance (up to 93%) for RC-B after
10 000 cycles, indicating the good stability of material and
excellent ion accessibility in porous perforated graphene
during long term cyclability. A double-layer supercapacitor fab-
Fig. 7 Cyclic voltammetry (CV) loops of (a) RC-A and (b) RC-B at ricated using RC-B samples produced an excellent bright glow
different scan rates in aqueous 1 M Na2SO4. Galvanostatic charge– of an LED for 1 min (see Fig. S5 of ESI V†).
discharge curves of (c) RC-A and (d) RC-B in aqueous 1 M Na2SO4 and at For energy storage devices, it is essential to know the
different current densities.
energy and power densities. The energy density (E) and power
density (P) were calculated by the following equations:
1
E ¼ Csp ðΔVÞ2 ð3Þ
Table 1 Specific capacitance, areal capacitance, power densities, and 2
energy densities of the RC-A and RC-B samples at different current
E
densities P¼ ð4Þ
tdis
Current density (A g−1)
where Csp is the specific capacitance of the active material, t is
Measurements Sample 2.28 3.33 4.66 5.82 the discharging time, and ΔV is the potential window in 1 M
Na2SO4 for charging and discharging. For different current
Specific capacitance (F g−1)RC-A 316.2 140.7 75.9 41.3
RC-B 458.3 391.1 178.5 105.8 densities, energy density, power density, and specific capaci-
Areal capacitance (mF cm−2) RC-A 57.0 34.2 23.0 16.2 tance for carbon pyrolyzed at 600 and 800 °C is presented in
RC-B 37.2 39.0 25.6 18.0 Table 1. Note that at 2.58 Ag−1, RC-B shows an excellent
Energy density (Wh kg−1) RC-A 43.9 19.5 10.5 5.7
RC-B 63.7 54.3 24.8 14.6 energy and power density i.e. 63.7 Wh kg−1 and 273.2 W kg−1,
Power density (W kg−1) RC-A 1126 1628 2108 2870 respectively. It also shows that the energy density increases
RC-B 273.2 3878 4960 7300 with the decreasing current density. At high current density,
very fast discharge occurs because very few pores at the surface
are accessed by ions of the electrolyte, whereas at low current
For the electrolytic double-layer capacitor, areal capacitance density, all the pores are used by the electrolyte, which exhibits
is one of the important parameters in supercapacitor devices. slower discharge. The energy and power densities of the
The areal capacitance was calculated using the following carbon derived from dead flowers (see Table 1) are much
equation: higher than those for other carbon materials synthesized from
natural waste (see Table 2 and Table S1†).
2I
CA ¼ ð2Þ The relationship between the energy density and power
dv
A density i.e. Ragone plot, for both RC-A and RC-B is shown
dt in Fig. 9. It also shows that the highest energy density of
where A is the area of the supercapacitor device. In the present 63.7 Wh kg−1 can be achieved for RC-B at the power density of
case, the area of the device is about 3 cm2. The study shows a 273.2 W kg−1 and retains 14.6 Wh kg−1 at 7300 W kg−1, which

Table 2 Comparison of the properties of graphene synthesized from natural waste and their supercapacitance and energy density

Natural waste material Maximum capacitance (F g−1) Electrolyte Energy density (Wh kg−1) Ref.
−1 −1
Coconate [Editor33]shell 268 at 1.0 A g 6 M KOH 54.7 at 10 000 W kg 42
Fungus 374 at 1.0 A g−1 6 M KOH 22 at 784 W kg−1 43
Bougainvillea flower 458 at 2.28 A g−1 1 M Na2SO4 63.7 at 273.2 W kg−1 Present work

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Fig. 8 Cycling stability performance at the current density of 5.81 A g−1.
Fig. 9 Ragone plot for carbon derived from dead flowers ( plot of
energy density vs. power density).
is higher than that of recently reported carbon–carbon
symmetric supercapacitors in an aqueous electrolyte (see
Table 1).12,59–64 These results show that the synthesized RC-B
may be a superior electrode material for high power and cost-
effective supercapacitors.
Electrochemical impedance spectroscopy (EIS) is significant
tool to examine the conductivity of electrode materials.65 The
typical Nyquist plot for RC-B in 1 M Na2SO4 for the frequency
range from 10 kHz to 10 mHz is shown in Fig. 10a. It clearly
demonstrates an almost vertical straight line parallel to the
imaginary impedance axis (Z″) at a low frequency region, indi-
cating typical EDLC behaviour. In the middle frequency
region, the curve is a straight line, which indicates the
diffusion of the ions of the electrolyte through the porous
network of the electrode.66,67 The semicircle in the magnified
high frequency region is shown in Fig. 10a, which represents
the charge transfer resistance due to the electroactive surface
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Fig. 10 (a) Nyquist plot for RC-B in 1 M Na2SO4, and the inset shows
the magnified higher frequency region. (b) Plot of the Bode phase angle
(circle) and plot of the total impedance vs. frequency with frequency
(square).
area of the electrodes.68 We identified the equivalent circuit
using the NOVA 1.11 software. The circuit was composed of an
equivalent series resistance (ESR) in series with a parallel com-
bination of double-layer capacitor (Cd) and resistor (Rf ) in
series with the Warburg impedance element (W) analogous to
the electrolyte ion diffusion into the porous network of the
carbon material used for electrode fabrication. The ESR rep-
resents the combined contact resistance between the current
collector electrode or conducting substrate material and the
ohmic resistance of the electrode–electrolyte interface. In the
present study, the equivalent series resistance was approxi-
mately 12.3 Ω for RC-B, showing good conducting behaviour.57
Hence, further studies will be needed to optimize the
reduction of ESR using proper contacts in devices. Fig. 10(b
and c) shows the Bode phase plot and plot of the total impe-
dance (Z) vs. frequency (Hz) for RC-B (Fig. 10c). The Bode
phase plot indicates that the phase shift is 69° for RC-B in the
low frequency region, indicating full double layer charge
storage phenomenon without a faradaic (redox)-type charge
storage process.68
In the total impedance vs. frequency plot, the impedance or
resistance |Z| decreased with the increasing frequency
(Fig. 10b). It has been reported that the penetration depth of
electrolyte ions in the pores increases with the decreasing
applied frequency. A straight line was obtained at a low fre-
quency region due to the accumulation of ions at the bottom
of the pores, whereas in the middle frequency region, a
straight line was obtained due to the semi-infinite ion
migration (dipoles) through various mesopores. At the high
frequency region, a horizontal line appeared, which is due to
the dominance of electronic transport over this regime.69 The
electrochemical impedance study of RC-B reveals that carbon
derived from the Bougainvillea flower is a potential candidate
for supercapacitors. The carbon material used herein shows
ideal and stable capacitive behaviour as well as double charge
storage mechanism.
4. Conclusion
Overall, we demonstrated the high surface area mesoporous
functional (conducting) and perforated graphene from dead
Nanoscale, 2017, 9, 4801–4809 | 4807

Paper
flowers of Bougainvillea for the first time. Further, we
used graphene for supercapacitor applications without any
external activation. The perforated graphene synthesized using
Bougainvillea flowers at 800 °C demonstrated a very high
charge storage capability with a specific capacitance of 458
Published on 15 March 2017. Downloaded by National Institute of Technology - Rourkela on 12/8/2022 5:55:38 AM.
F g−1 and an energy density of 63.7 Wh kg−1 in 1 M Na2SO4 as
an electrolyte. This high supercapacitance may be due to the
extraordinary mesoporosity and perforated nature with high
specific surface area, i.e. 850 m2 g−1. The present study demon-
strates the solution for waste management as it has always
been a large problem in big cities, and the preparation of
value-added products from natural waste.
Acknowledgements
The authors would like to thank C-MET, Pune for technical
support and MeitY, New Delhi for the financial support.
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