DOI: 10.1002/slct.
202000101 Full Papers
z Sustainable Chemistry
A Novel Strategy for Sustainable Synthesis of Soluble-
Graphene by a Herb Delphinium denudatum Root Extract
for Use as Light-Weight Supercapacitors
Saikumar Manchala,[a, b] VSRK Tandava,[a] Deshetti Jampaiah,[c] Suresh K. Bhargava,*[c] and
Vishnu Shanker*[a, b]
Synthesis of high-quality graphene nanosheets under eco-
friendly strategies is of enormous interest today hence
graphene-based materials offer unique advantages in a wide
range of applications including light-weight supercapacitors.
The reduction of graphene oxide (GO) by chemical reagents
frequently involves hazardous reductants that are also danger-
ous to humans. In view of sustainability, we develop a facile
and green procedure to synthesize soluble-graphene by
reducing the GO in delphinium root extraction for the first time.
The reducing property of organic compounds that exist in the
aqueous delphinium root extract may be accountable for the
reduction of exfoliated GO to D-graphene under reflux
condition. The efficient elimination of oxygen functionalities
from GO was verified by powder X-ray diffraction (PXRD), UV-
1. Introduction
Since the publishing of twelve principles of green chemistry
from 1998 to present, a lot of efforts have been led to develop
new eco-friendly strategies in the fields of sustainable nano-
science and technology.[1] A sp2 hybridized planar sheet of
continuous carbon atoms, namely graphene, first discovered in
2004 by an easy isolation using mechanical exfoliation of
graphite by Geim and Novoselov, can be a wonder carbon
nanomaterial for a wide range of emerging applications, has
gained an utmost attention from the scientific community since
then and still needs to be explored to a larger extent.[2,3]
Perhaps it is the thinnest form of carbon allotrope and simple
than any other material ever produced. Graphene is found to
have a honeycomb lattice structure that possesses highly
unique properties. Owing to its large in-plane electrical
conductivity (∼ 104/ Ώ.cm), used in electrodes preparation as
[a] S. Manchala, V. Tandava, Dr. V. Shanker
Department of Chemistry, National Institute of Technology, Warangal-
506004, Telangana, India
E-mail: vishnu@nitw.ac.in
[b] S. Manchala, Dr. V. Shanker
Centre for Advanced Materials, National Institute of Technology,
Warangal-506004, Telangana, India
[c] Dr. D. Jampaiah, Prof. S. K. Bhargava
Centre for Advanced Materials & Industrial Chemistry (CAMIC), School of
Science, RMIT University, GPO BOX 2476, Melbourne-3001, Australia
E-mail: suresh.bhargava@rmit.edu.au
Supporting information for this article is available on the WWW under
https://doi.org/10.1002/slct.202000101
ChemistrySelect 2020, 5, 2701 – 2709
Visible spectroscopy (UV-Vis), Fourier transform infrared (FT-IR),
and X-ray photoelectron spectroscopy (XPS) studies. Atomic
force microscopy (AFM) and transmission electron microscopy
(TEM) studies indicate the successful development of few-layer
graphene. The electrochemical activities are delivered by cyclic
voltammetry (CV) and galvanic charge-discharge (GCD) studies.
This uniquely-synthesized D-graphene electrode offers superior
electrochemical performance at 2 A g 1 with an utmost specific
capacitance (Cs) of 158 F g 1 and high energy density (E) of
22 Wh Kg 1. Taking the above remarkable results, the character-
istics of eco-friendly, easy synthesis and cheap endow this
green approach as a promising avenue for the exploitation of
graphene-based materials in numerous applications, particu-
larly for graphene-based light-weight supercapacitors.
well as exploited in industrial blast furnaces as it possesses
superior thermal conductivity (∼ 3000 W/m.K).[4] To date, di-
verse approaches have been developed for the abundant
production of graphene comprising either a top-down or
bottom-up approach. Various methods include chemical
intercalation,[5,6] thermal or chemical reduction of GO,[7] epitaxial
growth,[8] mechanical or ultrasonic exfoliation,[9] electric arc
discharge,[10] chemical vapor deposition,[11] and microwave
plasma-enhanced chemical vapor deposition.[12] The as-synthe-
sized graphene with required fabrication is found to have
innumerable applications in the areas of photocatalysis,[13,14]
catalysis,[15] Li-ion batteries,[16,17] Ni- and Zn-ion batteries,[18]
supercapacitors,[19,20] solar cells,[21,22] photovoltaic cells,[23]
biosensors,[24,25] fuel cells,[26,27] heavy metals removal,[28] etc. Of
all the reported methods and methodologies, the chemical
reduction of GO is most widely employed as it is aids in bulk
synthesis and highly cost-effective.
The use of common reducing agents like sodium borohy-
dride (NaBH4),[29] and hydrazine hydrate (HH)[30] are not
advisable as they are hazardous being toxic to the
environment.[31] Alternatively, several green and environmen-
tally benign reducing agents were investigated for the
production of graphene-like bovine serum albumin,[32] reducing
sugar,[33] heparin,[34] wild carrot roots,[35] ascorbic acid or
Vitamin-C,[36] Tea polyphenols,[37] aloe vera,[38] vancomycin,[39]
etc. But the results show poor C/O ratio. However, a lot of work
is still to be focused on developing natural green reductants
for the huge production of graphene nanosheets. Therefore,
2701 © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

we have explored an interesting medicinal plant, Delphinium
denudatum, whose roots are of extremely propitious properties
in the fields of medicine and indigenous drugs.
Delphinium genus belongs to the family of Ranunculaceae,
is found to be famous for its beautiful flowers. There are
around 15 species that exist in India, and most of the species
abundantly found in the western Himalayas from Kumaon to
Kashmir. Among 15 species, Delphinium denudatum Wall has
been studied extensively in the traditional medicine system to
cure many ailments in India. Delphinium denudatum Wall, most
vernacularly known as Jadwar, is said to be one of the most
prominent drugs used as a medicine, more specifically an
Unani Medicine in India. Particularly, the rhizome and roots of
Delphinium denudatam Wall were found to be rich in several
alkaloids such as diterpenoids like denudatine, condelphine,
talatizidine, panicutine, denudatidine, vilmorrianone, isotalatizi-
dine, 8-acetylhetero-phyllisine, 3-hydroxy-2-methyl-4H-pyran-4-
one. Some sterols, phenols, proteins, fatty acids, and reducing
sugars along with oils were also reported in approximate
quantities in alcoholic and aqueous extracts of the roots. The
rhizome and adventitious roots of Jadwar are blackish-brown in
color, and they seem to be dark brown or greyish in color
when they were grounded to powder and are bitter in taste
without any specific odor. The additional advantages of root
extracts of Delphinium denudatam Wall include antifungal
activity, antibacterial activity, antiasthmatic activity, and anti-
oxidant activity.[40–47] Recently, reducing property of Jadwar root
extract has been investigated by Gopal Suresh, et al., for the
production of silver nanoparticles.[48]
Scheme 1. Schematic depiction of D-graphene synthesis by using Delphinium root extract.
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As for our knowledge, no report has been found on Jadwar
root extract for the production of soluble-graphene and there
has been a lot of interest to be explored further. In the present
work, graphene was synthesized by a facile reflux strategy
using aqueous Jadwar root extract. The total synthesis
procedure was shown in Scheme 1. The presented novel
strategy shows distinctive features for the abundant production
of graphene for miscellaneous applications and it exhibits
several advantages such as i) the used reduction strategy is
eco-friendly, and no hazardous chemicals used. ii) The method
is economical and simple. And iii) safe, and no hazardous waste
was produced. iv) The efficiency of reduction is high (C/O ratio-
8.07) compare to several reported green reductants.
2. Results and Discussions
2.1 Characterization of synthesized D-graphene
To monitor the reduction of GO by Delphinium root extract, UV-
Vis was employed and the results were displayed in Figure 1a.
As presented in Figure 1a, GO exhibits absorption peak around
at 230 nm corresponding to the π-π* transitions, whereas D-
graphene exhibits absorption peak around at 270 nm ascribed
to the π-π* transitions indicates that the majority of the oxygen
functionalities eliminated from the GO surface and conjugation
(C=C) remains stored.[49] Additionally, as the reaction progress,
the colour of the solution turned from brownish to deep black,
specifying the reduction of GO solution.
To confirm the atomic structures of the graphite and as-
prepared GO and D-graphene, PXRD was employed and the
2702 © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

Figure 1. (a) UV-Vis spectra, (c) Raman spectra, (d) FT-IR spectra of synthesized GO and D-graphene, and (b) PXRD patterns of Graphite and synthesized GO
and D-graphene.
typical diffraction patterns of the samples were shown in
Figure 1b. The nano graphite powder shows a characteristic
diffraction peak at 26.6° assigned to the basal plane of (002),
with a dspacing of 0.334 nm. After oxidation, the GO exhibited a
diffraction peak at 12.6° with a dspacing of 0.702 nm. The high
dspacing value of GO compare to that of pure graphite is due to
the development of oxygen functional groups and the
adsorbed H2O molecules between the sheets of graphite. After
the reduction of GO with Delphinium root extract, a broad peak
appeared at 24.5° with a dspacing of 0.362 nm while the reflection
peak at 12.6° was disappeared, designating that the develop-
ment of D-graphene. Moreover, the dspacing of D-graphene was
largely reduced, suggesting that the elimination of oxygen
functionalities from GO, which are in line with UV-Vis results.[50]
To determine the nature (ordered or disordered) of carbon
nanomaterials Raman spectroscopy was performed, and the
results were exhibited in Figure 1c. The GO showed two major
peaks typically at 1339 and 1585 cm 1, which were similar to
the reported literature.[51,52] The first one at 1339 cm 1 for D-
band can be assigned to breathing mode and the intensity of
the D-band determined by the population of defects and
staging disorder. The second one at 1585 cm 1 for G-band can
be allotted to the E2g symmetry phonon mode of in-plane
vibrations of all sp2 carbons network. After reduction, one
additional peak noticed at 2670 cm 1 for a 2D band, which can
be corresponding to the two-phonon mode with opposite
wave vectors and the intensity ratios of both D and G bands
obviously increased from 0.95 to 1.06 confirms the formation
D-graphene which is compatible with the previous reports.[53]
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Therefore, the higher intensity of D-band demonstrates the
origin of new and more sp3 isolated graphitic domains in D-
graphene compared to that of GO.[54] And also the lower
intensity and redshift in the G-band position ( 1585 to
1573 cm 1) explain the formation of new sp2 carbon domains
(number of double bonds) which are smaller in number
compared to the sp2 carbon domains present in GO before
reduction.[51] Altogether, it is deduced that the Delphinium root
extract can play a major role in the efficient reduction of GO by
the elimination of oxygen functionalities.
To verify the functional groups present in the synthesized
GO and D-graphene, FT-IR was carried out, and the observed
spectra were shown in Figure 1d. The GO displayed several
bands. The bands at 1243 and 1029 cm 1 can be assigned to
the stretching frequencies of epoxy C O-C and phenolic C O
groups. The bands observed at 2924 and 2853 cm 1 can be
ascribed to the asymmetric and symmetric stretching frequen-
cies of CH2 groups.[55] The bands noticed at 1735 and
1615 cm 1 corresponding to the stretching frequencies of C=O
and C=C groups. Finally, the broadband between 3100–
3650 cm 1 can be correlated to the stretching frequency of OH
groups and bands at 1386 and 1038 cm 1 can be assigned to
the deformation vibrations of OH groups present on the GO
surface, respectively.[37,51] Moreover, after the reduction of GO
by Delphinium root extract, the oxygen-containing functional
groups (C O C, phenolic C O, and OH) absorption bands’
intensity has been decreased remarkably and some of the
functional groups such as C=O completely eliminated, which
confirmed the reduction of GO to D-graphene.
2703 © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
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Figure 2. (a–d) TEM, (e) HR-TEM, and (f) SAED images of synthesized D-graphene.

To evaluate the morphological characteristics of D-gra-
phene, TEM investigation was carried out and the correspond-
ing images of D-graphene were shown in Figure 2a-d. It is
evidenced that the formation of few-layer 2D graphene nano-
sheets and commonly display scrolled, wrinkled and trans-
parent features. Moreover, the exact number of nanosheets
present in few-layer graphene cannot be determined. However,
it can be seen that there were no big graphitic lumps, which
indicates the successful development of few-layer graphene.
The HR-TEM image of D-graphene (Figure 2e), shows the dspacing
of 0.387 nm, which is near to the dspacing of D-graphene
(0.362 nm) acquired by PXRD.[56] Besides, the corresponding
SAED pattern displayed in Figure 2f further confirms the
diffraction plane (002) of formed D-graphene. These results
directly coincide with the results obtained by PXRD and HR-
TEM of synthesized D-graphene.
To investigate the reduction efficiency of delphinium root
extract by reducing GO to D-graphene, XPS studies were
employed. The reduction efficiency can be assessed by
Figure 3a-b, the high-resolution C 1s XPS spectra of GO and D-
graphene were deconvoluted into 4 peaks around the binding
energies of 284.8, 286.8, 287.7, and 289.5 eV corresponding to
the C=C (sp2-carbon), C O (epoxy/hydroxyl), C=O (carbonyl),
and O C=O (carboxyl) groups.[57,58] The peak intensity of D-
graphene corresponding to oxygen functional groups de-
creased and some of them (C=O) completely vanished, which
indicates the delphinium root extract is highly effective in the
reduction of GO to D-graphene and the C to O ratio also
apparently increased in the D-graphene (8.07) when compared
to GO (5.05) as shown in Table 1. The C to O ratio obtained in
this method (8.07) is higher than that of the several reported
green reductants as shown in Table 2. The above XPS results
Table 2. Comparisons of C/O and ID/IG ratios for the graphene synthesized
by different green reductants.
Reductants C/O ratio ID/IG Ref.
Tea polyphenols 3.1 - [37]

analyzing the C to O ratio in the D-graphene. The determined C Gallic acid 3.89-5.28 1.86-1.92 [59]

[60]
to O ratios were shown in Table 1. As displayed in the Tannic acid 2.44 1.15
[50]
Caffeic acid 7.15 1.15
[61]
Natural cellulose 5.47 1.53
[36]
L-Ascorbic acid 5.7 >1
[62]
Table 1. Comparisons of the C/O ratio of GO and D-graphene. Baker’s yeast 5.9 1.44
Delphinium 8.07 1.06 Present work
S.No. Sample C (Atomic %) O (Atomic %) C/O ratio root extract

1 GO 83.46 16.54 5.05 [a] Carbon to Oxygen ratio, [b] Intensity of D-band to Intensity of G-band
2 D-graphene 88.98 11.02 8.07 ratio

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Figure 3. High-resolution C 1s XPS spectra of (a) GO and (b) D-graphene.
describe that the Delphinium root extract serves as an efficient
green reductant for the bulk synthesis of D-graphene from GO
and the results are in consistence with FTIR-results.
To analyze the thickness of D-graphene, AFM was carried
out. Figure 4 represents the AFM images and corresponding
height profiles of D-graphene. Literature reports revealed that
the thickness of the graphene sheet was decreased possibly
due to the elimination of oxygen functional groups from GO
during reduction.[7] As exhibited in the Figure. 4, the average
thickness of D-graphene was observed to be around 3–5 nm.
From the literature reports the thickness of single-layer
graphene was 0.335 nm,[63,64] which means two single graphene
layers can measure approximately 1 nm thick when accounting
for the dspacing. Therefore, D-graphene might be composed of 6–
10 graphene sheets.
Figure 4. AFM images and depth profiles of D-graphene.
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2.2 Solubility studies of D-graphene
At the side of the water, the suspension nature of D-graphene
in various non-aqueous solvents were studied. As indicated in
the Figure 5, the D-graphene powder has been dispersed
successfully in water and different non-aqueous solvents such
as MeOH, THF, EtAC, n-hexane, DMSO, DMF, and EtOH by using
sonication. After one week, it was noticed that most of the
dispersions were highly stable in nature with an insignificant
amount of D-graphene settled. But the D-graphene present in
the n-hexane dispersion was completely precipitated out,
whereas the D-graphene present in the THF dispersion
precipitated out to a large extent. Significantly, the high
dispersibility of D-graphene in a variety of solvents with a low
boiling point can create opportunities for the design and
manufacturing of new-class of devices and composites to a
2705 © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

Figure 5. As-prepared dispersions of D-graphene (1 mg/mL) in water and various non-aqueous solvents and their dispersion status after one week.
great extent. Altogether makes this Delphinium root extract-
based green reduction as an eco-friendly, cost-effective, and
efficient method to avoid the use of dangerous chemical
reagents such as hydrazine and NaBH4 for the abundant
production of solution-dispersible graphene from GO.
2.3 Electrochemical characterization for supercapacitor
application
The electrochemical activities, electron transfer resistance, and
Cs of prepared D-graphene supercapacitor electrode were
tested by CV, EIS, and GCD. As displayed in Figure 6a, the CV
curves of the D-graphene supercapacitor electrode at different
scan rates were similar in shape and shown an extraordinary
rate capability upon increase of scan rates. As exhibited in
Figure 6b, the CV curve of the D-graphene supercapacitor
electrode has shown good conductivity compared to that of
the GO supercapacitor electrode at 100 mV s 1 scan rate and
also shown well-broaden peaks with a rectangular shape,
significantly demonstrating that a capacitive behaviour of
electrical double-layer capacitance (EDLC).[65] Figure 6c repre-
sents the Nyquist plot for the D-graphene supercapacitor
electrode, exhibits a semicircle in the high-frequency region
and a straight line in the low-frequency region gives the
information about interfacial charge transfer resistance (Rct) and
resistance due to diffusion. D-graphene supercapacitor elec-
trode was displayed fabulous electrical conductivity due to a
small Rct value (3.7). The results obtained from the Bode plot of
the D-graphene supercapacitor electrode as shown in Figure 6d
are also well complimented with the results shown above. The
maximum phase angle (nearly 90°) of the D-graphene super-
capacitor electrode indicates the high capacitive behaviour
with a huge storage capacity.[66,67] As represented in Figure 6e,
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the GCD curves of the D-graphene supercapacitor electrode at
three different current densities were similar in shape and
shown an outstanding capacitive behaviour. The ‘Cs’ and power
density (P) for the D-graphene supercapacitor electrode were
estimated from the below equations (1-3) at three different
current densities.[68]
IDt
Cs ¼ (1)
mDV
Cs � ðDVÞ2
E¼ (2)
2
E
P¼ (3)
t
Where ‘I’ indicates current (A), ‘m’ represents mass of active
material (g), ‘~t’ is the discharging time, and ‘~V’ is the
potential window. As shown in Figure 6f, the ‘Cs’ of D-graphene
at 2, 3, and 5 A g 1 are 158, 125, and 92 F g 1, respectively. The
D-graphene supercapacitor electrode offers high ‘Cs’ than that
of some of the recently reported supercapacitors.[69–71] As
exhibited in Figure 6g, the Ragone plot of the D-graphene
supercapacitor electrode at three different current densities
offered the highest ‘E’ of 22 Wh kg 1 and ‘P’ of 500 W kg 1.
Figure 6h illustrates long-term electrochemical stability over
1000 cycles at 2 A g 1 of the D-graphene supercapacitor
electrode. Altogether, it can be believed that the D-graphene
supercapacitor electrode offers a significant combination of
high rate ability, high energy storage, and high long-term
stability makes this green approach as an ideal avenue to
realize high energy density supercapacitors.
2706 © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
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Figure 6. (a) CV curves of D-graphene supercapacitor electrode at different scan rates, (b) CV curves of synthesized GO and D-graphene supercapacitor
electrodes at 100 mV s 1 scan rate, (c) Nyquist and (d) Bode plots of D-graphene electrode, (e) GCD curves, (f) Specific capacitance, (g) Ragone plot of D-
graphene supercapacitor electrode at different current densities, and (h) Cyclic stability of D-graphene supercapacitor electrode at 2 A g 1 over 1000 cycles.

3. Conclusions
In conclusion, a novel green reductant possessing the potential
to remove oxygen-functional groups from GO was discovered
in the form of Delphinium root extract and synthesized D-
graphene produce stable suspensions in various solvents. Our
approach can be considered as an excellent methodology,
owing to its several distinguishing features over the formerly
reported strategies, which makes it rather effective, highly

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economical and attractive for the abundant production of
soluble-graphene for emerging miscellaneous applications: (1)
In this reduction process no other synthetic chemicals are used
except green solvent (water) and plant material, so it is eco-
friendly and no hazardous by-products were produced. (2) It
does not require a complex procedure and is very cheap and
safe. (3) The good efficiency of reduction. (4) The acquired D-
graphene able to disperse in both aqueous and various non-
aqueous solvents. These results revealed that the Delphinium
root extract illustrates as an ideal substitute for dangerous
reductants such as NaBH4, hydrazine, and HH in the extensive
development of solution-dispersible graphene. Besides, the D-
graphene supercapacitor electrode demonstrates high ‘Cs’ and
‘E’ (158 F g 1 and 22 Wh Kg 1 at 2 A g 1) with outstanding
supercapacitive cyclic stability over 1000 cycles. It can be
deduced that the significant characteristics of eco-friendly, easy
synthesis, high-efficiency, and cost-effective endow this green
approach as a promising route not only for the development of
light-weight supercapacitors but also in bio-related and other
energy-related applications.
Supporting Information
Experimental details including materials and methods such as
extraction from roots of Delphinium denudatum, synthesis of
GO, the procedure for the reduction of GO using the aqueous
Delphinium denudatum root extract, characterization techni-
ques, and electrochemical measurements employed were
discussed.
Acknowledgment
The author acknowledges the MHRD, Govt. of India for giving
fellowship and NIT-Warangal for providing facilities. The author
thanks the RMIT Microscopy and Microanalysis Facility (RMMF)
for use of their sophisticated set of instruments.
Keywords: Delphinium denudatum roots · Energy storage ·
Graphene · Green synthesis · Supercapacitor
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Submitted: January 8, 2020
Accepted: February 17, 2020
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