Abstract
The present work has reported a microwave-assisted green reduction approach for reducing graphene oxide (GO) to reduced graphene oxide (rGO) using Artemisia vulgaris plant leaf extract. GO has been synthesised following the modified Hummers method. The reduction of graphene oxide (GO) has been conducted in three sets resulting in six reduced graphene oxide (rGO) samples (R1–R6) with a maximum reduction time of 1 h. Three sets of parameters with changes in microwave input power, reduction reaction time and volume of plant extract have been investigated to acquire an optimised set of reduction conditions. The reported optimised set exhibited the highest specific capacitance (CS) value out of the parameters investigated. The study is based on the comparative analysis of structural, morphological, vibrational, optical, bonding and networks and electrochemical properties of GO and its reduced products (rGO) for supercapacitor application. The potential of this plant extract to reduce GO into rGO has been reported. Furthermore, it was discovered that only a particular volume of Artemisia vulgaris extract might be employed for effective reduction. The rGO samples have been studied for supercapacitor electrode application. Total charge resistance (RCT) analysis through electrochemical impedance spectroscopy (EIS) reveals the decrease in RCT value from 295.51 Ω for GO to as low as 42.09 Ω for R5. The CS of the synthesised GO and all rGO samples have been calculated using CD and CV plots. The highest value recorded for R5 was 111.62 Fg−1 at a scan rate of 0.005 Vs−1 and 94.80 Fg−1 at a current density of Ag−1. The cyclic stability after 5000 cycles at a current density of 3 Ag−1 was recorded as 74.2%.
Similar content being viewed by others
Data availability
The datasets generated during and/or analysed during the current study are available from the corresponding author on reasonable request.
References
K.S. Novoselov, A.K. Geim, S.V. Morozov, D. Jiang, Y. Zhang, S.V. Dubonos, I.V. Grigorieva, A.A. Firsov, Electric field effect in atomically thin carbon films. Science 306, 666 (2004)
U.A. Méndez-Romero, S.A. Pérez-García, X. Xu, E. Wang, L. Licea-Jiménez, Functionalized reduced graphene oxide with tunable band gap and good solubility in organic solvents. Carbon 146, 491 (2019)
Y. Shen, S. Yang, P. Zhou, Q. Sun, P. Wang, L. Wan, J. Li, L. Chen, X. Wang, S. Ding, D.W. Zhang, Evolution of the bandgap and optical properties of graphene oxide with controllable reduction level. Carbon 62, 157 (2013)
R. Bhujel, S. Rai, U. Deka, B.P. Swain, Electrochemical, bonding network and electrical properties of reduced graphene oxide-Fe2O3 nanocomposite for supercapacitor electrodes applications. J. Alloys Compd. 792, 250 (2019)
C. Zhou, Y. Zhang, Y. Li, J. Liu, Construction of high-capacitance 3D CoO@Polypyrrole nanowire array electrode for aqueous asymmetric supercapacitor. Nano Lett. 13, 2078 (2013)
K.H. An, K.K. Jeon, J.K. Heo, S.C. Lim, D.J. Bae, Y.H. Lee, High-capacitance supercapacitor using a nanocomposite electrode of single-walled carbon nanotube and polypyrrole. J. Electrochem. Soc. 149, A1058 (2002)
Z. Gan, N. Song, H. Zhang, Z. Ma, Y. Wang, C. Chen, One-Step Electrofabrication of reduced graphene oxide/poly(n-methylthionine) composite film for high performance supercapacitors. J. Electrochem. Soc. 167, 085501 (2020)
Q. Meng, K. Cai, Y. Chen, L. Chen, Research progress on conducting polymer based supercapacitor electrode materials. Nano Energy 36, 268 (2017)
A.C. Dhanemozhi, V. Rajeswari, S. Sathyajothi, Green synthesis of zinc oxide nanoparticle using green tea leaf extract for supercapacitor application. Mater. Today Proc. 4, 660 (2017)
S. Maiti, A. Pramanik, S. Mahanty, Electrochemical energy storage in Mn2O3 porous nanobars derived from morphology-conserved transformation of benzenetricarboxylate-bridged metal-organic framework. CrystEngComm 18, 450 (2016)
S. Sardana, A. Gupta, A.S. Maan, S. Dahiya, K. Singh, A. Ohlan, Design and synthesis of polyaniline/MWCNT composite hydrogel as a binder-free flexible supercapacitor electrode. Indian J. Phys. 96, 433 (2022)
B. Sharma, S. Thakur, D. Trache, H.Y. Nezhad, V.K. Thakur, Microwave-assisted rapid synthesis of reduced graphene oxide-based gum tragacanth hydrogel nanocomposite for heavy metal ions adsorption. Nanomaterials 10, 1616 (2020)
A. Moyseowicz, A. Śliwak, E. Miniach, G. Gryglewicz, Polypyrrole/iron oxide/reduced graphene oxide ternary composite as a binderless electrode material with high cyclic stability for supercapacitors. Compos. B 109, 23 (2017)
C.H. Kim, B.H. Kim, Zinc oxide/activated carbon nanofiber composites for high-performance supercapacitor electrodes. J. Power Sources 274, 512 (2015)
F. Liu, C. Wu, Y. Dong, C. Zhu, C. Chen, Poly (azure C)-coated CoFe Prussian blue analogue nanocubes for high-energy asymmetric supercapacitors. J. Colloid Interface Sci. 628, 682 (2022)
C.K. Chua, M. Pumera, Chemical reduction of graphene oxide: a synthetic chemistry viewpoint. Chem. Soc. Rev. 43, 291 (2014)
R. Muszynski, B. Seger, P.V. Kamat, Decorating graphene sheets with gold nanoparticles. J. Phys. Chem. C 112, 5263 (2008)
W. Guoxiu, Y. Juan, P. Jinsoo, G. Xinglong, W. Bei, L. Hao, Y. Jane, Facile synthesis and characterisation of graphene nanosheets. J. Phys. Chem. C 112, 8192 (2008)
D. Perumal, E.L. Albert, C.A.C. Abdullah, Green reduction of graphene oxide involving extracts CS of plants from different taxonomy groups. J. Compos. Sci. 6, 58 (2022)
M. Agharkar, S. Kochrekar, S. Hidouri, M.A. Azeez, Trends in green reduction of graphene oxides, issues and challenges: a review. Mater. Res. Bull. 59, 323 (2014)
J. Liu, S. Fu, B. Yuan, Y. Li, Z. Deng, Toward a universal “Adhesive Nanosheet” for the assembly of multiple nanoparticles based on a protein-induced reduction/decoration of graphene oxide. J. Am. Chem. Soc. 132, 7279 (2010)
O. Akhavan, E. Ghaderi, A. Esfandiar, Wrapping bacteria by Graphene nanosheets for isolation from environment, reactivation by sonication, and inactivation by near-infrared irradiation. J. Phys. Chem. B 115, 6279 (2011)
J. Gao, F. Liu, Y. Liu, N. Ma, Z. Wang, X. Zhang, Environment-friendly method to produce graphene that employs vitamin C and amino acid. Chem. Mater. 22, 2213 (2010)
C. Zhu, S. Guo, Y. Fang, S. Dong, Reducing sugar, new functional molecules for the green synthesis of graphene nanosheets. ACS Nano 4, 2429 (2010)
S. Rai, R. Bhujel, J. Biswas, B.P. Swain, Biocompatible synthesis of rGO from ginger extract as a green reducing agent and its supercapacitor application. Bull. Mater. Sci. 44, 40 (2021)
Z. Lin, X. Weng, L. Ma, B. Sarkar, Z. Chen, Mechanistic insights into Pb (II) removal from aqueous solution by green reduced graphene oxide. J. Colloid Interface Sci. 550, 1 (2019)
S. Thakur, N. Karak, Green reduction of graphene oxide by aqueous phytoextracts. Carbon 50, 5331 (2012)
B. Li, X. Jin, J. Lin, Z. Chen, Green reduction of graphene oxide by sugarcane bagasse extract and its application for the removal of cadmium in aqueous solution. J. Clean. Prod. 189, 128 (2018)
R.K. Upadhyay, N. Soin, G. Bhattacharya, S. Saha, A. Barman, S.S. Roy, Grape extract assisted green synthesis of reduced graphene oxide for water treatment application. Mater. Lett. 160, 355 (2015)
M.Z. Ansari, W.A. Siddiqui, Deoxygenation of graphene oxide using biocompatible reducing agent Ficus carica (dried ripe fig). J. Nanostruct. Chem. 8, 431 (2018)
D. Hou, Q. Liu, H. Cheng, K. Li, Graphene synthesis via chemical reduction of graphene oxide using lemon extract. J. Nanosci. Nanotechnol. 17, 6518 (2017)
S. Ramanathan, E. Elanthamilan, A. Obadiah, A. Durairaj, J.P. Merlin, S. Ramasundaram, S. Vasanthkumar, Aloe vera (L.) Burm.f. extract reduced graphene oxide for supercapacitor application. J. Mater. Sci. Mater. Electron. 28, 16648 (2017)
D.R. Madhuri, K. Kavyashree, A.R. Lamani, H.S. Jayanna, G. Nagaraju, S. Mundinamani, Reduction of graphene oxide by Phyllanthus Emblica as a reducing agent: a green approach for supercapacitor application. Mater. Today Proc. 49, 865 (2022)
N.J. Panicker, P.P. Sahu, Green reduction of graphene oxide using phytochemicals extracted from Pomelo Grandis and Tamarindus indica and its supercapacitor applications. J. Mater. Sci. Mater. Electron. 32, 15265 (2021)
H. Ekiert, J. Pajor, P. Klin, A. Rzepiela, H. Ślesak, A. Szopa, Significance of Artemisia Vulgaris L. (Common Mugwort) in the history of medicine and its possible contemporary applications substantiated by phytochemical and pharmacological studies. Molecules 25, 4415 (2020)
P. Chettri, V.S. Vendamani, A. Tripathi, A.P. Pathak, A. Tiwari, Self assembly of functionalised graphene nanostructures by one step reduction of graphene oxide using aqueous extract of Artemisia vulgaris. Appl. Surf. Sci. 362, 221 (2016)
D.A.P. Hernández, E.R. Parra, P.J.A. Arango, B.S. Giraldo, C.D.A. Medina, Innovative method for coating of natural corrosion inhibitor based on Artemisia vulgaris. Materials 14, 2234 (2021)
A. Temraz, W.H. El-Tantawy, Characterisation of antioxidant activity of extract from Artemisia vulgaris. Pak. J. Pharm. Sci. 21, 321 (2008)
S. Rai, R. Bhujel, J. Biswas, B.P. Swain, in Nanostructured materials and their applications. ed. by B.P. Swain (Springer, Singapore, 2021), p.115
S.N. Alam, N. Sharma, L. Kumar, Synthesis of graphene oxide (GO) by modified hummers method and its thermal reduction to obtain reduced graphene oxide (rGO)*. Graphene 6, 1 (2017)
N.M.S. Hidayah, W.-W. Liu, C.-W. Lai, N.Z. Noriman, C.-S. Khe, U. Hashim, H.C. Lee, Comparison on graphite, graphene oxide and reduced graphene oxide: Synthesis and characterization. AIP Conf. Proc. 1892, 150002 (2017)
K. Bansal, J. Singh, A.S. Dhaliwal, Synthesis and characterisation of Graphene Oxide and its reduction with different reducing agents. IOP Conf. Ser. Mater. Sci. Eng. 1225, 012050 (2022)
W.H. Bragg, W.L. Bragg, The reflection of X-rays by crystals. Proc. R. Soc. Lond. A 88, 428 (1913)
U. Holzwarth, N. Gibson, The Scherrer equation versus the ‘Debye-Scherrer equation.’ Nat. Nanotechnol. 6, 534 (2011)
S.R. Meitei, C. Ngangbam, N.K. Singh, Microstructural and optical properties of Ag assisted β-Ga2O3 nanowires on silicon substrate. Opt. Mater. 117, 111190 (2021)
A. Kaushal, S.K. Dhawan, V. Singh, Determination of crystallite size, number of graphene layers and defect density of graphene oxide (GO) and reduced graphene oxide (RGO). AIP Conf. Proc. 2115, 030106 (2019)
K. Chaudhary, M. Aadil, S. Zulfiqar, S. Ullah, S. Haider, P.O. Agboola, M.F. Warsi, I. Shakir, Graphene oxide and reduced graphene oxide supported ZnO nanochips for removal of basic dyes from the industrial effluents. Fuller. Nanotub. Carbon Nanostruct. 29, 915 (2021)
R. Siburian, H. Sihotang, S.L. Raja, M. Supeno, C. Simanjuntak, New route to synthesise of Graphene Nano sheets. Orient. J. Chem. 34, 182 (2018)
R. Al-Gaashani, A. Najjar, Y. Zakaria, S. Mansour, M.A. Atieh, XPS and structural studies of high quality graphene oxide and reduced graphene oxide prepared by different chemical oxidation methods. Ceram. Int. 45, 14439 (2019)
D. Khalili, Graphene oxide: a promising carbocatalyst for the regioselective thiocyanation of aromatic amines, phenols, anisols and enolisable ketones by hydrogen peroxide/KSCN in water. New J. Chem. 40, 2547 (2016)
C.H. Manoratne, S.R.D. Rosa, I.R.M. Kottegoda, XRD-HTA, UV visible, FTIR and SEM interpretation of reduced graphene oxide synthesised from high purity vein graphite. Mater. Sci. Res. India 14, 19 (2017)
N.M.N. Huynh, Z.A. Boeva, J.-H. Smått, M. Pesonen, T. Lindfors, Reduced graphene oxide as a water, carbon dioxide and oxygen barrier in plasticised poly(vinyl chloride) films. RSC Adv. 8, 17645 (2018)
A.C. Ferrari, J.C. Meyer, V. Scardaci, C. Casiraghi, M. Lazzeri, F. Mauri, S. Piscanec, D. Jiang, K.S. Novoselov, S. Roth, A.K. Geim, Raman spectrum of graphene and graphene layers. Phys. Rev. Lett. 97, 187401 (2006)
S. Rai, R. Bhujel, B.P. Swain, Electrochemical analysis of graphene oxide and reduced graphene oxide for super capacitor applications. IEEE Electron Devices Kolkata Conf. (EDKCON) 2018, 489–492 (2018). https://doi.org/10.1109/EDKCON.2018.8770433
H. Martinho, C. Rettori, P.G. Pagliuso, A.A. Martin, N.O. Moreno, J.L. Sarrao, Role of the E2g phonon in the superconductivity of MgB2: a Raman scattering study. Solid State Commun. 125, 499 (2003)
S.M. Hafiz, R. Ritikos, T.J. Whitcher, N.M. Razib, D.C.S. Bien, N. Chanlek, H. Nakajima, T. Saisopa, P. Songsiriritthigul, N.M. Huang, S.A. Rahman, A practical carbon dioxide gas sensor using room-temperature hydrogen plasma reduced graphene oxide. Sens. Actuators B 193, 692 (2014)
W.I. Singh, S. Sinha, N.A. Devi, S. Nongthombam, S. Laha, B.P. Swain, Fabrication and characterisation of reduced graphene oxide/polyaniline/poly(caprolactone) electrospun nanofiber. Arab. J. Sci. Eng. 47, 925 (2022)
F. Ghasemi, M. Jalali, A. Abdollahi, S. Mohammadi, Z. Sanaee, S. Mohajerzadeh, A high performance supercapacitor based on decoration of MoS2/reduced graphene oxide with NiO nanoparticles. RSC Adv. 7, 52772 (2017)
Z. Li, S. Gadipelli, Y. Yang, G. He, J. Guo, J. Li, Y. Lu, C.A. Howard, D.J.L. Brett, I.P. Parkin, F. Li, Z. Guo, Exceptional supercapacitor performance from optimized oxidation of graphene-oxide. Energy Storage Mater. 17, 12 (2019)
J. Kim, J.H. Eum, J. Kang, O. Kwon, H. Kim, D.W. Kim, Tuning the hierarchical pore structure of graphene oxide through dual thermal activation for high-performance supercapacitor. Sci. Rep. 11, 1 (2021)
F.T. Johra, W.G. Jung, Hydrothermally reduced graphene oxide as a supercapacitor. Appl. Surf. Sci. 357, 1911 (2015)
B. Zhao, P. Liu, Y. Jiang, D. Pan, H. Tao, J. Song, T. Fang, W. Xu, Supercapacitor performances of thermally reduced graphene oxide. J. Power Sources 198, 423 (2012)
C. Xiang, M. Li, M. Zhi, A. Manivannan, N. Wu, A Reduced graphene oxide/Co3O4 composite for supercapacitor electrode. J. Power Sources 226, 65 (2013)
S.P. Lee, G.A.M. Ali, H.H. Hegazy, H.N. Lim, K.F. Chong, Optimizing Reduced graphene oxide aerogel for a supercapacitor. Energy Fuels 35, 4559 (2021)
V. Balasubramani, S. Chandraleka, T.S. Rao, R. Sasikumar, M.R. Kuppusamy, T.M. Sridhar, Review-recent advances in electrochemical impedance spectroscopy based toxic gas sensors using semiconducting metal oxides. J. Electrochem. Soc. 167, 037572 (2020)
Y. Yoon, J. Jo, S. Kim, I.G. Lee, B.J. Cho, M. Shin, W.S. Hwang, Impedance spectroscopy analysis and equivalent circuit modeling of graphene oxide solutions. Nanomaterials 7, 446 (2017)
B.A. Mei, O. Munteshari, J. Lau, B. Dunn, L. Pilon, Physical Interpretations of Nyquist Plots for EDLC electrodes and devices. J. Phys. Chem. C 122, 194 (2018)
S.-J. Lee, H.-Y. Chung, C.G.-A. Maier, A.R. Wood, R.A. Dixon, T.J. Mabry, Estrogenic flavonoids from Artemisia vulgaris L. J. Agric. Food Chem. 46, 3325 (1998)
S. Numonov, F. Sharopov, A. Salimov, P. Sukhrobov, S. Atolikshoeva, R. Safarzoda, M. Habasi, H. Aisa, Assessment of artemisinin contents in selected artemisia species from tajikistan (Central Asia). Medicines 6, 23 (2019)
M. Nganthoi, K. Sanatombi, Artemisinin content and DNA profiling of Artemisia species of Manipur. S. Afr. J. Bot. 125, 9 (2019)
Acknowledgements
The authors acknowledge the Centre of Excellence in Advanced Materials, NIT Durgapur, for their help in procuring FESEM micrographs and XRD spectra and the Institute Instrumentation Centre, IIT Roorkee, for providing the XPS spectra. We would also like to extend our gratitude to the Sophisticated Analytical Instrument Facility (SAIF), NEHU, Shillong, for providing the TEM micrographs. We sincerely acknowledge Sikkim Manipal University for providing PhD Research Fellowship to Miss Suveksha Tamang.
Funding
The present work is funded by TMA Pai Research Fellowship, Sikkim Manipal University (Ref. No.: 118/SMU/REG/00/53/2019).
Author information
Authors and Affiliations
Contributions
ST contributed to experimental design, performance, data analysis and manuscript preparation. SR contributed to data analysis and data verification. MKM contributed to structural investigation and analysis. NKB contributed to data verification and manuscript preparation. BPS contributed to data analysis and manuscript preparation. JB performed supervision, data analysis and manuscript preparation.
Corresponding author
Ethics declarations
Conflict of interest
On behalf of all authors, the corresponding authors state that there are no conflicts to declare.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary Information
Below is the link to the electronic supplementary material.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Tamang, S., Rai, S., Mondal, M.K. et al. Microwave-assisted reduction of graphene oxide using Artemisia vulgaris extract for supercapacitor application. J Mater Sci: Mater Electron 34, 575 (2023). https://doi.org/10.1007/s10854-023-09995-3
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s10854-023-09995-3