Abstract
The objective of this work is twofold: (1) to improve the electrochemical performance of reduced graphene oxide (RGO) by decorating RGO sheets with magnetic nanoparticles (MNPs) and (2) to evaluate the electrochemical performance of RGO and MNP-decorated RGO (MRGO) in various aqueous electrolyte solutions (phosphate buffer solution (PBS) containing ferricyanide, PBS containing ferricyanide and KCl, Na2SO4, and KOH). The morphological and structural characteristics of solvothermal synthesized RGO and MRGO revealed the decoration of phase pure Fe3O4 nanoparticles on RGO sheets. In FC-PBS-KCl electrolyte solution, MRGO showed higher redox peak current (83.89 μA) and lower peak potential separation (0.11 V) at 50 mV s−1 scan rate compared with that in FC-PBS electrolyte solution. MRGO showed 15.5% higher peak current than that for the RGO in FC-PBS-KCl electrolyte solution. Moreover, the peak current for MRGO in FC-PBS-KCl was increased by 30% when compared with that in FC-PBS electrolyte solution. These results suggest that MRGO in FC-PBS-KCl electrolyte solution can be a good electron pathway between electrode and electrolyte solution for sensing applications. On the other hand, in both Na2SO4 and KOH electrolyte solution, RGO and MRGO showed supercapacitive behavior. In KOH, MRGO exhibited higher specific capacitance (180 Fg−1 at 3 A g−1) and superior cyclic stability (87% after 2000 cycles) compared with that in Na2SO4. MRGO showed 219% increase in specific capacitance than that of the RGO in KOH electrolyte solution. The superior electrochemical performance of MRGO compared with that of RGO is attributed to the synergistic effect of conductivity of RGO and redox activity of MNPs.
Similar content being viewed by others
References
Ma S, Nam K, Yoon W, Yang X (2008) Electrochemical properties of manganese oxide coated onto carbon nanotubes for energy-storage applications. J Power Sources 178(1):483–489
Arie AA, Song JO, Lee JK (2009) Structural and electrochemical properties of fullerene-coated silicon thin film as anode materials for lithium secondary batteries. Mater Chem Phys 113(1):249–254
Yan JA, Chou MY (2010) Oxidation functional groups on graphene: structural and electronic properties. Phys Rev B - Condens Matter Mater Phys 82(12)
Ali MA, Kamil Reza K, Srivastava S, Agrawal VV, John R, Malhotra BD (2014) Lipid-lipid interactions in aminated reduced graphene oxide interface for biosensing application. Langmuir 30(14):4192–4201
Dubey R, Guruviah V (2019) Review of carbon-based electrode materials for supercapacitor energy storage. Ionics (Kiel) 25(4):1419–1445
Adhikari BR, Govindhan M, Chen A (2015) Carbon nanomaterials based electrochemical sensors/biosensors for the sensitive detection of pharmaceutical and biological compounds. Sensors (Switzerland) 15(9):22490–22508
Borenstein A, Hanna O, Attias R, Luski S (2017) Carbon-based composite materials for supercapacitor electrodes : a review. J Mater Chem A Mater Energy Sustain 5(25):12653–12672
Krishnamoorthy K, Veerapandian M, Yun K, Kim SJ (2013) The chemical and structural analysis of graphene oxide with different degrees of oxidation. Carbon N Y 53:38–49
Madhuvilakku R, Alagar S, Mariappan R, Piraman S (2017) Green one-pot synthesis of flowers-like Fe3O4/rGO hybrid nanocomposites for effective electrochemical detection of riboflavin and low-cost supercapacitor applications. Sensors Actuators B Chem 253:879–892
Pei S, Cheng HM (2012) The reduction of graphene oxide. Carbon N Y 50(9):3210–3228
Pumera M (2010) Graphene-based nanomaterials and their electrochemistry. Chem Soc Rev 39(11):4146–4157
Bai H, Li C, Shi G (2011) Functional composite materials based on chemically converted graphene. Adv Mater:1089–1115
Schniepp HC, Li J, Mcallister MJ et al (2006) Functionalized single graphene sheets derived from splitting graphite oxide. J Phys Chem B 2:8535–8539
Schwenke AM, Hoeppener S, Schubert US (2015) Microwave synthesis of carbon nanofibers-the influence of MW irradiation power, time, and the amount of catalyst. J Mater Chem A 3(47):23778–23787
Dubin S, Gilje S, Wang K, et al (2010) A one-step, solvothermal reduction method for producing reduced graphene oxide dispersions in organic solvents. Am Chem Soc 4:3845–3852
Sinan N, Unur E (2016) Fe3O4/carbon nanocomposite: investigation of capacitive & magnetic properties for supercapacitor applications. Mater Chem Phys 183:571–579
Li L, Gao P, Gai S, He F, Chen Y, Zhang M, Yang P (2016) Ultra small and highly dispersed Fe3O4 nanoparticles anchored on reduced graphene for supercapacitor application. Electrochim Acta 190:566–573
Zhang X, Sun X, Chen Y, Zhang D, Ma Y (2012) One-step solvothermal synthesis of graphene / Mn 3 O 4 nanocomposites and their electrochemical properties for supercapacitors. Mater Lett 68:336–339
Stankovich S, Dikin DA, Dommett GHB, Kohlhaas KM, Zimney EJ, Stach EA, Piner RD, Nguyen SBT, Ruoff RS (2006) Graphene-based composite materials. Nature 442(7100):282–286
Nguyen ST, Jung I, Dikin DA et al (2007) Graphene−silica composite thin films as transparent conductors. Nano Lett 7:1888–1892
Jadhav HS, Thorat GM, Kale BB, Seo JG (2017) Mesoporous Mn reduced graphene oxide (rGO) composite with enhanced electrochemical performance for Li-ion battery. Dalton Trans 46(30):9777–9783
Juan Yang A, Yu C (2016) Electroactive Edge site-enriched nickel-cobalt sulfide into graphene Frameworks for high-performance asymmetric supercapacitors. R Soc Chem 9:1299–1307
Zhao Y, Song X, Song Q, Yin Z (2012) A facile route to the synthesis copper oxide/reduced graphene oxide nanocomposites and electrochemical detection of catechol organic pollutant. R Soc Chem:6710–6719
Sreeprasad TS, Maliyekkal SM, Lisha KP, Pradeep T (2011) Reduced graphene oxide-metal/metal oxide composites : facile synthesis and application in water purification. J Hazard Mater 186(1):921–931
Chang MS, Kim T, Kang JH et al (2015) The effect of surface characteristics of reduced graphene oxide on the performance of a pseudocapacitor. 2D Mater 2:14007
Usman AA, Mashuri (2019) Magnetic properties of rGO/Fe3O4 microparticles composites based on natural materials. In: AIP Conference Proceedings
Mondal S, Rana U, Malik S (2017) Reduced graphene oxide/Fe3O4/polyaniline nanostructures as electrode materials for an all-solid-state hybrid supercapacitor. J Phys Chem C 121(14):7573–7583
Liang C, Zhai T, Wang W, Chen J, Zhao W, Lu X, Tong Y (2014) Fe3O4/reduced graphene oxide with enhanced electrochemical performance towards lithium storage. J Mater Chem A 2(20):7214–7220
Waifalkar PP, Chougale AD, Kollu P, Patil PS, Patil PB (2018) Magnetic nanoparticle decorated graphene based electrochemical nanobiosensor for H2O2 sensing using HRP. Colloids Surf B: Biointerfaces 167:425–431
Wasiński K, Walkowiak M, Półrolniczak P, Lota G (2015) Capacitance of Fe3O4/rGO nanocomposites in an aqueous hybrid electrochemical storage device. J Power Sources 293:42–50
Yu L, Wu H, Wu B (2014) Magnetic Fe3 O4-reduced graphene oxide nano-composites-based electrochemical biosensing. Nano Lett 6(3):258–267
Hoan NTV, Thu NTA, Van Duc H et al (2016) Fe3O4/Reduced graphene oxide nanocomposite: synthesis and its application for toxic metal ion removal. J Chemother 2016
Qin Y, Long M, Tan B, Zhou B (2014) RhB adsorption performance of magnetic adsorbent Fe3O4/RGO Composite and its regeneration through a Fenton-like reaction. Nano-Micro Lett 6(2):125–135
Liu S, Zhou L, Yao L, Chai L, Li L, Zhang G, Kankan, Shi K (2014) One-pot reflux method synthesis of cobalt hydroxide nanoflake-reduced graphene oxide hybrid and their NOx gas sensors at room temperature. J Alloys Compd 612:126–133
Zhu S, Chen M, Ren W, Yang J, Qu S, Li Z, Diao G (2015) Microwave assisted synthesis of α-Fe2O3/reduced graphene oxide as anode material for high performance lithium ion batteries. New J Chem 39(10):7923–7931
Liu Y, Guan M, Feng L, Deng S (2013) Facile and straightforward synthesis of superparamagnetic reduced graphene oxide – Fe 3 O 4 hybrid composite by a solvothermal reaction. Nanotechnology:025604
Singh RK, Kumar R, Singh DP (2016) Graphene oxide: strategies for synthesis, reduction and frontier applications. RSC Adv 6(69):64993–65011
Ullah W, Anwar AW, Majeed A et al (2015) Cost-effective and facile development of Fe 3 O 4 –reduced graphene oxide electrodes for supercapacitors. Mater Technol 30:144–149
Li T, Qin A, Yang L, Chen J, Wang Q, Zhang D, Yang H (2017) In situ grown Fe 2 O 3 single crystallites on reduced graphene oxide nanosheets as high performance conversion anode for sodium-ion batteries. ACS Appl Mater Interfaces 9(23):19900–19907
Yang S, Cao C, Li G, Sun Y, Huang P, Wei F, Song W (2015) Improving the electrochemical performance of Fe3O4 nanoparticles via a double protection strategy through carbon nanotube decoration and graphene networks. Nano Res 8(4):1339–1347
Peik-See T, Pandikumar A, Nay-Ming H, Hong-Ngee L, Sulaiman Y (2014) Simultaneous electrochemical detection of dopamine and ascorbic acid using an iron oxide/reduced graphene oxide modified glassy carbon electrode. Sensors (Switzerland) 14(8):15227–15243
Gao Y, Wu D, Wang T, Jia D, Xia W, Lv Y, Cao Y, Tan Y, Liu P (2016) One-step solvothermal synthesis of quasi-hexagonal Fe2O3 nanoplates/graphene composite as high performance electrode material for supercapacitor. Electrochim Acta 191:275–283
Qu QT, Wang B, Yang LC, Shi Y, Tian S, Wu YP (2008) Study on electrochemical performance of activated carbon in aqueous Li2SO4, Na2SO4 and K2SO4 electrolytes. Electrochem Commun 10(10):1652–1655
Barzegar F, Momodu DY, Fashedemi OO, Bello A, Dangbegnon JK, Manyala N (2015) Investigation of different aqueous electrolytes on the electrochemical performance of activated carbon-based supercapacitors. RSC Adv 5(130):107482–107487
Zhou D, Zhang TL, Han BH (2013) One-step solvothermal synthesis of an iron oxide-graphene magnetic hybrid material with high porosity. Microporous Mesoporous Mater 165:234–239
Habte AT, Ayele DW, Hu M (2019) Synthesis and characterization of reduced graphene oxide (rGO) started from graphene oxide (GO) using the tour method with different parameters. Adv Mater Sci Eng 2019:1–9
Online VA, Feng Z, Zhang C et al (2013) RSC Advances An easy and eco-friendly method to prepare reduced additive for LiFePO 4 cathode materials 3. R Soc Chem 3(4408–44):4408–4415
Shalaby A, Nihtianova D, Markov P et al (2015) Structural analysis of reduced graphene oxide by transmission electron microscopy. Bulg Chem Commun 47:291–295
Shen X, Wu J, Bai S, Zhou H (2010) One-pot solvothermal syntheses and magnetic properties of graphene-based magnetic nanocomposites. J Alloys Compd 506(1):136–140
Hardiansyah A, Rahimi Chaldun E, Fadyah Idzni A (2018) Magnetic reduced graphene oxide as advanced materials for adsorption of metal ions. J Sains Mater Indones 18(4):185
Li Y, Zhao C, Wen Y, Wang Y, Yang Y (2018) Adsorption performance and mechanism of magnetic reduced graphene oxide in glyphosate contaminated water. Environ Sci Pollut Res 25(21):21036–21048
Yan F, Ding J, Liu Y, Wang Z, Cai Q, Zhang J (2015) Fabrication of magnetic irregular hexagonal-Fe3O4 sheets/reduced graphene oxide composite for supercapacitors. Synth Met 209:473–479
Kumar R, Singh RK, Vaz AR, Savu R, Moshkalev SA (2017) Self-assembled and one-step synthesis of interconnected 3D network of Fe3O4/reduced graphene oxide nanosheets hybrid for high-performance supercapacitor electrode. ACS Appl Mater Interfaces 9(10):8880–8890
Devi P, Sharma C, Kumar P, Kumar M, Bansod BKS, Nayak MK, Singla ML (2017) Selective electrochemical sensing for arsenite using rGO/Fe 3 O 4 nanocomposites. J Hazard Mater 322(Pt A):85–94
Sriprachuabwong C, Karuwan C, Wisitsorrat A, Phokharatkul D, Lomas T, Sritongkham P, Tuantranont A (2012) Inkjet-printed graphene-PEDOT:PSS modified screen printed carbon electrode for biochemical sensing. J Mater Chem 22(12):5478–5485
Chandel M, Moitra D, Makkar P, Sinha H, Hora HS, Ghosh NN (2018) Synthesis of multifunctional CuFe 2 O 4 -reduced graphene oxide nanocomposite: an efficient magnetically separable catalyst as well as high performance supercapacitor and first-principles calculations of its electronic structures. RSC Adv 8(49):27725–27739
Alam M, Karmakar K, Pal M, Mandal K (2016) Electrochemical supercapacitor based on double perovskite Y2NiMnO6 nanowires. RSC Adv 6(115):114722–114726
Liu J, Dong S, He Q, Yang S, Xie M, Deng P, Xia Y, Li G (2019) Facile preparation of Fe3O4/C nanocomposite and its application for cost-effective and sensitive detection of tryptophan. Biomolecules 9(6)
Cai Z, Ye Y, Wan X et al (2019) Morphology–dependent electrochemical sensing properties of iron oxide–graphene oxide nanohybrids for dopamine and uric acid. Nanomaterials 9:1–19
Radhakrishnan S, Krishnamoorthy K, Sekar C et al (2014) Applied Catalysis B : Environmental A highly sensitive electrochemical sensor for nitrite detection based on Fe 2 O 3 nanoparticles decorated reduced graphene oxide nanosheets. Appl Catal B Environ 148–149:22–28
Srivastava S, Kumar V, Ali MA, Solanki PR, Srivastava A, Sumana G, Saxena PS, Joshi AG, Malhotra BD (2013) Electrophoretically deposited reduced graphene oxide platform for food toxin detection. Nanoscale 5(7):3043–3051
Thu NTA, Van Duc H, Hai Phong N et al (2018) Electrochemical determination of paracetamol using Fe3O4/reduced graphene-oxide-based electrode. J Nanomater 2018
Kiryushov VN, Skvortsova LI, Aleksandrova TP (2011) Electrochemical behavior of the system ferricyanide-ferrocyanide at a graphite-epoxy composite electrode. J Anal Chem 66(5):510–514
Xie Z, Xu J, Xie F, Xiong S (2016) Electrochemical detection of as(III) by a rGO/Fe 3 O 4 -modified screen-printed carbon electrode. Anal Sci 32(10):1053–1058
Zhang X, Wang X, Jiang L, Wu H, Wu C, Su J (2012) Effect of aqueous electrolytes on the electrochemical behaviors of supercapacitors based on hierarchically porous carbons. J Power Sources 216:290–296
Morris JB, Schempf JM (1959) Voltammetric studies at the graphite electrode in quiet solutions. Anal Chem 31(2):286–291
Liao W, Guo C, Sun L et al (2015) The electrochemical behavior of nafion/reduced graphene oxide modified carbon electrode surface and its application to ascorbic acid determination. Int J Electrochem Sci 10:5747–5755
Ghosh S, Mathews T, Gupta B, Das A, Gopala Krishna N, Kamruddin M (2017) Supercapacitive vertical graphene nanosheets in aqueous electrolytes. Nano-Struct Nano-Objects 10:42–50
Wang Z, Ma C, Wang H, Liu Z, Hao Z (2013) Facilely synthesized Fe2O3-graphene nanocomposite as novel electrode materials for supercapacitors with high performance. J Alloys Compd 552:486–491
Cheng JP, Shou QL, Wu JS, Liu F, Dravid VP, Zhang XB (2013) Influence of component content on the capacitance of magnetite/reduced graphene oxide composite. J Electroanal Chem 698:1–8
Ramachandran R, Saranya M, Velmurugan V, Raghupathy BPC, Jeong SK, Grace AN (2015) Effect of reducing agent on graphene synthesis and its influence on charge storage towards supercapacitor applications. Appl Energy 153:22–31
Wang D, Li Y, Wang Q, Wang T (2012) Nanostructured Fe 2O 3-graphene composite as a novel electrode material for supercapacitors. J Solid State Electrochem 16(6):2095–2102
Qi T, Jiang J, Chen H, Wan H, Miao L, Zhang L (2013) Synergistic effect of Fe3O4/reduced graphene oxide nanocomposites for supercapacitors with good cycling life. Electrochim Acta 114:674–680
Pal B, Yang S, Ramesh S, Thangadurai V, Jose R (2019) Electrolyte selection for supercapacitive devices: a critical review. Nanoscale Adv 1(10):3807–3835
Funding
The study was funded by the Science and Engineering Research Board, Department of Science and Technology (DST-SERB), Government of India (no. EMR/2017/001810) and Human Resources Development Program (no. 20194030202470) of the Korea Institute of Energy Technology Evaluation and Planning (KETEP) grant funded by the Korean Government Ministry of Trade, Industry and Energy.
Author information
Authors and Affiliations
Corresponding author
Additional information
Publisher’s note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary information
ESM 1
(DOCX 10109 kb)
Rights and permissions
About this article
Cite this article
Patil, S.M., Shingte, S.R., Karade, V.C. et al. Electrochemical performance of magnetic nanoparticle-decorated reduced graphene oxide (MRGO) in various aqueous electrolyte solutions. J Solid State Electrochem 25, 927–938 (2021). https://doi.org/10.1007/s10008-020-04866-x
Received:
Revised:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10008-020-04866-x