najoNanosystems: Physics, Chemistry, MathematicsНаносистемы: физика, химия, математика2220-80542305-7971Университет ИТМО10.17586/2220-8054-2023-14-3-380-389najo-330Research ArticleCHEMISTRY AND MATERIALS SCIENCEХИМИЯ И НАУКА О МАТЕРИАЛАХSynthesis and characterization of one pot electrochemical graphene for supercapacitor applicationsОдностадийный синтез и характеристика электрохимического графена для применения в суперконденсаторах»https://orcid.org/0000-0002-4998-7497Нареш МутхуР.Naresh MuthuR.

Р. Нареш Мутху - Кафедра физики

Тенкаси – 627852, Тамилнад

R. Naresh Muthu – Department of Physics

Tenkasi – 627852, Tamilnadu

rnaresh7708@gmail.comКолледж искусств и наук JP (филиал Университета Манонманиам Сундаранар, Тирунелвели)J. P. College of Arts and Science (affiliated to Manonmaniam Sundaranar University)202330062025143380389Copyright © Naresh Muthu R., 20252025Нареш Мутху Р.Naresh Muthu R.Данная работа распространяется под лицензией Creative Commons Attribution 4.0.This work is licensed under a Creative Commons Attribution 4.0 License.https://nanojournal.ifmo.ru/jour/article/view/330

Graphene can be used to store energy as well as a supercapacitor material because of its unique physical and chemical properties, including high specific surface area, high chemical stability, high mechanical strength, and oxidation resistance. In this report, a facile, green, and cost-effective approach has been adopted to synthesize graphene sheets through an electrochemical exfoliation technique for supercapacitor applications. Graphene sheets were synthesized using aqueous electrolyte (Ag/AgCl, 0.1 M H2SO4) with four different exfoliation potentials such as 3, 5, 7 and 9 V. The prepared graphene sheets were subjected to characterization techniques such as Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and atomic force microscopy (AFM). The Raman results revealed that the defect density and thickness of the graphene layers increased with increased in the exfoliation potential and then eventually decreased. Among all potentials, the maximum crystalline size of graphene was observed for the potential of 5 V, an intermediate crystalline size of 9 V, and minimum for 7 V, showing that the exfoliated graphene layer was sensitive to the exfoliation potential. XPS study shows the structural oxidation (relative percentage of carbon and oxygen) of the exfoliated graphene at different potentials. The results indicate that electrochemically exfoliated graphene (5 V) has been successfully produced. The behaviour of 5 V graphene has been examined using a charge-discharge (CD) curve and cyclic voltammetry (CV) for supercapacitor applications. The maximum value of specific capacitance obtained is 198 F g-1 at a current density of 0.14 A g-1 in 6 M KOH. The highest value obtained for energy density and power density is 17 W h kg-1 and 1176 W kg-1.

Графен можно использовать для хранения энергии, а также в качестве материала для суперконденсаторов благодаря его уникальным физическим и химическим свойствам, включая высокую удельную поверхность, высокую химическую стабильность, высокую механическую прочность и стойкость к окислению.

 В представленной работе использовался простой, экологически чистый и экономичный подход к синтезу листов графена с помощью метода электрохимического расслоения для дальнейшего применения в суперконденсаторах.

Листы графена были синтезированы с использованием водного электролита (Ag/AgCl, 0,1 М H2SO4) с четырьмя различными потенциалами расслаивания – 3В, 5В, 7В и 9В. Подготовленные листы графена были охарактеризованы набором методов физико-химического анализа, включающим рамановскую спектроскопию, фотоэлектронную спектроскопию (XPS), рентгеновскую дифракцию (XRD) и атомно-силовую микроскопию (АСМ).

Результаты комбинационного рассеяния показали, что плотность дефектов и толщина графеновых слоев увеличивались с увеличением потенциала расслоения, а затем в конечном итоге уменьшались. Среди всех потенциалов максимальный размер кристаллов графена наблюдался при потенциале 5В, промежуточный размер кристаллов 9В и минимум при 7В, что свидетельствует о том, что эксфолиированный слой графена чувствителен к потенциалу эксфолиации.

Исследование XPS показывает структурное окисление (относительное процентное содержание углерода и кислорода) расслоенного графена при различных потенциалах. Поведение графена при напряжении 5В было исследовано с использованием кривой заряда-разряда (CD) и циклической вольтамперометрии (CV) для применения в суперконденсаторах. Максимальное полученное значение удельной емкости составляет 198 Ф∙г-1 при плотности тока 0,14 А∙г-1 в 6М растворе КОН. Наибольшее значение, полученное для плотности энергии и удельной мощности, составляет 17 Вт·ч·кг-1 и 1176 Вт·кг-1.

графенэлектрохимическое расслоениесуперконденсатор и EDLCgrapheneelectrochemical exfoliationsupercapacitorEDLCReferencesZhong C., Deng Y., Hu W., Qiao J., Zhang L., Zhang J. A review of electrolyte materials and compositions for electrochemical supercapacitors. Chem. Soc. Rev., 2015, 44 (21), P. 7484–7539.Zhong C., Deng Y., Hu W., Qiao J., Zhang L., Zhang J. A review of electrolyte materials and compositions for electrochemical supercapacitors. Chem. Soc. Rev., 2015, 44 (21), P. 7484–7539.Muthu R.N., Tatiparti S.S.V. Electrochemical Behavior of Cobalt Oxide/Boron-Incorporated Reduced Graphene Oxide Nanocomposite Electrode for Supercapacitor Applications. J. of Mater. Eng. and Perform., 2020, 29, P. 6535–6549.Muthu R.N., Tatiparti S.S.V. Electrochemical Behavior of Cobalt Oxide/Boron-Incorporated Reduced Graphene Oxide Nanocomposite Electrode for Supercapacitor Applications. J. of Mater. Eng. and Perform., 2020, 29, P. 6535–6549.Zhong Y., Zhen Z., Zhu H. Graphene: Fundamental research and potential applications. FlatChem, 2017, 4, P. 20–32.Zhong Y., Zhen Z., Zhu H. Graphene: Fundamental research and potential applications. FlatChem, 2017, 4, P. 20–32.Rodr´ıguez-Pe´rez L., Herranz M.A´., Mart´ın N. The chemistry of pristine graphene. Chem. Commun., 2013, 49 (36), P. 3721–3735.Rodr´ıguez-Pe´rez L., Herranz M.A´., Mart´ın N. The chemistry of pristine graphene. Chem. Commun., 2013, 49 (36), P. 3721–3735.Liu C., Yu Z., Neff D., Zhamu A., Jang B.Z. Graphene-based supercapacitor with an ultrahigh energy density. Nano Lett., 2010, 10 (12), P. 4863– 4868.Liu C., Yu Z., Neff D., Zhamu A., Jang B.Z. Graphene-based supercapacitor with an ultrahigh energy density. Nano Lett., 2010, 10 (12), P. 4863– 4868.Jibrael R.I., Mohammed M.K.A. Production of graphene powder by electrochemical exfoliation of graphite electrodes immersed in aqueous solution. Optik (Stuttg)., 2016, 127 (16), P. 6384–6389.Jibrael R.I., Mohammed M.K.A. Production of graphene powder by electrochemical exfoliation of graphite electrodes immersed in aqueous solution. Optik (Stuttg)., 2016, 127 (16), P. 6384–6389.Chen J., Li Y., Huang L., Li C., Shi G. High-yield preparation of graphene oxide from small graphite flakes via an improved Hummers method with a simple purification process. Carbon N.Y., 2015, 81 (1), P. 826–834.Chen J., Li Y., Huang L., Li C., Shi G. High-yield preparation of graphene oxide from small graphite flakes via an improved Hummers method with a simple purification process. Carbon N.Y., 2015, 81 (1), P. 826–834.Pei S., Wei Q., Huang K., Cheng H.M., Ren W. Green synthesis of graphene oxide by seconds timescale water electrolytic oxidation. Nat. Commun., 2018, 9 (1), P. 1–9.Pei S., Wei Q., Huang K., Cheng H.M., Ren W. Green synthesis of graphene oxide by seconds timescale water electrolytic oxidation. Nat. Commun., 2018, 9 (1), P. 1–9.Muthu R.N, Tatiparti S.S.V. Electrode and symmetric supercapacitor device performance of boron-incorporated reduced graphene oxide synthesized by electrochemical exfoliation. Energy Storage, 2020, 2, e134.Muthu R.N, Tatiparti S.S.V. Electrode and symmetric supercapacitor device performance of boron-incorporated reduced graphene oxide synthesized by electrochemical exfoliation. Energy Storage, 2020, 2, e134.Arunkumar M., Amit P. Importance of Electrode Preparation Methodologies in Supercapacitor Applications. ACS Omega, 2017, 2 (11), P. 8039– 8050.Arunkumar M., Amit P. Importance of Electrode Preparation Methodologies in Supercapacitor Applications. ACS Omega, 2017, 2 (11), P. 8039– 8050.Pandit B., Dubal D.P., Sankapal B.R. Large scale flexible solid state symmetric supercapacitor through inexpensive solution processed V2O5 complex surface architecture. Electrochim. Acta, 2017, 242, P. 382–389.Pandit B., Dubal D.P., Sankapal B.R. Large scale flexible solid state symmetric supercapacitor through inexpensive solution processed V2O5 complex surface architecture. Electrochim. Acta, 2017, 242, P. 382–389.Rold´an S., Barreda D., Granda M., Men´endez R., Santamar´ıa R., Blanco C. An approach to classification and capacitance expressions in electrochemical capacitors technology. Phys. Chem. Chem. Phys., 2015, 17 (2), P. 1084–1092.Rold´an S., Barreda D., Granda M., Men´endez R., Santamar´ıa R., Blanco C. An approach to classification and capacitance expressions in electrochemical capacitors technology. Phys. Chem. Chem. Phys., 2015, 17 (2), P. 1084–1092.Das A.K., et al. Iodide-mediated room temperature reduction of graphene oxide: A rapid chemical route for the synthesis of a bifunctional electrocatalyst. J. Mater. Chem. A, 2014, 2 (5), P. 1332–1340.Das A.K., et al. Iodide-mediated room temperature reduction of graphene oxide: A rapid chemical route for the synthesis of a bifunctional electrocatalyst. J. Mater. Chem. A, 2014, 2 (5), P. 1332–1340.Kakaei K., Alidoust E., Ghadimi G. Synthesis of N- doped graphene nanosheets and its composite with urea choline chloride ionic liquid as a novel electrode for supercapacitor. J. Alloys Compd., 2018, 735, P. 1799–1806.Kakaei K., Alidoust E., Ghadimi G. Synthesis of N- doped graphene nanosheets and its composite with urea choline chloride ionic liquid as a novel electrode for supercapacitor. J. Alloys Compd., 2018, 735, P. 1799–1806.Nguyen V.T., Le H.D., Nguyen V.C., Ngo T.T.T., Le D.Q., Nguyen X.N., Phan N.M. Synthesis of multi-layer graphene films on copper tape by atmospheric pressure chemical vapor deposition method. Adv. Nat. Sci. Nanosci. Nanotechnol., 2013, 4 (3), 035012.Nguyen V.T., Le H.D., Nguyen V.C., Ngo T.T.T., Le D.Q., Nguyen X.N., Phan N.M. Synthesis of multi-layer graphene films on copper tape by atmospheric pressure chemical vapor deposition method. Adv. Nat. Sci. Nanosci. Nanotechnol., 2013, 4 (3), 035012.Bindumadhavan K., Chang P-Y., Doong R-a. Silver nanoparticles embedded boron-doped reduced graphene oxide as anode material for high performance lithium ion battery. Electrochimica Acta, 2017, 243, P. 282–290.Bindumadhavan K., Chang P-Y., Doong R-a. Silver nanoparticles embedded boron-doped reduced graphene oxide as anode material for high performance lithium ion battery. Electrochimica Acta, 2017, 243, P. 282–290.Pullamsetty A., Subbiah M., Sundara R. Platinum on boron doped graphene as cathode electrocatalyst for proton exchange membrane fuel cells. Int. J. Hydrogen Energy, 2015, 40 (32), P. 10251–10261.Pullamsetty A., Subbiah M., Sundara R. Platinum on boron doped graphene as cathode electrocatalyst for proton exchange membrane fuel cells. Int. J. Hydrogen Energy, 2015, 40 (32), P. 10251–10261.Muthu R.N, Rajashabala S., Kannan R. Facile synthesis and characterization of a reduced graphene oxide/halloysite nanotubes/hexagonal boron nitride (RGO/HNT/h-BN) hybrid nanocomposite and its potential application in hydrogen storage. RSC Adv., 2016, 6, P. 79072.Muthu R.N, Rajashabala S., Kannan R. Facile synthesis and characterization of a reduced graphene oxide/halloysite nanotubes/hexagonal boron nitride (RGO/HNT/h-BN) hybrid nanocomposite and its potential application in hydrogen storage. RSC Adv., 2016, 6, P. 79072.Gong Y., Li D., Fu Q., Pan C. Influence of graphene microstructures on electrochemical performance for supercapacitors. Progress in Natural Science: Materials International, 2015, 25 (5), P. 379–385.Gong Y., Li D., Fu Q., Pan C. Influence of graphene microstructures on electrochemical performance for supercapacitors. Progress in Natural Science: Materials International, 2015, 25 (5), P. 379–385.

The authors declare that there are no conflicts of interest present.