Investigation of Evolution in the Synthesis of Graphene Oxide and Reduced Graphene Oxide

Document Type : Research Article

Authors

1 Department of Physics, University of Agriculture, Faisalabad, PAKISTAN

2 Pakistan Nuclear Regulatory Authority (PNRA), Islamabad, PAKISTAN

3 National Institute of Fundamental Studies, SRI LANKA

Abstract

Hummer’s method, in which potassium permanganate (KMnO4) acts as the oxidant and concentrated sulfuric acid (H2SO4) serves as the intercalator is commonly used to prepare Graphene Oxide (GO). The amount of the intercalator, oxidant, and graphite are important factors that affect the properties and structure of graphene oxide. In this work, a detailed investigation is carried out to optimize the mechanism of Hummer’s method in order to get the maximum yield of GO and reduced graphene oxide (rGO). XRD, SEM, TEM, FT-IR, TGA, Raman spectroscopy, and UV-Visible spectroscopy are used for characterization. XRD results of optimized samples (Opt-3-GO and Opt-3-rGO) clearly showed that the value of interlayer spacing is increased due to increasing the amount of oxidant and intercalator. SEM and TEM results revealed that the Opt-3-rGO was highly wrinkled nanosheets as compared to the Opt-3-GO. The FT-IR results showed that the double amount of oxidant and intercalator had an effect on the functional groups in the structure of Opt-3-GO and Opt-3-rGO. TGA results indicated that Opt-3-rGO has higher thermal stability as compared to Opt-3-GO due to the lower defect density. The ratio of intensities of D and G bands (ID/IG) increased for Opt-3-rGO as compared to Opt-3-GO. UV-Vis spectra of Opt-3-GO showed a maximum absorption peak at 237 nm attributable to π-π* transition of the atomic C-C bonds. The prepared samples have their use in different applications such as electrode materials for batteries, capacitors, and solar cells.

Keywords

Main Subjects


[1] Alkhouzaam A., Qiblawey H., Khraisheh M., Atieh M., Al-Ghouti M., Synthesis of Graphene Oxides Particle of High Oxidation Degree Using a Modified Hummers Method, J. Ceramics International, 46(15): 23997–24007 (2020).
[2] Benzait Z., Chen P., Trabzon L., Enhanced Synthesis Method of Graphene Oxide, J. Nanoscale Adv, 3(1): 223–230 (2021).
[3] Abaszade R.G., Mamedova S.A., Agayev F.H., Budzulyak S.I., Kapush O.A., Mamedova M.A., Nabiyev A.M., Kotsyubynsky V.O., Synthesis and Characterization of Graphene Oxide Flakes for Transparent Thin Films, J. Phys. Chem. Solid State, 22(3): 595–60 (2021).
[5] Nasreen F., Anwar A. W., Ahmad M. A., Majeed A., Afzal A., Hussain T., A Facile Improved Oxidation Method for Ecological Production of Graphene Oxide, J. Dig. J. Nanomater. Biostructures, 16(1): 119–124 (2021).
[6] Alkhouzaam A., Qiblawey H., Khraisheh M., Atieh M., Al-Ghouti M., Synthesis of Graphene Oxides Particle of High Oxidation Degree using a Modified Hummers Method, J. Ceramics International, 46(15): 23997-24007 (2020).
[7] Manabe S., Kiliyankil S.A., Takiguchi S., Kumashiro T., Fugetsu B., Sakata I., Graphene Nanosheets Homogeneously Incorporated in Polyurethane Sponge for the Elimination of Water-Soluble Organic DyesJ. of Colloid and Interface Science, 584: 816-826 (2021).  
[8] Lee K.E., Kim J.E., Maiti U.N., Lim J., Hwang J.O., Shim J., Kim S.O., Liquid Crystal Size Selection of Large-Size Graphene Oxide for Size-Dependent N-Doping and Oxygen Reduction CatalysisJ. ACS Nano8(9): 9073-9080 (2014).
[9] Ma H., Li C., Zhang M., Hong J.D., Shi G., Graphene Oxide Induced Hydrothermal Carbonization of Egg Proteins for High-Performance Supercapacitors, J. Materials Chemistry A, 5(32): 17040-17047 (2017).  
[11] El-Khodary S.A., El-Enany G.M., El-Okr M., Ibrahim M., Preparation and Characterization of Microwave Reduced Graphite Oxide for High-Performance Supercapacitors, J. Electrochimica Acta, 150: 269-278 (2014).
[12] Quitain A.T., Sumigawa Y., Mission E.G., Sasaki M., Assabumrungrat S., Kida T., Graphene Oxide and Microwave Synergism for Efficient Esterification of Fatty AcidsJ. Energy & Fuels32(3): 3599-3607 (2018).
[13] Chen J., Yao B., Li C., Shi G., An Improved Hummers Method for Eco-Friendly Synthesis of Graphene OxideJ. Carbon, 64: 225-229 (2013).
[14] Wu T.T., Ting J.M., Preparation and Characteristics of Graphene Oxide and its Thin FilmsJ. surface and coatings technology, 231: 487-491 (2013).
[15] Mombeshora E.T., Ndungu P.G., Nyamori V.O., Effect of Graphite/Sodium Nitrate Ratio and Reaction Time
on the Physicochemical Properties of Graphene Oxide
, J. New Carbon Materials32(2): 174-187 (2017).
[16] Holm A., Park J., Goodman E.D., Zhang J., Sinclair R., Cargnello M., Frank C.W., Synthesis, Characterization, and Light-Induced Spatial Charge Separation in Janus Graphene Oxide, J. Chem. of Materials30(6): 2084-2092 (2018).
[17] Marcano D.C., Kosynkin D.V., Berlin J.M., Sinitskii A., Sun Z., Slesarev A., Tour J.M., Improved Synthesis of Graphene OxideJ. ACS Nano, 4(8): 4806-4814 (2010).
[18] Chen Z, Liu Y., Luo J., Tribological Properties of Few-Layer Graphene Oxide Sheets as Oil-Based Lubricant Additives, Chinese J. Mechanical Engineering29(2): 439-444 (2016).
[19] Shojaeenezhad S.S., Farbod M., Kazeminezhad I., Effects of Initial Graphite Particle Size and Shape on Oxidation Time in Graphene Oxide Prepared by Hummers' Method, J. Sci. Adv. Materials and Devices, 2(4): 470-475 (2017).
[20] Dimiev A.M., Bachilo S.M, Saito R., Tour J.M., Reversible Formation of Ammonium Persulfate/Sulfuric Acid Graphite Intercalation Compounds and Their Peculiar Raman Spectra, J. ACS Nano6(9): 7842-7849 (2012).
[21] Liou Y.J., Tsai B.D., Huang W.J, An Economic Route to Mass Production of Graphene Oxide Solution for Preparing Graphene Oxide Papers, J. Materials Science and Engineering: B193: 37-40 (2015).
[22] Cao J., Wang Y., Xiao P., Chen Y., Zhou Y., Ouyang J.H., Jia D, Hollow Graphene Spheres Self-Assembled from Graphene Oxide Sheets by a One-Step Hydrothermal Process, J. Carbon56: 389-391 (2013).
[23] Guo P., Song H., Chen X, Hollow Graphene Oxide Spheres Self-Assembled by W/O Emulsion, J. Materials Chemistry20(23): 4867-4874 (2010).
[24] Sharifzadeh E., Parsnasab M, Direct and Reverse Desymmetrization Process in O/W Pickering Emulsions to Produce Hollow Graphene Oxide Janus Micro/Nano-Particles, J. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 619: 126522 (2021).
[27] Huh S.H., Choi S.H., Ju H.M., Song C.K., Park S.H., Kim B.M, A Catalytic Graphene Oxide Film for a Dye-Sensitized Solar Cell, J. the Korean Physical Society57(6): 1653-1656 (2010).
[28] Chen J., Yao B., Li C., Shi G., An Improved Hummers Method for Eco-Friendly Synthesis of Graphene Oxide, J. Carbon, 64: 225-229 (2013).
[29] Guo H.L., Wang X.F., Qian Q.Y., Wang F.B., Xia X.H., A Green Approach to the Synthesis of Graphene Nanosheets, J. ACS Nano3(9): 2653-2659 (2009).  
[31] Teong S.P., Li X., Zhang Y., Hydrogen Peroxide as An Oxidant in Biomass-to-Chemical Processes of Industrial Interest, J. Green Chemistry21(21): 5753-5780 (2019).
[32] Zhu Y., Murali S., Cai W., Li X., Suk J.W., Potts J.R., Ruoff R.S., Graphene and Graphene Oxide: Synthesis, Properties, and Applications, J. Adv. Materials22(35): 3906-3924 (2010).
[33] Shahriary L., Athawale A.A., Graphene Oxide Synthesized by using Modified Hummers ApproachInt. J. Renew. Energy Environ. Eng, 2(1): 58-63 (2014).
[34] Kumar D., Singh K., Verma V., Bhatti H.S., Synthesis, Structural and Optical Characterization of Graphene Oxide and Reduced Graphene Oxide, J. Nanoelectronics and Optoelectronics, 9(4): 458-467 (2014). 
[35] Lai Q., Zhu S., Luo X., Zou M., Huang S., Ultraviolet-Visible Spectroscopy of Graphene Oxides, J. Aip. Adv., 2(3): 032146 (2012).