Role of Temperature and Time Exposure for Controlled and Accelerated Synthesis of Graphene Oxide Using Tour Method

https://doi.org/10.22146/ijc.71817

Uswatul Chasanah(1), Wega Trisunaryanti(2*), Haryo Satriya Oktaviano(3), Triyono Triyono(4), Dyah Ayu Fatmawati(5)

(1) Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Gadjah Mada, Sekip Utara, Yogyakarta 55281, Indonesia
(2) Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Gadjah Mada, Sekip Utara, Yogyakarta 55281, Indonesia
(3) Research & Technology Center, PT. Pertamina (Persero), Sopo Del Tower A, Floor 51, Jl. Mega Kuningan Barat III, Kawasan Mega Kuningan, Jakarta Selatan, DKI Jakarta, 12950, Indonesia
(4) Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Gadjah Mada, Sekip Utara, Yogyakarta 55281, Indonesia
(5) Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Gadjah Mada, Sekip Utara, Yogyakarta 55281, Indonesia
(*) Corresponding Author

Abstract


Synthesis of graphene oxide (GO) with the Tour method has been studied. In this procedure, phosphoric acid was mixed with sulfuric acid in the ratio of 1:9, and then potassium permanganate and graphite with the ratio of 6:1 was added in an ice bath at the variation of oxidation times of 1, 7 and 24 h and temperatures of 40, 50 and 60 °C. The GOs were characterized by UV–Visible spectroscopy, Fourier Transform InfraRed (FT-IR) spectroscopy, X-ray Diffraction (XRD), Scanning Electron Microscopy-Energy Dispersive X-Ray (SEM-EDX), and Transmission Electron Microscopy (TEM). The results show that the GO oxidized at 40 °C for 7 h (GO-7-40) has been successfully formed indicating that GO-7-40 is the most efficient GO. The GO-7-40 is characterized by a peak at 2θ = 10.89° in the XRD diffractogram, resulting calculation of the average distance between graphene layer (d) of 0.81 nm. The average number of graphene layers (n) is 4, the oxidation level (C/O) is 1.50 according to EDX data, λmax at 226 nm attributes to π→π* transitions of C=C bond in UV-Vis spectrum, and the functional groups such as O-H, C=C, C-OH, and C-OC are observed in FT-IR spectrum.

Keywords


graphene oxide; reducing time; temperature; Tour method

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References

[1] Thangavel, S., and Venugopal, G., 2014, Understanding the adsorption property of graphene-oxide with different degrees of oxidation levels, Powder Technol., 257, 141–148.

[2] Georgakilas, V., Otyepka, M., Bourlinos, A.B., Chandra, V., Kim, N., Kemp, K.C., Hobza, P., Zboril, R., and Kim, K.S., 2012, Functionalization of graphene: Covalent and non-covalent approaches, derivatives and applications, Chem. Rev., 112 (11), 6156–6214.

[3] Malik, R., Tomer, V.K., and Chaudhary, V., 2019, "Hybridized graphene for chemical sensing" in Functionalized Graphene Nanocomposites and Their Derivatives, Eds. Jawaid, M., Bouhfid, R., and Qaiss, A.K., Elsevier, Amsterdam, Netherlands, 323–338

[4] Gupta, K., and Khatri, O.P., 2017, Reduced graphene oxide as an effective adsorbent for removal of malachite green dye: Plausible adsorption pathways, J. Colloid Interface Sci., 501, 11–21.

[5] Gao, Y., Wu, J., Ren, X., Tan, X., Hayat, T., Alsaedi, A., Cheng, C., and Chen, C., 2017, Impact of graphene oxide on the antibacterial activity of antibiotics against bacteria, Environ. Sci.: Nano, 4 (5), 1016–1024.

[6] Saleh, T.A., and Fadillah, G., 2019, Recent trends in the design of chemical sensors based on graphene–metal oxide nanocomposites for the analysis of toxic species and biomolecules, TrAC, Trends Anal. Chem., 120, 115660.

[7] Tan, H.L., Denny, F., Hermawan, M., Wong, R.J., Amal, R., and Ng, Y.H., 2017, Reduced graphene oxide is not a universal promoter for photocatalytic activities of TiO2, J. Materiomics, 3 (1), 51–57.

[8] Gopalakrishnan, A., Krishnan, R., Thangavel, S., Venugopal, G., and Kim, S.J., 2015, Removal of heavy metal ions from pharma-effluents using graphene-oxide nanosorbents and study of their adsorption kinetics, J. Ind. Eng. Chem., 30, 14–19.

[9] Ajala, O.J., Tijani, J.O., Bankole, M.T., and Abdulkareem, A.S., 2022, A critical review on graphene oxide nanostructured material: Properties, synthesis, characterization and application in water and wastewater treatment, Environ. Nanotechnol. Monit. Manage., 18, 100673.

[10] Marcano, D.C., Kosynkin, D.V., Berlin, J.M., Sinitskii, A., Sun, Z., Slesarev, A., Alemany, L.B., Lu, W., and Tour, J.M., 2010, Improved synthesis of graphene oxide, ACS Nano, 4 (8), 4806–4814.

[11] Alshamkhani, M.T., Teong, L.K., Putri, L.K., Mohamed, A.R., Lahijani, P., and Mohammadi, M., 2021, Effect of graphite exfoliation routes on the properties of exfoliated graphene and its photocatalytic applications, J. Environ. Chem. Eng., 9 (6), 106506.

[12] Brodie, B.C., 1859, On the atomic weight of graphite, Philos. Trans. R. Soc. London, 149, 249–259.

[13] Staudenmaier, L., 1898, Verfahren zur darstellung der draphitsäure, Ber. Dtsch. Chem. Ges., 31, 1481–1487.

[14] Hummers, W.S., and Offeman, R.E., 1958, Preparation of graphitic oxide, J. Am. Chem. Soc., 80 (6), 1339.

[15] Zhu, Y., Kong, G., Pan, Y., Liu, L., Yang, B., Zhang, S., Lai, D., and Che, C., 2022, An improved Hummers method to synthesize graphene oxide using much less concentrated sulfuric acid, Chin. Chem. Lett., 33 (10), 4541–4544.

[16] Sali, S., Mackey, H.R., and Abdala, A.A., 2019, Effect of graphene oxide synthesis method on properties and performance of polysulfone-graphene oxide mixed matrix membranes, Nanomaterials, 9 (5), 769.

[17] Zaaba, N.I., Foo, K.L., Hashim, U., Tan, S.J., Liu, W.W., and Voon, C.H., 2017, Synthesis of graphene oxide using modified Hummers method: Solvent influence, Procedia Eng., 184, 469–477.

[18] Marcano, D.C., Kosynkin, D.V., Berlin, J.M., Sinitskii, A., Sun, Z., Slesarev, A.S., Alemany, L.B., Lu, W., and Tour, J.M., 2018, Correction to improved synthesis of graphene oxide, ACS Nano, 12 (2), 2078.

[19] Bychko, I., Abakumov, A., Didenko, O., Chen, M., Tang, J., and Strizhak, P., 2022, Differences in the structure and functionalities of graphene oxide and reduced graphene oxide obtained from graphite with various degrees of graphitization, J. Phys. Chem. Solids, 164, 110614.

[20] Romero, A., Lavin-Lopez, M.P., Sanchez-Silva, L., Valverde, J.L., and Paton-Carrero, A., 2018, Comparative study of different scalable routes to synthesize graphene oxide and reduced graphene oxide, Mater. Chem. Phys., 203, 284–292.

[21] Chen, J., Li, Y., Huang, L., Li, C., and Shi, G., 2015, High-yield preparation of graphene oxide from small graphite flakes via an improved Hummers method with a simple purification process, Carbon, 81, 826–834.

[22] Lavin-Lopez, M.P., Romero, A., Garrido, J., Sanchez-Silva, L., and Valverde, J.L., 2016, Influence of different improved hummers method modifications on the characteristics of graphite oxide in order to make a more easily scalable method, Ind. Eng. Chem. Res., 55 (50), 12836–12847.

[23] Park, J., Cho, Y.S., Sung, S.J., Byeon, M., Yang, S.J., and Park, C.R., 2018, Characteristics tuning of graphene-oxide-based-graphene to various end-uses, Energy Storage Mater., 14, 8–21.

[24] Benzait, Z., Chen, P., and Trabzon, L., 2021, Enhanced synthesis method of graphene oxide, Nanoscale Adv., 3 (1), 223–230.

[25] Boychuk, V.M., Kotsyubynsky, V.O., Bandura, K.V., Yaremiy, I.P., and Fedorchenko, S.V., 2019, Reduced graphene oxide obtained by Hummers and Marcano-Tour methods: Comparison of electrical properties, J. Nanosci. Nanotechnol., 19 (11), 7320–7329.

[26] Pendolino, F., Armata, N., Masullo, T., and Cuttitta, A., 2015, Temperature influence on the synthesis of pristine graphene oxide and graphite oxide, Mater. Chem. Phys.,164, 71–77.

[27] Olorunkosebi, A.A., Eleruja, M.A., Adedeji, A.V., Olofinjana, B., Fasakin, O., Omotoso, E., Oyedotun, K.O., Ajayi, E.O.B., and Manyala, N., 2021, Optimization of graphene oxide through various Hummers’ methods and comparative reduction using green approach, Diamond Relat. Mater., 117, 108456.

[28] Habte, A.T., and Ayele, D.W., 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, 5058163.

[29] Ranjan, P., Agrawal, S., Sinha, A., Rao, T.R., Balakrishnan, J., and Thakur, A.D., 2018, A low-cost non-explosive synthesis of graphene oxide for scalable applications, Sci. Rep., 8 (1), 12007.

[30] Kang, J.H., Kim, T., Choi, J., Park, J., Kim, Y.S., Chang, M.S., Jung, H., Park, K.T., Yang, S.J., and Park, C.R., 2016, Hidden second oxidation step of Hummers method, Chem. Mater., 28 (3), 756–764.

[31] Jara, A.D., and Kim, J.Y., 2020, Chemical purification processes of the natural crystalline flake graphite for Li-ion Battery anodes, Mater. Today Commun., 25, 101437.

[32] Suhaimin, N.S., Hanifah, M.F.R., Jusin, J.W., Jaafar, J., Aziz, M., Ismail, A.F., Othman, M.H.D., Abd Rahman, M., Aziz, F., Yusof, N., and Muhamud, M., 2021, Tuning the oxygen functional groups in graphene oxide nanosheets by optimizing the oxidation time, Phys. E, 131, 114727.

[33] Meng, L.Y., and Park, S.J., 2012, Preparation and characterization of reduced graphene nanosheets via pre-exfoliation of graphite flakes, Bull. Korean Chem. Soc., 33 (1), 209–214.

[34] Dimiev, A.M., and Tour, J.M., 2014, Mechanism of graphene oxide formation, ACS Nano, 8 (3), 3060–3068.

[35] Lee, D.W., De Los Santos V.L., Seo, J.W., Leon Felix, L., Bustamante D.A., Cole, J.M., and Barnes, C.H.W., 2010, The structure of graphite oxide: Investigation of its surface chemical groups, J. Phys. Chem. B, 114 (17), 5723–5728.

[36] Dubey, A., Bhavsar, N., Pachchigar, V., Saini, M., Ranjan, M., and Dube, C.L., 2021, Microwave assisted ultrafast synthesis of graphene oxide based magnetic nano composite for environmental remediation, Ceram. Int., 48 (4), 4821–4828.

[37] Roy, O., Jana, A., Pratihar, B., Saha, D.S., and De, S., 2021, Graphene oxide wrapped Mix-valent cobalt phosphate hollow nanotubes as oxygen evolution catalyst with low overpotential, J. Colloid Interface Sci., 610, 592–600.

[38] Shen, B., Lu, D., Zhai, W., and Zheng, W., 2013, Synthesis of graphene by low-temperature exfoliation and reduction of graphite oxide under ambient atmosphere, J. Mater. Chem. C, 1 (1), 50–53.

[39] Stobinski, L., Lesiak, B., Malolepszy, A., Mazurkiewicz, M., Mierzwa, B., Zemek, J., Jiricek, P., and Bieloshapka, I., 2014, Graphene oxide and reduced graphene oxide studied by the XRD, TEM and electron spectroscopy methods, J. Electron Spectrosc. Relat. Phenom., 195, 145–154.

[40] Kumar, V., Kumar, A., Lee, D.J., and Park, S.S., 2021, Estimation of number of graphene layers using different methods: A focused review, Materials, 14 (16), 4590.

[41] Paredes, J.I., Villar-Rodil, S., Martínez-Alonso, A., and Tascón, J.M.D., 2008, Graphene oxide dispersions in organic solvents, Langmuir, 24 (19), 10560–10564.

[42] Ding, H., Zhang, S., Chen, J.T., Hu, X.P., Du, Z.F., Qiu, Y.X., and Zhao, D.L., 2015, Reduction of graphene oxide at room temperature with vitamin C for RGO-TiO2 photoanodes in dye-sensitized solar cell, Thin Solid Films, 584, 29–36.

[43] Tammer, M., 2004, G. Sokrates: Infrared and Raman characteristic group frequencies: Tables and charts, Colloid Polym. Sci., 283 (2), 235.

[44] Lotfi, M., Yari, H., Sari, M.G., and Azizi, A., 2022, Fabrication of a highly hard yet tough epoxy nanocomposite coating by incorporating graphene oxide nanosheets dually modified with amino silane coupling agent and hyperbranched polyester-amide, Prog. Org. Coat., 162, 106570.

[45] Sahoo, P., Shubhadarshinee, L., Jali, B.R., Mohapatra, P., and Barick, A.K., 2021, Synthesis and characterization of graphene oxide and graphene from coal, Mater. Today: Proc., 56, 2421–2427.

[46] Fadillah, G., Saleh, T.A., Wahyuningsih, S., Ninda Karlina Putri, E., and Febrianastuti, S., 2019, Electrochemical removal of methylene blue using alginate-modified graphene adsorbents, Chem. Eng. J., 378, 122140.

[47] Cao, H., Wu, X., Yin, G., and Warner, J.H., 2012, Synthesis of adenine-modified reduced graphene oxide nanosheets, Inorg. Chem., 51 (5), 2954–2960.

[48] Liu, F., Cao, Y., Yi, M., Xie, L., Huang, W., Tang, N., Zhong, W., and Du, Y., 2013, Thermostability, photoluminescence, and electrical properties of reduced graphene oxide-carbon nanotube hybrid materials, Crystals, 3 (1), 28–37.

[49] Geng, J., Liu, L., Yang, S.B., Youn, S.C., Kim, D.W., Lee, J.S., Choi, J.K., and Jung, H.T., 2010, A simple approach for preparing transparent conductive graphene films using the controlled chemical reduction of exfoliated graphene oxide in an aqueous suspension, J. Phys. Chem. C, 114 (34), 14433–14440.

[50] Eda, G., and Chhowalla, M., 2010, Chemically derived graphene oxide: Towards large-area thin-film electronics and optoelectronics, Adv. Mater., 22 (22), 2392–2415.

[51] Fadillah, G., Wicaksono, W.P., Fatimah, I., and Saleh, T.A., 2020, A sensitive electrochemical sensor based on functionalized graphene oxide/SnO2 for the determination of eugenol, Microchem. J., 159, 105353.

[52] You, S., Luzan, S.M., Szabó, T., and Talyzin, A.V., 2013, Effect of synthesis method on solvation and exfoliation of graphite oxide, Carbon, 52, 171–180.

[53] Jung, I., Field, D.A., Clark, N.J., Zhu, Y., Yang, D., Piner, R.D., Stankovich, S., Dikin, D.A., Geisler, H., Ventrice, C.A., and Ruoff, R.S., 2009, Reduction kinetics of graphene oxide determined by electrical transport measurements and temperature programmed desorption, J. Phys. Chem. C, 113 (43), 18480–18486.

[54] Tambe, P., 2021, Synthesis and characterization of acid treated reduced graphene oxide, Mater. Today: Proc., 49, 1294–1297.

[55] Chasanah, U., Trisunaryanti, W., Triyono, T., Oktaviano, H.S., and Fatmawati, D.A., 2021, The performance of green synthesis of graphene oxide prepared by modified Hummers method with oxidation time variation, Rasayan J. Chem., 14 (3), 2017–2023.



DOI: https://doi.org/10.22146/ijc.71817

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