Optimization of Graphene Oxide Synthesis Using Hummers Method

Year 2024, , 1132 - 1152, 01.09.2024

Haluk Korucu

https://doi.org/10.35378/gujs.1357390

Cited By: 1

Abstract

In the processes of nanomaterial synthesis and characterization, it is important to explore and understand the relationships between variables and levels of processes by introducing experimental design methods and statistical approaches. The main goal of this work is to improve the quality of the graphene oxide (GO) that is made by using the TOPSIS-Based Taguchi Method and the L9(33) experimental design. Various parameters were chosen for experimentation, including samples of graphite with varying levels of purity (85%, 99%, and 99.99%). Prior to initiating the reaction, the graphite underwent pre-application, which involved diverse treatments such as no pre-processing, pre-heating at 200 °C, and ultrasonication. Additionally, different types of auxiliary oxidants (NaNO3, H3PO4, and Na2B4O710H2O) were employed. Raman spectroscopy was used to measure the peak intensity ratio (D/G) of the D peak and the G peak. X-ray diffraction (XRD) was employed to determine the crystal size (CS-nm). The surface area (SA-m2/g) was measured using the BET method. The average particle size (PS-nm) and the Zeta potential (ZP-mv) were determined using a Zeta-Sizer. The atomic ratio of carbon to oxygen (C/O) was also studied using scanning electron microscopy and energy-dispersive X-ray spectroscopy (SEM+EDX) to get a better understanding of graphene oxide (GO). The quality criteria's findings were assessed for each experiment using the TOPSIS-Based Taguchi Method, and the optimum circumstances were identified. The recovery rates for D/G, C/O, ZP, SA, PS, and CS were computed as 15.88%, 55.55%, 19.23%, -63.23%, -82.77%, and 20.79%, respectively. The utilization of low-purity graphite and boron compounds in the Hummers method yielded a favorable outcome in the synthesis of graphene oxide. When evaluating the experiment from an economic and environmentally conscious perspective, the results are quite impressive.

Keywords

Graphene oxide, Hummers method, Taguchi method, TOPSIS method

Ethical Statement

No conflict of interest was declared by the author. Ethical responsibility belongs to the author

Supporting Institution

Çankırı Karatekin Universty

Project Number

MF210621B08

Thanks

This research was carried out with the support of the Scientific Research Project (MF210621B08) funded by Çankırı Karatekin University. Author thank to Çankırı Karatekin University, Scientific Research Project Management Unit (ÇAKÜ-BAP).

References

• [1] Dreyer, D. R., Park, S., Bielawski, C.W., and Ruoff, R.S., “The chemistry of graphene oxide”, Chemical Society Reviews, 39: 228-240, (2009).
• [2] Chandio, A. D., Shaikh, A. A., Channa, I. A., Bacha, M. S., Bhatti, J., Khan, M. Y., Bhutto, S. “Synthesis of graphene oxide (GO) by modified Hummer's method with improved oxidation through Ozone Treatment”, Journal of the Chemical Society of Pakistan, 45: 128-136, (2023).
• [3] Silva, K. D., Huang, H. H., Joshi, R. K., Yoshimura, M., “Chemical reduction of graphene oxide using green reductants”, Carbon, 119:190-199, (2017).
• [4] Brodie, B. C., “On the atomic weight of graphite”, Philosophical Transactions of the Royal Society, 149: 249–259, (1859).
• [5] Staudenmaier, L., “Verfahren zur Darstellung der Graphitsäure”, Berichte der Deutschen Chemischen Gesellschaft, 31(2): 1481-1487, (1898)
• [6] Hummers, W. S., Offeman, R. E., “Preparation of graphitic oxide”, Journal of American Chemical Society, 80:1339, (1958),
• [7] Sujiono, E. H., Zumansyah, D., Dahlan M. Y., Amin B. D., Samnur, J., “Graphene oxide based coconut shell waste: synthesis by modified Hummers method and characterization”, Heliyon, 6: 4568-4566, (2020)
• [8] Bychko, I., Abakumov, A., Didenko, O., Chen, M., Tang, J., Strizhak P., “Differences in the structure and functionalities of graphene oxide and reduced graphene oxide obtained from graphite with various degrees of graphitization”, Journal of Physics and Chemistry of Solids, 164: 110614-110632, (2022),
• [9] Korucu, H., Mohamed, A. I., Yartaşı, A., Uğur, M., “The detailed Characterization of graphene oxide”, Chemical Papers, 77: 5787-57806, (2023).
• [10] Ahmad, H., Fan, M., Hui, D., “Graphene oxide incorporated meterials: A review”, Composites Part B, 145: 270-280, (2018).
• [11] Vazquez-Jaime, M., Arcibar-Orozco, J.A., Damian-Ascencio, C.E., Saldana-Robles, A.L., Martínez-Rosales M., Saldana-Robles A., Cano-Andrade, S., “Effective removal of arsenic from an aqueous solution by ferrihydrite/goethite graphene oxide composites using the modified Hummers method”, Journal of Environmental Chemical Engineering, 8: 104416-104428, (2020).
• [12] Zhu, Y., Kong, G., Pan, Y., Liu, L., Yang, B., Zhang, S., Lai, D., Che, C., “An improved Hummers method to synthesize graphene oxide using much less concentrated sulfuric acid”, Chinese Chemical Letters, 33(10): 4541-4544, (2022).
• [13] Zhang, J., Yang, H., Shen, G., Cheng, P., Zhang, J., Guo, S., “Reduction of graphene oxide via L-ascorbic acid”, Chemical Communications, 46(7): 1112-1114, (2010).
• [14] Zhang, Q., Yang, Y., Fan, H., Feng, L., Wen, G., Qin, L. C., “Synthesis of graphene oxide using boric acid in Hummers method”, Colloids and Surfaces A: Physicochemical and Engineering Aspects, 652: 129802-129011, (2022).
• [15] Mumcu Şımşek, H., and Gulıyev, R. A., ‘‘Taguchi Optimization Study about the Dissolution of Colemanite in Ammonium Bisulfate (NH4HSO4) Solution’’, Iranian Journal of Chemistry and Chemical Engineering, 41(8).2735-2742, (2022).
• [16] Küçük, Ö., Elfarah, K.T.T., Islak, S., Özarak, C., “Optimization by using Taguchi method of the production of magnesium-matrix carbide reinforced composites by powder metallurgy method”, Metals, 7(9): 352-364, (2017).
• [17] Çopur, M., Pekdemir, T., Kocakerim, M. M., Korucu, H., Guliyev, R., “Industrial symbiosis: Boron waste valorization through CO2 utilization”, Korean Journal of Chemical Engineering, 39(10): 2600-2614, (2022).
• [18] Taguchi, G., Chowdhury, S., Wu, Y., “Taguchi’s Quality Engineering Handbook” John Wiley and Sons, 1662, (2005).
• [19] Şimşek, B., “TOPSIS based taguchi design optimization for CVD growth of graphene using different carbon sources: Graphene thickness, defectiveness and homogeneity”, Chinese Journal of Chemical Enginnering, 27(3): 685-694, (2019).
• [20] Korucu, H., Şimşek B., Yartaşı A., “A TOPSIS-based Taguchi design to investigate optimum mixture proportions of graphene oxide powder synthesized by Hummers method”, Arabian Journal for Science and Engineering, 43(11): 6033–6055, (2018).
• [21] Korucu, H., “ Evaluation of the performance on reduced graphene oxide synthesized using ascorbic acid and sodium borohydride: experimental designs-based multi-response optimization applica tion”, Journal of Molecular Structure, 1268: 133715, (2022)
• [22] Simsek, B., Ultav, G.; Korucu, H.; Yartasi, A., “Improvement of the graphene oxide dispersion properties with the use of TOPSIS based Taguchi application”, Periodica Polytechnica-Chemical Engineering, 62(3): 11412-11425, (2018).