Research Article
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The Role of Water on the Oxidation Process of Graphene Oxide Structures

Year 2024, Volume: 28 Issue: 3, 567 - 578, 30.06.2024
https://doi.org/10.16984/saufenbilder.1337974

Abstract

Graphene oxide (GO) has recently attracted attention with its unique chemical and physical properties and serves as a raw material for graphene-based materials. GO has been produced for decades by the Hummers Method with the oxidation process of graphite. The properties and structure of GO are significantly affected by the production parameters of Hummers Method. In this study, the effect of the water content on the oxidation level of GO structure was investigated. GO was produced with different amounts of water in the oxidation stage of Hummers Method. The structural characterizations of produced GO were carried out by X-ray Diffraction Technique (XRD), Fourier Transform Infrared Spectroscopy (FTIR), X-ray Photoelectron Spectroscopy (XPS), Energy Dispersive X-ray Spectroscopy (EDS), UV-Visible Spectroscopy (UV-Vis) and Raman Spectroscopy. Additionally, morphological and thermal characterization of the produced GO samples were performed by Scanning Electron Microscopy (SEM) and Thermogravimetric Analysis (TGA)/Differential Thermal Analysis (DTA), respectively. According to XRD, FTIR, XPS, and EDS results, it was determined that the oxidation degree of GO decreased with increasing amount of water. Besides, it was revealed that the post-oxidation step generated more defects in the basal plane of graphene according to the results of the Raman Analysis. Also, it was observed that GO had a smoother surface and was found to have higher thermal stability with increasing amounts of water. The results show that the post-oxidation step reduces the oxidation degree of GO, increases the amount of the defect, provides a less wrinkled structure, and improves the thermal stability of GO.

Supporting Institution

Manisa Celal Bayar Üniversitesi

Project Number

2020-038

Thanks

Authors would like to thank Dokuz Eylul University (DEU) Department of Metallurgical and Materials Engineering and Center for Fabrication and Application of Electronic Materials for valuable supports. Authors would also like to thank Arifmert Cen, Ceyda Otlu, Yunus Emre Demir and Cem İnci for their support in laboratory studies.

References

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  • [3] J. Chen, B. Yao, C. Li, G. Shi, “An improved Hummers method for eco-friendly synthesis of graphene oxide,” Carbon, vol. 64, no. 1, pp. 225–229, 2013.
  • [4] W. S. Koe, J. W. Lee, W. C. Chong, Y. L. Pang, L. C. Sim, “An overview of photocatalytic degradation: photocatalysts, mechanisms, and development of photocatalytic membrane,” Environmental Science and Pollution Research, vol. 27, no. 3, pp. 2522–2565, 2020.
  • [5] T. A. Saleh, G. Fadillah, “Recent trends in the design of chemical sensors based on graphene–metal oxide nanocomposites for the analysis of toxic species and biomolecules,” Trends in Analytical Chemistry, vol. 120, 2019.
  • [6] R. K. Joshi, S. Alwarappan, M. Yoshimura, V. Sahajwalla, Y. Nishina, “Graphene oxide: the new membrane material,” Applied Materials Today, vol. 1, no. 1, pp. 1–12, 2015.
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  • [12] V. Panwar, A. Chattree, K. Pal, “A new facile route for synthesizing of graphene oxide using mixture of sulfuric-nitric-phosphoric acids as intercalating agent,” Physica E: Low-Dimensional Systems and Nanostructures, vol. 73, pp. 235–241, 2015.
  • [13] M. D. P. Lavin-Lopez, A. Romero, J. Garrido, L. Sanchez-Silva, J. L. Valverde, “Influence of Different Improved Hummers Method Modifications on the Characteristics of Graphite Oxide in Order to Make a More Easily Scalable Method,” Industrial & Engineering Chemistry Research, vol. 55, no. 50, pp. 12836–12847, 2016.
  • [14] D. Yang, A. Velamakanni, G. Bozoklu, S. Park, M. Stoller, R. D. Piner, S. Stankovich, I. Jung, D. A. Field, C. A. Ventrice, R. S. Ruoff, “Chemical analysis of graphene oxide films after heat and chemical treatments by X-ray photoelectron and Micro-Raman spectroscopy,” Carbon, vol. 47, no. 1, pp. 145–152, 2009.
  • [15] S. Eigler, A. M. Dimiev, “Characterization Techniques,” in Graphene Oxide: Fundamentals and Applications, A. M. Dimiev and S. Eigler, Eds., United Kingdom: John Wiley & Sons, 2016, pp. 85–118.
  • [16] B. C. Brodie, “XIII. On the atomic weight of graphite,” Philosophical Transactions of the Royal Society of London, vol. 149, no. 1, pp. 249–259, 1859.
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  • [19] F. Boran, S. Çetinkaya Gürer, “The effect of starting material types on the structure of graphene oxide and graphene,” Turkish Journal of Chemistry, vol. 43, no. 5, pp. 1322–1335, 2019.
  • [20] L. J. Cote, J. Kim, Z. Zhang, C. Sun, J. Huang, “Tunable assembly of graphene oxide surfactant sheets: wrinkles, overlaps and impacts on thin film properties,” Soft Matter, vol. 6, no. 24, p. 6096, 2010.
  • [21] J. H. Kang, T. Kim, J. Choi, J. Park, Y. S. Kim, M. S. Chang, H. Jung, K. T. Park, S. J. Yang, C. R. Park, “Hidden Second Oxidation Step of Hummers Method,” Chemistry of Materials, vol. 28, no. 3, pp. 756–764, 2016.
  • [22] A. M. Dimiev, J. M. Tour, “Mechanism of graphene oxide formation,” ACS Nano, vol. 8, no. 3, pp. 3060–3068, 2014.
  • [23] F. J. Tölle, K. Gamp, R. Mülhaupt, “Scale-up and purification of graphite oxide as intermediate for functionalized graphene,” Carbon, vol. 75, no. April, pp. 432–442, 2014.
  • [24] J. Chen, Y. Zhang, M. Zhang, B. Yao, Y. Li, L. Huang, C. Li, G. Shi, “Water-enhanced oxidation of graphite to graphene oxide with controlled species of oxygenated groups,” Chemical Science, vol. 7, no. 3, pp. 1874–1881, 2016.
  • [25] R. Muzyka, M. Kwoka, Ł. Smędowski, N. Díez, G. Gryglewicz, “Oxidation of graphite by different modified Hummers methods,” New Carbon Materials, vol. 32, no. 1, pp. 15–20, 2017.
  • [26] A. A. Muhsan, K. Lafdi, “Numerical study of the electrochemical exfoliation of graphite,” SN Applied Sciences, vol. 1, no. 3, p. 276, 2019.
  • [27] J. Epp, “X-ray diffraction (XRD) techniques for materials characterization,” in Materials Characterization Using Nondestructive Evaluation (NDE) Methods, G. Huebschen, I. Altpeter, R. Tschuncky, and H.-G. Herrmann, Eds., Elsevier Inc., 2016, pp. 81–124.
  • [28] A. L. Higginbotham, D. V Kosynkin, A. Sinitskii, Z. Sun, J. M. Tour, “Lower-Defect Graphene Oxide Nanotubes Nanoribbons from Multiwalled Carbon Nanotubes,” ACS nano, vol. 4, no. 4, p. 2059, 2010.
  • [29] M. F. R. Hanifah, J. Jaafar, M. H. D. Othman, A. F. Ismail, M. A. Rahman, N. Yusof, W. N. W. Salleh, F. Aziz, “Facile synthesis of highly favorable graphene oxide: Effect of oxidation degree on the structural, morphological, thermal and electrochemical properties,” Materialia, vol. 6, no. May, p. 100344, 2019.
  • [30] K. Krishnamoorthy, M. Veerapandian, K. Yun, S.-J. Kim, “The chemical and structural analysis of graphene oxide with different degrees of oxidation,” Carbon, vol. 53, pp. 38–49, 2013.
  • [31] M. Wojtoniszak, D. Rogińska, B. Machaliński, M. Drozdzik, E. Mijowska, “Graphene oxide functionalized with methylene blue and its performance in singlet oxygen generation,” Materials Research Bulletin, vol. 48, no. 7, pp. 2636–2639, 2013.
  • [32] M. J. Yoo, H. B. Park, “Effect of hydrogen peroxide on properties of graphene oxide in Hummers method,” Carbon, vol. 141, pp. 515–522, 2019.
  • [33] S. Thakur, N. Karak, “Green reduction of graphene oxide by aqueous phytoextracts,” Carbon, vol. 50, no. 14, pp. 5331–5339, 2012.
  • [34] V. Ţucureanu, A. Matei, A. M. Avram, “FTIR Spectroscopy for Carbon Family Study,” Critical Reviews in Analytical Chemistry, vol. 46, no. 6, pp. 502–520, 2016.
  • [35] Y. Hou, S. Lv, L. Liu, X. Liu, “High-quality preparation of graphene oxide via the Hummers’ method: Understanding the roles of the intercalator, oxidant, and graphite particle size,” Ceramics International, vol. 46, no. 2, pp. 2392–2402, 2020.
  • [36] R. Al-Gaashani, A. Najjar, Y. Zakaria, S. Mansour, M. A. Atieh, “XPS and structural studies of high quality graphene oxide and reduced graphene oxide prepared by different chemical oxidation methods,” Ceramics International, vol. 45, no. 11, pp. 14439–14448, 2019.
  • [37] A. Allahbakhsh, F. Sharif, S. Mazirani, “The Influence of Oxygen-Containing Functional Groups on The Surface Behavior and Roughness Characteristics of Graphene Oxide,” Nano, vol. 08, no. 04, p. 1350045, 2013.
  • [38] S. Eigler, C. Dotzer, F. Hof, W. Bauer, A. Hirsch, “Sulfur Species in Graphene Oxide,” Chemistry - A European Journal, vol. 19, no. 29, pp. 9490–9496, 2013.
  • [39] R. Ikram, B. M. Jan, W. Ahmad, “An overview of industrial scalable production of graphene oxide and analytical approaches for synthesis and characterization,” Journal of Materials Research and Technology, vol. 9, no. 5, pp. 11587–11610, 2020.
  • [40] Q. Zhang, Y. Yang, H. Fan, L. Feng, G. Wen, L. Qin, “Roles of water in the formation and preparation of graphene oxide,” RSC Advances, vol. 11, pp. 15808–15816, 2021.
  • [41] P. S. Narayan, N. L. Teradal, S. Jaldappagari, A. K. Satpati, “Eco-friendly reduced graphene oxide for the determination of mycophenolate mofetil in pharmaceutical formulations,” Journal of Pharmaceutical Analysis, vol. 8, no. 2, pp. 131–137, 2018.
  • [42] N. Yadav, B. Lochab, “A comparative study of graphene oxide: Hummers, intermediate and improved method,” FlatChem, vol. 13, no. February, pp. 40–49, 2019.
Year 2024, Volume: 28 Issue: 3, 567 - 578, 30.06.2024
https://doi.org/10.16984/saufenbilder.1337974

Abstract

Project Number

2020-038

References

  • [1] M. P. Araújo, O. S. G. P. Soares, A. J. S. Fernandes, M. F. R. Pereira, C. Freire, “Tuning the surface chemistry of graphene flakes: new strategies for selective oxidation,” RSC Advances, vol. 7, no. 23, pp. 14290–14301, 2017.
  • [2] J. Guerrero-Contreras, F. Caballero-Briones, “Graphene oxide powders with different oxidation degree, prepared by synthesis variations of the Hummers method,” Materials Chemistry and Physics, vol. 153, pp. 209–220, 2015.
  • [3] J. Chen, B. Yao, C. Li, G. Shi, “An improved Hummers method for eco-friendly synthesis of graphene oxide,” Carbon, vol. 64, no. 1, pp. 225–229, 2013.
  • [4] W. S. Koe, J. W. Lee, W. C. Chong, Y. L. Pang, L. C. Sim, “An overview of photocatalytic degradation: photocatalysts, mechanisms, and development of photocatalytic membrane,” Environmental Science and Pollution Research, vol. 27, no. 3, pp. 2522–2565, 2020.
  • [5] T. A. Saleh, G. Fadillah, “Recent trends in the design of chemical sensors based on graphene–metal oxide nanocomposites for the analysis of toxic species and biomolecules,” Trends in Analytical Chemistry, vol. 120, 2019.
  • [6] R. K. Joshi, S. Alwarappan, M. Yoshimura, V. Sahajwalla, Y. Nishina, “Graphene oxide: the new membrane material,” Applied Materials Today, vol. 1, no. 1, pp. 1–12, 2015.
  • [7] D. Ege, A. R. Kamali, A. R. Boccaccini, “Graphene Oxide/Polymer-Based Biomaterials,” Advanced Engineering Materials, vol. 19, no. 12, p. 1700627, 2017.
  • [8] S. Thangavel, G. Venugopal, “Understanding the adsorption property of graphene-oxide with different degrees of oxidation levels,” Powder Technology, vol. 257, pp. 141–148, 2014.
  • [9] Y. Wei, X. Hu, Q. Jiang, Z. Sun, P. Wang, Y. Qiu, W. Liu, “Influence of graphene oxide with different oxidation levels on the properties of epoxy composites,” Composites Science and Technology, vol. 161, no. April, pp. 74–84, 2018.
  • [10] D. R. Dreyer, S. Park, C. W. Bielawski, R. S. Ruoff, “The chemistry of graphene oxide,” Chem. Soc. Rev., vol. 39, no. 1, pp. 228–240, 2010.
  • [11] S. Eigler, S. Grimm, F. Hof, A. Hirsch, “Graphene oxide: a stable carbon framework for functionalization,” Journal of Materials Chemistry A, vol. 1, no. 38, p. 11559, 2013.
  • [12] V. Panwar, A. Chattree, K. Pal, “A new facile route for synthesizing of graphene oxide using mixture of sulfuric-nitric-phosphoric acids as intercalating agent,” Physica E: Low-Dimensional Systems and Nanostructures, vol. 73, pp. 235–241, 2015.
  • [13] M. D. P. Lavin-Lopez, A. Romero, J. Garrido, L. Sanchez-Silva, J. L. Valverde, “Influence of Different Improved Hummers Method Modifications on the Characteristics of Graphite Oxide in Order to Make a More Easily Scalable Method,” Industrial & Engineering Chemistry Research, vol. 55, no. 50, pp. 12836–12847, 2016.
  • [14] D. Yang, A. Velamakanni, G. Bozoklu, S. Park, M. Stoller, R. D. Piner, S. Stankovich, I. Jung, D. A. Field, C. A. Ventrice, R. S. Ruoff, “Chemical analysis of graphene oxide films after heat and chemical treatments by X-ray photoelectron and Micro-Raman spectroscopy,” Carbon, vol. 47, no. 1, pp. 145–152, 2009.
  • [15] S. Eigler, A. M. Dimiev, “Characterization Techniques,” in Graphene Oxide: Fundamentals and Applications, A. M. Dimiev and S. Eigler, Eds., United Kingdom: John Wiley & Sons, 2016, pp. 85–118.
  • [16] B. C. Brodie, “XIII. On the atomic weight of graphite,” Philosophical Transactions of the Royal Society of London, vol. 149, no. 1, pp. 249–259, 1859.
  • [17] W. S. Hummers, R. E. Offeman, “Preparation of Graphitic Oxide,” Journal of the American Chemical Society, vol. 80, no. 6, pp. 1339–1339, 1958.
  • [18] D. C. Marcano, D. V. Kosynkin, J. M. Berlin, A. Sinitskii, Z. Sun, A. Slesarev, L. B. Alemany, W. Lu, J. M. Tour, “Improved synthesis of graphene oxide,” ACS Nano, vol. 4, no. 8, pp. 4806–4814, 2010.
  • [19] F. Boran, S. Çetinkaya Gürer, “The effect of starting material types on the structure of graphene oxide and graphene,” Turkish Journal of Chemistry, vol. 43, no. 5, pp. 1322–1335, 2019.
  • [20] L. J. Cote, J. Kim, Z. Zhang, C. Sun, J. Huang, “Tunable assembly of graphene oxide surfactant sheets: wrinkles, overlaps and impacts on thin film properties,” Soft Matter, vol. 6, no. 24, p. 6096, 2010.
  • [21] J. H. Kang, T. Kim, J. Choi, J. Park, Y. S. Kim, M. S. Chang, H. Jung, K. T. Park, S. J. Yang, C. R. Park, “Hidden Second Oxidation Step of Hummers Method,” Chemistry of Materials, vol. 28, no. 3, pp. 756–764, 2016.
  • [22] A. M. Dimiev, J. M. Tour, “Mechanism of graphene oxide formation,” ACS Nano, vol. 8, no. 3, pp. 3060–3068, 2014.
  • [23] F. J. Tölle, K. Gamp, R. Mülhaupt, “Scale-up and purification of graphite oxide as intermediate for functionalized graphene,” Carbon, vol. 75, no. April, pp. 432–442, 2014.
  • [24] J. Chen, Y. Zhang, M. Zhang, B. Yao, Y. Li, L. Huang, C. Li, G. Shi, “Water-enhanced oxidation of graphite to graphene oxide with controlled species of oxygenated groups,” Chemical Science, vol. 7, no. 3, pp. 1874–1881, 2016.
  • [25] R. Muzyka, M. Kwoka, Ł. Smędowski, N. Díez, G. Gryglewicz, “Oxidation of graphite by different modified Hummers methods,” New Carbon Materials, vol. 32, no. 1, pp. 15–20, 2017.
  • [26] A. A. Muhsan, K. Lafdi, “Numerical study of the electrochemical exfoliation of graphite,” SN Applied Sciences, vol. 1, no. 3, p. 276, 2019.
  • [27] J. Epp, “X-ray diffraction (XRD) techniques for materials characterization,” in Materials Characterization Using Nondestructive Evaluation (NDE) Methods, G. Huebschen, I. Altpeter, R. Tschuncky, and H.-G. Herrmann, Eds., Elsevier Inc., 2016, pp. 81–124.
  • [28] A. L. Higginbotham, D. V Kosynkin, A. Sinitskii, Z. Sun, J. M. Tour, “Lower-Defect Graphene Oxide Nanotubes Nanoribbons from Multiwalled Carbon Nanotubes,” ACS nano, vol. 4, no. 4, p. 2059, 2010.
  • [29] M. F. R. Hanifah, J. Jaafar, M. H. D. Othman, A. F. Ismail, M. A. Rahman, N. Yusof, W. N. W. Salleh, F. Aziz, “Facile synthesis of highly favorable graphene oxide: Effect of oxidation degree on the structural, morphological, thermal and electrochemical properties,” Materialia, vol. 6, no. May, p. 100344, 2019.
  • [30] K. Krishnamoorthy, M. Veerapandian, K. Yun, S.-J. Kim, “The chemical and structural analysis of graphene oxide with different degrees of oxidation,” Carbon, vol. 53, pp. 38–49, 2013.
  • [31] M. Wojtoniszak, D. Rogińska, B. Machaliński, M. Drozdzik, E. Mijowska, “Graphene oxide functionalized with methylene blue and its performance in singlet oxygen generation,” Materials Research Bulletin, vol. 48, no. 7, pp. 2636–2639, 2013.
  • [32] M. J. Yoo, H. B. Park, “Effect of hydrogen peroxide on properties of graphene oxide in Hummers method,” Carbon, vol. 141, pp. 515–522, 2019.
  • [33] S. Thakur, N. Karak, “Green reduction of graphene oxide by aqueous phytoextracts,” Carbon, vol. 50, no. 14, pp. 5331–5339, 2012.
  • [34] V. Ţucureanu, A. Matei, A. M. Avram, “FTIR Spectroscopy for Carbon Family Study,” Critical Reviews in Analytical Chemistry, vol. 46, no. 6, pp. 502–520, 2016.
  • [35] Y. Hou, S. Lv, L. Liu, X. Liu, “High-quality preparation of graphene oxide via the Hummers’ method: Understanding the roles of the intercalator, oxidant, and graphite particle size,” Ceramics International, vol. 46, no. 2, pp. 2392–2402, 2020.
  • [36] R. Al-Gaashani, A. Najjar, Y. Zakaria, S. Mansour, M. A. Atieh, “XPS and structural studies of high quality graphene oxide and reduced graphene oxide prepared by different chemical oxidation methods,” Ceramics International, vol. 45, no. 11, pp. 14439–14448, 2019.
  • [37] A. Allahbakhsh, F. Sharif, S. Mazirani, “The Influence of Oxygen-Containing Functional Groups on The Surface Behavior and Roughness Characteristics of Graphene Oxide,” Nano, vol. 08, no. 04, p. 1350045, 2013.
  • [38] S. Eigler, C. Dotzer, F. Hof, W. Bauer, A. Hirsch, “Sulfur Species in Graphene Oxide,” Chemistry - A European Journal, vol. 19, no. 29, pp. 9490–9496, 2013.
  • [39] R. Ikram, B. M. Jan, W. Ahmad, “An overview of industrial scalable production of graphene oxide and analytical approaches for synthesis and characterization,” Journal of Materials Research and Technology, vol. 9, no. 5, pp. 11587–11610, 2020.
  • [40] Q. Zhang, Y. Yang, H. Fan, L. Feng, G. Wen, L. Qin, “Roles of water in the formation and preparation of graphene oxide,” RSC Advances, vol. 11, pp. 15808–15816, 2021.
  • [41] P. S. Narayan, N. L. Teradal, S. Jaldappagari, A. K. Satpati, “Eco-friendly reduced graphene oxide for the determination of mycophenolate mofetil in pharmaceutical formulations,” Journal of Pharmaceutical Analysis, vol. 8, no. 2, pp. 131–137, 2018.
  • [42] N. Yadav, B. Lochab, “A comparative study of graphene oxide: Hummers, intermediate and improved method,” FlatChem, vol. 13, no. February, pp. 40–49, 2019.
There are 42 citations in total.

Details

Primary Language English
Subjects Material Production Technologies
Journal Section Research Articles
Authors

Kürşat Kanbur 0000-0001-6343-2992

Işıl Birlik 0000-0003-3098-2001

Fatih Sargın 0000-0002-2683-4543

Funda Ak Azem 0000-0002-4446-1437

Ahmet Türk 0000-0002-4260-6372

Project Number 2020-038
Early Pub Date June 14, 2024
Publication Date June 30, 2024
Submission Date August 4, 2023
Acceptance Date February 11, 2024
Published in Issue Year 2024 Volume: 28 Issue: 3

Cite

APA Kanbur, K., Birlik, I., Sargın, F., Ak Azem, F., et al. (2024). The Role of Water on the Oxidation Process of Graphene Oxide Structures. Sakarya University Journal of Science, 28(3), 567-578. https://doi.org/10.16984/saufenbilder.1337974
AMA Kanbur K, Birlik I, Sargın F, Ak Azem F, Türk A. The Role of Water on the Oxidation Process of Graphene Oxide Structures. SAUJS. June 2024;28(3):567-578. doi:10.16984/saufenbilder.1337974
Chicago Kanbur, Kürşat, Işıl Birlik, Fatih Sargın, Funda Ak Azem, and Ahmet Türk. “The Role of Water on the Oxidation Process of Graphene Oxide Structures”. Sakarya University Journal of Science 28, no. 3 (June 2024): 567-78. https://doi.org/10.16984/saufenbilder.1337974.
EndNote Kanbur K, Birlik I, Sargın F, Ak Azem F, Türk A (June 1, 2024) The Role of Water on the Oxidation Process of Graphene Oxide Structures. Sakarya University Journal of Science 28 3 567–578.
IEEE K. Kanbur, I. Birlik, F. Sargın, F. Ak Azem, and A. Türk, “The Role of Water on the Oxidation Process of Graphene Oxide Structures”, SAUJS, vol. 28, no. 3, pp. 567–578, 2024, doi: 10.16984/saufenbilder.1337974.
ISNAD Kanbur, Kürşat et al. “The Role of Water on the Oxidation Process of Graphene Oxide Structures”. Sakarya University Journal of Science 28/3 (June 2024), 567-578. https://doi.org/10.16984/saufenbilder.1337974.
JAMA Kanbur K, Birlik I, Sargın F, Ak Azem F, Türk A. The Role of Water on the Oxidation Process of Graphene Oxide Structures. SAUJS. 2024;28:567–578.
MLA Kanbur, Kürşat et al. “The Role of Water on the Oxidation Process of Graphene Oxide Structures”. Sakarya University Journal of Science, vol. 28, no. 3, 2024, pp. 567-78, doi:10.16984/saufenbilder.1337974.
Vancouver Kanbur K, Birlik I, Sargın F, Ak Azem F, Türk A. The Role of Water on the Oxidation Process of Graphene Oxide Structures. SAUJS. 2024;28(3):567-78.