Study of green reductant effects of highly reduced graphene oxide production and their characteristics
Main Article Content
The study of the green reductant effects to produce reduced graphene oxide (rGO) has been completed successfully. The reduction of graphene oxide (GO) was carried out chemically using various reductants such as ascorbic acid (rGO-AA), gallic acid (rGO-AG), and trisodium citrate (rGO-NS). The GO was prepared using the Tour method at a temperature of 65 ? for 6 hours with potassium permanganate: graphite weight ratio 1:3.5. The results showed that rGO-AA had the highest electrical conductivity value of 755.70 S/m, with characteristics such as a surface area of 255.93 m2/g, a pore volume of 0.61 cm3/g, an average pore diameter of 7.10 nm, ID/IG ratio of 1.93, and three graphene layers in the material nanostructure stack. Therefore, it can be concluded that the reduction of GO with ascorbic acid (rGO-AA) is the most effective in producing rGO.
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2. L. Huang, D. Santiago, P. Loyselle, L. Dai. Graphene-Based Nanomaterials for Flexible and Wearable Supercapacitors. Small, 14 (2018). 1-11.
3. M. Samanc?. Chemically and thermally reduced graphene oxide supported Pt catalysts prepared by supercritical deposition. Int. J. Hydrog. Energy, 47 (2022), 19669-19689.
4. A.E.F. Oliveira, G.B. Braga, C.R.T. Tarley and A.C. Pereira. Thermally reduced graphene oxide: synthesis, studies and characterization. J. Mater. Sci., 53 (2018), 12005-12015.
5. S. Yang, Q. Chen, M. Shi, Q. Zhang, S. Lan, T. Maimaiti et al. Fast identification and quantification of graphene oxide in aqueous environment by raman spectroscopy. Nanomaterials, 10 (2020), 770-781.
6. Y.I. Zhang, L. Zhang and C. Zhou. Graphene and Related Applications. Acc. Chem. Res, 46 (2013), 2329-2339.
7. T.B. Prayitno. Tuning the magnetic states in AA-stacked bilayer zigzag graphene nanoribbons. Commun. Sci. Technol., 7 (2022), 73-79.
8. W. Yu, L. Sisi, Y. Yaiyan, and L. Jie. Progress in the functional modification of graphene/graphene oxide: A review. RSC. Adv, 10 (2020), 15328-15345.
9. M. T. Alshamkhani, L. K. Teong, L. K. Putri, A. R. Mohamed, P.Lahijani, M. Mohammadi. Effect of graphite exfoliation routes on the properties of exfoliated graphene and its photocatalytic applications. J. Environ. Chem. Eng., 9 (2021), 1-40.
10. B.C. Brodie, XIII. On the atomic weight of graphite. Philos. Trans. R. Soc, 149 (1859), 249–259.
11. L. Staudenmaier, Verfahren zur Darstellung der Graphitsäure, Berichte der Dtsch. Chem. Gesellschaft, 31 (1898), 1481–1487.
12. W.S. Hummers and R.E. Offeman, Preparation of Graphitic Oxide, J. Am. Chem. Soc. 80 (1958), 1339.
13. Y. Zhu, G. Kong, Y. Pan, L. Liu, B. Yang, S. Zhang et al. An improved Hummers method to synthesize graphene oxide using much less concentrated sulfuric acid. Chinese Chem. Lett. 33 (2022), 8–11.
14. D.C. Marcano, D. V. Kosynkin, J.M. Berlin, A. Sinitskii, Z. Sun, A. Slesarev et al. Improved synthesis of graphene oxide, ACS Nano, 4 (2010), . 4806–4814.
15. D.C. Marcano, D. V. Kosynkin, J.M. Berlin, A. Sinitskii, Z. Sun, A.S. Slesarev et al. Correction to Improved Synthesis of Graphene Oxide. ACS Nano, 12 (2018), 2078.
16. I. Bychko, A. Abakumov, O. Didenko, M. Chen, J. Tang and P. Strizhak. 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 (2022), 110614.
17. A. Romero, M.P. Lavin-Lopez, L. Sanchez-Silva, J.L. Valverde and A. Paton-Carrero. Comparative study of different scalable routes to synthesize graphene oxide and reduced graphene oxide, Mater. Chem. Phys., 203 (2018), 284-292.
18. J. Chen, Y. Li, L. Huang, C. Li and G. Shi. High-yield preparation of graphene oxide from small graphite flakes via an improved Hummers method with a simple purification process. Carbon N. Y. 81 (2015), 826-834.
19. M.D.P. Lavin-Lopez, A. Romero, J. Garrido, L. Sanchez-Silva and 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. Ind. Eng. Chem. Res. 55 (2016), 12836-12847.
20. C.K. Chua, and M. Pumera. Chemical reduction of graphene oxide: A synthetic chemistry viewpoint. Chem. Soc. Rev, 1 (2014), 291-312.
21. K.K.H De Silva, H.H Huang, R.K Joshi, and M. Yoshimura. Chemical reduction of graphene oxide using green reductants. Carbon, 119 (2017), 190-199.
22. M. Samanc? and A. Bayrakçeken Yurtcan. Chemically and thermally reduced graphene oxide supported Pt catalysts prepared by supercritical deposition. Int. J. Hydrogen Energy, 47 (2022). 19669–19689.
23. T.A. Saleh and G. Fadillah. 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 (2019), 115660.
24. Y. Wang, Z.X. Shi and J. Yin. Facile synthesis of soluble graphene via a green reduction of graphene oxide in tea solution and its biocomposites. ACS Appl. Mater. Interfaces, 3 (2011), 1127-1133.
25. D. Hou, Q. Liu, H. Cheng, K. Li, D. Wang and H. Zhang. Chrysanthemum extract assisted green reduction of graphene oxide. Mater. Chem. Phys., 183 (2016), 76-82 .
26. T. Kuila, S. Bose, P. Khanra, A.K. Mishra, N.H. Kim and J.H. Lee. A green approach for the reduction of graphene oxide by wild carrot root. Carbon N. Y., 50 (2012), 94-921.
27. S. Thakur and N. Karak. Green reduction of graphene oxide by aqueous phytoextracts. Carbon N. Y, 50 (2012), 5331-5339.
28. F. Tavakoli, M. Salavati-Niasari, A. Badiei and F. Mohandes. Green synthesis and characterization of graphene nanosheets. Mater. Res. Bull., 63 (2015), 51-57.
29. D. Hou, Q. Liu, H. Cheng, H. Zhang and S. Wang. Green reduction of graphene oxide via Lycium barbarum extract. J. Solid State Chem., 246 (2017), 351-356.
30. Y. Gao, J. Wu, X. Ren, X. Tan, T. Hayat, A. Alsaedi et al. Impact of graphene oxide on the antibacterial activity of antibiotics against bacteria. Environ. Sci. Nano, 4 (2017), 1016–1024.
31. W. Wan, Z. Zhao, H. Hu, Y. Gogotsi and J. Qiu. Highly controllable and green reduction of graphene oxide to flexible graphene film with high strength. Mater. Res. Bull., 48 (2013), 4797-4803.
32. Z. Bo, X. Shuai, S. Mao, H. Yang, J. Qian, J. Chen et al. Green preparation of reduced graphene oxide for sensing and energy storage applications. Sci. Rep., 4 (2014), 1-8.
33. T.F. Emiru and D.W. Ayele. Controlled synthesis, characterization and reduction of graphene oxide: A convenient method for large scale production. Egypt. J. Basic Appl., Sci. 4 (2017), 74-79.
34. S. Bose, T. Kuila, A.K. Mishra, N.H. Kim and J.H. Lee. Dual role of glycine as a chemical functionalizer and a reducing agent in the preparation of graphene: An environmentally friendly method. J. Mater. Chem., 22 (2012), 9696-9703.
35. J. Wang, E.C. Salihi and L. Šiller. Green reduction of graphene oxide using alanine. Mater. Sci. Eng. C, 72 (2017), 1-6.
36. J. Liu, S. Fu, B. Yuan, Y. Li and Z. Deng. Toward a universal “adhesive nanosheet” for the assembly of multiple nanoparticles based on a protein-induced reduction/decoration of graphene oxide. J. Am. Chem. Soc., 132 (2010), .
37. J. Li, G. Xiao, C. Chen, R. Li and D. Yan, Superior dispersions of reduced graphene oxide synthesized by using gallic acid as a reductant and stabilizer, J. Mater. Chem. A 1 (2013), 7279-7281.
38. M.J. Fernández-Merino, L. Guardia, J.I. Paredes, S. Villar-Rodil, P. Solís-Fernández, A. Martínez-Alonso et al. Vitamin C is an ideal substitute for hydrazine in the reduction of graphene oxide suspensions. J. Phys. Chem. C, 114 (2010), 6426-6432 .
39. D.Y. Kim, J. Suk Sung, M. Kim and G. Ghodake. Rapid production of silver nanoparticles at large-scale using gallic acid and their antibacterial assessment. Mater. Lett., 155 (2015), 62-64.
40. J. Lee, S. Oh, M. Jang, J. Kim, J. Lee and H. Zhou. Synthesis of silver nanoparticles using analogous reducibility of phytochemicals. Curr. Appl. Phys., 16 (2016), 738-747.
41. Y. Zhou, M. Xu, Y. Liu, Y. Bai, Y. Deng, J. Liu et al. Green synthesis of Se/Ru alloy nanoparticles using gallic acid and evaluation of theiranti-invasive effects in HeLa cells. Colloids Surfaces B Biointerfaces, 144 (2016), 118-124.
42. A. Sood, V. Arora, J. Shah, R.K. Kotnala and T.K. Jain. Ascorbic acid-mediated synthesis and characterisation of iron oxide/gold core–shell nanoparticles. J. Exp. Nanosci., 11 (2016), 370-382.
43. S. Yokoyama, K. Sato, M. Muramatsu, T. Yamasuge, T. Itoh, K. Motomiya et al. Green synthesis and formation mechanism of nanostructured Bi2Te3 using ascorbic acid in aqueous solution. Adv. Powder Technol., 26 (2015), 789-796.
44. Z. Zhang, H. Chen, C. Xing, M. Guo, F. Xu, X. Wang et al. Sodium citrate: A universal reducing agent for reduction / decoration of graphene oxide with au nanoparticles. Nano Res., 4 (2011), 599-611.
45. C. Xu, X. Shi, A. Ji, L. Shi, C. Zhou and Y. Cui. Fabrication and characteristics of reduced graphene oxide produced with different green reductants. PLoS One, 10 (2015), 1-15.
46. J. Zhang, H. Yang, G. Shen, P. Cheng, J. Zhang and S. Guo. Reduction of graphene oxide via L-ascorbic acid._Supporting Information. Chem. Commun. (Camb). 2 (2010), 112-114.
47. U. Chasanah, W. Trisunaryanti, H.S. Oktaviano And D.A. Fatmawati, The Performance Of Green Synthesis Of Graphene Oxide Prepared By Modified Hummers Method With Oxidation Time Variation, Rasayan J. Chem. 14 (2021), 2017–2023.
48. G. Fadillah, T.A. Saleh, S. Wahyuningsih, E. Ninda Karlina Putri and S. Febrianastuti. Electrochemical removal of methylene blue using alginate-modified graphene adsorbents. Chem. Eng. J., 378 (2019), 122140.
49. G. Fadillah, R. Hidayat and T.A. Saleh. Hydrothermal assisted synthesis of titanium dioxide nanoparticles modified graphene with enhanced photocatalytic performance. J. Ind. Eng. Chem., 113 (2022), 411–418.
50. M.P. Lavin-Lopez, A. Paton-Carrero, L. Sanchez-Silva, J.L. Valverde and A. Romero. Influence of the reduction strategy in the synthesis of reduced graphene oxide. Adv. Powder Technol., 28 (2017), 3195-3203.
51. M. Coros, F. Pogacean, A. Turza, M. Dan, C. Berghian-Grosan, I.O. Pana et al. Green synthesis, characterization and potential application of reduced graphene oxide. Phys. E Low-Dimensional Syst. Nanostructures, 119 (2020), .
52. J.C. Silva Filho, E.C. Venancio, S.C. Silva, H. Takiishi, L.G. Martinez and R.A. Antunes, A thermal method for obtention of 2 to 3 reduced graphene oxide layers from graphene oxide, SN Appl. Sci. 2 (2020), 113971.
53. N.M.S. Hidayah, W.W. Liu, C.W. Lai, N.Z. Noriman, C.S. Khe, U. Hashim et al. Comparison on graphite, graphene oxide and reduced graphene oxide: Synthesis and characterization. in AIP Conference Proceedings, 1892 (2017), 150092.
54. R. Siburian, H. Sihotang, S. Lumban Raja, M. Supeno and C. Simanjuntak. New route to synthesize of graphene nano sheets. Orient. J. Chem., 34 (2018), 182-187.
55. S. Sadhukhan, T.K. Ghosh, D. Rana, I. Roy, A. Bhattacharyya, G. Sarkar et al. Studies on synthesis of reduced graphene oxide (RGO) via green route and its electrical property. Mater. Res. Bull., 79 (2016), 41-51.
56. L. long Dong, W. ge Chen, N. Deng and C. hao Zheng. A novel fabrication of graphene by chemical reaction with a green reductant. Chem. Eng. J. 306 (2016), 754-762.
57. I. Srivastava, R.J. Mehta, Z.Z. Yu, L. Schadler and N. Koratkar. Raman study of interfacial load transfer in graphene nanocomposites. Appl. Phys. Lett. 98 (2011), 1-3.
58. L.M. Malard, M.A. Pimenta, G. Dresselhaus, and M.S. Dresselhaus. Raman spectroscopy in graphene. Phys. Rep., 473 (2009), 51-87.
59. I. Childres, L.A. Jauregui, W. Park, H. Caoa and Y.P. Chena. Raman spectroscopy of graphene and related materials. in New Developments in Photon and Materials Research, 19 (2013), 1-20.
60. A.C. Ferrari, J.C. Meyer, V. Scardaci, C. Casiraghi, M. Lazzeri, F. Mauri et al. Raman spectrum of graphene and graphene layers. Phys. Rev. Lett. 97 (2006), 187401.
61. V. ?ucureanu, A. Matei, and M. Avram. FTIR Spectroscopy for Carbon Family Study. Crit. Rev. Anal. Chem., 46 (2016), 502-520.
62. B.D. Ossonon and D. Bélanger. Synthesis and characterization of sulfophenyl-functionalized reduced graphene oxide sheets. RSC Adv., 7 (2017), 27224-27234.
63. G. Surekha, K.V. Krishnaiah, N. Ravi and R. Padma Suvarna. FTIR, Raman and XRD analysis of graphene oxide films prepared by modified Hummers method. in Journal of Physics: Conference Series, 1495 (2020), 1-7.
64. A. Marinoiu, M. Andrulevicius, A. Tamuleviciene, T. Tamulevicius, M. Raceanu and M. Varlam. Synthesis of well dispersed gold nanoparticles on reduced graphene oxide and application in PEM fuel cells. Appl. Surf. Sci. 504 (2020), 144511.
65. T.A. Zegeye, M.C. Tsai, J.H. Cheng, M.H. Lin, H.M. Chen, J. Rick et al. Controllable embedding of sulfur in high surface area nitrogen doped three dimensional reduced graphene oxide by solution drop impregnation method for high performance lithium-sulfur batteries. J. Power Sources, 353 (2017), 298-311.
66. R. Al-Gaashani, A. Najjar, Y. Zakaria, S. Mansour and M.A. Atieh. XPS and structural studies of high quality graphene oxide and reduced graphene oxide prepared by different chemical oxidation methods. Ceram. Int. 45 (2019), 14439-14448.
67. A.K. Mishra and S. Ramaprabhu. Functionalized graphene-based nanocomposites for supercapacitor application. J. Phys. Chem. C 115 (2011), 14006-14013.
68. X.M. Wang, M.E. Wang, D.D. Zhou and Y.Y. Xia. Structural design and facile synthesis of a highly efficient catalyst for formic acid electrooxidation. Phys. Chem. Chem. Phys., 13 (2011), 13594-13597.
69. A. Shalaby, D. Nihtianova, P. Markov, A.D. Staneva, R.S. Iordanova and Y.B. Dimitriev. Structural analysis of reduced graphene oxide by transmission electron microscopy. Bulg. Chem. Commun., 47 (2015), 291-295.
70. Y. Geng, S.J. Wang and J.K. Kim. Preparation of graphite nanoplatelets and graphene sheets. J. Colloid Interface Sci., 336 (2009), 592-598.
71. Y. Zhang, Z. Chu, C.A. Dreiss, Y. Wang, C. Fei and Y. Feng. Smart wormlike micelles switched by CO2 and air. Soft Matter, 9 (2013), 6217-6222.
72. V.B. Mohan, K. Jayaraman and D. Bhattacharyya. Brunauer–Emmett–Teller (BET) specific surface area analysis of different graphene materials: A comparison to their structural regularity and electrical properties. Solid State Commun., 320 (2020), 114004.
73. V.B. Mohan, L. Jakisch, K. Jayaraman and D. Bhattacharyya. Role of chemical functional groups on thermal and electrical properties of various graphene oxide derivatives: A comparative x-ray photoelectron spectroscopy analysis. Mater. Res. Express, 5 (2018), 1-8.
74. J. ?wiatowska, V. Lair, C. Pereira-Nabais, G. Cote, P. Marcus and A. Chagnes. XPS, XRD and SEM characterization of a thin ceria layer deposited onto graphite electrode for application in lithium-ion batteries. Appl. Surf. Sci., 257 (2011), 9110-9119.
75. S. Park, J. An, J.R. Potts, A. Velamakanni, S. Murali and R.S. Ruoff. Hydrazine-reduction of graphite- and graphene oxide. Carbon N. Y., 49 (2011), 3019-3023.
76. S. Eigler, M. Enzelberger-Heim, S. Grimm, P. Hofmann, W. Kroener, A. Geworski et al. Wet chemical synthesis of graphene. Adv. Mater., 25 (2013), 3583-3587.
77. S. Jin, Q. Gao, X. Zeng, R. Zhang, K. Liu, X. Shao et al. Effects of reduction methods on the structure and thermal conductivity of free-standing reduced graphene oxide films. Diam. Relat. Mater., 58 (2015), 54-61.
78. T.H.T. Vu, T.T.T. Tran, H.N.T. Le, P.H.T. Nguyen, N.Q. Bui and N. Essayem. A new green approach for the reduction of graphene oxide nanosheets using caffeine. Bull. Mater., Sci. 38 (2015), 667-671.