CVD GROWTH AND CHARACTERIZATION OF MULTILAYER GRAPHENE DOMAINS ON COPPER WITH POLYMER-ASSISTED TRANSFER ONTO SiO₂/Si SUBSTRATES
Keywords:
Multilayer graphene domains, CVD, copper foil, silicon substrateAbstract
This work presents the synthesis of multilayer graphene domains on copper substrates by thermal chemical vapor deposition (CVD). A detailed description of the CVD reactor system is provided, including the use of argon as a cooling medium and methane as the carbon precursor. Optimal process parameters temperature regimes, gas flow rates, working pressure, and cooling profiles were experimentally determined. Surface morphology was examined using optical and field-emission scanning electron microscopy, revealing discrete rectangular graphene domains with heterogeneous orientations. Raman spectroscopy confirmed the multilayer nature of the domains, the presence of structural defects, and variations in crystallinity. PMMA-assisted transfer of graphene onto SiO2/Si substrates was also investigated; microscopy revealed the presence of polymer residues, wrinkles, and surface contamination. These findings demonstrate both the effectiveness of thermal CVD for producing domain-structured multilayer graphene and the limitations of polymer-mediated transfer. The results contribute to improving synthesis and transfer strategies for advanced graphene-based electronic, sensing, and energy devices.
Keywords: Multilayer graphene domains, CVD, copper foil, silicon substrate.
References
1. Geim, A.K. and Novoselov, K.S., 2007. The rise of graphene. Nature Materials, 6, pp.183–191.
2. Geim, A.K., 2009. Graphene: status and prospects. Science, 324, pp.1530–1534.
3. Singh, V., Daehajoung, L., Zhai, L., Das, S., Khondaker, S.I. and Seal, S., 2011. Graphene based materials: past, present and future. Progress in Materials Science, 56, pp.1178–1271.
4. Huang, X., Yin, Z., Wu, S., Qi, X., et al., 2011. Graphene-based materials: synthesis, characterization, properties, and applications. Small, 7(14), pp.1876–1902.
5. Mattevi, C., Kim, H. and Chhowalla, M., 2011. A review of chemical vapour deposition of graphene on copper. Journal of Materials Chemistry, 21, pp.3324–3334.
6. Brownson, D.A.C., Kampouris, D.K. and Banks, C.E., 2011. An overview of graphene in energy production and storage applications. Journal of Power Sources, 196, pp.4873–4885.
7. Kashyap, A. et al., 2025. Recent progress on graphene-based derivatives for enhanced [full title not specified]. [Journal not specified], 202401794, pp.1–49.
8. Neto, A.C., Guinea, F., Peres, N.M.R., Novoselov, K.S. and Geim, A.K., 2009. The electronic properties of graphene. Reviews of Modern Physics, 81, pp.109–116.
9. Urade, A.R., Lahiri, I. and Suresh, K.S., 2023. Graphene properties, synthesis and applications: a review. JOM, 75(3), pp.614–630.
10. Novoselov, K.S., Geim, A.K., Morozov, S.V., Jiang, D., Zhang, Y., Dubonos, S.V., Grigorieva, I.V. and Firsov, A.A., 2004. Electric field effect in atomically thin carbon films. Science, 306, pp.666–669.
11. Jain, P. et al., 2024. Recent advances in graphene-enabled materials for photovoltaic applications: a comprehensive review. ACS Omega, 9(11), pp.12403–12425.
12. Muchuweni, E. et al., 2025. Towards high-performance dye-sensitized solar cells by utilizing reduced graphene oxide-based composites as potential alternatives to conventional electrodes: a review. Next Materials, 6(December 2024), p.100477.
13. De Arco, L.G., Zhang, Y., Schlenker, C.W., Ryu, K., Thompson, M.E. and Zhou, C., 2010. Continuous, highly flexible, and transparent graphene films by chemical vapor deposition for organic photovoltaics. ACS Nano, 4(5), pp.2865–2873.
14. Pasadas, F. et al., 2023. Exploiting ambipolarity in graphene field-effect transistors for novel designs on high-frequency analog electronics. [Journal not specified], 2303595, pp.1–15.
15. Kiranakumar, H.V., Thejas, R., Naveen, C.S., Khan, M.I. et al., 2024. A review on electrical and gas-sensing properties of reduced graphene oxide-metal oxide nanocomposites. Biomass Conversion and Biorefinery, 14(12), pp.12625–12635.
16. Park, J., Lee, W.H., Huh, S., Sim, S.H., Kim, S.H., Kim, S.B., Cho, K., Hong, B.H. and Kim, K.S., 2011. Work-function engineering of graphene electrodes by self-assembled monolayers for high-performance organic field-effect transistors. Journal of Physical Chemistry Letters, 2, pp.841–845.
17. Lee, W.H., Park, J., Kim, Y., Kim, K.S., Hong, B.H. and Cho, K., 2010. Control of graphene field-effect transistors by interfacial hydrophobic self-assembled monolayers. Advanced Materials, 23, pp.3460–3464.
18. Song, I., Kim, Y., Kim, K.S., Ozyilmaz, B., Ahn, J. and Hong, B.H., 2010. Roll-to-roll production of 30-inch graphene films for transparent electrodes. Nature Nanotechnology, 5, pp.574–578.
19. Jo, G., Choe, M., Cho, C.Y., Kim, J.H., Park, W., Lee, S., Lee, T. et al., 2010. Large-scale patterned multi-layer graphene films as transparent conducting electrodes for GaN light-emitting diodes. Nanotechnology, 21, p.175201.
20. Recum, P. and Hirsch, T., 2024. Graphene-based chemiresistive gas sensors. Nanoscale Advances, 6(1), pp.11–31.
21. Thejas, R. et al., 2024. A review on electrical and gas-sensing properties of reduced graphene oxide-metal oxide nanocomposites. Biomass Conversion and Biorefinery, 14(12), pp.12625–12635.
22. Madhav, G. and Jayatissa, A.H., 2011. Gas sensing properties of graphene synthesized by chemical vapor deposition. Materials Science and Engineering C, 31, pp.1405–1411.
23. Zhang, H., Fan, L., Dong, H., Zhang, P., Nie, K., Zhong, J., Li, Y., Guo, J. and Sun, X., 2016. Spectroscopic investigation of plasma-fluorinated monolayer graphene and application for gas sensing. ACS Applied Materials & Interfaces, 8(13), pp.8652–8661.
24. Basu, S. and Bhattacharyya, P., 2012. Recent developments on graphene and graphene oxide based solid state gas sensors. Sensors and Actuators B: Chemical, 173, pp.1–21.
25. Avouris, P., 2010. Graphene: electronic and photonic properties and devices. Nano Letters, 10, pp.4285–4294.
26. Jung, I., Pelton, M., Piner, R. et al., 2007. Simple approach for high-contrast optical imaging and characterization of graphene-based sheets. Nano Letters, 7, pp.3569–3575.
27. Zheng, Y., Ni, G.X., Bae, S., Cong, C.X., Kahya, O., Hong, B.H. and Ozyilmaz, B., 2011. Wafer-scale graphene/ferroelectric hybrid devices for low-voltage electronics. EPL (Europhysics Letters), 93, p.17002.
28. Sevincli, H., Topsakal, M., Durgun, E. and Ciraci, S., 2008. Electronic and magnetic properties of 3d transition-metal atom adsorbed graphene and graphene nanoribbons. Physical Review B, 77, p.195434.
29. Sadiq, I., Ali, S.A. and Ahmad, T., 2023. Graphene-based derivatives heterostructured catalytic systems for sustainable hydrogen energy via overall water splitting. Catalysts, 13(1), p.109.
30. Bongu, C.S. et al., 2024. Graphene-based 2D materials for rechargeable batteries and hydrogen production and storage: a critical review. Sustainable Energy & Fuels, 8(18), pp.4039–4070.
31. Arya, A.K. et al., 2024. Graphene-coated Ni–Cu alloys for durable degradation resistance of bi-polar plates for proton exchange membrane fuel cells: remarkable role of alloy composition. Advanced Energy Materials, 14, p.2305320.
32. Wu, W., Liu, Z., Jauregui, L.A., Yu, Q., Pillai, R., Cao, H., Bao, J., Chen, Y.P. and Pei, S.S., 2010. Wafer-scale synthesis of graphene by chemical vapor deposition and its application in hydrogen sensing. Sensors and Actuators B: Chemical, 150(1), pp.296–300.
33. Ilnicka, A. and Lukaszewicz, J.P., 2020. Graphene-based hydrogen gas sensors: a review. Processes, 8, p.633.
34. Lonkar, S.P. and Abdala, A.A., 2014. Applications of graphene in catalysis. Journal of Thermodynamics & Catalysis, 5(2), p.1000132.
35. Yam, K.M., Guo, N., Jiang, Z., Li, S. and Zhang, C., 2020. Graphene-based heterogeneous catalysis: role of graphene. Catalysts, 10, p.53.
36. Jin, M., Jeong, H.K., Kim, T.H., So, K.P., Cui, Y., Yu, W.J., Ra, E. and Lee, Y.H., 2010. Synthesis and systematic characterization of functionalized graphene sheets generated by thermal exfoliation at low temperature. Journal of Physics D: Applied Physics, 43, p.275402.
37. Khan, U., O’Neill, A., Lotya, M., De, S. and Coleman, J.N., 2010. High-concentration solvent exfoliation of graphene. Small, 6(7), pp.864–871.
38. Peng, X. and Ahuja, R., 2008. Symmetry breaking induced bandgap in epitaxial graphene layers on SiC. Nano Letters, 8, pp.4464–4468.
39. Nomani, M.W.K., Shishir, R., Qazi, M., Diwan, D., Shields, V.B., Spencer, M.G., Tompa, G.S., Sbrockey, N.M. and Koley, G., 2010. Highly sensitive and selective detection of NO₂ using epitaxial graphene on 6H-SiC. Sensors and Actuators B: Chemical, 150, pp.301–307.
40. Stankovich, S., Dikin, D.A., Piner, R.D., Kohlhaas, K.A., Kleinhammes, A., Jia, Y., Wu, Y., Nguyen, S.T. and Ruoff, R.S., 2007. Synthesis of graphene-based nanosheets via chemical reduction of exfoliated graphite oxide. Carbon, 45, pp.1558–1565.
41. Moradizadeh, L., Yazdanpanah, P. and Karimi, G., 2023. Investigating the role of graphite and reduced graphene oxide in the fabrication of microporous layers for proton exchange membrane fuel cells. Journal of Materials Science, 58(31), pp.12706–12723.
42. Kim, E., Lee, W.G. and Jung, J., 2011. Agglomeration effects of thin metal catalyst on graphene film synthesized by chemical vapor deposition. Electronic Materials Letters, 7(3), pp.261–264.
43. Wang, Y. et al., 2011. Electrochemical delamination of CVD-grown graphene film: toward the recyclable use of copper catalyst. ACS Nano, 5(12), pp.9927–9933.
44. Ishihara, M., Koga, Y., Kim, J., Tsugawa, K. and Hasegawa, M., 2011. Direct evidence of advantage of Cu (111) for graphene synthesis by using Raman mapping and electron backscatter diffraction. Materials Letters, 65, pp.2864–2867.
45. Kim, W., Yoo, K., Seo, E.K., Kim, S.J. and Hwang, C., 2011. Scanning tunneling microscopy study on a graphene layer grown on a single-crystal Cu (111) surface by using chemical vapor deposition. Journal of the Korean Physical Society, 59(1), pp.71–74.
46. Guermoune, A., Chari, T., Popescu, F., Sabri, S.S., Guillemette, J., Skulason, H.S., Szkopek, T. and Siaj, M., 2011. Chemical vapor deposition synthesis of graphene on copper with methanol, ethanol, and propanol precursors. Carbon, 49, pp.4204–4210.
47. Miyata, Y., Kamon, K., Ohashi, K., Kitaura, R., Yoshimura, M. and Shinohara, H., 2010. A simple alcohol-chemical vapor deposition synthesis of single-layer graphenes using flash cooling. Applied Physics Letters, 96, p.263105.
Published
How to Cite
Issue
Section
License
Copyright (c) 2025 «JOURNAL OF MODERN CHEMISTRY»
This work is licensed under a Creative Commons Attribution-NonCommercial-ShareAlike 4.0 International License.
