Innovative Approach to Graphene Film Synthesis: Factorial Design in PECVD Experiments

Siwasit Pitjamit; Norrapon Vichiansan; Komgrit Leksakul

doi:10.5614/j.eng.technol.sci.2025.57.1.6

Innovative Approach to Graphene Film Synthesis: Factorial Design in PECVD Experiments

Published: 2025-01-01 | DOI: 10.5614/j.eng.technol.sci.2025.57.1.6 | Vol 57, Issue 1 (2025) | Cited by: 2

Authors

Siwasit Pitjamit

Department of Industrial Engineering, Faculty of Engineering, Rajamangala University of Technology Lanna, Tak 63000

ORCID: 0000-0002-4842-5871 · OpenAlex: A5012270799

Norrapon Vichiansan

Multidisciplinary Center, Faculty of Engineering, Chiang Mai University, Chiang Mai 50200

ORCID: 0009-0002-1232-4486 · OpenAlex: A5060072940

Komgrit Leksakul

Department of Industrial Engineering, Faculty of Engineering, Chiang Mai University, Chiang Mai 50200

OpenAlex: A5108345295

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Abstract

Graphene, a two-dimensional carbon allotrope, has garnered significant interest due to its exceptional properties and diverse applications. This study investigates the optimization of graphene synthesis parameters using plasma-enhanced chemical vapor deposition (PECVD) to enhance film properties and broaden their application potentials. Using a comprehensive factorial design approach, factors including electric power (ranging from 60 to 100 W), the acetylene-to-hydrogen ratio (ranging from 30:70 to 50:50), and discharge time (ranging from 10 to 30 minutes) were systematically varied, and film thickness and the D/G ratio served as response variables. The experimental results revealed the significant effects of these parameters on film thickness, with optimal conditions identified as an electric power of 100 W, an acetylene-to-hydrogen ratio of 50:50, and a discharge time of 10 min. The average film thickness ranged from 41.51 to 253.80 nm. Morphological and structural analyses using atomic force microscopy and Raman spectroscopy elucidated the impact of synthesis parameters on film characteristics, with the D/G ratio varying from 0.75 to 1.8, indicating the degree of graphitization and defect density. Furthermore, surface properties and wettability were assessed using contact angle measurements, providing insights into surface interactions crucial for various applications. This study culminates in discussions on the implications for graphene synthesis optimization and its potential applications across diverse fields. Overall, this research contributes to advancing the understanding of graphene synthesis methodologies and underscores its significance in driving technological innovations.

Keywords

factorial design; film thickness; graphene synthesis; graphitization; raman spectroscopy; thin film characterization

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Graphene research and applications Primary

0.60

Materials Chemistry › Materials Science › Physical Sciences

Molecular Junctions and Nanostructures

0.51

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2025

2026

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Year	Citations
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Graphene 0.78

level 2

Factorial experiment 0.75

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Materials science 0.46

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Mathematics 0.35 Composite material 0.33 Engineering drawing 0.32 Nanotechnology 0.32 Engineering 0.26 Statistics 0.24

Institution Network

Rajamangala University of Technology Lanna TH
Siwasit Pitjamit
Chiang Mai University TH
Norrapon Vichiansan · Komgrit Leksakul

References

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Song, Y., Zou, W., Lu, Q., Lin, L., & Liu, Z. (2021). Graphene transfer: Paving the road for applications of chemical vapor deposition graphene. Small, 17(8), 2007600. https://doi.org/10.1002/smll.202007600 DOI: 10.1002/smll.202007600
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Sui, C., Zhao, Y., Zhang, Z., He, J., Zhang, Z., He, X., … & Wu, J. (2017). Morphology-controlled tensile mechanical characteristics in graphene allotropes. ACS Omega, 2(7), 3977–3988. https://doi.org/10.1021/acsomega.7b00732 DOI: 10.1021/acsomega.7b00732
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[ref-1] Abdelrahman, M. M. (2015). Study of plasma and ion beam sputtering processes. Journal of Physical Science and Application, 5(2), 128–142. https://doi.org/10.17265/2159-5348/2015.02.007 DOI: 10.17265/2159-5348/2015.02.007

[ref-2] Dasari, B. L., Nouri, J. M., Brabazon, D., & Naher, S. (2017). Graphene and derivatives–Synthesis techniques, properties and their energy applications. Energy, 140, 766–778. https://doi.org/10.1016/j.energy.2017.08.048 DOI: 10.1016/j.energy.2017.08.048

[ref-3] Fu, R., Yang, Y., Lu, C., Ming, Y., Zhao, X., Hu, Y., … & Chen, W. (2018). Large-scale fabrication of high-performance ionic polymer–metal composite flexible sensors by in situ plasma etching and magnetron sputtering. ACS Omega, 3(8), 9146–9154. https://doi.org/10.1021/acsomega.8b00877 DOI: 10.1021/acsomega.8b00877

[ref-4] Iqbal, M., Dinh, D. K., Abbas, Q., Imran, M., Sattar, H., & Ul Ahmad, A. (2019). Controlled surface wettability by plasma polymer surface modification. Surfaces, 2(2), 349–371. https://doi.org/10.3390/surfaces2020026 DOI: 10.3390/surfaces2020026

[ref-5] Kalita, G., Ayhan, M. E., Sharma, S., Shinde, S. M., Ghimire, D., Wakita, K., … & Tanemura, M. (2014). Low-temperature deposited graphene by surface wave plasma CVD as effective oxidation resistive barrier. Corrosion Science, 78, 183–187. https://doi.org/10.1016/j.corsci.2013.09.013 DOI: 10.1016/j.corsci.2013.09.013

[ref-6] Kalita, G., Kayastha, M. S., Uchida, H., Wakita, K., & Umeno, M. (2012). Direct growth of nanographene films by surface wave plasma chemical vapor deposition and their application in photovoltaic devices. RSC Advances, 2(8), 3225–3230. https://doi.org/10.1039/C2RA01024K DOI: 10.1039/c2ra01024k

[ref-7] Kalita, G., Sharma, S., Wakita, K., Umeno, M., Hayashi, Y., & Tanemura, M. (2012). Synthesis of graphene by surface wave plasma chemical vapor deposition from camphor. Physica Status Solidi (a), 209(12), 2510–2513. https://doi.org/10.1002/pssa.201228554 DOI: 10.1002/pssa.201228554

[ref-8] Kalita, G., Wakita, K., & Umeno, M. (2012). Low-temperature growth of graphene film by microwave-assisted surface wave plasma CVD for transparent electrode application. RSC Advances, 2(7), 2815–2820. https://doi.org/10.1039/C2RA00648K DOI: 10.1039/c2ra00648k

[ref-9] Khan, K., Tareen, A. K., Iqbal, M., Shi, Z., Zhang, H., & Guo, Z. (2021). Novel emerging graphdiyne-based two-dimensional materials: Synthesis, properties and renewable energy applications. Nano Today, 39, 101207. https://doi.org/10.1016/j.nantod.2021.101207 DOI: 10.1016/j.nantod.2021.101207

[ref-10] Kleijn, C. R., Dorsman, R., Kuijlaars, K. J., Okkerse, M., & van Santen, H. V. (2007). Multi-scale modeling of chemical vapor deposition processes for thin-film technology. Journal of Crystal Growth, 303(2), 362–380. https://doi.org/10.1016/j.jcrysgro.2006.12.062 DOI: 10.1016/j.jcrysgro.2006.12.062

[ref-11] Kruszelnicki, M., Polowczyk, I., & Kowalczuk, P. B. (2024). Insight into the influence of surface wettability on flotation properties of solid particles–Critical contact angle in flotation. Powder Technology, 431, 119056. https://doi.org/10.1016/j.powtec.2023.119056 DOI: 10.1016/j.powtec.2023.119056

[ref-12] Li, X., Colombo, L., & Ruoff, R. S. (2016). Synthesis of graphene films on copper foils by chemical vapor deposition. Advanced Materials, 28(31), 6247–6252. https://doi.org/10.1002/adma.201504760 DOI: 10.1002/adma.201504760

[ref-13] Li, Z., Deng, L., Kinloch, I. A., & Young, R. J. (2023). Raman spectroscopy of carbon materials and their composites: Graphene, nanotubes and fibres. Progress in Materials Science, 135, 101089. https://doi.org/10.1016/j.pmatsci.2023.101089 DOI: 10.1016/j.pmatsci.2023.101089

[ref-14] Liu, W., Li, M., Jiang, G., Li, G., Zhu, J., Xiao, M., … & Chen, Z. (2020). Graphene quantum dots-based advanced electrode materials: Design, synthesis and their applications in electrochemical energy storage and electrocatalysis. Advanced Energy Materials, 10(26), 2001275. https://doi.org/10.1002/aenm.202001275 DOI: 10.1002/aenm.202001275

[ref-15] Ma, T., Liu, Z., Wen, J., Gao, Y., Ren, X., Chen, H., … & Ren, W. (2017). Tailoring the thermal and electrical transport properties of graphene films by grain size engineering. Nature Communications, 8, 14486. https://doi.org/10.1038/ncomms14486 DOI: 10.1038/ncomms14486

[ref-16] Moene, R., Dekker, J. P., Makkee, M., Schoonman, J., & Moulijn, J. A. (1994). Evaluation of isothermal chemical vapor infiltration with Langmuir‐Hinshelwood type kinetics. Journal of the Electrochemical Society, 141(2), 282–286. https://doi.org/10.1149/1.2054700 DOI: 10.1149/1.2054700

[ref-17] Phiri, J., Johansson, L. S., Gane, P., & Maloney, T. (2018). A comparative study of mechanical, thermal and electrical properties of graphene-, graphene oxide-and reduced graphene oxide-doped microfibrillated cellulose nanocomposites. Composites Part B: Engineering, 147, 104–113. https://doi.org/10.1016/j.compositesb.2018.04.018 DOI: 10.1016/j.compositesb.2018.04.018

[ref-18] Roy, D., Kanojia, S., Mukhopadhyay, K., & Eswara Prasad, N. (2021). Analysis of carbon-based nanomaterials using Raman spectroscopy: Principles and case studies. Bulletin of Materials Science, 44, 31. https://doi.org/10.1007/s12034-020-02327-9 DOI: 10.1007/s12034-020-02327-9

[ref-19] Scardaci, V., & Compagnini, G. (2021). Raman spectroscopy investigation of graphene oxide reduction by laser scribing. Journal of Carbon Research, 7(2), 48. https://doi.org/10.3390/c7020048 DOI: 10.3390/c7020048

[ref-20] Song, Y., Zou, W., Lu, Q., Lin, L., & Liu, Z. (2021). Graphene transfer: Paving the road for applications of chemical vapor deposition graphene. Small, 17(8), 2007600. https://doi.org/10.1002/smll.202007600 DOI: 10.1002/smll.202007600

[ref-21] Stephen, D. T., & Hong, H. (2023). Using combustion synthesis to convert emissions into useful solid materials. In Combustion Chemistry and the Carbon Neutral Future, 599–630. Elsevier. https://doi.org/10.1016/B978-0-323-99213-8.00016-3 DOI: 10.1016/b978-0-323-99213-8.00016-3

[ref-22] Sui, C., Zhao, Y., Zhang, Z., He, J., Zhang, Z., He, X., … & Wu, J. (2017). Morphology-controlled tensile mechanical characteristics in graphene allotropes. ACS Omega, 2(7), 3977–3988. https://doi.org/10.1021/acsomega.7b00732 DOI: 10.1021/acsomega.7b00732

[ref-23] Thomas, T. M., Chowdhury, I. U., Dhivyaraja, K., Mahapatra, P. S., Pattamatta, A., & Tiwari, M. K. (2021). Droplet dynamics on a wettability patterned surface during spray impact. Processes, 9(3), 555. https://doi.org/10.3390/pr9030555 DOI: 10.3390/pr9030555

[ref-24] Vasić, B., Matković, A., & Gajić, R. (2017). Phase imaging and nanoscale energy dissipation of supported graphene using amplitude modulation atomic force microscopy. Nanotechnology, 28(46), 465708. https://doi.org/10.1088/1361-6528/aa8e3b DOI: 10.1088/1361-6528/aa8e3b

[ref-25] Wahab, H., Heil, J., Tyrrell, A. S., Muller, T., Ackerman, J., Kotthoff, L., & Johnson, P. A. (2024). Optimization of structural and electrical properties of graphene-based TiO2 thin-film nanocomposites using machine learning. Journal of Materials Chemistry C, 12(6), 1389–1399. https://doi.org/10.1039/D3TC05069H DOI: 10.1039/d3tc05069h

[ref-26] Wei, X., Wang, X., Tan, J., Sun, X., Jiang, H., & Chen, W. (2016). Graphene nanosheets–Decorated silicon composites as high-performance anodes for lithium-ion batteries. Energy Storage Materials, 3, 30–37. https://doi.org/10.1016/j.ensm.2015.12.001 DOI: 10.1016/j.ensm.2015.12.001

[ref-27] Yang, C., Tang, C., Zhou, Q., Hu, J., Xue, X., Huang, Y., & Wang, C. (2020). Mechanically strengthened graphene aerogels via rational assembly for enhanced thermal insulation. ACS Applied Materials & Interfaces, 12(36), 40467–40475. https://doi.org/10.1021/acsami.0c09481 DOI: 10.1021/acsami.0c09481

[ref-28] Zhao, H., Zhou, L., & Zhang, C. (2022). Molecular insights into the impact of graphene oxide on microbial cell membranes. Environmental Science: Nano, 9(4), 1116–1126. https://doi.org/10.1039/D2EN00167E DOI: 10.1039/d2en00167e

[ref-29] Zhu, J., Li, S., & Zeng, X. (2023). Raman spectroscopic insights into carbon nanomaterials: Techniques, challenges, and applications. Carbon Trends, 10, 100257. https://doi.org/10.1016/j.cartre.2023.100257 DOI: 10.1016/j.cartre.2023.100257

[ref-30] Zhu, X., Liu, S., Yang, Y., Wang, Y., Sun, H., Chen, H., … & Wang, C. (2019). Multi-scale understanding of graphene-based membranes: From fundamentals to advanced water purification applications. Nano Research, 12(1), 183–200. https://doi.org/10.1007/s12274-018-2236-6 DOI: 10.1007/s12274-018-2236-6