Application of Box Behnken Design to Optimize the Parameters to Synthesis Graphene by CVD Process

Document Type : Research Paper


1 Faculty member of Research Institute of Petroleum Industry (RIPI)

2 Research Institute of Petroleum Industry (RIPI), West Blvd. Azadi Sport Complex, Tehran, I. R. Iran

3 Transport phenomena and Nanotechnology Laboratory, Department of Chemical Eng, University of Tehran, Tehran, I. R. Iran


This paper discusses the use of Box Behnken design (BBD) approach to plan the experiments for turning the yield of CVD, thickness and layer number of graphene sheets with an overall objective of optimizing the process to provide higher graphene production volume, fewer layers and thinness structure of graphene. BBD is having the maximum efficiency for an experiment involving four factors such as total gas flow, gas ratio (H2/CH4), temperature, and reaction time in three levels. The proposed BBD requires 25 runs of experiment for data acquisition and modeling the response surface. Three regression models were developed and their adequacies were verified to predict the output values at nearly all conditions. Further, the models were validated by performing experiments, taking three sets of random input values. The output parameters measured through experiments (actual) are in good consistency with the predicted values using the models. This work resulted in identifying the optimized set of turning parameters for CVD process to achieve high yield value and good structure of graphene. In the best condition, yield of process is 6.1%.


[1] K.S. Novoselov, A.K. Geim, S.V. Morozov, D. Jiang, Y. Zhang, S.V. Dubonos, I.V. Grigorieva, A.A. Firsov, (2004). “Electric field effect in atomically thin carbon films.” J. Science., Vol. 6, No. 13, pp. 666-672.
[2] C. Berger, Z. Song, X.Li, X. Wu, N. Brown, C. Naud, D. Mayou, T. Li, J. Hass, A.N. Marchenkov, E.H. Conrad, P.N., First, W.A. de Heer, (2006). “Electronic Confinement and Coherence in Patterned Epitaxial Graphene.” J. Science., Vol. 312, No. 4, pp. 1191-1201.
[3] Z Chen, YM Lin, MJ Rooks, P Avouris Physica E, (2007). “Low-dimensional Systems and Nanostructures.”J. Carbon., Vol. 40, No. 1, pp. 911-928.
[4] F. Schedin, A.K. Geim, S.V. Morozov, E.W. Hill, P. Blake, M.I. Katsnelson, L.S. Novoselov, (2007). “Detection of individual gas molecules adsorbed on graphene.” J. Nature Mater., Vol. 6, No. 1, pp. 652.
[5] Li X, Wang X, Zhang L, Lee S, Dai H. (2008). “Chemically derived, ultrasmooth graphene nanoribbon semiconductors.” J. Science., Vol. 319, No. 1, pp. 1229.
[6] Fukushima H, Drzal LT. (2003). “A carbon nanotube alternative, graphite nanoplatelets as reinforcements for polymers.” J. Annu Tech Conf Soc Plast Eng., Vol. 61, No. 36, pp. 2230-2241.
[7] Stankovich S, Dikin DA, Piner RD, Kohlhaas KA, Kleinhammes A, Jia Y., (2007). “Synthesis of graphene-based nanosheets via chemical reduction of exfoliated graphite oxide.” J. Carbon , Vol.45, No. 1, pp. 1558-1566.
[8] Wang JJ, Zhu MY, Outlaw RA, Zhao X, Manos DM, Holoway BC., (2004). “Synthesis of carbon nanosheets by inductively coupled radio-frequency plasma enhanced chemical vapor deposition.” J. Carbon., Vol. 42, No. 1, pp. 2867.
[9] Forbeaux I, Themlin JM, Debever JM. (1998). “Heteroepitaxial graphite on 6H–SiC (0001), interface formation through conduction-band electronic structure.” J. Phys Rev B., Vol. 58, No. 1, pp. 16396-402.
[10] Stankovich S, Dikin DA, Dommett GHB, Kohlhaas KM, Zimney EJ, Stach EA, (2006). “Graphene-based composite materials.” J. Nature., Vol. 442, No. 2, pp. 44-52.
[11] Stankovich S, Piner RD, Nguyen ST, Ruoff RS., (2006). “Synthesis and exfoliation of isocyanate-treated graphene oxide nanoplatelets.” J. Carbon., Vol. 44, No. 1, pp. 3342-3355.
[12] Chen J-H, Cullen WG, Jang C, Fuhrer MS, Williams ED., (2009). “Defect scattering in graphene.” J. Phys Rev Lett., Vol. 102, No. 1, pp. 805-812.
[13] Wu J, Pisula W, Mullen K. (2007). “Graphenes as potential material for electronics.” J. Chem Rev., Vol. 107, No. 8, pp. 83-96.
[14] Barone V, Hod O, Scuseria GE., (2006). “Electronic structure and stability of semiconducting grapheme nanoribbons.” J. Nano Lett., Vol. 6, No. 2, pp. 44-59.
[15] Cao H, Yu Q, Colby R, Pandey D, Park CS, Lian J, (2010). “Large scale graphitic thin films synthesized on Ni and transferred to insulators: Structural and electronic properties.” J. Appl Phys., Vol. 107, No. 4, pp. 44310-19.
[16] Bhaviripudi S, Jia X, Dresselhaus MS, Kong J., (2010). “Role of kinetic factors in chemical vapor deposition synthesis of uniform large area graphene using copper catalyst.” J. Nano Lett , Vol. 10, No. 2, pp. 4128-4134.
[17] Kim KS, Zhao Y, Jang H, Lee SY, Kim JM, Kim KS, (2009). “Large-scale pattern growth of graphene films for stretchable transparent electrodes.” J. Nature., Vol. 457, No. 3, pp. 706-717.
[18] Li X, Cai W, An J, Kim S, Nah J, Yang D, (2009). “Large-area synthesis of high-quality and uniform graphene films on copper foils.” J. Science., Vol. 324, No. 2, pp. 1312-1319.
[19] V. Suresh Babu, S. Sriram Kumar, R. V. Murali and M. Madhava Rao, (2011). “Investigation and validation of optimal cutting parameters for least surface roughness in EN24 with response surface method.” J. International Journal of Engineering, Science and Technology., Vol. 3, No. 6, pp. 146-155
[20] Long Wu, Kit-lun Yick, Sun-pui Ng, Joanne Yip, (2012). “Application of the Box–Behnken design to the optimization of process parameters in foam cup molding.” J. Expert Systems with Applications., Vol. 39, No. 9, pp. 7585-7596.
[21] Ross PJ, (1996). “Taguchi techniques for quality engineering.” McGraw- Hill., New York,
[22] Montgomery D.C, (1991). “Design and Analysis of Experiments.” John Wiley and sons., New York,
[23] C.H., Dong, X.Q., Xie, X.L., Wang, Y. Zhan, and Y.J., Yao, (2009). “Application of Box-Behnken design inoptimisation for polysaccharides extraction from cultured mycelium of Cordyceps sinensis.” J. Food and Bioproducts Processing., Vol. 87, No. 2, pp. 139-151.
[24] A. Ghozatloo, M. Shariaty-Niasar and A.M. Rashidi, (2013). “Preparation of nanofluids from functionalized Graphene by new alkaline method and study on the thermal conductivity and stability.” J. International  Communications in Heat and Mass Transfer., Vol. 42, No. 3, pp. 89-96.