Recent Progress on CVD Growth of Graphene from a Liquid Carbon Precursor


  • Azzafeerah Mahyuddin Universiti Teknologi Malaysia
  • Abd. Khamim Ismail Universiti Teknologi Malaysia
  • Muhammad Firdaus Omar Universiti Teknologi Malaysia
  • Ainul Hakimah Karim Universiti Kuala Lumpur



Graphene, Chemical Vapor Deposition, Liquid Precursor, Synthesis Method


Graphene has become a remarkable highlight of advanced material research because of its far superior properties compared to other materials. Chemical vapor deposition (CVD) has emerged as an essential method for scalable production and large area graphene for various applications. Various carbon precursors have been reported for graphene production as they can dramatically impact the graphene growth yield. In the early years of graphene CVD growth, hydrocarbon gases such as methane and acetylene have become favorable carbon precursors because of their stability at elevated temperature and controllable growth. However, hydrocarbon gases are known as explosives and toxic, therefore require a growth system with a high degree of safety and handling precautions. With the limitations mentioned above, liquid carbon source may change the graphene growth landscape as it is relatively inexpensive, non-explosive compared to the conventional gaseous precursor. This article aims to review a detailed synthesis of large-area graphene using liquid carbon precursors via the CVD technique. Challenges and future perspectives are highlights.


A. K. Geim and K. S. Novoselov, “The rise of graphene,” Nat. Mater., vol. 6, no. 3, pp. 183–191, Mar. 2007.

R. K. Singh Raman et al., “Protecting copper from electrochemical degradation by graphene coating,” Carbon N. Y., vol. 50, no. 11, pp. 4040–4045, Sep. 2012.

M.-S. Kim, J.-M. Woo, D.-M. Geum, J. R. Rani, and J.-H. Jang, “Effect of copper surface pre-treatment on the properties of CVD grown graphene,” AIP Adv., vol. 4, no. 12, p. 127107, Dec. 2014.

T. J. Gnanaprakasa et al., “The role of copper pretreatment on the morphology of graphene grown by chemical vapor deposition,” Microelectron. Eng., vol. 131, pp. 1–7, Jan. 2015.

R. Addou, A. Dahal, P. Sutter, and M. Batzill, “Monolayer graphene growth on Ni (111) by low temperature chemical vapor deposition,” Appl. Phys. Lett., vol. 100, no. 2, p. 021601, Jan. 2012.

E. Ozceri and Y. Selamet, “Influence of buffer layers on Ni thin film structure and graphene growth by CVD,” J. Phys. D. Appl. Phys., vol. 48, no. 45, p. 455302, Nov. 2015.

G. W. Cushing, V. Johánek, J. K. Navin, and I. Harrison, “Graphene Growth on Pt(111) by Ethylene Chemical Vapor Deposition at Surface Temperatures near 1000 K,” J. Phys. Chem. C, vol. 119, no. 9, pp. 4759–4768, Mar. 2015.

T. Gao et al., “Growth and Atomic-Scale Characterizations of Graphene on Multifaceted Textured Pt Foils Prepared by Chemical Vapor Deposition,” ACS Nano, vol. 5, no. 11, pp. 9194–9201, Nov. 2011.

E. Sutter, P. Albrecht, and P. Sutter, “Graphene growth on polycrystalline Ru thin films,” Appl. Phys. Lett., vol. 95, no. 13, p. 133109, Sep. 2009.

S. Nie et al., “Growth from Below: Graphene Bilayers on Ir(111),” ACS Nano, vol. 5, no. 3, pp. 2298–2306, Mar. 2011.

M. A. Azam et al., “Review—Critical Considerations of High Quality Graphene Synthesized by Plasma-Enhanced Chemical Vapor Deposition for Electronic and Energy Storage Devices,” ECS J. Solid State Sci. Technol., vol. 6, no. 6, pp. M3035–M3048, Jan. 2017.

C.-M. Seah, S.-P. Chai, and A. R. Mohamed, “Mechanisms of graphene growth by chemical vapour deposition on transition metals,” Carbon N. Y., vol. 70, pp. 1–21, Apr. 2014.

M. Marchena, D. Janner, T. L. Chen, V. Finazzi, and V. Pruneri, “Low temperature direct growth of graphene patterns on flexible glass substrates catalysed by a sacrificial ultrathin Ni film,” Opt. Mater. Express, vol. 6, no. 8, p. 2487, Aug. 2016.

I. Vlassiouk et al., “Electrical and thermal conductivity of low temperature CVD graphene: the effect of disorder,” Nanotechnology, vol. 22, no. 27, p. 275716, Jul. 2011.

Y. Gong et al., “Layer-Controlled and Wafer-Scale Synthesis of Uniform and High-Quality Graphene Films on a Polycrystalline Nickel Catalyst,” Adv. Funct. Mater., vol. 22, no. 15, pp. 3153–3159, Aug. 2012.

Y. Miyata, K. Kamon, K. Ohashi, R. Kitaura, M. Yoshimura, and H. Shinohara, “A simple alcohol-chemical vapor deposition synthesis of single-layer graphenes using flash cooling,” Appl. Phys. Lett., vol. 96, no. 26, p. 263105, Jun. 2010.

X. Dong et al., “Growth of large-sized graphene thin-films by liquid precursor-based chemical vapor deposition under atmospheric pressure,” Carbon N. Y., vol. 49, no. 11, pp. 3672–3678, Sep. 2011.

J. Campos-Delgado et al., “CVD synthesis of mono- and few-layer graphene using alcohols at low hydrogen concentration and atmospheric pressure,” Chem. Phys. Lett., vol. 584, pp. 142–146, Oct. 2013.

X. Chen et al., “Chemical vapor deposition growth of 5 mm hexagonal single-crystal graphene from ethanol,” Carbon N. Y., vol. 94, pp. 810–815, Nov. 2015.

A. Gnisci et al., “Ethanol-CVD Growth of Sub-mm Single-Crystal Graphene on Flat Cu Surfaces,” J. Phys. Chem. C, vol. 122, no. 50, pp. 28830–28838, Dec. 2018.

R. John, A. Ashokreddy, C. Vijayan, and T. Pradeep, “Single- and few-layer graphene growth on stainless steel substrates by direct thermal chemical vapor deposition,” Nanotechnology, vol. 22, no. 16, p. 165701, Apr. 2011.

A. Srivastava et al., “Novel Liquid Precursor-Based Facile Synthesis of Large-Area Continuous, Single, and Few-Layer Graphene Films,” Chem. Mater., vol. 22, no. 11, pp. 3457–3461, Jun. 2010.

C. B. Flores and D. M. López, “Multilayer Graphene Synthesized by CVD Using Liquid Hexane as the Carbon Precursor,” World J. Condens. Matter Phys., vol. 01, no. 04, pp. 157–160, 2011.

Z. Li et al., “Low-Temperature Growth of Graphene by Chemical Vapor Deposition Using Solid and Liquid Carbon Sources,” ACS Nano, vol. 5, no. 4, pp. 3385–3390, Apr. 2011.

C. Kang, D. H. Jung, and J. S. Lee, “Atmospheric Pressure Chemical Vapor Deposition of Graphene Using a Liquid Benzene Precursor,” J. Nanosci. Nanotechnol., vol. 15, no. 11, pp. 9098–9103, Nov. 2015.

J. Jang et al., “Low-temperature-grown continuous graphene films from benzene by chemical vapor deposition at ambient pressure,” Sci. Rep., vol. 5, no. 1, p. 17955, Dec. 2015.

Y. Xue et al., “Low Temperature Growth of Highly Nitrogen-Doped Single Crystal Graphene Arrays by Chemical Vapor Deposition,” J. Am. Chem. Soc., vol. 134, no. 27, pp. 11060–11063, Jul. 2012.

R. Shanmugam, M. Rangarajan, S. Devanathan, V. G. Sathe, R. Senthilkumar, and N. K. Kothurkar, “A design of experiments investigation of the effects of synthesis conditions on the quality of CVD graphene,” Mater. Res. Express, vol. 3, no. 12, p. 125601, Dec. 2016.

M. H. Khan et al., “Hydrogen sieving from intrinsic defects of benzene-derived single-layer graphene,” Carbon N. Y., vol. 153, pp. 458–466, Nov. 2019.

B. Zhang et al., “Low-temperature chemical vapor deposition growth of graphene from toluene on electropolished copper foils,” ACS Nano, vol. 6, no. 3, pp. 2471–2476, 2012.

J. G. Kim, W. S. Kim, Y. H. Kim, C. H. Lim, and D. J. Choi, “Formation of graphene on SiC by chemical vapor deposition with liquid sources,” Surf. Coatings Technol., vol. 231, pp. 189–192, Sep. 2013.

D. H. Seo et al., “Single-step ambient-air synthesis of graphene from renewable precursors as electrochemical genosensor,” Nat. Commun., vol. 8, no. 1, p. 14217, Apr. 2017.

M. V. Jacob et al., “Catalyst-Free Plasma Enhanced Growth of Graphene from Sustainable Sources,” Nano Lett., vol. 15, no. 9, pp. 5702–5708, Sep. 2015.

B. Ouyang, Y. Zhang, Z. Zhang, H. J. Fan, and R. S. Rawat, “Green synthesis of vertical graphene nanosheets and their application in high-performance supercapacitors,” RSC Adv., vol. 6, no. 28, pp. 23968–23973, 2016.

S. F. A. Rahman, M. R. Mahmood, and A. M. Hashim, “Growth of graphene on nickel using a natural carbon source by thermal chemical vapor deposition,” Sains Malaysiana, vol. 43, no. 8, pp. 1205–1211, 2014.

M. J. Salifairus, S. B. Abd Hamid, T. Soga, S. A. H. Alrokayan, H. A. Khan, and M. Rusop, “Structural and optical properties of graphene from green carbon source via thermal chemical vapor deposition,” J. Mater. Res., vol. 31, no. 13, pp. 1947–1956, 2016.

M. Robaiah, M. Rusop, S. Abdullah, Z. Khusaimi, H. Azhan, and N. A. Asli, “Synthesis graphene layer at different waste cooking palm oil temperatures,” in AIP Conference Proceedings, 2017, p. 030008.

S. Maarof, A. A. Ali, and A. M. Hashim, “Synthesis of Large-Area Single-Layer Graphene Using Refined Cooking Palm Oil on Copper Substrate by Spray Injector-Assisted CVD,” Nanoscale Res. Lett., vol. 14, no. 1, p. 143, Dec. 2019.

L. M. Malard, M. A. Pimenta, G. Dresselhaus, and M. S. Dresselhaus, “Raman spectroscopy in graphene,” Phys. Rep., vol. 473, no. 5–6, pp. 51–87, Apr. 2009.

J. Wang et al., “A review of graphene synthesisatlow temperatures by CVD methods,” New Carbon Mater., vol. 35, no. 3, pp. 193–208, Jun. 2020.

S. Naghdi, K. Y. Rhee, and S. J. Park, “A catalytic, catalyst-free, and roll-to-roll production of graphene via chemical vapor deposition: Low temperature growth,” Carbon N. Y., vol. 127, pp. 1–12, Feb. 2018.