Role of hydrogen in chemical vapor deposition growth of large single-crystal graphene.

We show that graphene chemical vapor deposition growth on copper foil using methane as a carbon source is strongly affected by hydrogen, which appears to serve a dual role: an activator of the surface bound carbon that is necessary for monolayer growth and an etching reagent that controls the size and morphology of the graphene domains. The resulting growth rate for a fixed methane partial pressure has a maximum at hydrogen partial pressures 200-400 times that of methane. The morphology and size of the graphene domains, as well as the number of layers, change with hydrogen pressure from irregularly shaped incomplete bilayers to well-defined perfect single layer hexagons. Raman spectra suggest the zigzag termination in the hexagons as more stable than the armchair edges.

[1]  M. Chi,et al.  Electrical and thermal conductivity of low temperature CVD graphene: the effect of disorder , 2011, Nanotechnology.

[2]  J. Warner,et al.  Hexagonal single crystal domains of few-layer graphene on copper foils. , 2011, Nano letters.

[3]  Luigi Colombo,et al.  Large-area graphene single crystals grown by low-pressure chemical vapor deposition of methane on copper. , 2011, Journal of the American Chemical Society.

[4]  Jinlong Yang,et al.  First-Principles Thermodynamics of Graphene Growth on Cu Surfaces , 2011, 1101.3851.

[5]  D. Vvedensky,et al.  Novel growth mechanism of epitaxial graphene on metals. , 2010, Nano letters.

[6]  S. Pei,et al.  Control and characterization of individual grains and grain boundaries in graphene grown by chemical vapour deposition. , 2010, Nature materials.

[7]  Hui‐Ming Cheng,et al.  Efficient growth of high-quality graphene films on Cu foils by ambient pressure chemical vapor deposition , 2010 .

[8]  Carl W. Magnuson,et al.  Graphene films with large domain size by a two-step chemical vapor deposition process. , 2010, Nano letters.

[9]  Klaus von Klitzing,et al.  Raman scattering at pure graphene zigzag edges. , 2010, Nano letters.

[10]  Pinshane Y. Huang,et al.  Grains and grain boundaries in single-layer graphene atomic patchwork quilts , 2010, Nature.

[11]  R. Ruoff,et al.  Graphene and Graphene Oxide: Synthesis, Properties, and Applications , 2010, Advanced materials.

[12]  Jing Kong,et al.  Role of kinetic factors in chemical vapor deposition synthesis of uniform large area graphene using copper catalyst. , 2010, Nano letters.

[13]  Kwang S. Kim,et al.  Roll-to-roll production of 30-inch graphene films for transparent electrodes. , 2010, Nature nanotechnology.

[14]  J. Smet,et al.  Hot phonons in an electrically biased graphene constriction. , 2010, Nano letters.

[15]  Luigi Colombo,et al.  Evolution of graphene growth on Ni and Cu by carbon isotope labeling. , 2009, Nano letters.

[16]  SUPARNA DUTTASINHA,et al.  Graphene: Status and Prospects , 2009, Science.

[17]  S. Banerjee,et al.  Large-Area Synthesis of High-Quality and Uniform Graphene Films on Copper Foils , 2009, Science.

[18]  Daniel Knapp,et al.  Density functional theory studies of methane dissociation on anode catalysts in solid-oxide fuel cells: Suggestions for coke reduction , 2007 .

[19]  Andre K. Geim,et al.  The rise of graphene. , 2007, Nature materials.

[20]  Andre K. Geim,et al.  Electric Field Effect in Atomically Thin Carbon Films , 2004, Science.

[21]  I. Chorkendorff,et al.  The interaction of CH4 at high temperatures with clean and oxygen precovered Cu(100) , 1992 .

[22]  A. Gelb,et al.  Classical trajectory study of the dissociation of hydrogen on copper single crystals: II. Cu(100) and Cu(110) , 1977 .

[23]  A. Gelb,et al.  Classical trajectory studies of hydrogen dissociation on a Cu(100) surface , 1976 .