Self-regulating homogenous growth of high-quality graphene on Co-Cu composite substrate for layer control.

The composite substrate of Co and Cu was proposed to grow homogenous high quality wafer-size graphene films by an atmosphere pressure CVD method. The composite substrate consists of a moderate-carbon-solubility metal top (Co coating) as a C-dissolving layer and a low-carbon-solubility metal base (Cu foil) as a C-rejecting layer. During the CVD process, the interdiffusion of Co and Cu atoms occurs in the composite. With the dynamic control on Co and Cu alloying process to affect the carbon solubility, active carbon atoms captured by the Co layer were segregated to form spontaneously a high-quality graphene film on the top of Cu-Co substrate. The tunable layer-number of the graphene films can be precisely controlled by adjusting the thickness of the Co layer. High quality single-layered graphene films with a 98% yield were prepared on an 80 nm-Co-coated Cu foil and insensitive to growth temperature and time. More importantly, this type of composite substrate has also been developed to grow AB-stacked bilayers and three-layer graphene with 99% surface coverage and absence of defects. The approach is opening up a new avenue for high-quality graphene production with precise layer control through composite substrate design.

[1]  B. Dlubak,et al.  Kinetic control of catalytic CVD for high-quality graphene at low temperatures. , 2012, ACS nano.

[2]  R. Piner,et al.  Growth mechanism and controlled synthesis of AB-stacked bilayer graphene on Cu-Ni alloy foils. , 2012, ACS nano.

[3]  X. Lü,et al.  The production of large bilayer hexagonal graphene domains by a two-step growth process of segregation and surface-catalytic chemical vapor deposition , 2012 .

[4]  M. Jiang,et al.  Autonomously Controlled Homogenous Growth of Wafer‐Sized High‐Quality Graphene via a Smart Janus Substrate , 2012 .

[5]  Zhongfan Liu,et al.  Rational design of a binary metal alloy for chemical vapour deposition growth of uniform single-layer graphene. , 2011, Nature communications.

[6]  P. Ajayan,et al.  Growth of bilayer graphene on insulating substrates. , 2011, ACS nano.

[7]  Fu-Rong Chen,et al.  Direct formation of wafer scale graphene thin layers on insulating substrates by chemical vapor deposition. , 2011, Nano letters.

[8]  S. Banerjee,et al.  CMOS-compatible synthesis of large-area, high-mobility graphene by chemical vapor deposition of acetylene on cobalt thin films. , 2011, ACS nano.

[9]  M. Jiang,et al.  Transparent Conductive Graphene Films Synthesized by Ambient Pressure Chemical Vapor Deposition Used as the Front Electrode of CdTe Solar Cells , 2011, Advanced materials.

[10]  Zhongfan Liu,et al.  Segregation Growth of Graphene on Cu–Ni Alloy for Precise Layer Control , 2011 .

[11]  Tianquan Lin,et al.  A facile preparation route for boron-doped graphene, and its CdTe solar cell application , 2011 .

[12]  Hui Li,et al.  Formation of bilayer bernal graphene: layer-by-layer epitaxy via chemical vapor deposition. , 2011, Nano letters.

[13]  Lei Fu,et al.  Universal segregation growth approach to wafer-size graphene from non-noble metals. , 2011, Nano letters.

[14]  N. Hanagata,et al.  Production of extended single-layer graphene. , 2011, ACS nano.

[15]  Zheng Yan,et al.  Growth of graphene from solid carbon sources , 2010, Nature.

[16]  Z. Zhong,et al.  Wafer scale homogeneous bilayer graphene films by chemical vapor deposition. , 2010, Nano letters.

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

[18]  Kwang S. Kim,et al.  Roll-to-roll production of 30-inch graphene films for transparent electrodes. , 2009, Nature nanotechnology.

[19]  R. Piner,et al.  Transfer of large-area graphene films for high-performance transparent conductive electrodes. , 2009, Nano letters.

[20]  G. Flynn,et al.  Structure and electronic properties of graphene nanoislands on Co(0001). , 2009, Nano letters.

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

[22]  Eun Sung Kim,et al.  Synthesis of Large‐Area Graphene Layers on Poly‐Nickel Substrate by Chemical Vapor Deposition: Wrinkle Formation , 2009 .

[23]  T. Tang,et al.  Direct observation of a widely tunable bandgap in bilayer graphene , 2009, Nature.

[24]  A. Reina,et al.  Growth of large-area single- and Bi-layer graphene by controlled carbon precipitation on polycrystalline Ni surfaces , 2009, 0906.2236.

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

[26]  A. Morpurgo,et al.  Trilayer graphene is a semimetal with a gate-tunable band overlap , 2009, Nature Nanotechnology.

[27]  Kwang S. Kim,et al.  Large-scale pattern growth of graphene films for stretchable transparent electrodes , 2009, Nature.

[28]  A. M. Dobrotvorskii,et al.  Experimental and theoretical study of the morphology of commensurate and incommensurate graphene layers on Ni single-crystal surfaces , 2008 .

[29]  J. Flege,et al.  Epitaxial graphene on ruthenium. , 2008, Nature materials.

[30]  N. Peres,et al.  Fine Structure Constant Defines Visual Transparency of Graphene , 2008, Science.

[31]  T. Michely,et al.  Structural coherency of graphene on Ir(111). , 2008, Nano letters.

[32]  F. Guinea,et al.  The electronic properties of graphene , 2007, Reviews of Modern Physics.

[33]  S. Marchini,et al.  Scanning tunneling microscopy of graphene on Ru(0001) , 2007 .

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

[35]  Jannik C. Meyer,et al.  The structure of suspended graphene sheets , 2007, Nature.

[36]  Andre K. Geim,et al.  Raman spectrum of graphene and graphene layers. , 2006, Physical review letters.

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

[38]  E. .. Mittemeijer,et al.  The solubility of C in solid Cu , 2004 .

[39]  W. Hofmeister,et al.  Carbon nanotube growth from Cu-Co alloys for field emission applications , 2003, IEEE/CPMT/SEMI. 28th International Electronics Manufacturing Technology Symposium (Cat. No.03CH37479).

[40]  M. Hecker,et al.  Interdiffusion, stress, and microstructure evolution during annealing in Co/Cu/Co trilayers , 2002 .

[41]  R. Mclellan,et al.  The diffusion of carbon in solid cobalt , 1992 .

[42]  K. Ishida,et al.  The C-Co(Carbon-Cobalt) system , 1991 .

[43]  B. S. Berry.  Diffusion of carbon in nickel , 1973 .

[44]  J. C. Swartz.  Solubility of graphite in cobalt and nickel , 1971 .

[45]  J. J. Lander,et al.  Solubility and Diffusion Coefficient of Carbon in Nickel: Reaction Rates of Nickel‐Carbon Alloys with Barium Oxide , 1952 .

[46]  H. Sørum,et al.  Interdiffusion in Cu‐Ni, Co‐Ni, and Co‐Cu , 1964 .