Improved synthesis of graphene oxide.

An improved method for the preparation of graphene oxide (GO) is described. Currently, Hummers' method (KMnO(4), NaNO(3), H(2)SO(4)) is the most common method used for preparing graphene oxide. We have found that excluding the NaNO(3), increasing the amount of KMnO(4), and performing the reaction in a 9:1 mixture of H(2)SO(4)/H(3)PO(4) improves the efficiency of the oxidation process. This improved method provides a greater amount of hydrophilic oxidized graphene material as compared to Hummers' method or Hummers' method with additional KMnO(4). Moreover, even though the GO produced by our method is more oxidized than that prepared by Hummers' method, when both are reduced in the same chamber with hydrazine, chemically converted graphene (CCG) produced from this new method is equivalent in its electrical conductivity. In contrast to Hummers' method, the new method does not generate toxic gas and the temperature is easily controlled. This improved synthesis of GO may be important for large-scale production of GO as well as the construction of devices composed of the subsequent CCG.

[1]  W. E. Billups,et al.  Reductive Alkylation of Fluorinated Graphite , 2008 .

[2]  C. Berger,et al.  Electronic Confinement and Coherence in Patterned Epitaxial Graphene , 2006, Science.

[3]  S. Stankovich,et al.  Synthesis and exfoliation of isocyanate-treated graphene oxide nanoplatelets , 2006 .

[4]  M. Wissler,et al.  Graphite and carbon powders for electrochemical applications , 2006 .

[5]  E. Samulski,et al.  Synthesis of water soluble graphene. , 2008, Nano letters.

[6]  Kang L. Wang,et al.  A chemical route to graphene for device applications. , 2007, Nano letters.

[7]  Roberto Car,et al.  Functionalized single graphene sheets derived from splitting graphite oxide. , 2006, The journal of physical chemistry. B.

[8]  R. Yazami,et al.  Insertion compounds of graphite with improved performances and electrochemical applications of those compounds , 1987 .

[9]  Dongmin Chen,et al.  Synthesis and Solid-State NMR Structural Characterization of 13C-Labeled Graphite Oxide , 2008, Science.

[10]  Xin Lu,et al.  Fast and Facile Preparation of Graphene Oxide and Reduced Graphene Oxide Nanoplatelets , 2009 .

[11]  D. A. Corley,et al.  Kinetics of diazonium functionalization of chemically converted graphene nanoribbons. , 2010, ACS nano.

[12]  J. Tour,et al.  Graphite oxide flame-retardant polymer nanocomposites. , 2009, ACS applied materials & interfaces.

[13]  C. A. Wilkie,et al.  Preparation of nanocomposites from styrene and modified graphite oxides , 2004 .

[14]  J. Coleman,et al.  Liquid phase production of graphene by exfoliation of graphite in surfactant/water solutions , 2008, 0809.2690.

[15]  J. D. Lopez-Gonzalez,et al.  Study of oxygen-containing groups in a series of graphite oxides: Physical and chemical characterization , 1995 .

[16]  L. Staudenmaier,et al.  Verfahren zur Darstellung der Graphitsäure , 1898 .

[17]  W. S. Hummers,et al.  Preparation of Graphitic Oxide , 1958 .

[18]  R. Ruoff,et al.  Graphene: calling all chemists. , 2008, Nature nanotechnology.

[19]  W. D. Heer Electronic coherence and confinement in patterned epitaxial graphene , 2006 .

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

[21]  Jacek Klinowski,et al.  A new structural model for graphite oxide , 1998 .

[22]  Cheol-Woong Yang,et al.  Evidence of graphitic AB stacking order of graphite oxides. , 2008, Journal of the American Chemical Society.

[23]  J. Tour,et al.  Longitudinal unzipping of carbon nanotubes to form graphene nanoribbons , 2009, Nature.

[24]  S. Stankovich,et al.  Synthesis of graphene-based nanosheets via chemical reduction of exfoliated graphite oxide , 2007 .

[25]  S. Stankovich,et al.  Stable aqueous dispersions of graphitic nanoplatelets via the reduction of exfoliated graphite oxide in the presence of poly(sodium 4-styrenesulfonate) , 2006 .

[26]  J. Tour,et al.  Lower-defect graphene oxide nanoribbons from multiwalled carbon nanotubes. , 2010, ACS nano.

[27]  Chun Li,et al.  Flexible graphene films via the filtration of water-soluble noncovalent functionalized graphene sheets. , 2008, Journal of the American Chemical Society.

[28]  G. Eda,et al.  Large-area ultrathin films of reduced graphene oxide as a transparent and flexible electronic material. , 2008, Nature nanotechnology.

[29]  Klaus Kern,et al.  Atomic structure of reduced graphene oxide. , 2010, Nano letters.

[30]  G. Wallace,et al.  Processable aqueous dispersions of graphene nanosheets. , 2008, Nature nanotechnology.

[31]  Wei Gao,et al.  New insights into the structure and reduction of graphite oxide. , 2009, Nature chemistry.

[32]  K. A. Mkhoyan,et al.  Atomic and Electronic Structure of Graphene-Oxide , 2010 .

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

[34]  K. Novoselov,et al.  Detection of individual gas molecules adsorbed on graphene. , 2006, Nature materials.

[35]  Micah J. Green,et al.  Spontaneous high-concentration dispersions and liquid crystals of graphene. , 2010, Nature nanotechnology.

[36]  James M Tour,et al.  Diazonium functionalization of surfactant-wrapped chemically converted graphene sheets. , 2008, Journal of the American Chemical Society.

[37]  R. Ruoff,et al.  The chemistry of graphene oxide. , 2010, Chemical Society reviews.

[38]  J. Tour,et al.  Graphene nanoribbon devices produced by oxidative unzipping of carbon nanotubes. , 2010, ACS nano.

[39]  Y. Aoi,et al.  Preparation of amorphous CNx thin films by pulsed laser deposition using a radio frequency radical beam source , 1999 .

[40]  J. Maire,et al.  Membranes de carbone et de graphite et leurs proprietes , 1968 .

[41]  Klaus Kern,et al.  Electronic transport properties of individual chemically reduced graphene oxide sheets. , 2007, Nano letters.

[42]  Xingfa Gao,et al.  Hydrazine and Thermal Reduction of Graphene Oxide: Reaction Mechanisms, Product Structures, and Reaction Design , 2010 .

[43]  J. Tour,et al.  Electronic transport in monolayer graphene nanoribbons produced by chemical unzipping of carbon nanotubes , 2009 .

[44]  Jacek Klinowski,et al.  Structure of Graphite Oxide Revisited , 1998 .

[45]  Benjamin Collins Brodie,et al.  On the Atomic Weight of Graphite , 1859 .

[46]  Inhwa Jung,et al.  Tunable electrical conductivity of individual graphene oxide sheets reduced at "low" temperatures. , 2008, Nano letters.