High-quality few layer graphene produced by electrochemical intercalation and microwave-assisted expansion of graphite

Few-layer graphene is synthesized from electrochemically-produced graphite intercalation compounds in aqueous perchloric acid. Although anodic intercalation is more efficient in terms of time, cathodic pre-treatment is preferred to avoid the formation of graphite oxide. The materials are characterized by high resolution transmission electron microscopy and scanning electron microscopy, UV–visible, infrared and Raman spectroscopy. We demonstrate that the method, under the experimental conditions used in this work, does not produce damage to the sp2 carbon lattice. The synthetic approach using electrochemical-potential control is very promising to obtain, in a controllable manner, graphene with different degrees of oxidation.

[1]  M. C. Miras,et al.  Characterization of monolithic porous carbon prepared from resorcinol/formaldehyde gels with cationic surfactant , 2010 .

[2]  R. Ruoff,et al.  Graphene-based ultracapacitors. , 2008, Nano letters.

[3]  J. Tour,et al.  High-yield organic dispersions of unfunctionalized graphene. , 2009, Nano letters.

[4]  G. Fudenberg,et al.  Ultrahigh electron mobility in suspended graphene , 2008, 0802.2389.

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

[6]  P. Novák,et al.  In situ atomic force microscopy study of exfoliation phenomena on graphite basal planes , 2008 .

[7]  M. Noel,et al.  Electrochemistry of graphite intercalation compounds , 1998 .

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

[9]  D.D.L. Chung,et al.  Exfoliation of graphite , 1987 .

[10]  E. Wang,et al.  STM investigation of HOPG superperiodic features caused by electrochemical pretreatment , 1995 .

[11]  A. Green,et al.  Solution phase production of graphene with controlled thickness via density differentiation. , 2009, Nano letters.

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

[13]  R. Kötz,et al.  Electrochemical intercalation of perchlorate ions in HOPG: an SFM/LFM and XPS study , 2001 .

[14]  R. Murray,et al.  Imaging the incipient electrochemical oxidation of highly oriented pyrolytic graphite , 1993 .

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

[16]  C. Barbero,et al.  Spectroscopic ellipsometry of carbon electrodes during electrochemical activation , 1993 .

[17]  H. Möhwald,et al.  Preparation and characterization of graphite compounds by electrochemical techniques , 1981 .

[18]  Yuyan Shao,et al.  Facile and controllable electrochemical reduction of graphene oxide and its applications , 2010 .

[19]  R. Kötz,et al.  Anion intercalation into highly oriented pyrolytic graphite studied by electrochemical atomic force microscopy , 1999 .

[20]  J. Coleman,et al.  High-concentration solvent exfoliation of graphene. , 2010, Small.

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

[22]  R. Kaner,et al.  Intercalation and exfoliation routes to graphite nanoplatelets , 2005 .

[23]  Mark C Hersam,et al.  Emerging Methods for Producing Monodisperse Graphene Dispersions. , 2010, The journal of physical chemistry letters.

[24]  U Zeitler,et al.  Room-Temperature Quantum Hall Effect in Graphene , 2007, Science.

[25]  A. Geim,et al.  Two-dimensional gas of massless Dirac fermions in graphene , 2005, Nature.

[26]  R. Kaner,et al.  Honeycomb carbon: a review of graphene. , 2010, Chemical reviews.

[27]  F. Béguin,et al.  Towards the mechanism of electrochemical hydrogen storage in nanostructured carbon materials , 2004 .

[28]  D. Aurbach,et al.  Chronoamperometric measurements and modeling of nucleation and growth, and moving boundary stages during electrochemical lithiation of graphite electrode , 2007 .

[29]  R. Holze,et al.  Carbon anode materials for lithium ion batteries , 2003 .

[30]  K. Loh,et al.  One-pot synthesis of fluorescent carbon nanoribbons, nanoparticles, and graphene by the exfoliation of graphite in ionic liquids. , 2009, ACS nano.

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

[32]  X. Xia,et al.  A green approach to the synthesis of graphene nanosheets. , 2009, ACS nano.

[33]  P. Novák,et al.  The influence of electrolyte and graphite type on the PF 6 - intercalation behaviour at high potentials , 2009 .

[34]  A. Geim,et al.  Unconventional quantum Hall effect and Berry’s phase of 2π in bilayer graphene , 2006, cond-mat/0602565.

[35]  A. Bard,et al.  In situ scanning tunneling microscopy of the anodic oxidation of highly oriented pyrolytic graphite surfaces , 1988 .

[36]  M. Dresselhaus,et al.  Perspectives on carbon nanotubes and graphene Raman spectroscopy. , 2010, Nano letters.

[37]  J. Coleman,et al.  High-yield production of graphene by liquid-phase exfoliation of graphite. , 2008, Nature nanotechnology.

[38]  R. McCreery,et al.  In situ Raman monitoring of electrochemical graphite intercalation and lattice damage in mild aqueous acids , 1992 .

[39]  Zhenhua Ni,et al.  Probing layer number and stacking order of few-layer graphene by Raman spectroscopy. , 2010, Small.

[40]  A. Ferrari,et al.  Raman spectroscopy of graphene and graphite: Disorder, electron phonon coupling, doping and nonadiabatic effects , 2007 .

[41]  Chao Zhang,et al.  One‐Step Ionic‐Liquid‐Assisted Electrochemical Synthesis of Ionic‐Liquid‐Functionalized Graphene Sheets Directly from Graphite , 2008 .

[42]  Allen J. Bard,et al.  Electrochemical Methods: Fundamentals and Applications , 1980 .

[43]  P. Kim,et al.  Experimental observation of the quantum Hall effect and Berry's phase in graphene , 2005, Nature.

[44]  F. Beck,et al.  Graphite intercalation compounds as positive electrodes in galvanic cells , 1981 .

[45]  S. Iijima,et al.  Direct evidence for atomic defects in graphene layers , 2004, Nature.