Evaluation Criteria for Reduced Graphene Oxide

Reduced graphene oxide (RGO) is an intriguing nanomaterial with tremendous potential for many applications. Although considerable efforts have been devoted to develop the reduction methods, it still needs further improvement, and how to choose an appropriate one for a specific application is a troublesome problem. In this study, RGOs were prepared by six typical reduction methods: N2H4·H2O, NaOH, NaBH4, solvothermal, high-temperature, and two-step. The samples were systematic compared by four aspects: dispersibility, reduction degree, defect repair degree, and electrical conductivity. On the basis of the comparison, a simple evaluation criterion was proposed for qualitatively judging the quality of RGO. This evaluation criterion would be helpful to understand the mechanism of reduction and design more ideal reduction methods.

[1]  James M Tour,et al.  Reduction of graphene oxide via bacterial respiration. , 2010, ACS nano.

[2]  Hong-Bo Sun,et al.  Direct imprinting of microcircuits on graphene oxides film by femtosecond laser reduction , 2010 .

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

[4]  Peng Chen,et al.  Centimeter-long and large-scale micropatterns of reduced graphene oxide films: fabrication and sensing applications. , 2010, ACS nano.

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

[6]  Ming Zhou,et al.  Controlled synthesis of large-area and patterned electrochemically reduced graphene oxide films. , 2009, Chemistry.

[7]  TaeYoung Kim,et al.  Synthesis of phase transferable graphene sheets using ionic liquid polymers. , 2010, ACS nano.

[8]  S. Stankovich,et al.  Chemical analysis of graphene oxide films after heat and chemical treatments by X-ray photoelectron and Micro-Raman spectroscopy , 2009 .

[9]  Zhongyuan Huang,et al.  Electrochemical co-reduction synthesis of graphene/Au nanocomposites in ionic liquid and their electrochemical activity , 2010 .

[10]  J. Tascón,et al.  Graphene oxide dispersions in organic solvents. , 2008, Langmuir : the ACS journal of surfaces and colloids.

[11]  T. Belytschko,et al.  Computational Studies of the Structure, Behavior upon Heating, and Mechanical Properties of Graphite Oxide , 2007 .

[12]  Can Xue,et al.  In Situ Synthesis of Metal Nanoparticles on Single-Layer Graphene Oxide and Reduced Graphene Oxide Surfaces , 2009 .

[13]  Qian Liu,et al.  Organic Photovoltaic Devices Based on a Novel Acceptor Material: Graphene , 2008 .

[14]  Yizhong Huang,et al.  Highly efficient restoration of graphitic structure in graphene oxide using alcohol vapors. , 2010, ACS nano.

[15]  Nobutoshi Ito,et al.  Development of a novel selective inhibitor of the Down syndrome-related kinase Dyrk1A. , 2010, Nature communications.

[16]  R. Ruoff,et al.  All-organic vapor sensor using inkjet-printed reduced graphene oxide. , 2010, Angewandte Chemie.

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

[18]  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 .

[19]  A. Govindaraj,et al.  Graphene: the new two-dimensional nanomaterial. , 2009, Angewandte Chemie.

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

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

[22]  S. Stankovich,et al.  Graphene-silica composite thin films as transparent conductors. , 2007, Nano letters.

[23]  L. Brinson,et al.  Functionalized graphene sheets for polymer nanocomposites. , 2008, Nature nanotechnology.

[24]  J. Robinson,et al.  Reduction of graphene oxide by electron beam generated plasmas produced in methane/argon mixtures , 2010 .

[25]  M. Rajamathi,et al.  CHEMICALLY MODIFIED GRAPHENE SHEETS PRODUCED BY THE SOLVOTHERMAL REDUCTION OF COLLOIDAL DISPERSIONS OF GRAPHITE OXIDE , 2008 .

[26]  R. Sundaram,et al.  Graphene Monolayers: Chemical Vapor Deposition Repair of Graphene Oxide: A Route to Highly‐Conductive Graphene Monolayers (Adv. Mater. 46/2009) , 2009 .

[27]  Peng Chen,et al.  Interfacing live cells with nanocarbon substrates. , 2010, Langmuir : the ACS journal of surfaces and colloids.

[28]  Hua Zhang,et al.  Conjugated-polyelectrolyte-functionalized reduced graphene oxide with excellent solubility and stability in polar solvents. , 2010, Small.

[29]  T. Ohta,et al.  Controlling the Electronic Structure of Bilayer Graphene , 2006, Science.

[30]  Liheng Wu,et al.  Direct fabrication of photoconductive patterns on LBL assembled graphene oxide/PDDA/titania hybrid films by photothermal and photocatalytic reduction , 2010 .

[31]  Jing Sun,et al.  pH-Sensitive Highly Dispersed Reduced Graphene Oxide Solution Using Lysozyme via an in Situ Reduction Method , 2010 .

[32]  R. Car,et al.  Single Sheet Functionalized Graphene by Oxidation and Thermal Expansion of Graphite , 2007 .

[33]  K. Loh,et al.  Multilayer Hybrid Films Consisting of Alternating Graphene and Titania Nanosheets with Ultrafast Electron Transfer and Photoconversion Properties , 2009 .

[34]  Yuyan Shao,et al.  Polyelectrolyte-induced reduction of exfoliated graphite oxide: a facile route to synthesis of soluble graphene nanosheets. , 2011, ACS nano.

[35]  Lifeng Yan,et al.  Preparation of graphene by a low-temperature thermal reduction at atmosphere pressure. , 2010, Nanoscale.

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

[37]  Qiyuan He,et al.  Electrochemical Deposition of Semiconductor Oxides on Reduced Graphene Oxide-Based Flexible, Transparent, and Conductive Electrodes , 2010 .

[38]  Kian Ping Loh,et al.  Microstructuring of Graphene Oxide Nanosheets Using Direct Laser Writing , 2010, Advanced materials.

[39]  Julio Gómez-Herrero,et al.  Chemical Vapor Deposition Repair of Graphene Oxide: A Route to Highly‐Conductive Graphene Monolayers , 2009 .

[40]  S. Stankovich,et al.  Graphene-based composite materials , 2006, Nature.

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

[42]  Fei Zhao,et al.  Bulk heterojunction polymer memory devices with reduced graphene oxide as electrodes. , 2010, ACS nano.

[43]  Efthimios Kaxiras,et al.  Graphene nanoFlakes with large spin. , 2008, Nano letters.

[44]  Chun-yan Liu,et al.  Electrochemical detection of hydroquinone by graphene and Pt-graphene hybrid material synthesized through a microwave-assisted chemical reduction process , 2011 .

[45]  Zhiqiang Wang,et al.  Environment-Friendly Method To Produce Graphene That Employs Vitamin C and Amino Acid , 2010 .

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

[47]  Thomas M. Orlando,et al.  Formation of Graphene Features from Direct Laser-Induced Reduction of Graphite Oxide , 2010 .

[48]  Shixin Wu,et al.  Reduced graphene oxide-templated photochemical synthesis and in situ assembly of Au nanodots to orderly patterned Au nanodot chains. , 2010, Small.

[49]  S. Sampath,et al.  Electrochemical Reduction of Oriented Graphene Oxide Films: An in Situ Raman Spectroelectrochemical Study , 2009 .

[50]  Jin Suk Chung,et al.  Fast and simple fabrication of a large transparent chemically-converted graphene film by spray-coating , 2010 .

[51]  Shixin Wu,et al.  Amphiphilic graphene composites. , 2010, Angewandte Chemie.

[52]  T. Feng,et al.  The field emission of vacuum filtered graphene films reduced by microwave , 2011 .

[53]  Mianqi Xue,et al.  Processing of graphene for electrochemical application: noncovalently functionalize graphene sheets with water-soluble electroactive methylene green. , 2009, Langmuir : the ACS journal of surfaces and colloids.

[54]  J. Crain,et al.  Scattering and Interference in Epitaxial Graphene , 2007, Science.

[55]  R. Stoltenberg,et al.  Evaluation of solution-processed reduced graphene oxide films as transparent conductors. , 2008, ACS nano.

[56]  Jianfei Che,et al.  A new approach to fabricate graphene nanosheets in organic medium: combination of reduction and dispersion , 2010 .

[57]  Huaping Zhao,et al.  Electric Current Induced Reduction of Graphene Oxide and Its Application as Gap Electrodes in Organic Photoswitching Devices , 2010, Advanced materials.

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

[59]  O. Akhavan The effect of heat treatment on formation of graphene thin films from graphene oxide nanosheets , 2010 .

[60]  Yang Yang,et al.  A one-step, solvothermal reduction method for producing reduced graphene oxide dispersions in organic solvents. , 2010, ACS nano.

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

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

[63]  Xiao-li Cheng,et al.  A novel strategy for making soluble reduced graphene oxide sheets cheaply by adopting an endogenous reducing agent , 2011 .

[64]  H. Dai,et al.  Solvothermal reduction of chemically exfoliated graphene sheets. , 2009, Journal of the American Chemical Society.

[65]  F. Wei,et al.  Facile synthesis of graphene nanosheets via Fe reduction of exfoliated graphite oxide. , 2011, ACS nano.

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

[67]  A. Krasheninnikov,et al.  Structural defects in graphene. , 2011, ACS nano.

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

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

[70]  Shaojun Dong,et al.  Reducing sugar: new functional molecules for the green synthesis of graphene nanosheets. , 2010, ACS nano.

[71]  Sang Yup Lee,et al.  Solution chemistry of self-assembled graphene nanohybrids for high-performance flexible biosensors. , 2010, ACS nano.

[72]  Vivek B Shenoy,et al.  Structural evolution during the reduction of chemically derived graphene oxide. , 2010, Nature chemistry.

[73]  Yang Yang,et al.  High-throughput solution processing of large-scale graphene. , 2009, Nature nanotechnology.

[74]  Die Reduktion von Graphitoxyd mit Schwefelwasserstoff , 1934 .

[75]  Lifeng Yan,et al.  Preparation of graphene by the rapid and mild thermal reduction of graphene oxide induced by microwaves , 2010 .

[76]  Omid Akhavan,et al.  Photocatalytic Reduction of Graphene Oxide Nanosheets on TiO2 Thin Film for Photoinactivation of Bacteria in Solar Light Irradiation , 2009 .

[77]  M I Katsnelson,et al.  Modeling of graphite oxide. , 2008, Journal of the American Chemical Society.

[78]  Hee‐Tae Jung,et al.  A Simple Approach for Preparing Transparent Conductive Graphene Films Using the Controlled Chemical Reduction of Exfoliated Graphene Oxide in an Aqueous Suspension , 2010 .

[79]  A. Govindaraj,et al.  Uptake of H2 and CO2 by Graphene , 2008 .

[80]  Quan-hong Yang,et al.  Self‐Assembled Free‐Standing Graphite Oxide Membrane , 2009 .

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

[82]  Seth R. Marder,et al.  Nanoscale Tunable Reduction of Graphene Oxide for Graphene Electronics , 2010, Science.

[83]  C. Macosko,et al.  Aqueous only route toward graphene from graphite oxide. , 2011, ACS nano.

[84]  M. Ashokkumar,et al.  Sonolytic Design of Graphene−Au Nanocomposites. Simultaneous and Sequential Reduction of Graphene Oxide and Au(III) , 2010 .

[85]  Hua Zhang,et al.  Organic photovoltaic devices using highly flexible reduced graphene oxide films as transparent electrodes. , 2010, ACS nano.

[86]  Freddy Yin Chiang Boey,et al.  Direct Electrochemical Reduction of Single-Layer Graphene Oxide and Subsequent Functionalization with Glucose Oxidase , 2009 .

[87]  Yongsheng Chen,et al.  High-Efficiency Loading and Controlled Release of Doxorubicin Hydrochloride on Graphene Oxide , 2008 .

[88]  X. Jia,et al.  Bulk production of a new form of sp(2) carbon: crystalline graphene nanoribbons. , 2008, Nano letters.

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

[90]  S. Jiang,et al.  Microwave-assisted one-pot synthesis of metal/metal oxide nanoparticles on graphene and their electrochemical applications , 2011 .

[91]  R. Car,et al.  Raman spectra of graphite oxide and functionalized graphene sheets. , 2008, Nano letters.

[92]  Xiong Zhang,et al.  High performance supercapacitors based on reduced graphene oxide in aqueous and ionic liquid electrolytes , 2011 .

[93]  C. Berger,et al.  Ultrathin epitaxial graphite: 2D electron gas properties and a route toward graphene-based nanoelectronics. , 2004, cond-mat/0410240.

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

[95]  Yang Liu,et al.  Pulsed laser assisted reduction of graphene oxide , 2011 .

[96]  Sandip Niyogi,et al.  Solution properties of graphite and graphene. , 2006, Journal of the American Chemical Society.

[97]  M. S. El-shall,et al.  Microwave synthesis of graphene sheets supporting metal nanocrystals in aqueous and organic media , 2009 .

[98]  P. Kamat,et al.  TiO2-graphene nanocomposites. UV-assisted photocatalytic reduction of graphene oxide. , 2008, ACS nano.

[99]  Hui-Ming Cheng,et al.  Synthesis of high-quality graphene with a pre-determined number of layers , 2009 .

[100]  R. Ruoff,et al.  Chemical methods for the production of graphenes. , 2009, Nature nanotechnology.

[101]  Shixin Wu,et al.  Electrochemical deposition of ZnO nanorods on transparent reduced graphene oxide electrodes for hybrid solar cells. , 2010, Small.

[102]  Jiali Zhang,et al.  Reduction of graphene oxide via L-ascorbic acid. , 2010, Chemical communications.

[103]  M. S. El-shall,et al.  Photothermal Deoxygenation of Graphite Oxide with Laser Excitation in Solution and Graphene-Aided Increase in Water Temperature , 2010 .

[104]  R. Ruoff,et al.  Reduced graphene oxide by chemical graphitization. , 2010, Nature communications.

[105]  Rodolfo Cruz-Silva,et al.  Flash reduction and patterning of graphite oxide and its polymer composite. , 2009, Journal of the American Chemical Society.

[106]  Bei Wang,et al.  Synthesis of enhanced hydrophilic and hydrophobic graphene oxide nanosheets by a solvothermal method , 2009 .

[107]  S. Hur,et al.  Chemical functionalization of graphene sheets by solvothermal reduction of a graphene oxide suspension in N-methyl-2-pyrrolidone , 2011 .

[108]  Lifeng Yan,et al.  Chemical Reduction of Graphene Oxide to Graphene by Sulfur-Containing Compounds , 2010 .

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

[110]  J. Tascón,et al.  Vitamin C Is an Ideal Substitute for Hydrazine in the Reduction of Graphene Oxide Suspensions , 2010 .

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

[112]  Jie Yin,et al.  Facile synthesis of soluble graphene via a green reduction of graphene oxide in tea solution and its biocomposites. , 2011, ACS applied materials & interfaces.

[113]  Jinbin Liu,et al.  Toward a universal "adhesive nanosheet" for the assembly of multiple nanoparticles based on a protein-induced reduction/decoration of graphene oxide. , 2010, Journal of the American Chemical Society.

[114]  Jun Yan,et al.  An environmentally friendly and efficient route for the reduction of graphene oxide by aluminum powder , 2010 .

[115]  Qiang Fu,et al.  A simple and efficient method to prepare graphene by reduction of graphite oxide with sodium hydrosulfite , 2011, Nanotechnology.

[116]  Hui-Ming Cheng,et al.  Direct reduction of graphene oxide films into highly conductive and flexible graphene films by hydrohalic acids , 2010 .

[117]  S. Saxena,et al.  Investigation of the Local Structure of Graphene Oxide , 2010 .

[118]  Z. Yin,et al.  All‐Carbon Electronic Devices Fabricated by Directly Grown Single‐Walled Carbon Nanotubes on Reduced Graphene Oxide Electrodes , 2010, Advanced materials.

[119]  Sung Min Kang,et al.  Simultaneous Reduction and Surface Functionalization of Graphene Oxide by Mussel‐Inspired Chemistry , 2011 .

[120]  M. Chhowalla,et al.  UV-reduction of graphene oxide and its application as an interfacial layer to reduce the back-transport reactions in dye-sensitized solar cells , 2009 .

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

[122]  S. Luo,et al.  Direct electrodeposition of reduced graphene oxide on glassy carbon electrode and its electrochemical application , 2011 .

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

[124]  Lei Wang,et al.  Stable Aqueous Dispersion of Graphene Nanosheets: Noncovalent Functionalization by a Polymeric Reducing Agent and Their Subsequent Decoration with Ag Nanoparticles for Enzymeless Hydrogen Peroxide Detection , 2010 .

[125]  Z. Yin,et al.  Multilayer stacked low-temperature-reduced graphene oxide films: preparation, characterization, and application in polymer memory devices. , 2010, Small.

[126]  Jili Wu,et al.  Stable aqueous dispersions of graphene prepared with hexamethylenetetramine as a reductant. , 2011, Journal of colloid and interface science.

[127]  Qiyuan He,et al.  Reduced graphene oxide films used as matrix of MALDI-TOF-MS for detection of octachlorodibenzo-p-dioxin. , 2010, Chemical Communications.

[128]  Philip Kim,et al.  Electric field modulation of galvanomagnetic properties of mesoscopic graphite. , 2004, Physical Review Letters.

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

[130]  Inhwa Jung,et al.  Colloidal suspensions of highly reduced graphene oxide in a wide variety of organic solvents. , 2009, Nano letters.

[131]  Kian Ping Loh,et al.  Hydrothermal Dehydration for the “Green” Reduction of Exfoliated Graphene Oxide to Graphene and Demonstration of Tunable Optical Limiting Properties , 2009 .

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

[133]  H. Dai,et al.  Chemically Derived, Ultrasmooth Graphene Nanoribbon Semiconductors , 2008, Science.

[134]  Bei Wang,et al.  FACILE SYNTHESIS AND CHARACTERIZATION OF GRAPHENE NANOSHEETS , 2008 .

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

[136]  Ji Won Suk,et al.  Graphene-based actuators. , 2010, Small.

[137]  Sarnjeet S. Dhesi,et al.  Catalyst‐Free Efficient Growth, Orientation and Biosensing Properties of Multilayer Graphene Nanoflake Films with Sharp Edge Planes , 2008 .

[138]  Prashant V. Kamat,et al.  Decorating Graphene Sheets with Gold Nanoparticles , 2008 .

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

[140]  W. Poirier,et al.  Can graphene set new standards? , 2010, Nature nanotechnology.

[141]  A. Reina,et al.  Large area, few-layer graphene films on arbitrary substrates by chemical vapor deposition. , 2009, Nano letters.

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

[143]  F. Stavale,et al.  Measuring disorder in graphene with the G and D bands , 2010 .

[144]  Yan Wang,et al.  Infrared-Triggered Actuators from Graphene-Based Nanocomposites , 2009 .

[145]  Guoliang Zhang,et al.  Deoxygenation of Exfoliated Graphite Oxide under Alkaline Conditions: A Green Route to Graphene Preparation , 2008 .

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

[147]  K. Tu,et al.  Solution-processable graphene oxide as an efficient hole transport layer in polymer solar cells. , 2010, ACS nano.

[148]  Michio Koinuma,et al.  Simple photoreduction of graphene oxide nanosheet under mild conditions. , 2010, ACS applied materials & interfaces.

[149]  S. Chou,et al.  Graphene transistors fabricated via transfer-printing in device active-areas on large wafer , 2007 .

[150]  R. Kaner,et al.  Graphene-like nano-sheets for surface acoustic wave gas sensor applications , 2009 .

[151]  Sheng-Zhen Zu,et al.  Aqueous Dispersion of Graphene Sheets Stabilized by Pluronic Copolymers: Formation of Supramolecular Hydrogel , 2009 .

[152]  S. Stankovich,et al.  Preparation and characterization of graphene oxide paper , 2007, Nature.

[153]  K. Novoselov,et al.  Graphene-based liquid crystal device. , 2008, Nano letters (Print).

[154]  Hui‐Ming Cheng,et al.  Efficient preparation of large-area graphene oxide sheets for transparent conductive films. , 2010, ACS nano.

[155]  Zhongqing Wei,et al.  Reduced graphene oxide molecular sensors. , 2008, Nano letters.