A Computational Investigation of the Catalytic Properties of Graphene Oxide: Exploring Mechanisms by using DFT Methods

Boukhvalov, Danil W.; Dreyer, Daniel R.; Bielawski, Christopher W.; Son, Young Kap

doi:10.1002/cctc.201200210

Cited by 133 publications

(133 citation statements)

References 47 publications

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“…63-65 Shortly after, a new O-H bond forms, and the C-O bond in hydroxyl and the C-H bond in thiophene are cleaved, yielding water molecule, sp2-hybridized C=C restored RGO (E) 1 without any epoxides and ketones (C=O), and new thiophene radical. This process is analogous to theoretically and experimentally observed recombinative desorption of the hydrogen atom on graphene andgraphite surfaces, which results in the disappearance of radical 66. Next, the radical dimer formed via step 2 bounds to epoxide on the GO (E) 2 due to the electrostatic attraction between positively charged H in radical dimer and negatively charged O…”

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confidence: 51%

Fabrication of Various Conducting Polymers Using Graphene Oxide as a Chemical Oxidant

et al. 2015

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Recently, using graphene oxide (GO) for "carbocatalysis" has great attraction as a novel application of graphene-based nanomaterials and expected to opens a host of possibilities for chemical synthesis because of the abundance of natural carbon sources, as well as the low density, extensive chemical functionalization, hydrophilicity, low cost, and ease of preparation.Here, we demonstrate that the GO can play a role as a chemical oxidant for various CPs (polythiophene, polyaniline, and polypyrrole), and diverse graphene-CP composites (graphenepolythiophene, graphene-polyaniline, and graphene-polypyrrole) can simply and rapidly be synthesized by using the GO as both graphene precursor and chemical oxidant. The UV-vis analysis confirms that the GO has successfully polymerized the CPs and been transformed to reduced graphene oxide (RGO). The SEM and TEM analyses show that the CPs have successfully been coated on the few-layered graphene sheets. Raman analysis and series of FT-IR analyses have been conducted to survey what functional group in the GO polymerized the monomers, and they reveal that hydroxyl and epoxy groups in the GO polymerized the monomers. Finally, plausible polymerization mechanisms have specifically and deeply proposed based on the IR result, classical radical polymerization mechanisms of the CPs, and widely adopted thermal reduction mechanism of the GO.The conducting polymers (CPs), prepared by typical oxidative polymerization method, 1-3 has attracted great attention in vast fields of energy storage/conversion, 4-8 electronic, 9-11 and biological 12-16 applications due to their fascinating properties such as unique redox behavior, tunable electrical conductivity, inherent biocompatibility, and high flexibility. 4-16 Despite a large number of advantages, however, inferior properties of CPs (e.g., low electrochemical stability, weak mechanical strength, etc.) often hinder their practical usage. 12,17,18 The need to overcome this limitation has led to the growing interest in hybridization of CPs with other additives. 12,17,18 For example, many kinds of nanostructured carbon materials (e.g., carbon nanotube, mesoporous carbon, etc.) have been incorporated with CPs to produce composites with desirable properties (e.g., enhanced thermal stability, increased electrochemical stability, or improved mechanical strength). [17][18][19][20][21][22] In particular, of the various nanostructured carbon additives, graphene has recently drawn significant attention because of its exceptional electrical, thermal, electrochemical, and mechanical properties. 17,18,23 With the burgeoning interest in the graphene additives, indeed, combination of graphene and CP has extensively been studied and the produced graphene-CP composites have shown the superior properties compared with other carbon-CP composites through the remarkable properties of graphene and synergistic effects between CP and graphene. [24][25][26][27][28] Majorly, the graphene-CP composites have been fabricated by following two methods; (i) mixing of preform...

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confidence: 51%

Fabrication of Various Conducting Polymers Using Graphene Oxide as a Chemical Oxidant

et al. 2015

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“…3 At present, this compound was proposed to be a source of graphene by exfoliation 4 and reduction 5 and as a material for catalyst, 6,7 filters, 8,9 solar cells, 10 magnetic materials, 11 ink-jet printing of electronic devices 12 and various biological applications. 13 These great prospects of GO require improving its large-scale fabrication methods.…”

Section: Introductionmentioning

confidence: 99%

Oxidation of a Graphite Surface: The Role of Water

Boukhvalov

2014

J. Phys. Chem. C

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“…23 For 1LG, the energetic favorability of this process at a lower level of graphene oxidation corresponds with the transformation of all C-O-C groups to C-OH (Supplementary Figure S12). In particular, the formation energy of the C-OH groups for 2LG is higher than that for 1LG and 3LG.…”

Section: Electrical Control Of Nanoscale Functionalization I-s Byun Ementioning

confidence: 99%

Electrical control of nanoscale functionalization in graphene by the scanning probe technique

et al. 2014

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Functionalized graphene is a versatile material that has well-known physical and chemical properties depending on functional groups and their coverage. However, selective control of functional groups on the nanoscale is hardly achievable by conventional methods utilizing chemical modifications. We demonstrate electrical control of nanoscale functionalization of graphene with the desired chemical coverage of a selective functional group by atomic force microscopy (AFM) lithography and their full recovery through moderate thermal treatments. Surprisingly, our controlled coverage of functional groups can reach 94.9% for oxygen and 49.0% for hydrogen, respectively, well beyond those achieved by conventional methods. This coverage is almost at the theoretical maximum, which is verified through scanning photoelectron microscope measurements as well as first-principles calculations. We believe that the present method is now ready to realize 'chemical pencil drawing' of atomically defined circuit devices on top of a monolayer of graphene.

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A Computational Investigation of the Catalytic Properties of Graphene Oxide: Exploring Mechanisms by using DFT Methods

Cited by 133 publications

References 47 publications

Fabrication of Various Conducting Polymers Using Graphene Oxide as a Chemical Oxidant

Fabrication of Various Conducting Polymers Using Graphene Oxide as a Chemical Oxidant

Oxidation of a Graphite Surface: The Role of Water

Electrical control of nanoscale functionalization in graphene by the scanning probe technique

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