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A 3D insight on the catalytic nanostructuration of few-layer graphene.

ABSTRACT: The catalytic cutting of few-layer graphene is nowadays a hot topic in materials research due to its potential applications in the catalysis field and the graphene nanoribbons fabrication. We show here a 3D analysis of the nanostructuration of few-layer graphene by iron-based nanoparticles under hydrogen flow. The nanoparticles located at the edges or attached to the steps on the FLG sheets create trenches and tunnels with orientations, lengths and morphologies defined by the crystallography and the topography of the carbon substrate. The cross-sectional analysis of the 3D volumes highlights the role of the active nanoparticle identity on the trench size and shape, with emphasis on the topographical stability of the basal planes within the resulting trenches and channels, no matter the obstacle encountered. The actual study gives a deep insight on the impact of nanoparticles morphology and support topography on the 3D character of nanostructures built up by catalytic cutting.

SUBMITTER: Melinte G

PROVIDER: S-EPMC4082640 | biostudies-literature | 2014 Jun

REPOSITORIES: biostudies-literature

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A 3D insight on the catalytic nanostructuration of few-layer graphene.

Melinte G G Florea I I Moldovan S S Janowska I I Baaziz W W Arenal R R Wisnet A A Scheu C C Begin-Colin S S Begin D D Pham-Huu C C Ersen O O

Nature communications 20140611

The catalytic cutting of few-layer graphene is nowadays a hot topic in materials research due to its potential applications in the catalysis field and the graphene nanoribbons fabrication. We show here a 3D analysis of the nanostructuration of few-layer graphene by iron-based nanoparticles under hydrogen flow. The nanoparticles located at the edges or attached to the steps on the FLG sheets create trenches and tunnels with orientations, lengths and morphologies defined by the crystallography and ...[more]

PMID: 24916201

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Project description:The mechanism for the functionalization of graphene layers with pyrrole compounds was investigated. Liquid 1,2,5-trimethylpyrrole (TMP) was heated in air in the presence of a high surface area nanosized graphite (HSAG), at temperatures between 80 °C and 180 °C. After the thermal treatments solid and liquid samples, separated by centrifugation, were analysed by means of Raman, Fourier Transform Infrared (FT-IR) spectroscopy, X-Rays Photoelectron Spectroscopy (XPS) and ¹H-Nuclear Magnetic Resonance (¹H NMR) spectroscopy and High Resolution Transmission Electron Microscopy (HRTEM). FT-IR spectra were interpreted with the support of Density Functional Theory (DFT) quantum chemical modelling. Raman findings suggested that the bulk structure of HSAG remained substantially unaltered, without intercalation products. FT-IR and XPS spectra showed the presence of oxidized TMP derivatives on the solid adducts, in a much larger amount than in the liquid. For thermal treatments at T ≥ 150 °C, IR spectral features revealed not only the presence of oxidized products but also the reaction of intra-annular double bond of TMP with HSAG. XPS spectroscopy showed the increase of the ratio between C(sp²)N bonds involved in the aromatic system and C(sp³)N bonds, resulting from reaction of the pyrrole moiety, observed while increasing the temperature from 130 °C to 180 °C. All these findings, supported by modeling, led to hypothesize a cascade reaction involving a carbocatalyzed oxidation of the pyrrole compound followed by Diels-Alder cycloaddition. Graphene layers play a twofold role: at the early stages of the reaction, they behave as a catalyst for the oxidation of TMP and then they become the substrate for the cycloaddition reaction. Such sustainable functionalization, which does not produce by-products, allows us to use the pyrrole compounds for decorating sp² carbon allotropes without altering their bulk structure and smooths the path for their wider application.

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A 3D insight on the catalytic nanostructuration of few-layer graphene.

Publications

A 3D insight on the catalytic nanostructuration of few-layer graphene.

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