Abstract

Nanometer-thick and crystalline sp3-bonded carbon sheets are promising new wide band-gap semiconducting materials for electronics, photonics, and medical devices. Diamane was prepared from the exposure of bi-layer graphene to hydrogen radicals produced by the hot-filament process at low pressure and temperature. A sharp sp3-bonded carbon stretching mode was observed in ultraviolet Raman spectra at around 1344–1367 cm−1 while no sp2-bonded carbon peak was simultaneously detected. By replacing bi-layer graphene with few-layer graphene, diamanoid/graphene hybrids were formed from the partial conversion of few-layer graphene, due to the prevalent Bernal stacking sequence. Raman spectroscopy, electron diffraction, and Density Functional Theory calculations show that partial conversion generates twisted bi-layer graphene located at the interface between the upper diamanoid domain and the non-converted graphenic domain underneath. Carbon-hydrogen bonding in the basal plane of hydrogenated few-layer graphene, where carbon is bonded to a single hydrogen over an area of 150 μm2, was directly evidenced by Fourier transform infrared microscopy and the actual full hydrogenation of diamane was supported by first-principle calculations. Those results open the door to large-scale production of diamane, diamanoids, and diamanoid/graphene hybrids.

Highlights

  • Centre d’Elaboration des Matériaux et d’Etudes Structurales (CEMES), CNRS, Université de Toulouse, Laboratoire de Physico-Chimie des Nano-Objets (LPCNO), CNRS, INSA, Université de Toulouse, Department of Chemistry, University of Manitoba, Winnipeg, MB R3T 2N2, Canada; Abstract: Nanometer-thick and crystalline sp3 -bonded carbon sheets are promising new wide bandgap semiconducting materials for electronics, photonics, and medical devices

  • Hot-filament chemical vapor deposition (CVD) has been employed for the industrial production of diamond films for about 40 years because it efficiently produces atomic hydrogen (H), which has been shown to play a critical role for the conventional synthesis of metastable diamond at low pressure from a dilute mixture of a hydrocarbon in H2 [38,39,40,41]

  • We have shown that the hot-filament-promoted hydrogenation process can be successfully used to produce genuine diamane from bi-layer graphene at low pressure and at low temperature

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Summary

Introduction

Electron diffraction, and Density Functional Theory calculations show that partial conversion generates twisted bi-layer graphene located at the interface between the upper diamanoid domain and the non-converted graphenic domain underneath. Carbon-hydrogen bonding in the basal plane of hydrogenated few-layer graphene, where carbon is bonded to a single hydrogen over an area of 150 μm , was directly evidenced by Fourier transform infrared microscopy and the actual full hydrogenation of diamane was supported by first-principle calculations. Those results open the door to large-scale production of diamane, diamanoids, and diamanoid/graphene hybrids. Because of the expected low friction coefficient of the hydrogenated surface, diamane may be used to improve published maps and institutional affiliations

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