Annealing of C in hydrogen at temperatures above the stability limit of C-H bonds in CH (500-550 °C) is found to result in direct collapse of the cage structure, evaporation of light hydrocarbons, and formation of solid mixture composed of larger hydrocarbons and few-layered graphene sheets. Only a minor part of this mixture is soluble; this was analyzed using matrix-assisted laser desorption/ionization MS, Fourier transform infrared (FTIR), and nuclear magnetic resonance spectroscopy and found to be a rather complex mixture of hydrocarbon molecules composed of at least tens of different compounds. The sequence of most abundant peaks observed in MS, which corresponds to CH mass difference, suggests a stepwise breakup of the fullerene cage into progressively smaller molecular fragments edge-terminated by hydrogen. A simple model of hydrogen-driven C unzipping is proposed to explain the observed sequence of fragmentation products. The insoluble part of the product mixture consists of large planar polycyclic aromatic hydrocarbons, as evidenced by FTIR and Raman spectroscopy, and some larger sheets composed of few-layered graphene, as observed by transmission electron microscopy. Hydrogen annealing of C thin films showed a thickness-dependent results with reaction products significantly different for the thinnest films compared to bulk powders. Hydrogen annealing of C films with the thickness below 10 nm was found to result in formation of nanosized islands with Raman spectra very similar to the spectra of coronene oligomers and conductivity typical for graphene.
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http://dx.doi.org/10.1021/jp500377s | DOI Listing |
ACS Nano
October 2024
School of Physics, CRANN & AMBER Research Centres, Trinity College Dublin, Dublin 2, Ireland.
Ultrasonics
January 2025
Department of Chemistry, University of Calicut, Calicut University (PO), Malappuram DT, Kerala - 673635, India. Electronic address:
ACS Appl Mater Interfaces
October 2024
Robert Fredrick Smith School of Chemical and Biomolecular Engineering, Cornell University, Ithaca, New York 14853, United States.
While chemically doped graphene has shown great promise, the lack of cost-effective manufacturing has hindered its use. This study utilizes a facile fabrication approach for modality-tunable N-doped graphene via thermal annealing of aqueous-phase-exfoliated few-layered graphene from a Taylor-Couette reactor. This method demonstrates a high level of N-doping (27 atom % N) and offers modality tunability of the C-N bond without foregoing scalability and green chemistry principles.
View Article and Find Full Text PDFNat Commun
September 2024
International Center for Quantum Materials, School of Physics, Peking University, Beijing, 100871, China.
The magnetism of Kitaev materials has been widely studied, but their charge properties and the coupling to other degrees of freedom are less known. Here we investigate the charge states of α-RuCl, a promising Kitaev quantum spin liquid candidate, in proximity to graphite. We discover that few-layered α-RuCl experiences a clear modulation of charge states, where a Mott-insulator to weak charge-transfer-insulator transition in the 2D limit occurs by means of heterointerfacial polarization.
View Article and Find Full Text PDFSmall
November 2024
Zernike Institute for Advanced Materials, University of Groningen, Nijenborgh 4, Groningen, 9747 AG, the Netherlands.
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