Abstract:A new hydrocarbonhydrographitewith the composition close to CH is shown to form from graphite and gaseous hydrogen at pressures above 2 GPa and temperatures from 450 to 700°C. Hydrographite is a black solid thermally stable under ambient conditions. If heated in vacuum, it decomposes into graphite and molecular hydrogen at temperatures from 500 to 650°C. Powder X-ray diffraction characterizes hydrographite as a multilayer "graphane II" phase predicted by ab initio calculations [Wen X-D et al. PNAS 2011;108:683… Show more
“…P.S. When this article was under preparation, it was reported in [40] that weakly ordered graphane-leke materials with stoichiometry close to 1:1 were obtained by the hydration of a disordered graphite nanopowder at a high pressure. The degree of ordering of the materials obtained in [40] is much lower than that in our samples.…”
The discovery of graphene stimulated an intensive search for its analogs and derivatives. One of the most interesting derivatives is hydrographene called graphane. Calculations indicate that bulk graphane is thermodynamically more favorable than all CH hydrocarbons including benzene. At the same time, pressureinduced polymerization of hydrocarbons and their derivatives at room temperature leads to the formation of amorphous products or poorly ordered one-dimensional products such as polyacetylene and benzene-derived carbon nanothreads.Here, we report a high-pressure high-temperature synthesis of several millimetersized samples of bulk graphanes with the composition C-H(D) from benzene and graphene-derivative C-H-N 0.2 from pyridine. X-ray diffraction, transmission electron microscopy, and infrared spectroscopy of new materials reveal relatively large (several nanometers in size) crystalline grains of an sp 3 -bonded graphane lattice (3-cycle-4step, the orthorhombic structure with P bca space-group and parameters a = 9.5-9.8Å, b = 8.9-9.1Å, c = 17.1-17.3Å). The main hydrogen groups in samples are C-H groups connected by aliphatic bonds. The synthesized graphanes at atmospheric pressure are stable up to 500 • C. The macroscopic density of CH samples is 1.5-1.57 g cm −3 and the refractive index is 1.78-1.80. The absorption spectra of samples with a high degree of crystallization exhibits a weak absorption maximum at 2.8 eV, which is responsible for the yellow-orange color, large absorption maximum at 4 eV and an absorption edge associated with the width of the optical gap at 5.2 eV. The bulk modulus (30-37 GPa) and shear modulus (15-18 GPa) of the fabricated samples, as well as their hardness (1-1.5 GPa), are about twice as high as the respective values for polycrystalline graphite. The solution of metalorganic complexes in benzene and pyridine makes it possible to obtain doped graphanes, which can have extraordinary electron transport and magnetic properties.arXiv:1608.07221v1 [cond-mat.mtrl-sci]
“…P.S. When this article was under preparation, it was reported in [40] that weakly ordered graphane-leke materials with stoichiometry close to 1:1 were obtained by the hydration of a disordered graphite nanopowder at a high pressure. The degree of ordering of the materials obtained in [40] is much lower than that in our samples.…”
The discovery of graphene stimulated an intensive search for its analogs and derivatives. One of the most interesting derivatives is hydrographene called graphane. Calculations indicate that bulk graphane is thermodynamically more favorable than all CH hydrocarbons including benzene. At the same time, pressureinduced polymerization of hydrocarbons and their derivatives at room temperature leads to the formation of amorphous products or poorly ordered one-dimensional products such as polyacetylene and benzene-derived carbon nanothreads.Here, we report a high-pressure high-temperature synthesis of several millimetersized samples of bulk graphanes with the composition C-H(D) from benzene and graphene-derivative C-H-N 0.2 from pyridine. X-ray diffraction, transmission electron microscopy, and infrared spectroscopy of new materials reveal relatively large (several nanometers in size) crystalline grains of an sp 3 -bonded graphane lattice (3-cycle-4step, the orthorhombic structure with P bca space-group and parameters a = 9.5-9.8Å, b = 8.9-9.1Å, c = 17.1-17.3Å). The main hydrogen groups in samples are C-H groups connected by aliphatic bonds. The synthesized graphanes at atmospheric pressure are stable up to 500 • C. The macroscopic density of CH samples is 1.5-1.57 g cm −3 and the refractive index is 1.78-1.80. The absorption spectra of samples with a high degree of crystallization exhibits a weak absorption maximum at 2.8 eV, which is responsible for the yellow-orange color, large absorption maximum at 4 eV and an absorption edge associated with the width of the optical gap at 5.2 eV. The bulk modulus (30-37 GPa) and shear modulus (15-18 GPa) of the fabricated samples, as well as their hardness (1-1.5 GPa), are about twice as high as the respective values for polycrystalline graphite. The solution of metalorganic complexes in benzene and pyridine makes it possible to obtain doped graphanes, which can have extraordinary electron transport and magnetic properties.arXiv:1608.07221v1 [cond-mat.mtrl-sci]
“…Instead, the expanded layer spacing may be attributed to graphane forms composed of hydrogenated carbon sheets. Multilayer graphane also referred to as hydro-graphite or graphate, has been theoretically predicted and synthesized 45 , 46 . Experimentally, stable hydro-graphite adopts a graphate-II or “buckled” structure composed of weakly coupled single graphane layers in a chair conformation.…”
Benzene (C6H6), while stable under ambient conditions, can become chemically reactive at high pressures and temperatures, such as under shock loading conditions. Here, we report in situ x-ray diffraction and small angle x-ray scattering measurements of liquid benzene shocked to 55 GPa, capturing the morphology and crystalline structure of the shock-driven reaction products at nanosecond timescales. The shock-driven chemical reactions in benzene observed using coherent XFEL x-rays were a complex mixture of products composed of carbon and hydrocarbon allotropes. In contrast to the conventional description of diamond, methane and hydrogen formation, our present results indicate that benzene’s shock-driven reaction products consist of layered sheet-like hydrocarbon structures and nanosized carbon clusters with mixed sp2-sp3 hybridized bonding. Implications of these findings range from guiding shock synthesis of novel compounds to the fundamentals of carbon transport in planetary physics.
“…The pyrolysis of toluene in the arc can be accompanied by the formation of methyl radicals [ 50 , 51 , 52 ], methylene molecules, and CCH 2 radicals [ 53 ], which interact with the CNH surface to form –CH 3 and –CH 2 groups. Asymmetric and symmetric vibrations in CH 3 cause peaks 1 and 5 in Figure 5 b,c, respectively; peak 2 is due to the asymmetric vibration of CH 2 and CH fragments; peak 3 corresponds to the asymmetric vibration of the CH 2 fragment; peak 4 is due to the bending in CH 3 and CH 2 fragments [ 54 , 55 ]. As the toluene content increases from 2.4 to 8.0 mL, the intensities of these peaks increase significantly.…”
Carbon nanohorns (CNHs) are attractive for various applications, where a high specific surface area and long dispersion stability in water are important. In the present work, we study these parameters of CNHs prepared by arc evaporation of graphite depending on the conditions of the synthesis and subsequent oxidation in air. It is shown that the addition of toluene in the reactor during the arcing allows obtaining CNHs functionalized with −CHx groups. Heating of CNHs in air at 400 °C leads to substitution of −CHx groups for oxygen-containing groups. Moreover, the CNH endcaps are opened at 500 °C, and as a result, the specific surface area of CNHs increases 4 times. Aqueous suspensions with a concentration of oxidized CNHs of 100 µg/mL are stable for 8 months.
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