Abstract

Thermal plasma processing of carbon sources using a plasma jet with high heat capacity is one of the most promising methods for the synthesis of new materials. This paper describes the low-temperature deposition of carbon nanomaterials by remote plasma-enhanced chemical vapor deposition (PECVD) in the absence of catalysts. The remote PECVD process differs from conventional and direct PECVD process in two ways: (a) only a subset of the process reactants and/or diluents are directly plasma excited; and (b) thin film deposition takes place on a substrate that is outside of the plasma glow region. In conventional CVD methods, carbon is produced from the decomposition of carbon sources such as hydrocarbons, carbon monoxide, alcohols, and so on, over a metal catalyst. The unavoidable metal species remaining in carbon nanomaterials would lead to obvious disadvantages for property characterization and application exploration. Despite sustained efforts, it is still an intractable problem to remove metal catalysts completely from carbon nanomaterials samples without introducing defects and contaminations. Good reactor design allowed to overcome problems of chemical and structural purity, and poor process robustness in terms of phase composition of product from run to run. For the synthesis of graphene materials, carbon black, carbon nanotubes, nanowires we used the thermal plasma generator which is a high current divergent anode-channel DC plasma torch. The experiment involved a simultaneous input of hydrocarbons (methane, propane, butane, acetylene) with the plasma forming gas (helium, argon, nitrogen) into the plasma torch, wherein heating and decompositions occurred in the plasma jet and in the region of the arc discharge, followed by condensation of the synthesis product on metallic surfaces. The deposition rate was varied with distance from the plasma. Consumption of carbon source, plasma forming gas and plasma torch power were changed independently from each other. For the experimental conditions the electric power of plasma torch was set up to 40 kW. Regularities of formation of carbon thread-like nanostructures and graphene in the course of hydrocarbons pyrolysis in thermal plasma without participation of catalytic particles were studied by means of electron microscopy, X-ray diffraction, IR-spectrometry and thermogravimetry. Depending on the pyrolytic synthesis parameters, different proportions of crystal carbon and soot may be obtained. It has been demonstrated that the phase composition is varied by hydrocarbons flow rate, plasma forming gas pressure and dc plasma torch power. It has been established through the experiments that carbon nucleation is volumetric and proceeds according to the model of explosive soot formation.

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