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Plasma based assembly and engineering of advanced carbon nanostructures

Abstract : Plasma environments constitute powerful tools in materials science by allowing the creation of innovative materials and the enhancement of long existing materials that would not otherwise be achievable. The remarkable plasma potential derives from its ability to simultaneously provide dense fluxes of charged particles, chemically active molecules, radicals, heat and photons which may strongly influence the assembly pathways across different temporal and space scales, including the atomic one.In this thesis, microwave plasma-based methods have been applied to the synthesis of advanced carbon nanomaterials including graphene, nitrogen-doped graphene (N-graphene) and diamond-like structures. To this end, the focus was placed on the optimization of the production processes of two-dimensional (2D) carbon nanostructures, such as graphene and N-graphene, by further elaboration and refinement of the microwave plasma-based method developed at the Plasma Engineering Laboratory (PEL). The scaling up of the synthesis process for high-quality graphene using surface-wave plasmas operating at atmospheric pressure and argon-ethanol mixtures was successfully achieved. Moreover, N-graphene was synthetized via a single-step process, by adding nitrogen to the argon-ethanol mixture, and via two-step process, by submitting previously synthetized graphene to the remote region of a low-pressure argon-nitrogen plasma. Nitrogen atoms were usefully incorporated into the hexagonal graphene lattice, mainly as pyrrolic, pyridinic and quaternary bonds. A doping level of 25% was attained.Different types of carbon nanostructures, including graphene and diamond-like nanostructures, were also produced by using methane and carbon dioxide as carbon precursors in an argon plasma.Additionally, capacitively-coupled radio-frequency plasmas have been employed in the functionalization of graphene and in the synthesis of Polyaniline (PANI)-graphene composites. The potential uses of these materials were studied, with both showing favourable characteristics for their applicability in biosensing applications.
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Ana Inês Vieitas de Amaral Dias. Plasma based assembly and engineering of advanced carbon nanostructures. Plasma Physics [physics.plasm-ph]. Université d'Orléans; Universidade técnica (Lisbonne), 2018. English. ⟨NNT : 2018ORLE2019⟩. ⟨tel-02436761⟩

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