Concentrations of Active Species in the Flowing Afterglow of a Nitrogen Microwave Plasma

Measurements of nitrogen atom density, by means of NO chemical titration, along with an evaluation of the densities of some excited species N ₂ (B, v=11), N ₂ (B, v=2), N ₂ (C, v=0), and N ₂ ⁺ (B,v=0), by means of a spectroscopic study of some bands of dinitrogen, are achieved along the flowing afterglow of a dinitrogen microwave plasma (2450 MHz) for several pressures. The concentrations obtained are in the following range: [N]10 ⁺¹⁵ , [N ₂ (B, 2)]10 ⁺⁹ –10 ⁺¹⁰ , [N ₂ (B, 11)]10 ⁺⁸ –10 ⁺⁹ , [N ₂ (C, 0)]10 ⁺⁶ –10 ⁺⁷ , [N ₂ ⁺ (B,0)]10 ⁺⁶ -10 ⁺⁸ (cm^-3). From a kinetic study of the formation and decay of excited and charged species, an estimation of N ₂ (A, v), N ₂ (X, v, and N ₂ ⁺ (X) densities can be derived: [N ₂ (A, v)]10 ⁺¹² , [N ₂ (X, v6)]10 ⁺¹⁵ –10 ⁺¹⁶ , [N ₂ (X, v12)]10 ⁺¹⁴ –10 ⁺¹⁵ , [N ₂ ⁺ (X)]10 ⁺¹⁰ (cm ^-3 ).     

Air microwave-induced plasma: Relation between ion density and atomic oxygen density

Electron temperature and ion density are measured in an air microwave-induced plasma (2450 MHz) by means of a floating double probe. A 'cinetic scheme for ion formation and decay is set up, and a relationship between atomic oxygen and ion densities is obtained. From this relationship an order-of-magnitude of atomic oxygen concentration in the discharge is derived and compared with results obtained by optical actinometry in another work.     

A kinetic study of methane conversion by a dinitrogen microwave plasma

Conversion of CH₄ with a N₂ microwave plasma (2.45 GHz) is studied. The experiments cover the absorbed microwave power range 300–700 W with 17–62% of methane in the gas mixture, with pressures of 10–40 mbar and flow rates of 140–650 ml· min^–1. The yields of C₂ hydrocarbons and dihydrogen are analyzed by gas chromatography. The distance of methane addition downstream of the plasma plays an important role on the composition and the concentration of the products obtained. This distance mainly determines the energy concentrated in the active species of the plasma when they react with methane. Different behaviors for acetylene formation, on the one hand, and for ethane and ethene formation, on the other hand, have been observed, and this finding allows us to propose a kinetic mechanism for the decay of methane and for the formation of C₂ hydrocarbons.     

Methane Conversion in the Flowing Afterglow of a Dinitrogen Microwave Plasma: Initiation of the Reaction

The reaction of methane in the nitrogen afterglow is studied by combination of direct measurements and computer experiment. The experimental data were obtained by optical emission spectroscopy of the discharge, by gas chromatography of resulting stable products and by probe diagnostics of charged species in afterglow plasma. The simulation was based on a macroscopic kinetic approach covering 24 species and 61 reactions with input data given by the afterglow experiment. In the present stage of the modelling the initiation of methane conversion was studied. It was found that, contrary to active discharge, in the afterglow plasma the active neutral species (mainly excited dinitrogen molecules) are most important for the dissociation of methane into CH_x and H radicals.     

Study of Spectral Emission Behaviour in the Glow and Microwave Discharges of Oxygen

Because of the very important role of oxygen plasmas in various applications, both direct current and microwave discharges have been analysed from the point of view of emission spectra properties. In both cases silica discharge tubes with practically the same diameters were used. The following transitions of the oxygen discharges were studied: the atomic lines at 777.4 nm (⁵P ‐ ⁵S)and 747.7 nm (³D ‐ ³P⁰), and the head at 759.4 nm of the atmospheric system (b ¹Σ⁺_g, v = 0 ‐ X ³Σ^—_g, v = 0).     

Methane conversion by an air microwave plasma

Activation of methane is carried out by means of an air microwave plasma (2.45 GHz). The experiments cover the absorbed microwave power range 350–650 W (20–50 W cm³ with 17–62%, of methane in the gas mixture, with pressures of 10–66 mbar and flow rates of 140700 ml min¹. Methane, dioxygen, and dinitrogen consumptions as well as C₂ hydrocarbons, carbon monoxide, and dihydrogen yields are analyzed hr gas chromatography. The distance of methane addition from the end of the discharge plays an important role in the composition and the concentration of the products obtained. This distance mainly determines the energy concentrated in the active species of the plasma when they react with methane. A kinetic mechanism jar the activation and decay of inethane and for the formation of C₂ hydrocarbons and carbon monoxide is discussed based on the experimental results and kinetic data in the literature.     

Experimental Study and Modelling of Formation and Decay of Active Species in an Oxygen Discharge

A microwave (2.45 GHz) oxygen discharge (3 hPa, 150 W, 50 mL.min^–1) is studied by optical emission spectroscopy of O(⁵P) (line 777.4 nm) and of the atmospheric system of O₂(head‐line 759.4 nm). Calibration of the spectral response of the optical setup is used to determine the concentrations of O(⁵P) and O₂(b). The concentration of the O(⁵P) atoms is in the range 108–109 cm^–3 and the concentration of the O₂(b) molecules is in the range 10¹⁴ – 2 × 10¹⁴ cm^–3 along the discharge tube. An attempt is made to simulate the experimental results by using coupling the Boltzmann equation, homogeneous energy transfer V‐V and V‐T, heterogeneous reactions on the walls (energy transfer and recombination of atoms) and a kinetic scheme (electronic transfer and chemical reactions). The Boltzmann equation includes momentum transfer, inelastic and superelastic processes and e‐e collisions. V‐V and V‐T transfer equations are obtained from the SSH theory and the kinetic scheme includes 65 reactions with 17 species [electrons e, ions O^– and O₂^–, fundamental electronic neutral species O(³P), O₂, O₂(X,v), O₃ and excited neutral species O₂(a), O₂(b), O₂(A), O(¹D), O(¹S), O(⁵P), O(4d ⁵D^o), O(5s ⁵S^o), O(3d ⁵D^o) and O(4s ⁵S^o)]. A fair agreement between experimental results and modelling is obtained with the following set of fitting values: – heterogeneous deactivation coefficient for O₂(b) γ = 2.6 × 10^–2; – rate constant of reaction [O(¹D) + O(³P) → 2 O(³P)] k₃₄ = 1.4 × 10^–11 cm³.s^–1; – electron concentration in the range 10¹⁰ – 10¹¹ cm^–3. Modelling shows that the recombination coefficient for oxygen atoms on the silica wall (range 1.4 × 10^–3 – 0.2 × 10^–3) is of the same order as the values obtained in a previous paper and that the ratio ([O] / 2 [O₂]initial) is about 33–50%. (© 2005 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)