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4.4. RESULTS AND DISCUSSION 4. FLUID MODELLING OF CO2 DISSOCIATION Even larger differences between the negative and the positive half-cycle are found in the spatiotemporal evolution of the negative charge carriers shown in figure 4.4b. In the negative half-cycle electrons are the dominant negatively charged species in the plasma region whereas negative ions dominate in the cathode fall region. Here, CO–3 is the dom- inant anion and its density contributes to more than 95 % to the total density of negative ions over the entire period. Due to their larger mass compared to the electron component, anions respond more inertly to the change of the electric field direction at t/T ≈ 18.8 (cf. figure 4.3d). As a result, most anions remain in the gap until re-ignition of the discharge in the positive half-cycle and constitute the the dominant negatively charged species here in contrast to the dominance of electrons during the negative half-cycle. Ion-ion recom- bination (processes I6 and I7 in table 4.5) as the dominant loss channel of negative ions is too slow for a marked depletion of its density within one voltage half-cycle. CO–3 has been found to be the dominant negative ions from numerical simulations (for example, [63]) and from experimental studies (for example, [197]) in pure CO2 plasmas. Mechanisms of CO2 dissociation In order to analyse the mechanisms of CO2 dissociation generating CO and O, the spa- tiotemporal distributions of CO and O particle densities are displayed in figure 4.5 for the standard condition. Starting from a spatially homogeneous distribution of these spe- cies with an initial particle density of 1000 cm−3 the densities of CO and O gradually increase in time. They are mainly generated around d0. The slight asymmetry of their spatial distribution is a consequence of the differences in the discharge behaviour the positive and negative half-cycle (cf. figure 4.3) At the end of the calculation the dens- ity of CO is slightly larger than that of O because the dissociative electron attachment to CO2 according to reaction E47 in table 4.2 leads to an additional generation of CO, while it does not produce O. Furthermore, the loss processes of CO and O in table 4.5 due to heavy particle collisions are comparatively inefficient during the period of time considered and the diffusion of both these species takes place with comparable velocity. To analyse the contribution of the different CO production channels, the rates of CO production due to electron impact dissociation (reaction E42 in table 4.2), by dissociative electron attachment to CO2 (reactions E47–E53 in table 4.2) and by dissociative electron- ion recombination (reaction E54 in table 4.2) are shown in figure 4.6 together with the temporal variation of the discharge current density and the spatially integrated CO density over one representative voltage cycle (t/T = 18.45–19.45 in figure 4.3) It is found that the CO density shows a step-like increase during the short discharge events, while it remains almost constant for the rest of the cycle (cf. figure 4.6a). The representation 95PDF Image | Understanding CO2 containing non-equilibrium plasmas
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