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2.4. DISCUSSION 2. HYDROGEN RADICAL ASSISTED METHANATION between them listed in tables 2.4 and 2.5, the densities of active species in the reactor are calculated. The calculations will be used to test if the reactions set considered will be sufficient to explain the results. Apart from the reactions listed in the tables, reaction R2 – reduction of CO2 with H – has been included to explain CO production at Φ = 1.0, when none of the other reactions will suffice. CO2 +H−→CO+OH (R2) The rate coefficient of this reaction is taken as 4.6× 10−22 m3s−1 [107]. The concentra- tion ni(t) of a species can be calculated with equation 2.2 ∫t∑ ∏ (−1)pkj nLl dt (2.2) ni(t)= The notation in equation 2.2 has the following definitions: t is the residence time (=0.25 s); kj is the rate coefficient of reaction j; nLl is the density of lth species in the left hand side of the reaction j; p is 1 when species i appears on left hand side of reaction j and 2 when it appears on the right hand side of reaction j. Combined initial concentration of all the species is set at 1016 cm−3. No spatial information or effect of the electric field is considered in this model. First, the concentrations of Ar+ ions and H radicals in the reactor after a residence time t is calculated as a function of Φ neglecting CO2. The results are plotted in the figure 2.6. From this figure it can be seen that when purely Ar flows through the arc (Φ=0.0), Ar+ ions account for 10% of the total concentration and similarly when purely H2 flows through the arc (Φ=1.0), 10% of the total species are H radicals; these follow directly from the initial conditions. With the addition of H2 to Ar, however, the Ar+ ions densities decrease very fast, producing H radicals. At Φ = 0.1, almost all the Ar+ ions are depleted with corresponding maximum in H radical densities. The loss of Ar+ ions with addition of H2 is established by others [94, 102]. With the addition of a constant amount of CO2, there exists a competition between CO2 and H2 for the charge transfer reactions and Ar+ ions are completely depleted even at Φ=0.0. This effect is illustrated in figure 2.7. In this figure, Ar+ ions are completely converted to produce either CO or H eventually. Because of its simplicity, only qualitat- ive trends in species densities could be captured with the model. Two of those important trends that match with the measured trends, when CO2 addition is considered are: max- imum CO density is produced when Φ=0.0; with the addition of H2, CO densities de- creases. Hence, the initial steep decline of CO can be attributed to fast loss of Ar+ ions, weakening the CT with CO2 (reaction C1) and subsequent DR of CO+2 with electrons (reaction D1) to produce CO. 0 jl 29PDF Image | Understanding CO2 containing non-equilibrium plasmas
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