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2. HYDROGEN RADICAL ASSISTED METHANATION 2.3. RESULTS a) -1 10 -2 10 -3 10 -4 10 0.0 0.2 0.4 0.6 0.8 1.0 b) -1 10 -2 10 -3 10 -4 10 0.0 0.2 0.4 0.6 0.8 1.0 CO input 2 O 2 CO 2 HO 2 CO CH 4 CO input CO CO 2 HO 2 CH 4 CH (CO ) 42 Figure 2.3: Product distributions measured with Ar + CO2 + H2 plasmas (a) and Ar + CO + H2 plasmas (b) as a function of Φ (see equation 2.1). CH4 produced in Ar + CO2 + H2 plasmas is also shown in (b) for comparison. slightly at very high to pure H2 conditions. Another major species, observed in both sets of experiments, is H2 O. Its production in Ar + CO2 + H2 plasmas peaks at a few percent addition of H2 before stabilizing to a lower value (≈ 20 % of input CO2). The peak in the H2O production can be explained taking into account the trends in the production of O and H radicals. This will be discussed in detail in section 2.4.4. In Ar + CO2 + H2 plasmas, in pure Ar condition (i.e., at Φ=0.0), O2 densities are maximally produced and in stoichiometric ratio dictated by unimolecular dissociation of CO2 CO2 −→ CO + 0.5 O2 (R1) and they decrease steeply with the addition of H2. with addition of H2 most of the atomic oxygen produced from CO2 dissociation ends up in H2O. Methane production increases with H2 ratio reaching a maximum value at the pure H2 condition (≈ 2% conversion of input CO2). Measurable quantities of methane are produced when Φ is ≈ 0.3. By contrast, methane production is detectable immediately with addition of H2 in Ar + CO + H2 plasmas (fig 2.3b), monotonically increasing with Φ, reaching a maximum value in pure H2 conditions (25% conversion of CO). The amount of H2O observed is approximately constant in all the conditions. The maximum amount of water produced is four times lower than the maximum amount measured in Ar + CO2 + H2 plasmas. CO2 was only produced when H2 addition is not significant and molecular oxygen was below detection limits in Ar + CO + H2 plasmas. The balance between total input of carbon and oxygen from CO in all the products is not complete. This unaccounted car- bon increases slowly with addition of H2 and reaches almost 50% in pure H2 condition. More investigations are required to understand this discrepancy. Methanation of CO is 24 Mixing Ratio Mixing RatioPDF Image | Understanding CO2 containing non-equilibrium plasmas
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