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2.1. INTRODUCTION 2. HYDROGEN RADICAL ASSISTED METHANATION ing syn-gas mixture and subsequently using F-T like mechanism [76]; such a general mechanism can be represented with equation M1. P1 P2+H P3 CO2 −→ CO −−−−→ CHxOy −→ CH4 (M1) Or methanation of CO2 can proceed without forming syn-gas but by forming oxygen- ates as intermediates [76]; such a general mechanism can be represented with equation M2. P1+H P2 CO2 −−−−→ CHxOy −→ CH4 (M2) The choice of catalyst is the dominant factor that determines which mechanism is active. In general, a chemical reaction involving saturated molecules is characterized by an activation barrier (Ea), the extra energy required by the reactants need to successfully produce products. In conventional catalysis (e.g M1 and M2), Ea of many chemical re- actions is significantly reduced by using a catalyst. The catalyst does this by creating chemically active intermediates that enhance the rates of desirable elementary chemical reactions. However, most catalyst systems suffer from reduction in efficiency due accu- mulation of nonreactive species on the surface over time and require regeneration period- ically [84]. Also the optimal catalysts, in most cases, are very expensive metals like Co, Ru etc., [83]. By comparison, reactions of many radicals with neutral molecules and ions with neutral molecules proceed with low or almost no activation barriers [85, 86]. High internal energies of the electronically and ro-vibrationally excited species can help in re- ducing Ea of reactions (including surface reactions) [87]. For example, internal energy of H2 is known to enhance the reaction rates of elementary reaction of reducing hydroxyl radical to water [88]. Hence by using plasma, which can generate significant concen- tration of active species such as radicals, ions, vibrationally and electronically excited species the choice of surfaces can be expanded. Even relatively inert stainless steel walls can become site of enhanced chemical reactivity. If principles of plasma activation are well understood, then plasma and conventional catalysts can be combined for synergistic effect – an area of research broadly called as plasma catalysis. For this work a cascaded arc has been used as a source for the production of active species; it can act as a very high flux radical source when molecular gases (H2 in this work) are used [29] and as a high flux ion source when noble gases (Ar in this work) are used [89]. This source has been thoroughly characterized in terms of parameters like electron temperature, radical densities ion densities etc [29, 89–91]. It injects radicals and ions into a reactor that is at a low pressure, resulting in expanding plasma jet (EPJ, see 19PDF Image | Understanding CO2 containing non-equilibrium plasmas
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