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2. HYDROGEN RADICAL ASSISTED METHANATION 2.2. EXPERIMENTAL DETAILS section 2.2.1) which works at low pressure and is recombining in nature. In EPJ, a high fraction of H radicals generated from the source undergo sequence of chemical reactions producing excited species: ro-vibrationally excited H2 and electronically excited H in particular [92]. Likewise ions such as Ar+ , H+2 recombine with electrons to produce excited species. In this work, mechanistic aspects of methanating CO2 – both on surface and in gas phases – with active species generated by Ar-H2 plasmas are described in detail; simil- arities and differences from F-T are highlighted i.e to ascertain if it is M1 or M2 that is dominant mechanism in methanation of CO2 in plasmas. A simple calculation is used to describe the role of the active species in the chemistry. Surface reactions are partic- ularly important in molecule formation in EPJ because of the low pressures used [93]. Therefore the role of surface reactions is tested by covering the walls of the stainless steel reactor with copper (Cu) and aluminum (Al) foils. Though the conditions used for this work may not be applicable to large scale directly, it gives insights into necessary and limiting conditions for methanation of CO2 in highly activated environments. 2.2 Experimental Details 2.2.1 Experimental set up and Characterization The experimental setup used in the current work has been described in detail elsewhere [89, 92] and only the key features are repeated here. The set-up consists of two parts, the first part generates plasma (plasma source) and the second part is the chamber into which the plasma expands (called as reactor in this work) and where the gas conversion takes place – expanding plasma jet (EPJ, figure 2.1). The plasma source consists of a wall stabilized cascaded arc through which the working gas mixture flows into the reactor. The plasma generated in the cascaded arc is at sub-atmospheric pressure (around 100 mbar) with an electron temperature, Te, of around 1eV [90, 94]. The plasma thus generated expands supersonically into the reactor through a copper nozzle. This plasma jet from the arc ends in a stationary shock front (few centimeters from the nozzle) after which it slows down into a subsonic expansion [95]. Te decreases to 0.2-0.3 eV at the end of expansion [89, 92] where most of the measurements are performed. Molecular gases like CO2, C2H2, SiH4 etc. can be admixed in the in the subsonic expansion region (see figure 2.1) [95]; for this work CO2 and CO are admixed. The flow dynamics are such that the chemical species are thoroughly mixed. The background pressure in the reactor of 1.1 mbar can be maintained independently of pressure in the arc. Since charged species are 20PDF Image | Understanding CO2 containing non-equilibrium plasmas
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