Understanding CO2 containing non-equilibrium plasmas

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Understanding CO2 containing non-equilibrium plasmas ( understanding-co2-containing-non-equilibrium-plasmas )

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1. GENERAL INTRODUCTION 1.2. FRAMEWORK AND GOALS OF THIS THESIS [40] or using plasma and a catalyst [41, 42]. Recently Sakai et al reported on convert- ing CO2 with H2 plasma generated from plasmas produced in water [43]. The lack of literature on approach I is quite surprising considering the fact that a lot of research on a related topic, dry-reforming using plasma is being pursued extensively [44–46]. The main focus of these works has been to optimize the parameter space to produce a desired product than to understand the mechanisms in detail. In contrast to approach I, a wealth of reports exist on approach II. The best results in terms of energy efficiency (between 60-80 %) have been obtained in microwaves at a pressure of 300 Torr [35, 47]. These exceptional results in microwave plasmas were explained with VV up-pumping [36] as mentioned before. Spencer et al by trying similar experiments at atmospheric pressure in RF discharges, could achieve converting 100 % of CO2 into CO, but were not successful in reproducing such high energy efficiencies [48]. Same group used Microwave plasmas with a catalyst (Rhodium) and had improved the energy efficiency to 30 % but at the cost of conversion [49]. In recent years non-equilibrium plasmas at atmospheric pres- sure have gained popularity due to availability of cheap power sources. These plasma sources were also investigated for CO2 conversion. Examples include using gliding arc discharges [50–52], corona discharges [53–55], nanosecond pulsed discharges [56], mi- crohollow cathode discharge [57], microplasmas [58] and in dielectric barrier discharges [59–62]. Again most of the research has been only to optimize the parameter space than to gain insights into the mechanistic aspects. In addition to the experimental research there has been efforts in theoretical and numerical modeling to understand these plasmas [62–66]. From this cursory glance at the literature it would become immediately obvious that there is an immense variety in plasma sources being used for CO2 conversion. Though this variety implies that thorough investigations into specific details of each type of plasma are required to be carried out, there can be some general features vis-à-vis chem- ical and physical mechanisms that are common to all (non-equilibrium) plasmas and these need to be explored even more. In this context, this thesis sets itself the goal of exploring some of these general features plasma assisted CO2 conversion. To this end two different plasma sources are explored from both experiments and numerical modeling. Detailed description of the plasma sources and the reasons for their selection will be discussed in the subsequent chapters. Some of the key issues that this thesis addresses are 6

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