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5.1. INTRODUCTION 5.1 Introduction For a sustainable future, it has become imperative to store the electric energy generated by renewable sources in chemical forms with an high energy density. Many research efforts are being pursued to develop closed loop chemical cycles that produce fuels (also called solar fuels) using renewable energy without any further increase of green house emissions. In this context, non thermal plasmas becomes especially attractive because they can be tuned in such a way that up to 95 % of total injected energy can be used for vibrational excitation in molecular gases [36, 63, 154]. Apart from being the optimal path for disso- ciation, in many cases vibrational energy is expected to enhance the chemical reactivity of endothermic reactions [36, 205]. For example, activation barrier of chemical reactions can be reduced, which will effectively enhance the rate coefficient of reaction. Such a reduction in activation energy and associated enhancement of reaction rate coefficient has been demonstrated by Schatz et al for the reaction, OH+H2 −→H2O+H (R1) Here it is found that the rate coefficient was enhanced by a factor of 300 at room temper- ature when H2 is excited to its first vibrational mode as compared with H2 in just ground state. Different modes of vibration might be required to enhance the rate of chemical re- actions of different molecules; for example, in the reaction R1, the vibrational excitation of OH has been found to have no effect on the rate coefficient. Other examples include, the excitation of symmetric mode in CH4 dissociation on surfaces [33] and the asymmet- ric mode excitation for CO2 dissociation in a plasma [35]. However, for most chemical systems it is not yet very clearly known how non equilibrium vibrational distributions effect specific chemical reactions. For example, in CO2 plasmas the effect of vibrational excitation of CO2 on the reaction CO2 + O −→ CO + O2 is not known and it is an active topic of research to understand the chemical reaction pathways of CO2 molecule excited to a selective vibrational mode [206]. In the following sections a detailed review of how vibrational energy can be used for CO2 dissociation will be given. The sections are divided so as to first discuss different reactions that create and ex- change vibrational energy. Secondly a discussion on preferred vibrational distributions is presented. Later, the discussion is extended to describe the vibrational energy exchange in CO2, a polyatomic molecule. Vibrational energy storage in asymmetric mode and its effect on dissociation is emphasized. Lastly, as a special note dissociation from vibra- tional quasi-continuum will be briefly touched upon. 111PDF Image | Understanding CO2 containing non-equilibrium plasmas
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