Insight into CO2 Dissociation in Plasma from Numerical Solution of a Vibrational Diffusion Equation

5 years ago

Insight into CO2 Dissociation in Plasma from Numerical Solution of a Vibrational Diffusion Equation

Savino Longo, Mauritius C. M. van de Sanden, Paola Diomede

Dissociation of CO₂ molecules in plasma is a subject of enormous importance for fundamental studies and in view of the recent interest in carbon capture and carbon-neutral fuels. Vibrational excitation of the CO₂ molecule plays an important role in the process. The complexity of the present state-to-state (STS) models makes it difficult to find the key parameters. In this paper we propose, as an alternative, a numerical method based on the diffusion formalism developed in the past for analytical studies. The nonlinear Fokker–Planck equation is solved by the time-dependent diffusion Monte Carlo method. Transport quantities are calculated from STS rate coefficients. The asymmetric stretching mode of CO₂ is used as a test case. We show that the method reproduces the STS results or a Treanor distribution depending on the choice of the boundary conditions. A positive drift, whose energy onset is determined by the vibrational to translational temperature ratio, brings molecules from mid-energy range to dissociation. Vibrational–translational energy transfers have negligible effect at the gas temperature considered in this study. The possibility of describing dissociation kinetics as a transport process provides insight toward the goal of achieving efficient CO₂ conversion.

Publisher URL: http://dx.doi.org/10.1021/acs.jpcc.7b04896

DOI: 10.1021/acs.jpcc.7b04896