A new methodology for the reduction of vibrational kinetics in non-equilibrium microwave plasma

A new methodology for the reduction of vibrational kinetics in non-equilibrium microwave plasma: Application to CO₂ dissociation

Fernandez de la Fuente, J. (TU Delft Intensified Reaction and Separation Systems)
Moreno Wandurraga, S.H. (TU Delft Intensified Reaction and Separation Systems)
Stankiewicz, A.I. (TU Delft Intensified Reaction and Separation Systems)
Stefanidis, G. (Katholieke Universiteit Leuven)

2016

Plasma reactor technologies have the potential to enable storage of green renewable electricity into fuels and chemicals. One of the major challenges for the implementation of these technologies is the energy efficiency. Empirical enhancement of plasma reactors' performance has proven to be insufficient in this regard. Numerical models are therefore becoming essential to get insight into the process for optimization purposes. The chemistry in non-thermal plasmas is the most challenging and complex part of the model due to the large number of species and reactions involved. The most recent reaction kinetics model for carbon dioxide (CO2) dissociation in non-thermal microwave plasma considers more than one hundred species and thousands of reactions. To enable the implementation of this model into multidimensional simulations, a new reduction methodology to simplify the state-to-state kinetic model is presented. It is based on four key elements: 1) all the asymmetric vibrational levels are lumped within a single group or fictitious species, Image ID:c6re00044d-t1.gif, 2) this group follows a non-equilibrium Treanor distribution, 3) an algebraic approximation is used to compute the vibrational temperature from the translational temperature based on the Landau–Teller formula and 4) weighted algebraic expressions are applied, instead of complex differential equations, to calculate the rates of the most influencing reactions; this decreases substantially the calculation time. Using this new approach, the dissociation and vibrational kinetics are captured in a reduced set of 44 reactions among 13 species. The predictions of the reduced kinetic model regarding the concentrations of the heavy species in the afterglow zone are in good agreement with those of the detailed model from which the former was derived. The methodology may also be applied to other state-to-state kinetic models in which interactions of vibrational levels have the largest share in the global set of reactions.

http://resolver.tudelft.nl/uuid:9a2af4ba-5ea3-4c23-a20e-617a309cf438

https://doi.org/10.1039/C6RE00044D

2017-08-17

2058-9883

Reaction Chemistry & Engineering, 1 (5), 540-554

Accepted Author Manuscript

Institutional Repository

journal article

© 2016 J. Fernandez de la Fuente, S.H. Moreno Wandurraga, A.I. Stankiewicz, G. Stefanidis