Taming microwave plasma to beat thermodynamics in CO2 dissociation

Author:

van Rooij G. J.123,van den Bekerom D. C. M.123,den Harder N.123,Minea T.123,Berden G.45673,Bongers W. A.123,Engeln R.8910113,Graswinckel M. F.123,Zoethout E.123,van de Sanden M. C. M.12389

Affiliation:

1. Dutch Institute for Fundamental Energy Research

2. 5600 HH Eindhoven

3. The Netherlands

4. Radboud University

5. Institute for Molecules and Materials

6. FELIX Laboratory

7. 6525 ED Nijmegen

8. Department of Applied Physics

9. Plasma and Materials Processing Group

10. Eindhoven University of Technology

11. 5600 MB Eindhoven

Abstract

The strong non-equilibrium conditions provided by the plasma phase offer the opportunity to beat traditional thermal process energy efficiencies via preferential excitation of molecular vibrations. Simple molecular physics considerations are presented to explain potential dissociation pathways in plasma and their effect on energy efficiency. A common microwave reactor approach is evaluated experimentally with Rayleigh scattering and Fourier transform infrared spectroscopy to assess gas temperatures (exceeding 104 K) and conversion degrees (up to 30%), respectively. The results are interpreted on a basis of estimates of the plasma dynamics obtained with electron energy distribution functions calculated with a Boltzmann solver. It indicates that the intrinsic electron energies are higher than is favorable for preferential vibrational excitation due to dissociative excitation, which causes thermodynamic equilibrium chemistry to dominate. The highest observed energy efficiencies of 45% indicate that non-equilibrium dynamics had been at play. A novel approach involving additives of low ionization potential to tailor the electron energies to the vibrational excitation regime is proposed.

Publisher

Royal Society of Chemistry (RSC)

Subject

Physical and Theoretical Chemistry

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