Abstract

Plasma-based greenhouse gas conversion (mainly CO₂ and CH₄) is gaining increasing interest. To improve this application in terms of conversion, energy efficiency and product formation, a good insight in the underlying mechanisms is desirable. We try to obtain this by computer modelling, supported by experiments.

We simulate both the plasma chemistry as well as the optimum reactor design, in the three types of plasma reactors most commonly used for gas conversion, i.e., (packed bed) dielectric barrier discharges (DBDs), gliding arc (GA) discharges and microwave (MW) plasmas. For the plasma reactor design, we use 2D or 3D computational fluid dynamics modelling. For the plasma chemistry, we make use of zero-dimensional chemical kinetics modeling, which solves continuity equations for the various plasma species, based on production and loss terms, as defined by the chemical reactions.

We focus especially on the the role of vibrationally excited CO₂ levels, which are the key species for enhanced energy efficiency of the CO₂ conversion. Our model reveals the relative importance of various processes, responsible for the CO₂ conversion, in a range of different conditions, and this is linked to the energy efficiency in the various types of plasma reactors.

We have also studied the plasma chemistry in CO₂/CH₄  and in CO₂/H₂O mixtures, with the purpose of producing value-added chemicals. The main products formed are a mixture of H₂ and CO, or syngas, with a tuneable H₂/CO ratio depending on the gas mixing ratio. The production of oxygenated compounds, such as methanol, formaldehyde, etc, is very limited, showing the need for combining with a catalyst. A detailed chemical kinetics analysis allows to elucidate the different pathways leading to the observed results.

Finally, we try to answer the question whether plasma can be formed inside catalyst pores, and what are the critical pore dimensions, by means of particle-in-cell Monte Carlo collision simulations of plasma streamer propagation inside catalyst pores.

Prof. Annemie Bogaerts简介

Annemie Bogaerts (age 46) is full professor and head of the research group PLASMANT. She has above 400 peer‐reviewed publications since 1995, and ca. 10,000 citations, with a H‐index of 49 (Web of Science) (above 14,000 citations and H‐index of 58 in Google Scholar). Furthermore, she has more than 140 invited lectures at international conferences (since 1998) and 60 invited seminars at universities/institutes (since 1995), in various countries. She was the supervisor of 29 finished PhD theses (since 2005), and is now supervising 16 PhD students (incl. 4 joint PhD students), and 14 postdocs. She has received 20 scientific awards, including the Prize of the Research Council of the University of Antwerp in Exact Sciences (1998), the Prize of the “Koninklijke Vlaamse Academie van België voor Wetenschappen en Kunsten” in de category Exact Sciences (2001), the Alumni Prize of the “Belgian‐American Educational Foundation” (2003), the “Lester W. Strock Award of the New England Section of the Society for Applied Spectroscopy”, in recognition for “Outstanding contributions in the areas of plasma and surface modeling” (2008) and the “Winter Plasma Award”, in recognition for “Outstanding contributions in the field of laser ablation modeling” (2009).