期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 124, 期 34, 页码 18401-18415出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.0c04257
关键词
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资金
- FWO project [G.0383.16N]
- European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program [810182]
- Hercules Foundation
- Flemish Government (department EWI)
- UAntwerpen
Plasma technology is gaining increasing interest for CO2 conversion. The gas temperature in (and after) the plasma reactor largely affects the performance. Therefore, we examine the effect of cooling/quenching, during and after the plasma, on the CO2 conversion and energy efficiency, for typical warm plasmas, by means of chemical kinetics modeling. For plasmas at low specific energy input (SEI similar to 0.5 eV/molecule), it is best to quench at the plasma end, while for high-SEI plasmas (SEI similar to 4 eV/molecule), quenching at maximum conversion is better. For low-SEI plasmas, quenching can even increase the conversion beyond the dissociation in the plasma, known as superideal quenching. To better understand the effects of quenching at different plasma conditions, we study the dissociation and recombination rates, as well as the vibrational distribution functions (VDFs) of CO2, CO, and O-2. When a high vibrational-translational (VT) nonequilibrium exists at the moment of quenching, the dissociation and recombination reaction rates both increase. Depending on the conversion degree at the moment of quenching, this can lead to a net increase or decrease of CO2 conversion. In general, however, and certainly for equilibrium plasmas at high temperature, quenching after the plasma helps prevent recombination reactions and clearly enhances the final CO2 conversion. We also investigate the effect of different quenching cooling rates on the CO2 conversion and energy efficiency. Finally, we compare plasma-based conversion to purely thermal conversion. For warm plasmas with typical temperatures of 3000-4000 K, the conversion is roughly thermal.
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