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Nanosecond Pulsed Discharge for CO2 Conversion: Kinetic Modeling To Elucidate the Chemistry and Improve the Performance
- Source :
- The journal of physical chemistry: C : nanomaterials and interfaces, Journal of physical chemistry. C 123 (2019): 12104–12116. doi:10.1021/acs.jpcc.9b01543, info:cnr-pdr/source/autori:Heijkers, Stijn; Martini, Luca Matteo; Dilecce, Giorgio; Tosi, Paolo; Bogaerts, Annemie/titolo:Nanosecond Pulsed Discharge for CO2 Conversion: Kinetic Modeling To Elucidate the Chemistry and Improve the Performance/doi:10.1021%2Facs.jpcc.9b01543/rivista:Journal of physical chemistry. C/anno:2019/pagina_da:12104/pagina_a:12116/intervallo_pagine:12104–12116/volume:123, Journal of Physical Chemistry C, 123(19), 12104-12116. American Chemical Society
- Publication Year :
- 2019
- Publisher :
- American Chemical Society (ACS), 2019.
-
Abstract
- We study the mechanisms of CO 2 conversion in a nanosecond repetitively pulsed (NRP) discharge, by means of a chemical kinetics model. The calculated conversions and energy efficiencies are in reasonable agreement with experimental results over a wide range of specific energy input values, and the same applies to the evolution of gas temperature and CO 2 conversion as a function of time in the afterglow, indicating that our model provides a realistic picture of the underlying mechanisms in the NRP discharge and can be used to identify its limitations and thus to suggest further improvements. Our model predicts that vibrational excitation is very important in the NRP discharge, explaining why this type of plasma yields energy-efficient CO 2 conversion. A significant part of the CO 2 dissociation occurs by electronic excitation from the lower vibrational levels toward repulsive electronic states, thus resulting in dissociation. However, vibration-translation (VT) relaxation (depopulating the higher vibrational levels) and CO + O recombination (CO + O + M → CO 2 + M), as well as mixing of the converted gas with fresh gas entering the plasma in between the pulses, are limiting factors for the conversion and energy efficiency. Our model predicts that extra cooling, slowing down the rate of VT relaxation and of the above recombination reaction, thus enhancing the contribution of the highest vibrational levels to the overall CO 2 dissociation, can further improve the performance of the NRP discharge for energy-efficient CO 2 conversion.
- Subjects :
- nanosecond discharges
02 engineering and technology
010402 general chemistry
Kinetic energy
01 natural sciences
Dissociation (chemistry)
Chemical kinetics
Specific energy
SDG 7 - Affordable and Clean Energy
Physical and Theoretical Chemistry
Chemistry
Physics
CO2 conversion
Plasma
Nanosecond
021001 nanoscience & nanotechnology
0104 chemical sciences
Surfaces, Coatings and Films
Electronic, Optical and Magnetic Materials
Afterglow
General Energy
Chemical physics
0210 nano-technology
Engineering sciences. Technology
SDG 7 – Betaalbare en schone energie
Excitation
Subjects
Details
- ISSN :
- 19327455 and 19327447
- Volume :
- 123
- Database :
- OpenAIRE
- Journal :
- The Journal of Physical Chemistry C
- Accession number :
- edsair.doi.dedup.....aa4aba94e4542dd6f3dfdd125b2f9bb5