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Global Pathway Selection/Analysis (GPSA) algorithm helps in analyzing the chemical kinetics of complex combustion systems by identifying important global reaction pathways that connects a source and a sink species. The present work aims to extend the application of GPSA to plasma assisted combustion systems in order to identify the dominant global pathways that govern the plasma and combustion kinetics at various conditions. The reaction cycles involving the excitation of nitrogen to its vibrational and electronic states and the subsequent de-excitation to its ground state are found to control the reactivity of plasma assisted systems. Provisions are made in the GPSA algorithm to capture the dominant reaction pathways and cycles of plasma assisted combustion (i.e., p-GPSA). Further, the analysis of plasma assisted ammonia combustion are presented as an example, which includes the results obtained using both the traditional path flux analysis and p-GPSA. The dominant pathways for the plasma assisted combustion of ammonia are identified along with the dominant excitation--de-excitation loops and their importance are ascertained and verified using path flux analysis.
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Plasma-based global pathway analysis to understand the chemical kinetics of plasma-assisted combustion and fuel reforming
The Global Pathway Analysis (GPA) algorithm helps analyze the chemical kinetics of complex combustion systems by identifying important global reaction pathways connecting a source species to a sink species through various important intermediate species (i.e., hub species). The present work aims to extend GPA algorithm to plasma-assisted combustion and fuel reforming systems to identify the dominant global pathways in such systems at various conditions. In addition, the present study extends the ability of GPA algorithm to identify reaction cycles involving the excitation of high-concentration species (e.g., O2, N2, and fuel) to their vibrational and electronic states and the subsequent de-excitation to their ground state, based on their significance on the reactivity of plasma-assisted systems in terms of gas heating and radical production. Provisions are made in the GPA algorithm to evaluate the reactivity of identified reaction pathways and cycles based on the element-flux transfer (i.e., dominance), heat release, and radical production rate. The newly developed Plasma-based Global Pathway Analysis (PGPA) algorithm is then used to analyze the plasma-assisted combustion of ammonia and reforming of methane. The PGPA analyses elucidated the significance of vibrational-translational cycles on the reactivity of NH3/air mixtures. Further, analyses on the production of NO ascribed the early reforming of NH3 to N2 and H2 in impeding the production of NO during plasma-assisted NH3 ignition. Lastly, the enhanced reforming of CH4/N2 mixtures using plasma has been attributed to electron impact dissociation of CH4 when compared to thermal reforming. In contrast, conventional path-Flux analysis (PFA) was found to require significant manual effort and pre-analysis intuitions from expert knowledge, making it arduous to provide valuable insights into plasma chemistry. The user-friendly and automated nature of PGPA thus provides a valuable tool for assessing the kinetics of plasma-assisted systems helpful in analyzing and, further, a foundation in reducing plasma-assisted chemistry, without the needs of expert knowledge.
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- Award ID(s):
- 2002635
- PAR ID:
- 10481922
- Editor(s):
- Pepiot, Perrine
- Publisher / Repository:
- Elsevier
- Date Published:
- Journal Name:
- Combustion and Flame
- Volume:
- 255
- Issue:
- C
- ISSN:
- 0010-2180
- Page Range / eLocation ID:
- 112927
- Subject(s) / Keyword(s):
- Global pathway analysis (GPA) Plasma assisted combustion (PAC) Fuel reforming Ammonia combustion Methane reforming Global reaction pathways
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1016/j.combustflame.2023.112927
