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The role of chemistry in the oscillating combustion of hydrocarbons : an experimental and theoretical study

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Abstract
The stable operation of low-temperature combustion processes is an open challenge, due to the presence of undesired deviations from steady-state conditions: among them, oscillatory behaviors have been raising significant interest. In this work, the establishment of limit cycles during the combustion of hydrocarbons in a wellstirred reactor was analyzed to investigate the role of chemistry in such phenomena. An experimental investigation of methane oxidation in dilute conditions was carried out, thus creating quasi-isothermal conditions and decoupling kinetic effects from thermal ones. The transient evolution of the mole fractions of the major species was obtained for different dilution levels (0.0025 <= X-CH4 <= 0.025), inlet temperatures (1080K <= T <= 1190K) and equivalence ratios (0.75 <= Phi <= 1). Rate of production analysis and sensitivity analysis on a fundamental kinetic model allowed to identify the role of the dominating recombination reactions, first driving ignition, then causing extinction. A bifurcation analysis provided further insight in the major role of these reactions for the reactor stability. One-parameter continuation allowed to identify a temperature range where a single, unstable solution exists, and where oscillations were actually observed. Multiple unstable states were identified below the upper branch, where the stable (cold) solution is preferred. The role of recombination reactions in determining the width of the unstable region could be captured, and bifurcation analysis showed that, by decreasing their strength, the unstable range was progressively reduced, up to the full disappearance of oscillations. This affected also the oxidation of heavier hydrocarbons, like ethylene. Finally, less dilute conditions were analyzed using propane as fuel: the coupling with heat exchange resulted in multiple Hopf Bifurcations, with the consequent formation of intermediate, stable regions within the instability range in agreement with the experimental observations.
Keywords
Industrial and Manufacturing Engineering, General Chemistry, General Chemical Engineering, Environmental Chemistry, Low-temperature combustion, Oscillations, Bifurcation, Reactor stability, Methane, PERFECTLY STIRRED REACTORS, METHANE MILD COMBUSTION, OPEN SYSTEM, BIFURCATION-ANALYSIS, PROPANE OXIDATION, DYNAMIC-BEHAVIOR, STEADY-STATE, IGNITION, HYDROGEN, REDUCTION

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Citation

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MLA
Stagni, Alessandro, et al. “The Role of Chemistry in the Oscillating Combustion of Hydrocarbons : An Experimental and Theoretical Study.” CHEMICAL ENGINEERING JOURNAL, vol. 385, 2020.
APA
Stagni, A., Song, Y., Vandewalle, L., Van Geem, K., Marin, G., Herbinet, O., … Faravelli, T. (2020). The role of chemistry in the oscillating combustion of hydrocarbons : an experimental and theoretical study. CHEMICAL ENGINEERING JOURNAL, 385.
Chicago author-date
Stagni, Alessandro, Yu Song, Laurien Vandewalle, Kevin Van Geem, Guy Marin, Olivier Herbinet, Frédérique Battin-Leclerc, and Tiziano Faravelli. 2020. “The Role of Chemistry in the Oscillating Combustion of Hydrocarbons : An Experimental and Theoretical Study.” CHEMICAL ENGINEERING JOURNAL 385.
Chicago author-date (all authors)
Stagni, Alessandro, Yu Song, Laurien Vandewalle, Kevin Van Geem, Guy Marin, Olivier Herbinet, Frédérique Battin-Leclerc, and Tiziano Faravelli. 2020. “The Role of Chemistry in the Oscillating Combustion of Hydrocarbons : An Experimental and Theoretical Study.” CHEMICAL ENGINEERING JOURNAL 385.
Vancouver
1.
Stagni A, Song Y, Vandewalle L, Van Geem K, Marin G, Herbinet O, et al. The role of chemistry in the oscillating combustion of hydrocarbons : an experimental and theoretical study. CHEMICAL ENGINEERING JOURNAL. 2020;385.
IEEE
[1]
A. Stagni et al., “The role of chemistry in the oscillating combustion of hydrocarbons : an experimental and theoretical study,” CHEMICAL ENGINEERING JOURNAL, vol. 385, 2020.
@article{8644547,
  abstract     = {The stable operation of low-temperature combustion processes is an open challenge, due to the presence of undesired deviations from steady-state conditions: among them, oscillatory behaviors have been raising significant interest. In this work, the establishment of limit cycles during the combustion of hydrocarbons in a wellstirred reactor was analyzed to investigate the role of chemistry in such phenomena. An experimental investigation of methane oxidation in dilute conditions was carried out, thus creating quasi-isothermal conditions and decoupling kinetic effects from thermal ones. The transient evolution of the mole fractions of the major species was obtained for different dilution levels (0.0025 <= X-CH4 <= 0.025), inlet temperatures (1080K <= T <= 1190K) and equivalence ratios (0.75 <= Phi <= 1). Rate of production analysis and sensitivity analysis on a fundamental kinetic model allowed to identify the role of the dominating recombination reactions, first driving ignition, then causing extinction.

A bifurcation analysis provided further insight in the major role of these reactions for the reactor stability. One-parameter continuation allowed to identify a temperature range where a single, unstable solution exists, and where oscillations were actually observed. Multiple unstable states were identified below the upper branch, where the stable (cold) solution is preferred. The role of recombination reactions in determining the width of the unstable region could be captured, and bifurcation analysis showed that, by decreasing their strength, the unstable range was progressively reduced, up to the full disappearance of oscillations. This affected also the oxidation of heavier hydrocarbons, like ethylene. Finally, less dilute conditions were analyzed using propane as fuel: the coupling with heat exchange resulted in multiple Hopf Bifurcations, with the consequent formation of intermediate, stable regions within the instability range in agreement with the experimental observations.},
  articleno    = {123401},
  author       = {Stagni, Alessandro and Song, Yu and Vandewalle, Laurien and Van Geem, Kevin and Marin, Guy and Herbinet, Olivier and Battin-Leclerc, Frédérique and Faravelli, Tiziano},
  issn         = {1385-8947},
  journal      = {CHEMICAL ENGINEERING JOURNAL},
  keywords     = {Industrial and Manufacturing Engineering,General Chemistry,General Chemical Engineering,Environmental Chemistry,Low-temperature combustion,Oscillations,Bifurcation,Reactor stability,Methane,PERFECTLY STIRRED REACTORS,METHANE MILD COMBUSTION,OPEN SYSTEM,BIFURCATION-ANALYSIS,PROPANE OXIDATION,DYNAMIC-BEHAVIOR,STEADY-STATE,IGNITION,HYDROGEN,REDUCTION},
  language     = {eng},
  pages        = {14},
  title        = {The role of chemistry in the oscillating combustion of hydrocarbons : an experimental and theoretical study},
  url          = {http://dx.doi.org/10.1016/j.cej.2019.123401},
  volume       = {385},
  year         = {2020},
}

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