The influence of the main process
parameters on the oscillatory
behavior of methane oxidation was analyzed in conditions relevant
for low-temperature combustion processes. The investigation was performed
by means of direct comparisons between experimental measurements realized
in two jet-stirred flow reactors used at atmospheric pressure. With
the operating conditions of the two systems coupled, wide ranges of
the inlet temperature (790–1225 K), equivalence ratio (0.5
< Φ < 1.5), methane mole fraction (X
CH4
from 0.01 to 0.05), bath gases (i.e., He, N2, CO2, or H2O) and different overall
mixture dilution levels were exploited in relation to the identification
of oscillatory regimes. Although the reference systems mainly differ
in thermal conditions (i.e., heat exchange to the surroundings), temperature
measurements suggested that the oscillatory phenomena occurred when
the system working temperature accessed a well-identifiable temperature
range. Experimental results were simulated by means of a detailed
kinetic scheme and commercial codes developed for complex chemistry
processes. Simulations were also extended considering systems with
different heat losses to the surroundings, thus passing from adiabatic
to isothermal systems. Results highlighted the kinetic nature of the
dynamic behavior. Because predictions were consistent with experimental
tests, further numerical analyses were realized to identify the kinetics
responsible for the establishment of oscillatory phenomena. Temperature
oscillations were predicted for a significant reactor working temperature
range, where oxidation and recombination kinetic routes, involving
carbon C1–2 species as well as reactions of the
H2/O2 sub-scheme, become competitive, thus boosting
limit cycle behaviors. Oscillatory phenomena cease when the system
working temperatures exceed characteristic threshold values with the
promotion of faster oxidation routes that diminish the inhibiting
effects of recombination reactions.