The
autoignition and oxidation behavior of CH4/H2S mixtures has been studied experimentally in a rapid compression
machine (RCM) and a high-pressure flow reactor. The RCM measurements
show that the addition of 1% H2S to methane reduces the
autoignition delay time by a factor of 2 at pressures ranging from
30 to 80 bar and temperatures from 930 to 1050 K. The flow reactor
experiments performed at 50 bar show that, for stoichiometric conditions,
a large fraction of H2S is already consumed at 600 K, while
temperatures above 750 K are needed to oxidize 10% methane. A detailed
chemical kinetic model has been established, describing the oxidation
of CH4 and H2S as well as the formation and
consumption of organosulfuric species. Computations with the model
show good agreement with the ignition measurements, provided that
reactions of H2S and SH with peroxides (HO2 and
CH3OO) are constrained. A comparison of the flow reactor
data to modeling predictions shows satisfactory agreement under stoichiometric
conditions, while at very reducing conditions, the model underestimates
the consumption of both H2S and CH4. Similar
to the RCM experiments, the presence of H2S is predicted
to promote oxidation of methane. Analysis of the calculations indicates
a significant interaction between the oxidation chemistry of H2S and CH4, but this chemistry is not well understood
at present. More work is desirable on the reactions of H2S and SH with peroxides (HO2 and CH3OO) and
the formation and consumption of organosulfuric compounds.
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