Experimental and Theoretical Study of the Mechanism of Chain Propagation in the Process of Thermal Gas-Phase Oxidation of Methane
E. M. Makaryan, S. D. Arsentyev, M. Dzh. Pogosyan
Nalbandyan Institute of Chemical Physics, National Academy of Sciences of Armenia, Yerevan, Armenia
Keywords: chain reactions, methane oxidation, peroxide radicals
Abstract
The mechanism of chain development during thermal gas-phase oxidation of methane was studied experimentally and theoretically. It was found that the rate-limiting step, which determines the overall process development, depends on the conditions. At a temperature of 728 K, the process is determined by the interaction of peroxide radicals with each other. Increasing the temperature to 873 K leads to an increased role for the reactions of peroxide radicals with formaldehyde, after which the rate-limiting step becomes the interaction of peroxide radicals with methane. Furthermore, changes in pressure and temperature have an equal effect on the concentration ratio of hydroperoxide and methylperoxide radicals, determined both by calculation and experiment.
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