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Abstract <p>A detailed kinetic model based on the NUI Galway mechanism for light hydrocarbon oxidation was used to investigate the effects of pressure on the non-catalytic conversion of methane in various gas atmospheres (Ar, H<sub>2</sub>, CO, CO<sub>2</sub>, H<sub>2</sub>O). The study also evaluated the impact of H<sub>2</sub>O addition on the conversion of CH<sub>4</sub> in mixtures with H<sub>2</sub> and CO. For CH<sub>4</sub> mixed with Ar, CO, or H<sub>2</sub>, the methane pyrolysis rate exhibits a power-law dependence on pressure (<i>W</i> = <i>AP</i><sup><i>n</i></sup>), with the exponent <i>n</i> ranging from ~0.4 to ~0.65 in the 1400–1800 K temperature range. The achievable CH<sub>4</sub> conversion decreases significantly with rising pressure, particularly for CH<sub>4</sub>–H<sub>2</sub> mixtures. For the non-catalytic conversion of CH<sub>4</sub> in mixtures with H<sub>2</sub>O and CO<sub>2</sub>, the initial pyrolysis rate is similar to that in an argon atmosphere. At high pressures, however, the CH<sub>4</sub> concentration profile subsequently passes through a rising region. This is attributed to the interaction of C<sub>2</sub>H<sub>2</sub> and CO products with H<sub>2</sub>O, which generates additional H<sub>2</sub> and consequently shifts the equilibrium of the reaction system (2CH<sub>4</sub> ↔ C<sub>2</sub>H<sub>4</sub> + 2H<sub>2</sub> ↔ C<sub>2</sub>H<sub>2</sub> + H<sub>2</sub>) to the left.</p>

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Effects of Pressure on the Non-Catalytic Thermal Conversion of Methane in Various Gases

  • 期刊论文

  • 发表日期：

    2025年12月1日

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  • V. I. Savchenko,
  • A. V. Ozerskii,
  • E. Busillo,
  • A. V. Nikitin,
  • I. V. Sedov,
  • V. S. Arutyunov

摘要

Abstract

A detailed kinetic model based on the NUI Galway mechanism for light hydrocarbon oxidation was used to investigate the effects of pressure on the non-catalytic conversion of methane in various gas atmospheres (Ar, H2, CO, CO2, H2O). The study also evaluated the impact of H2O addition on the conversion of CH4 in mixtures with H2 and CO. For CH4 mixed with Ar, CO, or H2, the methane pyrolysis rate exhibits a power-law dependence on pressure (W = APn), with the exponent n ranging from ~0.4 to ~0.65 in the 1400–1800 K temperature range. The achievable CH4 conversion decreases significantly with rising pressure, particularly for CH4–H2 mixtures. For the non-catalytic conversion of CH4 in mixtures with H2O and CO2, the initial pyrolysis rate is similar to that in an argon atmosphere. At high pressures, however, the CH4 concentration profile subsequently passes through a rising region. This is attributed to the interaction of C2H2 and CO products with H2O, which generates additional H2 and consequently shifts the equilibrium of the reaction system (2CH4 ↔ C2H4 + 2H2 ↔ C2H2 + H2) to the left.