Using natural gas and sustainable biogas as feed, high-temperature pyrolysis represents a potential technology for large-scale hydrogen production and simultaneous carbon capture. Further utilization of solid carbon accruing during the process (i. e., in battery industry or for metallurgy) increases the process's economic chances. This study demonstrated the feasibility of gas-phase methane pyrolysis for hydrogen production and carbon capture in an electrically heated high-temperature reactor operated between 1200 and 1600 °C under industrially relevant conditions. While hydrogen addition controlled methane conversion and suppressed the formation of undesired byproducts, an increasing residence time decreased the amount of byproducts and benefited high hydrogen yields. A temperature of 1400 °C ensured almost full methane conversion, moderate byproduct formation, and high hydrogen yield. A reaction flow analysis of the gas-phase kinetics revealed acetylene, ethylene, and benzene as the main intermediate products and precursors of carbon formation.
Keywords: carbon capture; decarbonization; gas-phase chemistry; hydrogen production; methane pyrolysis.
© 2022 The Authors. ChemSusChem published by Wiley-VCH GmbH.