Methane pyrolysis is a promising bridging technology to mitigate the effects of climate change. By decarbonizing natural gas, hydrogen can be produced from fossil fuels without creating CO2 emissions. The focus of future process optimization should not only be on the hydrogen yield and the energy efficiency but also on the carbon products and possible byproduct formation. During methane pyrolysis in a liquid metal (LM) bubble column reactor, at least two very distinct types of carbon are synthesized: soot particles and graphene‐like carbon sheets. A model is presented that couples a description of bubble dynamics in a LM bubble column reactor with a kinetic mechanism, originally developed for the combustion of natural gas that includes byproduct and soot formation. The model is validated by comparing it with an experimental dataset that covers a broad range of process conditions and the implications for carbon and byproduct formation are discussed. The good agreement of model results and experimental data shows that the combustion kinetic mechanism may be applied to methane pyrolysis and that the selected way of modeling bubble fluid dynamics in LM results in a good estimation of the actual bubble residence time in the optically nonaccessible liquid.

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Übersetzung wird gemeinsam mit der endgültigen englischen Fassung erscheinen. Die endgültige englische Fassung (Version of Record) wird ehestmöglich nach dem Redigieren und einem Korrekturgang als Early-View-Beitrag erscheinen und kann sich naturgemäß von der AA-Fassung unterscheiden. Leser sollten daher die endgültige Fassung, sobald sie veröffentlicht ist, verwenden. Für die AA-Fassung trägt der Autor die alleinige Verantwortung.

This contribution presents the results of continued investigations on the production of hydrogen by means of pyrolysis in a liquid metal bubble column reactor, as developed at the Karlsruhe Institute of Technology in recent years. Part I of this contribution described the motivation and the methodology of this study, as well as a significant scale-up, and discussed its results for pure methane pyrolysis. Here in part II, two additional experimental campaigns with methane–ethane mixtures (MEMs) and high-calorific natural gas (nGH) will be presented and discussed for the first time, using the up-scaled liquid metal bubble column reactor. It could be proven that an MEM as the feed gas led to an increase in methane conversion at low temperatures, which is consistent with the literature data. The nGH pyrolysis confirms this trend and also results in a significant rise in methane conversion compared to pure methane pyrolysis. Furthermore, the nGH pyrolysis leads to an increased methane conversion even at higher temperatures compared to MEM pyrolysis. Additionally, both MEM and nGH pyrolysis also showed a shift in the formation of by-products toward lower temperatures.

Hydrogen is not only an important industrial chemical but also an energy carrier with increasing demand. However, the current production techniques are based on technologies that result in massive CO2 emissions. In contrast, the pyrolysis of alkanes in a liquid metal bubble column reactor does not lead to direct CO2 emissions. In order to transfer this technology from lab-scale to industrial applications, it has to be scaled up and the influences of the most common constituent of natural gas on the pyrolysis process have to be determined. For this study, the liquid metal bubble column technology developed at the KIT was scaled up by a factor of 3.75, referred to as the reactor volume. In this article, the experimental setup containing the reactor is described in detail. In addition, new methods for the evaluation of experimental data will be presented. The reactor, as well as the experimental results from pure methane pyrolysis (PM), will be compared to the previous generation of reactors in terms of methane conversion. It could be proven that scaling up the reactor volume did not result in a decrease in methane conversion. For part II of this publication, methane-ethane (MEM) gas mixtures and high calorific natural gas (nGH) were pyrolyzed, and the results were discussed on the basis of the present part I.