Methane pyrolysis for hydrogen production: Modeling of soot deposition by computational fluid dynamics and experimental validation

Abstract

Methane pyrolysis is an attractive technology to reduce greenhouse gas emissions, since the carbonaceous part of the hydrocarbon is captured into a solid, easier to store than carbon dioxide. In this framework, computational fluid dynamics (CFD) is an excellent tool to simulate the catalyst deactivation and the complex phenomena arising on the carbon surface. We investigated thermal and catalytical pyrolysis of methane in a tubular quartz reactor with an internal diameter of 3.8cm. We modeled soot deposition and added a new surface mass balance that parametrize bed porosity as time-dependent variable. Our model predicts occlusion (clogging) time for empty and packed bed reactor: operating at 1373 K, an empty bed clogs in 15 d, which is coherent with industrial operations. The model well predicts methane conversion in the empty reactor even after 24h time on stream. When a packed bed is used, the experimental conversion follow the predicted activity decay, with deviations due to the size distribution of the carbon during experiments. Radiation is the main heat transfer mechanism (86% of the total heat absorbed by the system), compared to the others involved in this system, i.e., conduction, which is more than 50 times smaller, natural convection, more than 18 times smaller, and forced convection, more than 300 times smaller.