SiC-based structured catalysts for a high-efficiency electrified dry reforming of methane

Abstract

The process of dry reforming of methane (DRM) can allow the conversion of methane and carbon dioxide, the two main greenhouse gases (GHG), into syngas which can be either used as feedstock for chemicals production or it can undergo through separation step for H2 recovery. However, the heat required for the reaction is obtained by combustion of fossil fuels, so CO2 footprint of the process is significant. Another problematic aspect of the process concerns the heat transfer to the catalytic volume: for allowing the catalytic bed to reach and maintain the reaction temperature, the heating medium outside the tubes containing the catalyst must have a temperature higher than 1000 °C. A process intensification could be performed by combining two innovative technologies: (i) the use of electrification for the energy supply (microwave heating and direct electrification) and (ii) the adoption of structured catalysts with high thermal conductivity.This work proposed the study of electrified DRM process using two Ni-based structured catalysts prepared starting by different carriers, a Silicon carbide (SiC) honeycomb monolith and a Si–SiC open-cell foam. The electrification of the DRM process has been realized by using either microwave heating or electrification through Joule (or ohmic) heating, and the experimental tests have been performed at different space velocity values. The configuration of the carriers has been carefully chosen in order to enhance the heat and mass transport phenomena, allowing to assure a flat temperature profile along the entire catalytic bed.The results have shown that the SiC monolith is more suitable than the Si–SiC foam for a microwave-assisted catalytic test. In fact, the higher fraction of void in the foam determines a lower heat absorption, and a consequently higher energy consumption (8.29 kWh/Nm3 H2 and 4.2 kWh/Nm3 H2, for the foam and the monolith respectively). Moreover, the monolith-based catalyst approached the thermodynamic equilibrium values in terms of CH4 conversion in all the investigated temperature range, while in the same tests the foam-based catalyst reached these values only at the higher temperatures. Conversely, the foam-based catalyst has shown the best performance in the electrification tests through Joule heating: the CH4 conversion approached the equilibrium values in the investigated temperature range and, more important, the energy consumption value was of 2.6 kWh/Nm3 H2, very close to the theoretical one (1.90 kWh/Nm3 H2) and equal to about ¼ of that obtained with microwaves.