How reduction temperature influences the structure of perovskite-oxide catalysts during the dry reforming of methane†

Abstract

Dry reforming of methane is a promising reaction to convert CO₂ and combat climate change. However, the reaction is still not feasible in large-scale industrial applications. The thermodynamic need for high temperatures and the potential of carbon deposition leads to high requirements for potential catalyst materials. As shown in previous publications, the Ni-doped perovskite-oxide Nd_0.6Ca_0.4Fe_0.97Ni_0.03O₃ is a potential candidate as it can exsolve highly active Ni nanoparticles on its surface. This study focused on controlling the particle size by varying the reduction temperature. We found the optimal temperature that allows the Ni nanoparticles to exsolve while not yet enabling the formation of deactivating CaCO₃. Furthermore, the exsolution process and the behaviour of the phases during the dry reforming of methane were investigated using in situ XRD measurements at the DESY beamline P02.1 at PETRA III in Hamburg. They revealed that the formed deactivated phases would, at high temperatures, form a brownmillerite phase, thus hinting at a potential self-healing mechanism of these materials.