Regeneration of copper catalysts mediated by molybdenum-based oxides

Abstract

Cu catalysts, known for their unparalleled catalytic capabilities due to their unique electronic structure, have faced inherent challenges in maintaining long-term effectiveness under harsh hydrogenation conditions. Here, we demonstrate a molybdenum-mediated redispersion behavior of Cu under high-temperature oxidation conditions. The oxidized Cu nanoparticles with rich metal-support interfaces tend to dissolve into the MoO3 support upon heating to 600 °C, which facilitates the subsequent regeneration in a reducing atmosphere. A similar redispersion phenomenon is observed for Cu nanoparticles supported on ZnO-modified MoO3. The modification of ZnO significantly improves the performance of the Cu catalyst for CO2 hydrogenation to methanol, with the high activity being well maintained after four repeated oxidation-reduction cycles. In situ spectroscopic and theoretical analyses suggest that the interaction involved in the formation of the copper molybdate-like compound is the driving force for the redispersion of Cu. This method is applicable to various Mo-based oxide supports, offering a practical strategy for the regeneration of sintered Cu particles in hydrogenation applications.