Carbon-Supported Copper for Gas-Phase Hydrogenation Catalysis

Abstract

Fundamental studies in catalysis rely on well-defined catalyst materials and reactions. In this thesis we focused on the synthesis, characterization and performance of carbon-supported Cu-based materials in hydrogenation catalysis. The main aim was to investigate the effects of the Cu nanoparticle size, support interactions and metal oxide promotion, on the catalytic performance in three industrially-relevant gas-phase hydrogenation reactions, namely methanol synthesis by hydrogenation of CO and CO2, selective hydrogenation of butadiene in excess of propene, and hydrogenation of ethyl acetate to ethanol, a new reaction in our research group. In summary, the physicochemical phenomena involved in catalyst assembly were investigated on the nanometer scale for a series of carbon-supported Cu catalysts, which allowed us to prepare model catalysts with tailored structures. The work presented in this thesis showed that disentangling the effects of Cu particle size, supports and promoters, facilitated the establishment of structure-performance relationships in three important hydrogenation reactions. The advanced understanding of these relationships may assist in developing more active, selective and stable Cu-based hydrogenation catalysts, which may ultimately contribute to more efficient use of energy and materials resources.