Ammonia synthesis activity was improved by high crystallinity CeO2 covered by low crystallinity CeO2. However, too much low crystallinity CeO2 affects ammonia synthesis negatively.
Abstract
Ruthenium (Ru) catalysts supported on cerium oxide (CeO2), which was composed of high crystallinity (HC) CeO2 covered by low crystallinity (LC) CeO2 were investigated. The ammonia synthesis activities of a series of Ru/CeO2(LC)/CeO2(HC), having different LC/HC ratios were evaluated, and various characterizations, such as N2 adsorption, X-ray diffraction, hydrogen temperature-programmed reduction (H2-TPR), and hydrogen temperature-programmed desorption (H2-TPD), were performed. Ru/CeO2(LC)/CeO2(HC) (0.1) demonstrated higher activity. H2-TPR revealed that H2 consumption increased as the LC/HC ratio increased. This indicates that the larger the amount of low crystallinity CeO2, the higher the reducibility. However, the results of H2-TPD imply that the larger the amount of low crystallinity CeO2, the higher the interaction between adsorbed H2 and the catalyst surface. These results indicate that the balance of reducibility and hydrogen adsorption strength plays an important role in increasing the ammonia synthesis activity.