Preparation of tailor-made supported catalysts using asymmetric flow field flow fractionation and their application in hydrogenation

Abstract

AbstractThe optical, chemical, and catalytic properties of metallic nanoparticles (NPs) depend strongly on their particle size and shape. Therefore, the preparation of monodisperse metallic NPs is very important for fundamental studies and practical applications. However, the isolation of the different structures by separation from a polydisperse sample, especially in the size range below 10 nm, is not well applied so far. Here, the asymmetric flow field flow fractionation (AF4) is adapted for the preparative separation of the Pd NPs regarding their size and shape in the sub-10-nm size range. To prove the efficiency of the applied method, small-angle X-ray scattering (SAXS) and high-resolution transmission electron microscopy (TEM) were utilized to determine the particle size distribution at different stages of the separation process. A major benefit of this method compared to most of the other separation techniques, the removal of impurities during the separation process, was proven by proton nuclear magnetic resonance (NMR). The obtained results demonstrate that the AF4 is well suited for the rapid preparation of the purified uniform precious metal NPs at the applied size range. Single fractions of the different-sized and -shaped Pd NPs were deposited on titania (TiO2) and tested in the catalytic hydrogenation of 2,5 hydroxymethylfurfural (HMF) in aqueous solution under mild conditions. While the spherical-shaped particles show a high activity, the separated agglomerated particles show a higher selectivity to the desired products.