SINGLE-ATOM CATALYSTS SUPPORTED ON POLYOXOMETALATES – APPLICATIONS, SPECTROSCOPIC AND SPECTROMETRIC STUDIES

Abstract

In this thesis, the synthesis of single-atom catalysts supported on polyoxometalates as support with molecular precision is described. We employed those catalysts for different oxidation reactions (CO and benzyl alcohol oxidation) and the hydrogenation of different substrates (nitrobenzene and vinyl acetate among others) and we were able elucidated the mechanism of most of those reactions. This was done by means of in situ spectroscopy (XAS, XPS, IR, Raman, etc.) as well as mass spectrometry (ESI-MS). We demonstrate the power of model single-atom catalysts for the identification of reaction mechanisms and rate-determining steps as well as for the determination of scaling relations with the potential to even identify phenomena outside of the realm of single-atom catalysts. Besides serving as model systems, we found some of our catalysts to show extraordinary activity in the hydrodeoxygenation of various biomass-derived substrates, outperforming commercial and previously reported catalysts.