The connectivity and thermal stability of pores in heterogeneous, mesoporous metal oxide catalysts are key properties controlling their (long-term) efficacy. In this study, we investigate the influence of pH and temperature during a common hydrothermal aftertreatment step in the synthesis of mesoporous CeZrYLaO oxides obtained from molecular precursors via hydrothermal synthesis. This study has a strong focus on the methodological approach, elucidating whether and how even the smallest changes in morphology and connectivity may be unraveled and related to the underlying chemical processes to uncover key parameters for the ongoing improvement of material properties.
View Article and Find Full Text PDFPore size and pore connectivity control diffusion-based transport in mesopores, a crucial property governing the performance of heterogeneous catalysts. In many cases, transition-metal oxide catalyst materials are prepared from molecular precursors involving hydrothermal treatment followed by heat treatment. Here, we investigate the effects of such a hydrothermal aftertreatment step, using an aqueous ammonia solution, on the disordered mesopore network of CeZrYLaO mixed oxides.
View Article and Find Full Text PDFHere, we present a study of the development of the micro- and mesoporosity of a CeZrYLaO oxygen storage material upon treatment at temperatures up to 1050 °C. The investigated powder, obtained from nitrate-based metal oxide precursors in a specially developed hydrothermal synthesis, is highly crystalline, features a high surface area and does not show phase segregation at high temperatures. By employing an advanced methodology, consisting of state-of-the-art argon physisorption, thermogravimetric analysis coupled with mass spectrometry (TG-MS) and X-ray powder diffraction (XRD) along with Raman spectroscopy, we correlate the stability of the mesopore system to the presence of surface-bound nitrate groups introduced during synthesis, which prevent sintering up to a temperature of 600 °C.
View Article and Find Full Text PDFPorous carrier materials functionalized with organocatalysts offer substantial advantages compared to homogeneous catalysts, e.g., easy separation of the catalyst, scalability, and an improved implementation in continuous operations.
View Article and Find Full Text PDF