PRODUCTION, CONSOLIDATION, SINTERING, AND STABILITY OF NOVEL NANO-CRYSTALLINE ZIRCONIA CATALYST SUPPORT POWDERS

摘要

Nano-crystalline, zirconium oxide/oxyhydroxide particulates were produced using a novel, continuous, flow-through hydrothermal technology developed at the Pacific Northwest National Laboratory. Homogeneous aqueous solutions containing ZrO(NO_3)_2 and urea were pumped at pressures of 6000-8000 psi through a heated stainless steel reaction tube at 340-350°C. Flow at pressure was maintained using a nozzle at the down-stream end of the reaction tube. In this process, termed Rapid Thermal Decomposition of precursors in Solution (RTDS), the formation of zirconium oxide/oxyhydroxide nano-crystals (diameters of generally less than 15-nm) occurred during the solution's brief residence time (<15 seconds) in the reaction tube, yielding aqueous slurries of agglomerated particulates. Powders were separated from these slurries, washed, then dried. RTDS powder prepared from 0.3M ZrO(NO_3)_2 and 0.6M urea were mixed with binder and formed into pellets using a commercial screw extruder. These extrudates were subsequently sintered at 500°C, yielding zirconia catalyst support pellets with a measured surface area of 113 m~2/g. After application of 3% ruthenium metal to the sintered RTDS zirconia extrudates, the resulting catalyst was evaluated for catalytic activity using the hydrothermal hydrogenation of the sugar xylose to xylitol as a model reaction. After 3 hours at 140°C, the RTDS catalyst exhibited useful activity with 92% conversion and 66% selectivity to xylitol formation.