In this work novel Cu/ZrO2/CeO2Â materials prepared by co-precipitation and polymer templating have been investigated as catalysts in the steam reforming of methanol. Catalytic measurements were performed under continuous operation in a fixed bed reactor at atmospheric pressure. Experiments performed indicated that an initial period of deactivation in CZC samples with Cu contents exceeding 5% were stabilized and therefore such samples are recommended for prolonged catalytic applications. An increase in the Cu content from 5 to 15% was found to improve the long-term stability and suppress the CO production considerably, whereas the effect of a further enhancement was less significant. With respect to a reduced formation of CO during SRM, the samples with increased Cu loadings proved to be more efficient catalysts. A kinetic analysis of the catalysts was undertaken as a result of insignificant effect of mass transport on the catalytic reaction. The reaction scheme suggested for the overall transformation included the SRM, MD and RWGS reactions. In addition, the experimental data obtained in the range 503-573 K could be well fitted by the kinetic model employed.
The optimal temperature range for SRM on the CZC catalysts was 523-543 K, for which high methanol conversions and low carbon dioxide levels were obtained. For the SRM and RWGS reactions, the values of the activation energies were comparable and considerably lower than that of MD. The activation energy of each individual reaction exhibited a systematic decrease with an increasing Cu content of the catalyst. Evidently, the variation in the Cu concentration of the precursor material during preparation altered the microstructure of the Cu particles and, thus the active Cu surface, which considerably affected the catalytic behavior of the CZC catalysts.
Pellets of Zirconium oxynitride were isostatically pressed commercial Zirconia powder prepared at 1900Â°C in nitrogen atmosphere for 2 h in graphite heated resistance furnace. This resulted in a mixture of nitrogen-free monoclinic and beta-type Zirconium oxynitride phases. The resultant material was subsequently quenched from a vertical tube furnace from 1300Â°C (nitrogen atmosphere) in water. The X-ray analysis after quenching shows a reduced amount of monoclinic zirconia and metastable beta-phase of zirconium oxynitride (~Zr7O11N2). Samples containing 51 wt-% ZrO2 and 49 wt-% beta-phase were utilized during the analysis of the catalyst. Hot gas extraction of the as-prepared material yielded a total amount of nitrogen of 1.63 wt-% (theoretical 1.62 wt-%). A minor amount of nitrogen resulted after three month of ammonia decomposition.
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