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Development of Active and Stable Low Nickel Content Catalysts for Dry Reforming of Methane

2017-5-16, Ha, Quan Luu Manh, Armbruster, Udo, Atia, Hanan, Schneider, Matthias, Lund, Henrik, Agostini, Giovanni, Radnik, Jörg, Vuong, Huyen Thanh, Martin, Andreas

Methane dry reforming (DRM) was investigated over highly active Ni catalysts with low metal content (2.5 wt %) supported on Mg-Al mixed oxide. The aim was to minimize carbon deposition and metal sites agglomeration on the working catalyst which are known to cause catalyst deactivation. The solids were characterized using N2 adsorption, X-ray diffraction, temperature-programmed reduction, X-ray photoelectron spectroscopy, and UV-Vis diffuse reflectance spectroscopy. The results showed that MgO-Al2O3 solid solution phases are obtained when calcining Mg-Al hydrotalcite precursor in the temperature range of 550–800 °C. Such phases contribute to the high activity of catalysts with low Ni content even at low temperature (500 °C). Modifying the catalyst preparation with citric acid significantly slows the coking rate and reduces the size of large octahedrally coordinated NiO-like domains, which may easily agglomerate on the surface during DRM. The most effective Ni catalyst shows a stable DRM course over 60 h at high weight hourly space velocity with very low coke deposition. This is a promising result for considering such catalyst systems for further development of an industrial DRM technology.

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Nb-modified Ce/Ti oxide catalyst for the selective catalytic reduction of NO with NH3 at low temperature

2018, Mosrati, Jawaher, Atia, Hanan, Eckelt, Reinhard, Lund, Henrik, Agostini, Giovanni, Bentrup, Ursula, Rockstroh, Nils, Keller, Sonja, Armbruster, Udo, Mhamdi, Mourad

Recently, great attention has been paid to Ceria-based materials for selective catalytic reduction (SCR) with NH3 owing to their unique redox, oxygen storage, and acid-base properties. Two series of bimetallic catalysts issued from Titania modified by Ce and Nb were prepared by the one-step sol-gel method (SG) and by the sol-gel route followed by impregnation (WI). The resulting core-shell and bulk catalysts were tested in NH3-SCR of NOx. The impregnated Nb5/Ce40/Ti100 (WI) catalyst displayed 95% NOx conversion at 200 °C (GHSV = 60,000 mL·g−1·h−1, 1000 ppm NOx, 1000 ppm NH3, 5% O2/He) without forming N2O. The catalysts were characterized by various methods including ICP-OES, N2-physisorption, XRD, Raman, NH3-TPD, DRIFTS, XPS, and H2-TPR. The results showed that the introduction of Nb decreases the surface area and strengthens the surface acidity. This behavior can be explained by the strong interaction between Ceria and Titania which generates Ce-O-Ti units, as well as a high concentration of amorphous or highly dispersed Niobia. This should be the reason for the excellent performance of the catalyst prepared by the sol-gel method followed by impregnation. Furthermore, Nb5/Ce40/Ti100 (WI) has the largest NH3 adsorption capacity, which is helpful to promote the NH3-SCR reaction. The long-term stability and the effect of H2O on the catalysts were also evaluated.