We investigated the interactions between nickel oxide and silica–alumina supports, which were applied to the catalytic oligomerization of ethylene by powder X-ray diffraction, UV diffuse reflectance spectroscopy, H2 temperature-programmed reduction, and X-ray photoelectron spectroscopy. The catalytic activity was also correlated with the acidity of catalysts determined by NH3 temperature-programmed desorption and pyridine FT-IR spectroscopy. Although all the catalysts had similar Ni contents, their catalytic performances were strongly influenced by the strength of the metal oxide–support interaction. Strong interaction promoted the formation of nickel aluminate on the catalyst surface, and resulted in low catalytic activity due to reducing the amount of nickel oxide active sites. However, weak interaction favored the aggregation of nickel oxide species into larger particles, and thus resulted in low ethylene conversion and selectivity to oligomers. Eventually, the optimal activity was realized at the medium interaction strength, preserving a high amount of both active nickel oxides and acid sites.
High surface area (>170 m2 g−1) molybdenum nitride was prepared by the temperature-programmed nitridation of α-MoO3 with pure ammonia. The process was optimized by adjusting the experimental variables: the reaction temperature, heating rate, and molar flow rate of ammonia. The physicochemical properties of the as-formed molybdenum nitride were characterized by X-ray diffraction, N2 sorption, transmission electron microscopy, temperature-programmed oxidation/reduction, and X-ray photoelectron spectroscopy. Of the experimental variables, the nitridation temperature was found to be the most critical parameter determining the surface area of the molybdenum nitride. When the prepared molybdenum nitride was exposed to air, the specific surface area rapidly decreased because of the partial oxidation of molybdenum nitride to molybdenum oxynitride. However, the surface area recovered to 90% the initial value after H2 treatment. The catalyst with the highest degree of nitridation showed the best catalytic activity, superior to that of unmodified α-MoO3, for the decomposition of ammonia because of its high surface area.
Bioethanol dehydration was carried out in a bench scale reactor-loaded H-ZSM-5 molded catalyst, which increased by tens of times more than at lab scale (up to 60 and 24 times based on the amount of catalyst and ethanol flow rate, respectively). From the results of the lab scale reaction, we confirmed the optimum Si/Al ratio (14) of H-ZSM-5, reaction temperature (~250 °C), and weight hourly space velocity (WHSV) (<5 h−1) indicating high ethanol conversion and ethylene selectivity. Five types of cylindrical shaped molded catalysts were prepared by changing the type and/or amount of organic solid binder, inorganic solid binder, inorganic liquid binder, and H-ZSM-5 basis catalyst. Among them, the catalyst exhibiting the highest compression strength and good ethanol dehydration performance was selected. The bench scale reaction with varying reaction temperature of 245–260 °C and 1.2– 2.0 h−1 WHSV according to reaction time showed that the conversion and ethylene selectivity were more than 90% after 400 h on stream. It was also confirmed that even after the successive catalyst regeneration and the reaction for another 400 h, both the ethanol conversion and ethylene selectivity were still maintained at about 90%.
21 February 2022 in Catalysis Science & Technology
An active and stable Ni-BEA catalyst for dry reforming of methane was achieved by the in situ formation of highly dispersed Ni clusters that are stabilized by defect sites.