Nitrogen-doped carbon materials were prepared by ammoxidation of commercial carbon sources (carbon black and activated carbon) and applied as base catalysts for Knoevenagel and transesterification reactions. It was shown that these carbon materials were active and the activities were different depending on the ammoxidation conditions (temperature and ammonia concentration in air) and carbon sources used. The bulk, textural, and surface properties of the nitrogen-doped carbon materials were examined by several methods to clarify possible factors determining their final catalytic activities. The activated carbon-derived catalysts were more active than the carbon black-derived ones. The surface area and porosity were not responsible for this difference between the two carbon sources but the difference in the reactivity with oxygen was important. The reactivity of carbon sources with oxygen should influence the doping of nitrogen onto their surfaces by ammoxidation with ammonia and air and the resulting activities as base catalysts. The catalytic activity increases with the amount of nitrogen doped and, therefore, the nitrogen doped should be responsible for the catalytic activities. In addition, the activities are maximal at a ratio of nitrogen to oxygen of around 1, suggesting the importance of cooperative functions of nitrogen and oxygen on the surface of carbons.
Alkylation of aromatic compounds with various alkylating agents such as benzyl chloride, benzyl alcohol and isopropyl chloride were investigated using ZnCl 2 based ionic liquid (ILs) Lewis acid catalysts. Multi-component Lewis acid catalysts of ZnCl 2 and ionic liquids such as 1-butyl-3-methylimidazolium bromide, 1-butylpyridinium bromide, cholin chloride and tetrabutylammonium bromide were prepared, supported on silica gel, and compared for alkylation reactions with various alkylating agents. Among the IL-based catalysts, 1-butyl-3-methyl imidazolium-bromide-ZnCl 2 and 1-butylpyridinium bromide-ZnCl 2 are highly active.
Hydroformylation of cyclohexene was studied with a catalyst system of Ru 3 (CO) 12 and LiCl using H 2 and CO 2 instead of CO in NMP. The influence of H 2 and CO 2 pressures on the total conversion and the product distribution was examined. It was shown that increasing total pressure of H 2 and CO 2 promoted the reverse water gas shift reaction and increased the yield of cyclohexanecarboxaldehyde. Its hydrogenation to cyclohexanemethanol was promoted with increasing H 2 pressure but suppressed with increasing CO 2 pressure. Cyclohexane was also formed along with those products and this direct hydrogenation was suppressed with increasing CO 2 pressure. The roles of CO 2 as a promoter as well as a reactant were further examined by phase behavior observations and high pressure FTIR measurements.
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