In this work, the support effects on vapor-phase aldol condensation of methyl acetate (MeOAc) with formaldehyde (HCHO) over cesium catalysts are understood by the employment of Al 2 O 3 with different morphologies and crystal phases. The structural and electronic properties of these supported Cs catalysts are characterized by multiple techniques, such as XRD, HAADF-STEM, EDS-mapping, XPS, NH 3 -TPD and CO 2 -TPD. The Cs species are found to be highly dispersed on the Al 2 O 3 surfaces, and their compositions vary with the identity of Al 2 O 3 . A combined catalyst characterization and testing results indicates a balance between acidic and basic sites, i.e., an acid-base synergy, for the production of MA: the excess acidic sites lead to the lower MA selectivity due to the promoted further condensation, while the excess basic sites with the lower MeOAc conversion due to the insufficient activated HCHO species. These insights could be valuable for the design and optimization of catalysts for this reaction.
A variety of cesium supported catalysts with amorphous SiO2 as a carrier were prepared by vacuum impregnation and ultrasonic impregnation methods, which were used for the synthesis of methyl acrylate by aldol condensation of methyl acetate and formaldehyde. The as-prepared catalysts were characterized by XRD, N2 adsorption–desorption, NH3-TPD, CO2-TPD, XPS, ICP and TG. The results indicated that the bifunctional Cs–La–Sb/SiO2 showed a high conversion of methyl acetate as well as a high yield of methyl acrylate, which was attributed to the weak acid–base sites and the formation of basic Cs–O–Si species with the addition of antimony and lanthanum, respectively. Furthermore, Cs–La–Sb/SiO2-(V) prepared by vacuum impregnation showed a high initial catalytic activity, but its activity sharply decreased due to the loss of active species. Comparatively, Cs–La–Sb/SiO2-(U) prepared by ultrasonic impregnation showed a good stability owing to the cavitation effect of ultrasonic waves. The conversion of methyl acetate and yield of methyl acrylate remained above 20% and 9.0% (based on methyl acetate) for 100 h without obvious deactivation. Moreover, carbon deposition was the main factor for the deactivation of Cs–La–Sb/SiO2-(U), and the coked catalyst could be regenerated by calcination in air.
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