The heterogeneous catalytic synthesis of pyridine and methylpyridines (picolines) was carried out by the reaction of ethanol with formaldehyde and ammonia over aluminosilicates with different acidic properties and textural characteristics: zeolite framework-type FAU in H-form with microporous (H-Y) and micro-meso-macroporous structure (H-Y-mmm) and mesoporous aluminosilicates, obtained by sol-gel synthesis in an alkaline medium (ASM-1) and under variable pH (ASM-2). It is shown that the highest catalytic activity is characteristic of ASM-2 (Si/Al = 40) with a narrow pore size distribution within the range 2 to 5 nm and containing strongly acidic bridging Si–OH–Al groups on the surface. The products of the reaction of ethanol with formaldehyde and ammonia on the catalysts studied are dominated by picolines; the maximum amount of picolines (60%) is formed on the H-Y-mmm and aluminosilicate ASM-2 samples.
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