In the reaction of acetone, formaldehyde and methanol with ammonia over modified ZSM-5 catalysts, 2-picoline and 2,6-lutidine are synthesized selectively. The catalysts studied were H-ZSM-5 with Si/Al ratios, 30, 150 and 280, Pb-ZSM-5, W-ZSM-5 and modified silica-alumina. The yields of 2-picoline obtained were 30-47 wt.-% at 50-60 wt.-% conversions of acetone. The unconverted acetone and methanol can be recycled to increase the over-all yield. Pb-ZSM-5 was identified as the best catalyst.