The intercalation compound between alpha-zirconium phosphate and N,N'-bis-(3-aminopropyl)-1,3-propanediamine has two different modifications with respect to the conformation of the guess amine molecules: one is "bent form" and the other "straight form." Reactivity of each phase with a series of aldehydes was examined. C-13 CP/MAS NMR indicated that the tetraamine reacts stereoselectively with aldehydes to form cis-imine in the interlayer spacing. Depending on the molecular size of aldehyde, it is found that a significant difference can be recognized in the yields of the imine products for the two phases of intercalation compounds. It is also noted that residual water molecules in the interlayer spacing play an important role in the imine formation reaction.