Abstract: XRD, FT-IR, TG-DTAand ¹³C MAS NMRhave been used to characterize silicon zeolite CF-3 and ZSM-39 hydrothermally crystallized in TMEDA-Na₂O-SiO₂-H₂Osystem.The ¹³Cchemical shift and the relative intensity of resonance peak in CP (cross polarization) and HPDEC(high power decoupling) NMRspectra for different group of TMEDAreveal the position, the moving and the interaction with framework for the template molecule trapped in different size cages of zeolites.The narrowness, the unusual chemical shift to high field, and the obvious change of the intensity for the ¹³Cresonance peak of -C₂H₄- group related to that of -CH₃ group in the CPand HPDECspectra, indicate that one molecule of TMEDAis shared by two neighbours of [5¹²6⁴] cage of ZSM-39 and that the -C₂H₄- group of TMEDAinteracts strongly with oxygen atoms locating at the 6-oxygen-membered ring between the two cages.

Key words: Template molecule, TMEDA, Silicon zeolite CF-3, ZSM-39, ¹³C MAS NMR