Abstract:The dynamic behavior of tetrapropylammonium (TPA) cations in the clear precursor sols for silicalite synthesis has been investigated by 1 H diffusion ordered spectroscopy (DOSY), T 1 , T 2 , and T 1Ï 1 H relaxation, as well as 1 HĂ 13 C cross polarization (CP) nuclear magnetic resonance. The DOSY NMR experiments showed the presence of strong solute-solvent interactions in concentrated sols, which are decreasing upon dilution. Similarities in dependence of diffusion coefficients with fractional power of the viscosity constant observed for nanoparticles, TPA cations and water led to the conclusion that they aggregate as anisotropic silicate-TPA particles. Relaxation studies as well as 1 HĂ 13 C CP experiments provide information on dynamic properties of ethanol, water and TPA cations, which are function of silicate aggregates. The general tendency showed that the presence of silicate as oligomers and particles decreases the relaxation times, in particular T 2 and T 1ÏH , as a consequence of involvement of these latter in ion-pairing interactions with water-solvated TPA molecules slowing down their mobility. Furthermore, from the 1 HĂ 13 C CP dynamics curve profiles a change in the CP transfer regime was observed from fast (T CH << T 1ÏH ) for solutions without silicates to moderate (T CH~T1ÏH ) when silicates are interacting with the TPA cations that may reflect the occlusion of TPA into flexible silicate hydrate aggregates.