Alexander Aerts, Lana R. A. Follens, Mohamed Haouas, Tom P. Caremans, Marc-André Delsuc, Benoit Loppinet, Jan Vermant, Bart Goderis, Francis Taulelle, Johan A. Martens, and Christine E. A. Kirschhock
Concentrated clear solutions, as used for the preparation of Silicalite-1 zeolite, were synthesized from tetrapropylammonium hydroxide, tetraethylorthosilicate, and water. The solutions were analyzed using three techniques: quantitative 29Si NMR, synchrotron small-angle X-ray scattering (SAXS), and dynamic light scattering (DLS). 29Si NMR showed the coexistence of silicate oligomers and particles. For the first time, both fractions were analyzed simultaneously, providing a global, quantitative description of the clear solution microstructure. The SAXS patterns, typical of interacting particles, could be used together with the 29Si NMR deduced particle volume fraction to estimate a particle size. A careful analysis of DLS data of the dynamics of the suspensions revealed the occurrence of two diffusive processes. The faster process is a collective particle diffusion. The slower process corresponds to the particle self-diffusion and is present because of the presence of polydispersity in size, shape, and/or surface charge. The self-diffusion coefficient provides a means to estimate the equivalent hydrodynamic radius. The observations hence reveal a complex, polydisperse mixture of particles present at the onset of the Silicalite-1 zeolite formation. Implications on the proposed zeolite formation mechanisms are briefly discussed. [ABSTRACT FROM AUTHOR]