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Discrete colloidal particles of TPA-silicalite-1 with an average particle size of less than 100 nm and with a narrow particle-size distribution have been synthesized in clear homogeneous solutions. The factors influencing particle size have been investigated. High silica contents in conjunction with high alkalinities favor the synthesis of colloidal silicalite suspensions. Polymeric silica sources result in larger particles compared to those synthesized with tetraethoxy silane—presumably due to the different nucleation kinetics. It was found that the base concentration influences nucleation behavior in that high alkalinities result in the nucleation of a relatively large number of particles. The growth rates are constant for a given silica content irrespective of the alkalinity, at least within the alkalinity range studied. This result is ascribed to a rate-limiting surface reaction step that is a consequence of the synthesis mixture …