Silica species generated by the hydrolysis and condensation of tetraethyl orthosilicate (TEOS) could assemble with alkylamines to form silica gel. Herein, it was evidenced that part of the added amines, including butylamine (BA), octylamine (OA) or dodecylamine (DA), was protonated in the mixture of water and ethanol. Therefore, besides the hydrogen bonding between neutral silica species and the micelles composed of the non-protonated amines (Tanev and Pinnavaia, 1995), there existed strong electrostatic attraction between negatively charged silica species and the micelles composed of the protonated amines. This coexisting assembly mechanism could explain why the uncalcined BA- and OA-gels were millimeter-sized small blocks with large porosities and synthesized without waste water emission, while the uncalcined DA-gel was almost non-porous and formed via precipitation from its reaction medium. The uncalcined BA gel was proved to be efficient as a solid basic catalyst, replacing the commonly used ammonia solution which is easily volatilized and has a pungent smell, for the hydrolysis and condensation of TEOS to prepare silica microspheres.
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