Assessing Extreme Models of the Stober Synthesis Using Transients under a Range of Initial Composition.

29Si-NMR, conductimetry, and photon correlation spectroscopy are used to monitor the temporal profile of intermediate concentrations in Stober synthesis (i.e., ammonia-catalyzed hydrolysis of tetraethoxysilane in a batch reactor). Extreme models of the process are assessed by examining the effect of initial composition on these transients (over a wider range of composition than attempted previously). The trends with initial composition suggest that the nucleation is rate-limited by the hydrolysis of the singly hydrolyzed monomer, the product of which probably phase separates. Moreover, the trends are consistent with the aggregation model discussed by G. H. Bogush and C. F. Zukoski (J. Colloid Interface Sci. 142, 1, 19 (1991) and by M. T. Harris (Ph.D. dissertation, Univ. of Tennessee, 1992). The trends are not consistent with a growth model without aggregation. Copyright 1997 Academic Press. Copyright 1997Academic Press