Mechanistic studies of silica polymerization from supersaturated aqueous solutions by means of time-resolved light...

Silica polymerization in a supersaturated aqueous solution of sodium silicate is a fundamental mineralization process with broad relevance for technical applications as well as for biological processes. To contribute to a better understanding of the mechanism underlying the polymerization of sodium silicate under ambient conditions, a combined multiangle static and dynamic light scattering study on the evolution of particle mass and size is applied for the first time in a time-resolving manner. The light scattering experiments are complemented by a time-resolved analysis of the decay of the concentration of monomeric silicate by means of the silicomolybdate method. Particle formation was investigated at a variable concentration of silicate at pH 7 and 8. The joint experiments revealed a loss of monomers, which is parallel to the formation of compact, spherical particles growing by a monomer-addition process. An increase in the silicate content of up to 750 ppm increased the extent of nucleation and at the same time decreased the lag time observed between the start of the reaction and the actual onset of the growth of particles. Once the silica content is considerably larger than 1000 ppm, the formation of particles is succeeded by particle-particle agglomeration leading to larger fractal-like particles. By the time agglomeration becomes noticeable with light scattering, the monomer concentration has already reached its equilibrium value. An increase in the pH to 8 again revealed particle formation via a monomer-addition process. However, the extent of nucleation was increased and particle-particle agglomeration was inhibited even at an initial silica content of 2000 ppm.