Probing the Mechanism of Silica Polymerization at Ambient Temperatures using Monte Carlo Simulations

We have developed a model for silica polymerization at ambient temperatures and low densities and have studied this using reactive Monte Carlo simulations. The model focuses on SiO4 coordination with the energetics of hydrolysis and condensation reactions treated via the reaction ensemble. The simplicity of the model makes large system sizes accessible on a modest computation budget although it is necessary to make additional assumptions in order to use the reactive Monte Carlo method as a simulation of the system dynamics. Excellent agreement for the evolution of the Q(n) distribution is obtained upon comparing the simulation results to experimental observations. The analysis of simulation trajectories provides mechanistic insight into the polymerizations process, showing the following three regimes oligomerization (0-1 h), ring formation (1-2.6 h), and cluster aggregation (2.6-5.6 h).