Replica exchange reactive molecular dynamics simulations of initial reactions in zeolite synthesis

Abstract

Molecular simulation is a promising tool for the study of zeolite formation. However, sufficient sampling remains a grand challenge for the practical use of molecular simulation for this purpose. Here, we investigate the initial stage of zeolite synthesis under realistic conditions by using the replica-exchange method and the ReaxFF reactive force field. After a total simulation time of 480 ns, both energetic and structural properties approach convergence. Analyses of data collected at 600 K show that the inorganic structure directing agent NaOH promotes the aggregation of silicate, the formation of branched Si atoms and the formation of 5-membered rings. With the trajectories collected simultaneously at different temperatures, the effect of temperature is discussed.