Data science shows that entropy correlates with accelerated zeolite crystallization in Monte Carlo simulations

Abstract

We have performed a data science study of Monte Carlo (MC) simulation trajectories to understand factors that can accelerate the formation of zeolite nanoporous crystals, a process that can take days or even weeks. In previous work, MC simulations predicted and experiments confirmed that using a secondary organic structure-directing agent (OSDA) accelerates the crystallization of all-silica LTA zeolite, with experiments finding a three-fold speedup [Bores et al., Phys. Chem. Chem. Phys. 24, 142–148 (2022)]. However, it remains unclear what physical factors cause the speed-up. Here, we apply data science to analyze the simulation trajectories to discover what drives accelerated zeolite crystallization in MC simulations going from a one-OSDA synthesis (1OSDA) to a two-OSDA version (2OSDA). We encoded simulation snapshots using the smooth overlap of atomic positions approach, which represents all two- and three-body correlations within a given cutoff distance. Principal component analyses failed to discriminate datasets of structures from 1OSDA and 2OSDA simulations, while the Support Vector Machine (SVM) approach succeeded at classifying such structures with an area-under-curve (AUC) score of 0.99 (where AUC = 1 is a perfect classification) with all three-body correlations and as high as 0.94 with only two-body correlations. SVM decision functions reveal relatively broad/narrow histograms for 1OSDA/2OSDA datasets, suggesting that the two simulations differ strongly in information heterogeneity. Informed by these results, we performed pair (2-body) entropy calculations during crystallization, resulting in entropy differences that semi-quantitatively account for the speedup observed in the previous MC simulations. We conclude that altering synthesis conditions in ways that substantially change the entropy of labile silica networks may accelerate zeolite crystallization, and we discuss possible approaches for achieving such acceleration.