(569m) Explaining Mechanism of Zeolite Crystallization Via Data Science:Speed-up Caused By Entropic Effect

The increasing demand for zeolites in sustainable technology is challenged by the resource-intensive nature of conventional synthesis processes. Computational modeling has become essential in studying these processes, offering an enhanced understanding of reaction pathways and the potential for more efficient synthesis. The specific focus is on examining the function of organic structure directing agents(OSDAs), which play a guiding role in zeolite formation, although there remains uncertainty regarding the full implications of increasing OSDA addition.

Utilizing advanced Replica Exchange Reaction Ensemble Monte Carlo simulations, we have begun to unravel the mechanisms by which additional OSDAs enhance the crystallization rate of zeolites. The introduction of the Smooth Overlap of Atomic Positions(SOAP) descriptor has provided a nuanced view of atomic arrangements that are often overlooked by simpler models focused on bond angles and ring configurations, tracking the transition from a disordered amorphous state to an organized crystalline one.

Machine Learning methods were crucial in interpreting the dense structural information captured by SOAP. Principal Component Analysis(PCA), a technique for simplifying complex data, was used to reorient the dataset to highlight phase transitions. Despite PCA's benefits, it proved inadequate for discerning structures by OSDA quantity; this is where the Support Vector Machine(SVM) excelled, sharply dividing structures into clear categories. The categorized data sets revealed striking contrasts, with those from the multiple OSDA systems demonstrating a tendency towards uniformity—indicating lower configurational entropy. This homogeneity suggests that additional OSDAs hinder random configuration, thereby streamlining the path to crystallization. Beyond providing clarity on the crystallization process, this comprehensive understanding of the effect of OSDAs on zeolite formation could enable precise manipulation of synthesis conditions, paving the way for tailoring zeolite structures to specific applications.