Molecular Models to Predict the Influence of Templating Molecules on the Structure and Organization of Zeolites

Zeolites are crystalline aluminosilicate materials that are crucial in the modern chemical industry. Their material properties are defined mainly by their framework (FW) connectivity and the local arrangements of heteroatoms like Al or defects. Structure-directing agents (SDAs) are used during synthesis to control zeolite structure. In this dissertation, I used novel techniques to develop computational models and gain insights into the relationships between SDAs and their impact on the crystallization patterns of zeolite. First, I improve the efficacy of the traditional thermodynamic model in predicting the phase selectivity of organic SDAs between full siliceous CHA and AEI. Then, I introduced the Al into zeolite and explored the influence of SDAs on Al distributions in CHA with supercell density functional theory (DFT) models. Finally, I extended the model to further include charged vacancy defects and demonstrated their interaction with SDAs and other Al is indistinguishable from other framework Al. These works will serve as a guide for the industry, enabling the synthesis of zeolites with enhanced catalytic performance at reduced costs.