Abstract
This dissertation encapsulates a comprehensive exploration of zeolite crystallization, investigating the diverse functions and impacts of the reactants. The journey navigates an alternative synthesis approach, isotope labeling, nanoscale order manipulation, and nano-design of morphologies.The exploration commences by unraveling the significance of water's role in zeolite synthesis. The greener, solvent-free method is showcased for its accelerated crystallization, reduced water usage, and enhanced reactor volume utilization. Our findings highlight the importance of water participating in siloxane bond formation through a simple and highly efficient 17O isotope labelling method. Additionally, we present a pioneering grinding-free synthesis, demonstrating the wide adaptability of this approach.Varied organic structure-directing agents (OSDAs) elicit distinctive host-guest interactions, inducing local order and disorder variations. A thorough analysis of different OSDA-zeolite systems highlights the different forms of local disorder and deviations in unit cell parameters with implications for final properties. This investigation also identifies the most flexible sites within the MFI structure responding to such variations.The mineralizing agents are then examined through synthesizing various ZSM-5 samples with F- and OH-routes. This revealed an additional role in distributing Al sites, influencing the acidity. OH samples exhibited consistent Al site distribution regardless of Si/Al ratios, while F samples demonstrated gradual variation with increasing Si/Al ratios. Intensive NMR studies led to the conclusion that the specific location of F atoms influences the Al siting.The morphology design is addressed through dual templating to synthesize stacked zeolite nanosheets with customizable thickness. Commercially available OSDAs and straightforward literature-based protocols form the basis of this method. A linear correlation emerges between the measured thickness and introduced OSDAs mixture percentages. Furthermore, we establish the applicability of our technique to Al-containing zeolite synthesis.This work lays solid foundation for potential further investigations and applications including zeolites with controllable final properties.