The project focuses in particular on crystalline aluminosilicate zeolites. In these materials, aluminum heteroatoms within the zeolite framework are anionic charge centers. Increasing evidence indicates that the relative proximity of these aluminum centers has a significant impact on the ultimate properties of the zeolite, in particular in their function in Bronsted acid catalysis (methanol dehydration) and in redox catalysis (the selective catalytic reduction of NOx). The main hypotheses are cationically charged structure-directing agents (SDAs) present during the synthesis process have a determining effect on the location of those Al atoms within a given zeolite lattice, their effect can be inferred from the interactions between SDAs and the pre-formed, aluminum-substituted zeolite, and the same modeling approach can be used to predict speciation during post-synthetic ion exchange. To test these hypotheses, the project develops classical and first-principles models to predict zeolite compositional phase diagrams for organic SDAs and inorganic cations vs silicon-to-aluminum ratio in a series of zeolite frameworks. These models are validated against experimental observation on laboratory-synthesized zeolites, using both ex situ spectroscopic and chemical characterization as well kinetic evaluations under catalytic conditions, and informed by first-principles and microkinetic modeling predictions of the relationship between Al atom location and properties. The project advances the computational design of zeolite materials in the context of practically significant catalytic reactions in a computation/experiment and academic/industrial collaborative setting.