Interplay of water, extra-framework cations and framework atoms in the structure of low-silica zeolites: the case of the natural zeolite Goosecreekite as studied by computer simulation

Computational methods are described that model accurately the structure of hydrated Ca-bearing zeolites. Using Goosecreekite as a model system we probe the influence of framework ordering, cation siting and hydration of pores on the structure and its stability. We develop a methodology which allows the location of Al within the framework to be determined together with the position of extra-framework cations, in a stepwise fashion, progressing from an anhydrous model, via a dielectric continuum model, to finally, a fully atomistic model of the water in the intrazeolite pore space. Our methods reveal the complex interplay of short- and long-range interactions on the optimal structure of such materials.