MFI-type zeolites were characterized using powder x-ray diffraction (XRD), and positron annihilation lifetime spectroscopy (PALS) to uncover the hierarchical porous * Corresponding author. Tel: +61 3 9919 7682; fax: +61 3 9919 7696. Email: mikel.duke@vu.edu.au (M. Duke). overall release of ions, principally Na + and K + , which were liberated mainly from the zeolite channels, yet these materials adsorbed Ca 2+ in the microporous grain boundaries and Mg 2+ in the mesoporous grain boundaries. Si/Al = 100 appeared to be a unique ratio, allowing the material to possess the same Na + adsorption features (and hydrophilicity) of high alumina materials, but ion interactions resembling high silica materials. MFI-type zeolite is therefore shown to be highly configurable using Si/Al ratio for a wide variety of applications in the presence of ions.