The catalytic (propane dehydrocyclization) and reduction behaviors of near 1:1 cation (Ga, In)/framework-Al MFI zeolites were examined under conditions where the materials were initially either in fully protonated or zero-protonated states. Reductions at appropriate temperatures proceeded up to similar to 100% exchange of protons for reduced univalent cations. Further aqueous exchange of alkali (K+) or alkaline earth (Ba2+) cations increased the selectivity for dehydrogenation reactions at little or no sacrifice in overall activity.