Light alkanes in shale gas are an attractive source of carbon for the production of alkenes and aromatics compared to petroleum-derived naphtha. Zinc-exchanged zeolite H-MFI (Zn/ H-MFI) is active and selective for light alkane dehydrogenation and dehydroaromatization. In this study, Zn/H-MFI with varying Zn/Al ratios was prepared via solid-state ion exchange (SSIE) of ZnCl 2 and characterized by various methods. As-prepared Zn/H-MFI with Zn/Al ≤ 0.52 contains isolated [ZnCl] + and [ZnCl-(HCl)] + species; Zn/H-MFI with higher Zn loadings also contains ZnAl 2 O 4 /ZnAl 2 O 4−x Cl 2x nanoclusters. Postsynthetic treatment in He and subsequently in 2.5% H 2 in He at 773 K removes Cl and adsorbed HCl, resulting in the formation of [ZnH] + cations. Studies of C 3 H 8 dehydrogenation and cracking suggest that in the absence of cofed H 2 , [ZnH] + cations are transformed to bridging Zn 2+ cations, which exhibit higher C 3 H 8 dehydrogenation activity and selectivity relative to [ZnH] + cations. The kinetics of dehydrogenation and cracking over Zn/H-MFI were investigated as a function of Zn loading, C 3 H 8 partial pressure, and temperature. The turnover frequency for propane dehydrogenation and cracking increases with Zn loading, which we propose is due to localization of Zn 2+ cations either at increasingly distant pairs of Al atoms or at the β-site in the MFI framework. The selectivity to dehydrogenation over cracking over Zn 2+ is independent of C 3 H 8 partial pressure and temperature, consistent with dehydrogenation and cracking pathways that proceed via a common surface intermediate and have similar enthalpies of activation. The product distribution is thus determined by the entropy of activation for each pathway, which is less negative in the case of C 3 H 8 dehydrogenation.