In this article, an environmentally friendly non-noble-metal class of Mo/MgAl 2 O 4 catalysts is demonstrated to exhibit excellent performance in isobutane dehydrogenation. Results of activity tests indicated that an induction period is required for the catalysts to develop the active species. Further investigation revealed that high-valence-state Mo species are favorable for the initial oxidative reactions and Mo 4+ ions are probably the actual active species for catalytic dehydrogenation. Given the strongly endothermic characteristics and rapid catalyst deactivation of alkane dehydrogenation, a circulating fluidized-bed unit was further applied to evaluate the activity and stability of the catalysts. To avoid undesired oxidative reactions and improve the initial catalytic activity, a flow of hydrogen was introduced into the pilot-scale unit to prereduce the catalysts prior to reaction. In general, the catalysts exhibited highly active and stable performance in the pilot-scale evaluation, with an isobutene yield of up to 35 wt %, demonstrating great potential for industrial applications.