Ammonia (NHsub.3), which has a 17.7 wt% gravimetric hydrogen density, has been considered as a potential hydrogen storage material. This study looked at the thermocatalytic decomposition of NHsub.3 using a bulk Mosub.2N catalyst that was boosted by alkali metals (AM: 5 wt% Li, K, Cs). The K-Mosub.2N catalyst outperformed all other catalysts in this experiment in terms of catalytic performance. At 6000 hsup.−1 GHSV, 100% conversion of NHsub.3 was accomplished using the K-Mosub.2N, Cs-Mosub.2N, and Mosub.2N catalysts. However, when compared to other catalysts, K-Mosub.2N had the highest activity, or 80% NHsub.3 conversion, at a lower temperature, or 550 °C. The catalytic activity exhibited the following trend for the rate of hydrogen production per unit surface area: K-Mosub.2N > Cs-Mosub.2N > Li-Mosub.2N > Mosub.2N. Up to 20 h of testing the K-Mosub.2N catalyst at 600 °C revealed no considerable deactivation.