Hydrogen production from ammonia decomposition using Co/γ-Al₂O₃ catalysts – Insights into the effect of synthetic method

Chemical hydrogen storage in molecules such as ammonia (>17 wt% H₂) have the unique potential to overcome the current storage and transport limitations of the H₂ economy. However, sustainable on-demand production of hydrogen via ammonia decomposition, requires the development of novel transition metal-based catalysts beyond the current use of highly active but expensive ruthenium to ensure economic feasibility. In this paper, we provide fundamental understanding of the effects of a range of synthetic methods of Co/γ-Al₂O₃ catalysts on the resulting ammonia decomposition activity. The main activity determining factors are collectively the reducibility of the cobalt species and their particle size. This systematic work demonstrates that decreasing the cobalt particle size enhances the ammonia decomposition catalytic activity. However, a careful balance is required between a strong metal-support interaction leading to small particle sizes (promoted by precipitation methods) and the formation of inactive cobalt aluminate species (encouraged by adsorption methods). In addition, impurities such as boron and chloride remaining from particular synthetic methods were found to have detrimental effects on the activity.