An unsupported iron-nickel (Fe-Ni) alloy and several Fe-Ni alloy deposited on SBA-15 (Santa Barbara Amorphous-15) supports (Fe-Ni/SBA) with various Fe-Ni contents are prepared and used as catalysts in the hydrolysis of ammonia-borane (AB) for hydrogen generation. By maintaining a constant concentration of Fe-Ni in the AB aqueous solutions, we investigate the influence of the SBA-15 support on the Fe-Ni catalytic activity in the AB hydrolysis reaction. The SBA-15 support helps disperse the Fe-Ni alloy particles on its surface, which consequently improves the catalytic activity of the Fe-Ni. However, the presence of SBA-15 particles in the aqueous solution also retards the migration of the AB molecules in solution toward the Fe-Ni catalysts, increasing the induction time of the AB hydrolysis reaction. Therefore, there is an optimal Fe-Ni content in Fe-Ni/SBA for the catalysis of the AB hydrolysis reaction. Copyright (C) 2013, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.