Gas-phase hydrogenation of acetonitrile has been studied by using catalysts based on nickel supported on alumina- and mixedalumina/gallium oxide-pillared tin phosphate materials. The in situ thermal decomposition of nickel formate has demonstrated to be an interesting method to obtain dispersed nickel particles on pillared tin phosphate supports. These catalysts are active in this catalytic reaction, but all the catalysts exhibit important deactivation. The study of the influence of the structural and acid properties of the catalysts on their catalytic performance allows us to establish that both hydrogenation and condensation reaction leading to higher amines take place on the metal particles,