Inelastic Neutron Scattering (INS) spectroscopy was used to characterize the catalytic hydrogenation of butyronitrile on the surface of parent and LiOH-modified Raney-Co. At low pressure hydrogen is mainly adsorbed on 3-fold sites. Co-adsorbed butyronitrile and hydrogen react on the unmodified Raney-Co sample to several partially hydrogenated products that contain N-H bonds. The nature of the species suggests that bi-molecular condensation leading to N-Butylidene-1-butanamine is feasible.