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.