Identification of reaction intermediates during hydrogenation of CD3CN on Raney-Co

Reaction intermediates formed on the surface of Raney-Co after co-adsorption of acetonitrile-image (CD3CN) and hydrogen were investigated by inelastic neutron scattering (INS). Detailed information on the structure of the adsorbed molecules was obtained by comparison of the spectra of potential reaction intermediates with reference spectra of H2, CD3CN, and CD3CH2NH2 as well as INS spectra calculated by ab initio methods. We concluded that CD3CN reacted preferentially with hydrogen bound to image sites on the Co-001 plane. On the surface, a mixture of a nitrene-like intermediate and co-adsorbed CD3CH2NH2 was formed, as indicated by a strong CH2 twisting vibrational mode, which decreased in intensity relative to the other CH2 vibrational modes, when the amount of hydrogen was increased. The surface study is complemented with detailed catalyst characterisation as well as kinetic data on the hydrogenation of acetonitrile-image.