Theoretical study of the effect of hydrogen adsorption on the activation of supported rhodium catalysts

Abstract

As a first step in the study of the mechanism involved in the synthesis of bi- and organo-metallic catalysts, the interaction of a hydrogen atom with [Rh] 13 clusters is analyzed at the self-consistent-field multireference configuration interaction (SCF-MRCI) level by means of intermediate neglect of differential overlap (INDO) calculations. Structural characteristics are the result of gradient-driven geometry optimizations, while electronic descriptors and multiplicity values belong to MRCI. Larger binding energies are found in the higher coordinated sites, where the adsorption results in a spin quenching to zero magnetic moment.