This Thesis describes three broad areas: i) the synthesis of Fe and Ru complexes and the development of new catalytic systems for the dehydrocoupling of phosphine and amine-borane complexes, ii) mechanistic and reactivity studies of the dehydrocoupling of amine-borane adducts catalyzed by Rh complexes and (iii) the synthesis of a new amine-borane adduct and its dehydrogenation and hydrogenation reactivity studies.