The structural study of low coordinate uranium cations can provide fundamental information regarding the degree of covalency and f-orbital participation in organoactinide chemistry. In our group, we have successfully synthesised highly reactive organouranium (III) cations using bulky ligands, which have demonstrated reactivity with small unsaturated substrates such as dinitrogen (N2), oxides of carbon (CO, CO2) and aromatic systems such as benzene.The low coordination number to these reactive molecules has been suggested to be stabilised by intramolecular agostic C-H interactions, suggesting a degree of orbital participation normally associated with the transition elements. Studying uranium (III) compounds are useful as models for transuranic elements, in which the +3 oxidation state is more readily accessible, and can provide fundamental insights into the subtleties of covalent and ionic binding of 5f elements which are poorly understood. Understanding the fundamental chemistry of transuranic elements is critical to better understanding nuclear waste processing and separation.