Room Temperature Dinitrogen Cleavage and Hydrogenation with Organometallic Complexes of Uranium

The conversion of atmospheric nitrogen into ammonia is not just a crucial reaction for sustaining life on Earth; it is a pivotal cornerstone for our planet's future. The Haber-Bosch process, although a well-established method utilizing hydrogen and nitrogen, demands an extensive industrial infrastructure, limiting its accessibility and flexibility. Innovative technologies that harness hydrogen from renewable resources, combined with decarbonized electricity and nitrogen from the ambient air, are imperative to address the pressing need for sustainable ammonia production. The chemistry of molecular catalysts, whether supported or unsupported, offers numerous advantages. In this context, we present groundbreaking findings on the reactivity of dinitrogen with an organometallic uranium complex featuring the Cpttt ligand (Cpttt = 1,2,4-tris(tert-butyl)cyclopentadienyl). This complex demonstrates the ability to cleave and hydrogenate dinitrogen with notable kinetics at ambient temperature and pressure. Most notably, redox assistance from the hydrocarbon ligand is crucial to this reaction, highlighting the promise of such complexes as viable candidates for ammonia synthesis technologies.