One of the most important and challenging tasks in modern chemistry is the reduction of dinitrogen and its transformation into ammonia (NH<sub>3</sub>) or value-added N-containing organic compounds. In particular, uranium nitride materials (UN) have proven their activity as catalysts for the Haber-Bosch process which, combined with their potential application as nuclear fuels, attracted a large interest on their synthesis. Recently in our group, a multimetallic low valent uranium nitride complex was reported to perform the four-electron reduction of dinitrogen. The reduced dinitrogen could also be functionalized or converted into ammonia. A new multimetallic low valent uranium complex able to perform the four-electron reduction of dinitrogen will be presented in this work. The different nature of the bridging ligand revealed to have major effects on the functionalization and the reactivity of the reduced dinitrogen&lt;span style=font-size:10.8333px"&gt;.&lt;/span&gt; When the reduction of dinitrogen is performed in presence of a reducing agent, bis(µ-nitride) complexes are reported as possible products. Despite that, functionalization of those complexes has never been achieved in uranium chemistry and is very rare in d-block chemistry. In this work, the synthesis of a bis(µ-nitride) uranium(V) and the functionalization of the nitride ligand with small molecules is also presented. Uranium nitrides are also ideal target molecules for the investigation of magnetic communication between uranium atoms, whose examples remain limited. The magnetic properties of the bis(µ-nitride) uranium(V) and the complexes deriving from its small molecule reactivity will be presented in this work. The role of the coligands in uranium(IV) complexes bridged by a nitride ligand has also been investigated. The difference in the electronic structure of such complexes also reflects in dramatic changes in the reactivity towards small molecules, which will be presented in this work.

Dinitrogen reduction and N-functionalization by uranium multimetallic complexes

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.