Controlling electronics for the formation of high valent uranium imido complexes
Known primarily for its single electron chemistry, controlling the electronics at uranium to facilitate multi-electron processes remains a fundamental challenge in the actinide sciences. Our group has implemented the use of redox-active ligands to assist in the stabilization of low-valent uranium analogues, capable of performing multi-electron chemistry at a single uranium center. Of particular interest to our group are high-valent imido complexes, which are ubiquitous in organometallic and coordination chemistry due to their unique bonding properties and their ability to mediate bond-forming reactions. Uranium imido complexes, in particular, are the subject of much research to determine the degree of f-orbital involvement in the uranium-nitrogen multiple bonds. Thus, the formation of an unprecedented uranium tris(imido) species via multi-electron redox chemistry mediated by redox-active ligands as well as its bonding properties will be discussed. Additionally, the synthesis and characterization of other novel uranium imido species absent of redox active ligands will be presented, along with investigations of the reactive intermediates in solution. Finally, the reactivity of these novel tris(imido) complexes towards a variety of small molecules and organic substrates will be highlighted.
Bart, Purdue University.
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