Compared to the high-valent bis(imido) complexes U(NR)2X2Ln, mono(imido) U(IV) species exhibit N-based reactivity consistent with greater polarization of the U�N multiple bond. Characterization of this interaction has been hampered, however, by the lack of suitable starting materials for investigating this chemistry in a step-wise fashion. Nearly all of the known U(IV) mono(imido) compounds contain cyclopentadienide or bulky-amido co-ligands, stretching the relevance of comparisons between these different species. Building on a recently developed methodology for generating mononuclear, mono(imido) U(IV) dihalides, we report the synthesis and characterization of products resulting from imido-group reactivity at several U(IV)-imido-containing compounds. In particular, treatment of the U(NR)-complexes with aryl, alkyl, and silyl isocyanates is shown to lead to various reaction products, which highlights the divergent reactivity available to uranium imido complexes that span differing oxidation states.

Molecular U(IV) mono(imido) chemistry: New starting materials and imido-group reactivity

246th National Meeting (2013)

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