Synthesis and Structure of a Terminal Uranium Nitride Complex

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Science  28 Jun 2012:
DOI: 10.1126/science.1223488

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The terminal uranium nitride linkage is a fundamental target in the study of f-orbital participation in metal-ligand multiple bonding, but it has previously eluded characterization in an isolable molecule. Here, we report the preparation of the terminal uranium(V) nitride complex [UN(TrenTIPS)][Na(12-crown-4)2] (TrenTIPS = {N(CH2CH2NSiPri3)3}3– Pri = CH(CH3)2) by reaction of the uranium(III) complex [U(TrenTIPS)] with sodium azide followed by abstraction and encapsulation of the sodium cation by the polydentate crown ether 12-crown-4. Single-crystal X-ray diffraction reveals a uranium-terminal nitride bond length of 1.825(15) angstroms. The structural assignment is supported by 15N-isotopic labeling, electronic absorption spectroscopy, magnetometry, electronic structure calculations, elemental analyses, and liberation of ammonia following treatment with water.

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