Probing the chemistry, electronic structure and redox energetics in pentavalent organometallic actinide complexes

Graves, Christopher R; Vaughn, Anthony E; Morris, David E; Kiplinger, Jaqueline L

doi:10.1021/ic8017375

Probing the chemistry, electronic structure and redox energetics in pentavalent organometallic actinide complexes

Journal Article · Tue Jan 01 04:00:00 EST 2008 · Inorganic Chemistry

DOI:https://doi.org/10.1021/ic8017375· OSTI ID:960498

Graves, Christopher R ^[1]; Vaughn, Anthony E ^[1]; Morris, David E ^[1]; Kiplinger, Jaqueline L ^[1]

Los Alamos National Laboratory

Complexes of the early actinides (Th-Pu) have gained considerable prominence in organometallic chemistry as they have been shown to undergo chemistries not observed with their transition- or lanthanide metal counterparts. Further, while bonding in f-element complexes has historically been considered to be ionic, the issue of covalence remains a subject of debate in the area of actinide science, and studies aimed at elucidating key bonding interactions with 5f-orbitals continue to garner attention. Towards this end, our interests have focused on the role that metal oxidation state plays in the structure, reactivity and spectral properties of organouranium complexes. We report our progress in the synthesis of substituted U{sup V}-imido complexes using various routes: (1) Direct oxidation of U{sup IV}-imido complexes with copper(I) salts; (2) Salt metathesis with U{sup V}-imido halides; (3) Protonolysis and insertion of an U{sup V}-imido alkyl or aryl complex with H-N{double_bond}CPh{sub 2} or N{triple_bond}C-Ph, respectively, to form a U{sup V}-imido ketimide complex. Further, we report and compare the crystallographic, electrochemical, spectroscopic and magnetic characterization of the pentavalent uranium (C{sub 5}Me{sub 5}){sub 2}U({double_bond}N-Ar)(Y) series (Y = OTf, SPh, C{triple_bond}C-Ph, NPh{sub 2}, OPh, N{double_bond}CPh{sub 2}) to further interrogate the molecular, electronic, and magnetic structures of this new class of uranium complexes.

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Research Organization:: Los Alamos National Laboratory (LANL)

Sponsoring Organization:: DOE

DOE Contract Number:: AC52-06NA25396

OSTI ID:: 960498

Report Number(s):: LA-UR-08-05056; LA-UR-08-5056

Journal Information:: Inorganic Chemistry, Journal Name: Inorganic Chemistry; ISSN 0020-1669; ISSN INOCAJ

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
ACTINIDE COMPLEXES
ACTINIDES
BONDING
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COMPLEXES
COPPER
COVALENCE
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HALIDES
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OXIDATION
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Probing the chemistry, electronic structure and redox energetics in pentavalent organometallic actinide complexes

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