A Pseudotetrahedral Uranium(V) Complex

Tondreau, Aaron M.; Duignan, Thomas J.; Stein, Benjamin W.; Fleischauer, Valerie E.; Autschbach, Jochen; Batista, Enrique R.; Boncella, James M.; Ferrier, Maryline G.; Kozimor, Stosh A.; Mocko, Veronika; Neidig, Michael L.; Cary, Samantha K.; Yang, Ping

doi:10.1021/acs.inorgchem.7b03139

Title: A Pseudotetrahedral Uranium(V) Complex

Journal Article · 04 July 2018 · Inorganic Chemistry

DOI: https://doi.org/10.1021/acs.inorgchem.7b03139 · OSTI ID:1460655

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Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. at Buffalo, NY (United States). Dept. of Chemistry
Univ. of Rochester, NY (United States). Dept. of Chemistry
Univ. at Buffalo, NY (United States). Dept. of Chemistry

A series of uranium amides were synthesized from N,N,N-cyclohexyl(trimethylsilyl)lithium amide [Li][N(TMS)Cy] and uranium tetrachloride to give U(NCySiMe₃)_x(Cl)_4–x, where x = 2, 3, or 4. The diamide was then isolated as a bimetallic, bridging lithium chloride adduct ((UCl₂(NCyTMS)₂)₂-LiCl(THF)₂), and the tris(amide) was isolated as the lithium chloride adduct of the monometallic species (UCl(NCyTMS)₃-LiCl(THF)₂). The tetraamide complex was isolated as the four-coordinate pseudotetrahedron. Cyclic voltammetry revealed an easily accessible reversible oxidation wave, and upon chemical oxidation, the U^V amido cation was isolated in near-quantitative yields. The synthesis of this family of compounds allows a direct comparison of the electronic structure and properties of isostructural U^IV and U^V tetraamide complexes. Spectroscopic investigations consisting of UV–vis, NIR, MCD, EPR, and U L₃-edge XANES, along with density functional and wave function calculations, of the four-coordinate U^IV and U^V complexes have been used to understand the electronic structure of these pseudotetrahedral complexes.

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Research Organization:: Los Alamos National Laboratory (LANL)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-06NA25396; SC0016002; SC0001136; AC02-76SF00515

OSTI ID:: 1460655

Report Number(s):: LA-UR-18-21979

Journal Information:: Inorganic Chemistry, Journal Name: Inorganic Chemistry Journal Issue: 14 Vol. 57; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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