Coordination Chemistry of Homoleptic Actinide(IV)-Thiocyanate Complexes

Carter, Tyler J.; Wilson, Richard E.

doi:10.1002/chem.201502770

Coordination Chemistry of Homoleptic Actinide(IV)-Thiocyanate Complexes

Journal Article · Thu Sep 10 00:00:00 EDT 2015 · Chemistry - A European Journal

DOI:https://doi.org/10.1002/chem.201502770· OSTI ID:1237917

Carter, Tyler J. ^[1]; Wilson, Richard E. ^[1]

Argonne National Lab. (ANL), Argonne, IL (United States)

Here, the synthesis, X-ray crystal structure, vibrational and optical spectroscopy for the eight-coordinate thiocyanate compounds, [Et₄N]₄[Pu^IV(NCS)₈], [Et₄N]₄[Th^IV(NCS)₈], and [Et₄N]₄[Ce^III(NCS)₇(H₂O)] are reported. Thiocyanate was found to rapidly reduce plutonium to Pu^III in acidic solutions (pH<1) in the presence of NCS^–. The optical spectrum of [Et₄N][SCN] containing Pu^III solution was indistinguishable from that of aquated Pu^III suggesting that inner-sphere complexation with [Et₄N][SCN] does not occur in water. However, upon concentration, the homoleptic thiocyanate complex [Et₄N]₄[Pu^IV(NCS)₈] was crystallized when a large excess of [Et₄N][NCS] was present. This compound, along with its U^IV analogue, maintains inner-sphere thiocyanate coordination in acetonitrile based on the observation of intense ligand-to-metal charge-transfer bands. Spectroscopic and crystallographic data do not support the interaction of the metal orbitals with the ligand π system, but support an enhanced An^IV–NCS interaction, as the Lewis acidity of the metal ion increases from Th to Pu.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Chemical Sciences, Geosciences, and Biosciences Division

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1237917

Journal Information:: Chemistry - A European Journal, Journal Name: Chemistry - A European Journal Journal Issue: 44 Vol. 21; ISSN 0947-6539

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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Coordination Chemistry of Homoleptic Actinide(IV)-Thiocyanate Complexes

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