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Title: Coordination Chemistry of Homoleptic Actinide(IV)-Thiocyanate Complexes

Abstract

Here, the synthesis, X-ray crystal structure, vibrational and optical spectroscopy for the eight-coordinate thiocyanate compounds, [Et 4N] 4[Pu IV(NCS) 8], [Et 4N] 4[Th IV(NCS) 8], and [Et 4N] 4[Ce III(NCS) 7(H 2O)] 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 [Et 4N][SCN] containing Pu III solution was indistinguishable from that of aquated Pu III suggesting that inner-sphere complexation with [Et 4N][SCN] does not occur in water. However, upon concentration, the homoleptic thiocyanate complex [Et 4N] 4[Pu IV(NCS) 8] was crystallized when a large excess of [Et 4N][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.

Authors:
 [1];  [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1237917
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry - A European Journal
Additional Journal Information:
Journal Volume: 21; Journal Issue: 44; Journal ID: ISSN 0947-6539
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; actinoids; coordination chemistry; plutonium; thiocyanates

Citation Formats

Carter, Tyler J., and Wilson, Richard E. Coordination Chemistry of Homoleptic Actinide(IV)-Thiocyanate Complexes. United States: N. p., 2015. Web. doi:10.1002/chem.201502770.
Carter, Tyler J., & Wilson, Richard E. Coordination Chemistry of Homoleptic Actinide(IV)-Thiocyanate Complexes. United States. doi:10.1002/chem.201502770.
Carter, Tyler J., and Wilson, Richard E. Thu . "Coordination Chemistry of Homoleptic Actinide(IV)-Thiocyanate Complexes". United States. doi:10.1002/chem.201502770. https://www.osti.gov/servlets/purl/1237917.
@article{osti_1237917,
title = {Coordination Chemistry of Homoleptic Actinide(IV)-Thiocyanate Complexes},
author = {Carter, Tyler J. and Wilson, Richard E.},
abstractNote = {Here, the synthesis, X-ray crystal structure, vibrational and optical spectroscopy for the eight-coordinate thiocyanate compounds, [Et4N]4[PuIV(NCS)8], [Et4N]4[ThIV(NCS)8], and [Et4N]4[CeIII(NCS)7(H2O)] are reported. Thiocyanate was found to rapidly reduce plutonium to PuIII in acidic solutions (pH<1) in the presence of NCS–. The optical spectrum of [Et4N][SCN] containing PuIII solution was indistinguishable from that of aquated PuIII suggesting that inner-sphere complexation with [Et4N][SCN] does not occur in water. However, upon concentration, the homoleptic thiocyanate complex [Et4N]4[PuIV(NCS)8] was crystallized when a large excess of [Et4N][NCS] was present. This compound, along with its UIV 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 AnIV–NCS interaction, as the Lewis acidity of the metal ion increases from Th to Pu.},
doi = {10.1002/chem.201502770},
journal = {Chemistry - A European Journal},
number = 44,
volume = 21,
place = {United States},
year = {2015},
month = {9}
}

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Cited by: 6 works
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    • DOI: 10.1021/ic061798b

    Use of Soft Heterocyclic N-Donor Ligands To Separate Actinides and Lanthanides
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    Coordination Chemistry with f-Element Complexes for an Improved Understanding of Factors That Contribute to Extraction Selectivity
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    • Gorden, Anne E. V.; DeVore, Michael A.; Maynard, Branson A.
    • Inorganic Chemistry, Vol. 52, Issue 7
    • DOI: 10.1021/ic300887p

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    Synthesis and structure of the six-coordinate hexaisothiocyanatolanthanide(III) complexes
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    • DOI: 10.1021/ja01018a075

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    Comparison of Covalency in the Complexes of Trivalent Actinide and Lanthanide Cations
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    • Jensen, Mark P.; Bond, Andrew H.
    • Journal of the American Chemical Society, Vol. 124, Issue 33
    • DOI: 10.1021/ja0178620

    Structural Correspondence between Uranyl Chloride Complexes in Solution and Their Stability Constants
    journal, May 2011

    • Soderholm, L.; Skanthakumar, S.; Wilson, Richard E.
    • The Journal of Physical Chemistry A, Vol. 115, Issue 19
    • DOI: 10.1021/jp111551t

    Structures and Energetics of Erbium Chloride Complexes in Aqueous Solution
    journal, June 2009

    • Soderholm, L.; Skanthakumar, S.; Wilson, Richard E.
    • The Journal of Physical Chemistry A, Vol. 113, Issue 22
    • DOI: 10.1021/jp9012366

    How Hydrogen Bonds Affect the Growth of Reverse Micelles around Coordinating Metal Ions
    journal, March 2014

    • Qiao, Baofu; Demars, Thomas; Olvera de la Cruz, Monica
    • The Journal of Physical Chemistry Letters, Vol. 5, Issue 8
    • DOI: 10.1021/jz500495p

    Mesoscopic Aspects of Phase Transitions in a Solvent Extraction System
    journal, October 2012

    • Ellis, Ross J.; Audras, Matthieu; Antonio, Mark R.
    • Langmuir, Vol. 28, Issue 44
    • DOI: 10.1021/la3034879

    Thermochromic properties of low-melting ionic uranyl isothiocyanate complexes
    journal, January 2011

    • Aoyagi, Noboru; Shimojo, Kojiro; Brooks, Neil R.
    • Chemical Communications, Vol. 47, Issue 15
    • DOI: 10.1039/c0cc05550f

    Crystal structure versus solution for two new lutetium thiocyanato complexes
    journal, January 2011

    • Lozano-Rodriguez, M. J.; Copping, R.; Petit, S.
    • New Journal of Chemistry, Vol. 35, Issue 12
    • DOI: 10.1039/c1nj20494g

    Fingerprinting the oxidation state of U(iv) by emission spectroscopy
    journal, January 2013

    • Hashem, Emtithal; Lorusso, Giulia; Evangelisti, Marco
    • Dalton Transactions, Vol. 42, Issue 41
    • DOI: 10.1039/c3dt52151f

    Plutonium chlorido nitrato complexes: ligand competition and computational metrics for assembly and bonding
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