Divalent and trivalent gas-phase coordination complexes of californium: evaluating the stability of Cf(II)

Dau, Phuong D.; Shuh, David K.; Sturzbecher-Hoehne, Manuel; Abergel, Rebecca J.; Gibson, John K.

doi:10.1039/c6dt02414a

Title: Divalent and trivalent gas-phase coordination complexes of californium: evaluating the stability of Cf(II)

Abstract

The divalent oxidation state is increasingly stable relative to the trivalent state for the later actinide elements, with californium the first actinide to exhibit divalent chemistry under moderate conditions. Although there is evidence for divalent Cf in solution and solid compounds, there are no reports of discrete complexes in which Cf^II is coordinated by anionic ligands. Described here is the divalent Cf methanesulfinate coordination complex, Cf^II(CH₃SO₂)₃-, prepared in the gas phase by reductive elimination of CH₃SO₂ from Cf^III(CH₃SO₂)₄-. Comparison with synthesis of the corresponding Sm and Cm complexes reveals reduction of CfIII and SmIII, and no evidence for reduction of Cm^III. This reflects the comparative 3+/2+ reduction potentials: Cf³⁺ (-1.60 V) ≈ Sm³⁺ (-1.55 V) >> Cm³⁺ (-3.7 V). Association of O₂ to the divalent complexes is attributed to formation of superoxides, with recovery of the trivalent oxidation state. Lastly, the new gas-phase chemistry of californium, now the heaviest element to have been studied in this manner, provides evidence for Cf^II coordination complexes and similar chemistry of Cf and Sm.

Authors:

Dau, Phuong D. ^[1]; Shuh, David K. ^[1]; Sturzbecher-Hoehne, Manuel ^[1]; Abergel, Rebecca J. ^[1]; Gibson, John K. ^[1]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division

Publication Date:: Thu Jul 07 00:00:00 EDT 2016

Research Org.:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1435062

Grant/Contract Number:: AC02-05CH11231

Resource Type:: Accepted Manuscript

Journal Name:: Dalton Transactions

Additional Journal Information:: Journal Volume: 45; Journal Issue: 31; Journal ID: ISSN 1477-9226

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Dau, Phuong D., Shuh, David K., Sturzbecher-Hoehne, Manuel, Abergel, Rebecca J., and Gibson, John K. Divalent and trivalent gas-phase coordination complexes of californium: evaluating the stability of Cf(II).  United States: N. p., 2016. 
Web.  doi:10.1039/c6dt02414a.

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                    Dau, Phuong D., Shuh, David K., Sturzbecher-Hoehne, Manuel, Abergel, Rebecca J., & Gibson, John K. Divalent and trivalent gas-phase coordination complexes of californium: evaluating the stability of Cf(II).  United States.  https://doi.org/10.1039/c6dt02414a

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                    Dau, Phuong D., Shuh, David K., Sturzbecher-Hoehne, Manuel, Abergel, Rebecca J., and Gibson, John K. Thu .  
"Divalent and trivalent gas-phase coordination complexes of californium: evaluating the stability of Cf(II)".  United States.  https://doi.org/10.1039/c6dt02414a.  https://www.osti.gov/servlets/purl/1435062.

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@article{osti_1435062,

  title        = {Divalent and trivalent gas-phase coordination complexes of californium: evaluating the stability of Cf(II)},

  author       = {Dau, Phuong D. and Shuh, David K. and Sturzbecher-Hoehne, Manuel and Abergel, Rebecca J. and Gibson, John K.},

  abstractNote = {The divalent oxidation state is increasingly stable relative to the trivalent state for the later actinide elements, with californium the first actinide to exhibit divalent chemistry under moderate conditions. Although there is evidence for divalent Cf in solution and solid compounds, there are no reports of discrete complexes in which CfII is coordinated by anionic ligands. Described here is the divalent Cf methanesulfinate coordination complex, CfII(CH3SO2)3-, prepared in the gas phase by reductive elimination of CH3SO2 from CfIII(CH3SO2)4-. Comparison with synthesis of the corresponding Sm and Cm complexes reveals reduction of CfIII and SmIII, and no evidence for reduction of CmIII. This reflects the comparative 3+/2+ reduction potentials: Cf3+ (-1.60 V) ≈ Sm3+ (-1.55 V) >> Cm3+ (-3.7 V). Association of O2 to the divalent complexes is attributed to formation of superoxides, with recovery of the trivalent oxidation state. Lastly, the new gas-phase chemistry of californium, now the heaviest element to have been studied in this manner, provides evidence for CfII coordination complexes and similar chemistry of Cf and Sm.},

  doi          = {10.1039/c6dt02414a},

  journal      = {Dalton Transactions},

  number       = 31,

  volume       = 45,

  place        = {United States},

  year         = {Thu Jul 07 00:00:00 EDT 2016},

  month        = {Thu Jul 07 00:00:00 EDT 2016}

}

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Works referencing / citing this record:

Contemporary Chemistry of Berkelium and Californium
journal, June 2019

White, Frankie D.; Dan, David; Albrecht‐Schmitt, Thomas E.
Chemistry – A European Journal, Vol. 25, Issue 44
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Title: Divalent and trivalent gas-phase coordination complexes of californium: evaluating the stability of Cf(II)

Abstract

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Divalent Samarium Compounds with Heavier Chalcogenolate (EPh; E = Se, Te) Ligands
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Synthesis and Solid State Structures of Sterically Crowded d ⁰ -Metallocenes of Magnesium, Calcium, Strontium, Barium, Samarium, and Ytterbium
journal, July 2002

Expanding Dinitrogen Reduction Chemistry to Trivalent Lanthanides via the LnZ ₃ /Alkali Metal Reduction System: Evaluation of the Generality of Forming Ln ₂ (μ - η ² ^{: η ² ^{-N ₂ ) Complexes via LnZ ₃ /K}}
journal, November 2004

Evaluation of a Silylene Divalent Lanthanide Interaction in the Metallocene Complex (C ₅ Me ₅ ) ₂ Sm[SiN ^t ^{BuCHCHN ^t ^Bu]}
journal, March 2003

Studies of californium(II) and (III) iodides
journal, January 1978

Metastable charge-transfer state of californium( iii ) compounds
journal, January 2015

Completing the Series of +2 Ions for the Lanthanide Elements: Synthesis of Molecular Complexes of Pr ²⁺ , Gd ²⁺ , Tb ²⁺ , and Lu ²⁺
journal, May 2013

Effects of changing the M ²⁺ cation on the crystal structure and optical properties of divalent samarium-doped MAl ₂ Si ₂ O ₈ (M = Ca, Sr, Ba)
journal, January 2015

Lanthanide(II) complexes bearing mixed linked and unlinked cyclopentadienyl–monodentate-anionic ligands
journal, March 2002

Electron transfer dissociation of dipositive uranyl and plutonyl coordination complexes: ETD of Uranyl/Plutonyl Complexes
journal, December 2011

Polarographic evidence for the divalent oxidation state of californium
journal, May 1972

Contemporary Chemistry of Berkelium and Californium
journal, June 2019