Unexpected Actinyl Cation-Directed Structural Variation in Neptunyl(VI) A-Type Tri-lacunary Heteropolyoxotungstate Complexes
Abstract
A-type tri-lacunary heteropolyoxotungstate anions (e.g., [PW9O34]9-, [AsW9O34]9-, [SiW9O34]10- and [GeW9O34]10-) are multi-dentate oxygen donor ligands that readily form sandwich complexes with actinyl cations ({UO2}2+, {NpO2}+, {NpO2}2+ & {PuO2}2+) in near neutral/slightly alkaline aqueous solutions. Two or three actinyl cations are sandwiched between two trilacunary anions, with additional cations (Na+, K+ or NH4 +) also often held within the cluster. Studies thus far have indicated that it is these additional +I cations, rather than the specific actinyl cation, that direct the structural variation in the complexes formed. We now report the structural characterization of the neptunyl (VI) cluster complex (NH4)13 [Na(NpO2)2(A-α- PW9O34)2]·12H2O. The anion in this complex, [Na(NpO2)2(PW9O34)2]13-, contains one Na+ cation and two {NpO2}2+ cations held between two [PW9O34]9- anions – with an additional partial occupancy NH4 + or {NpO2}2+ cation also present. In the analogous uranium (VI) system, under similar reaction conditions that includes an excess of NH4Cl in the parent solution, it was previously shown that [(NH4)2(UVIO2)2(A-PW9O34)2]12- is the dominant species in both solution and the crystallized salt. Spectroscopic studies provide further proof of differences in the observed chemistry for the {NpO2}2+/[PW9O34]9- and {UO2}2+/[PW9O34]9- systems, both in solution and in solid state complexes crystallized from comparable salt solutions.more »
- Authors:
-
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1239107
- Report Number(s):
- LA-UR-14-27690
Journal ID: ISSN 0020-1669
- Grant/Contract Number:
- AC52-06NA25396
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Inorganic Chemistry
- Additional Journal Information:
- Journal Volume: 54; Journal Issue: 9; Journal ID: ISSN 0020-1669
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY; 12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
Citation Formats
Berg, John M., Gaunt, Andrew J., May, Iain, Pugmire, Alison L., Reilly, Sean D., Scott, Brian L., and Wilkerson, Marianne P. Unexpected Actinyl Cation-Directed Structural Variation in Neptunyl(VI) A-Type Tri-lacunary Heteropolyoxotungstate Complexes. United States: N. p., 2015.
Web. doi:10.1021/ic5024345.
Berg, John M., Gaunt, Andrew J., May, Iain, Pugmire, Alison L., Reilly, Sean D., Scott, Brian L., & Wilkerson, Marianne P. Unexpected Actinyl Cation-Directed Structural Variation in Neptunyl(VI) A-Type Tri-lacunary Heteropolyoxotungstate Complexes. United States. https://doi.org/10.1021/ic5024345
Berg, John M., Gaunt, Andrew J., May, Iain, Pugmire, Alison L., Reilly, Sean D., Scott, Brian L., and Wilkerson, Marianne P. Wed .
"Unexpected Actinyl Cation-Directed Structural Variation in Neptunyl(VI) A-Type Tri-lacunary Heteropolyoxotungstate Complexes". United States. https://doi.org/10.1021/ic5024345. https://www.osti.gov/servlets/purl/1239107.
@article{osti_1239107,
title = {Unexpected Actinyl Cation-Directed Structural Variation in Neptunyl(VI) A-Type Tri-lacunary Heteropolyoxotungstate Complexes},
author = {Berg, John M. and Gaunt, Andrew J. and May, Iain and Pugmire, Alison L. and Reilly, Sean D. and Scott, Brian L. and Wilkerson, Marianne P.},
abstractNote = {A-type tri-lacunary heteropolyoxotungstate anions (e.g., [PW9O34]9-, [AsW9O34]9-, [SiW9O34]10- and [GeW9O34]10-) are multi-dentate oxygen donor ligands that readily form sandwich complexes with actinyl cations ({UO2}2+, {NpO2}+, {NpO2}2+ & {PuO2}2+) in near neutral/slightly alkaline aqueous solutions. Two or three actinyl cations are sandwiched between two trilacunary anions, with additional cations (Na+, K+ or NH4 +) also often held within the cluster. Studies thus far have indicated that it is these additional +I cations, rather than the specific actinyl cation, that direct the structural variation in the complexes formed. We now report the structural characterization of the neptunyl (VI) cluster complex (NH4)13 [Na(NpO2)2(A-α- PW9O34)2]·12H2O. The anion in this complex, [Na(NpO2)2(PW9O34)2]13-, contains one Na+ cation and two {NpO2}2+ cations held between two [PW9O34]9- anions – with an additional partial occupancy NH4 + or {NpO2}2+ cation also present. In the analogous uranium (VI) system, under similar reaction conditions that includes an excess of NH4Cl in the parent solution, it was previously shown that [(NH4)2(UVIO2)2(A-PW9O34)2]12- is the dominant species in both solution and the crystallized salt. Spectroscopic studies provide further proof of differences in the observed chemistry for the {NpO2}2+/[PW9O34]9- and {UO2}2+/[PW9O34]9- systems, both in solution and in solid state complexes crystallized from comparable salt solutions. The work revealed that varying the actinide element (Np vs. U) can indeed measurably impact structure and complex stability in the cluster chemistry of actinyl (VI) cations with A-type tri-lacunary heteropolyoxotungstate anions.},
doi = {10.1021/ic5024345},
journal = {Inorganic Chemistry},
number = 9,
volume = 54,
place = {United States},
year = {Wed Apr 22 00:00:00 EDT 2015},
month = {Wed Apr 22 00:00:00 EDT 2015}
}
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The Coordination Geometry of Np(VII) in Alkaline Solution
journal, April 2001
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Direct Spectroscopic Characterization of Aqueous Actinyl(VI) Species: A Comparative Study of Np and U
journal, June 2009
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Crystal structure and spectroscopic measurements of room temperature intra-5f fluorescence of Cs2Np(VI)O2Cl4
journal, October 2007
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Synthesis and characterisation of two new lanthanide sandwich-type heteropolyoxometalates
journal, September 2003
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Raman spectroscopy of neptunyl and plutonyl ions in aqueous solution: hydrolysis of neptunium(VI) and plutonium(VI) and disproportionation of plutonium(V)
journal, June 1984
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Chemical Speciation of Neptunium(VI) under Strongly Alkaline Conditions. Structure, Composition, and Oxo Ligand Exchange
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Works referencing / citing this record:
Light-induced decarboxylation in a photo-responsive iron-containing complex based on polyoxometalate and oxalato ligands
journal, January 2017
- Duan, Yan; Waerenborgh, João C.; Clemente-Juan, Juan M.
- Chemical Science, Vol. 8, Issue 1