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Title: Extension of the Plutonium Oxide Nanocluster Family to Include {Pu 16} and {Pu 22}

Abstract

Plutonium(IV) oxide nanoclusters represent an interesting scientific problem regarding structure-function relationships and are also relevant to global concerns surrounding plutonium reprocessing, the remediation of plutonium-contaminated soils, and the storage or disposal of plutonium-containing wastes. Here we report the synthesis of five unique Pu IV oxide nanoclusters containing 38,22, or 16 metal centers and capped only with inorganic ligands, such as chlorine and water, which prevent formation of the extended PuO 2 structure. The products are interrogated through single-crystal X-ray diffraction, bond valence calculations, and comparisons to other known metal-oxide nanoclusters. Of particular interest is the in-corporation of hydroxide linkages into the smaller plutonium oxide nanoclusters, which underscores previous observations and hypotheses regarding the formation of plutonium polymers and colloids.

Authors:
 [1]; ORCiD logo [1]
  1. Univ. of Notre Dame, IN (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Materials Science of Actinides (MSA); Univ. of Notre Dame, IN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1492547
Alternate Identifier(s):
OSTI ID: 1491774
Grant/Contract Number:  
NA0003763; SC0001089
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry - A European Journal
Additional Journal Information:
Journal Volume: 25; Journal ID: ISSN 0947-6539
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Sigmon, Ginger E., and Hixon, Amy E. Extension of the Plutonium Oxide Nanocluster Family to Include {Pu16} and {Pu22}. United States: N. p., 2019. Web. doi:10.1002/chem.201805605.
Sigmon, Ginger E., & Hixon, Amy E. Extension of the Plutonium Oxide Nanocluster Family to Include {Pu16} and {Pu22}. United States. doi:10.1002/chem.201805605.
Sigmon, Ginger E., and Hixon, Amy E. Thu . "Extension of the Plutonium Oxide Nanocluster Family to Include {Pu16} and {Pu22}". United States. doi:10.1002/chem.201805605. https://www.osti.gov/servlets/purl/1492547.
@article{osti_1492547,
title = {Extension of the Plutonium Oxide Nanocluster Family to Include {Pu16} and {Pu22}},
author = {Sigmon, Ginger E. and Hixon, Amy E.},
abstractNote = {Plutonium(IV) oxide nanoclusters represent an interesting scientific problem regarding structure-function relationships and are also relevant to global concerns surrounding plutonium reprocessing, the remediation of plutonium-contaminated soils, and the storage or disposal of plutonium-containing wastes. Here we report the synthesis of five unique PuIV oxide nanoclusters containing 38,22, or 16 metal centers and capped only with inorganic ligands, such as chlorine and water, which prevent formation of the extended PuO2 structure. The products are interrogated through single-crystal X-ray diffraction, bond valence calculations, and comparisons to other known metal-oxide nanoclusters. Of particular interest is the in-corporation of hydroxide linkages into the smaller plutonium oxide nanoclusters, which underscores previous observations and hypotheses regarding the formation of plutonium polymers and colloids.},
doi = {10.1002/chem.201805605},
journal = {Chemistry - A European Journal},
number = ,
volume = 25,
place = {United States},
year = {2019},
month = {1}
}

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Cited by: 4 works
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Works referenced in this record:

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    Works referencing / citing this record:

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    Self-Assembly of Polyoxo Clusters and Extended Frameworks by Controlled Hydrolysis of Low-Valent Uranium
    journal, October 2007

    • Nocton, Grégory; Burdet, Fabien; Pécaut, Jacques
    • Angewandte Chemie, Vol. 119, Issue 40
    • DOI: 10.1002/ange.200702374

    The Structure of the Plutonium Oxide Nanocluster [Pu38O56Cl54(H2O)8]14−
    journal, January 2008

    • Soderholm, L.; Almond, Philip M.; Skanthakumar, S.
    • Angewandte Chemie, Vol. 120, Issue 2
    • DOI: 10.1002/ange.200704420

    Polyoxometallate als Bausteine für funktionelle Nanosysteme
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    • Long, De-Liang; Tsunashima, Ryo; Cronin, Leroy
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    • DOI: 10.1002/ange.200902483

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    • Biswas, Biplab; Mougel, Victor; Pécaut, Jacques
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    • Falaise, Clément; Volkringer, Christophe; Hennig, Christoph
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    • DOI: 10.1002/chem.201502207

    Coordination of Tetravalent Actinides (An=Th IV , U IV , Np IV , Pu IV ) with DOTA: From Dimers to Hexamers
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    • Tamain, Christelle; Dumas, Thomas; Hennig, Christoph
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    • DOI: 10.1002/chem.201700493

    First Hexanuclear U IV and Th IV Formate Complexes - Structure and Stability Range in Aqueous Solution : First Hexanuclear U
    journal, October 2009

    • Takao, Shinobu; Takao, Koichiro; Kraus, Werner
    • European Journal of Inorganic Chemistry, Vol. 2009, Issue 32
    • DOI: 10.1002/ejic.200900899

    Self-Assembly of Hexanuclear Clusters of 4f and 5f Elements with Cation Specificity
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    • DOI: 10.1002/ejic.201600656

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    • Costanzo, D. A.; Biggers, R. E.; Bell, J. T.
    • Journal of Inorganic and Nuclear Chemistry, Vol. 35, Issue 2
    • DOI: 10.1016/0022-1902(73)80575-5

    Uranyl Peroxide Cage Cluster Solubility in Water and the Role of the Electrical Double Layer
    journal, January 2017


    Clusters of Actinides with Oxide, Peroxide, or Hydroxide Bridges
    journal, October 2012

    • Qiu, Jie; Burns, Peter C.
    • Chemical Reviews, Vol. 113, Issue 2
    • DOI: 10.1021/cr300159x

    Lanthanide-Based Luminescent Hybrid Materials
    journal, September 2009


    Polyoxometalate-Based Molecular Materials
    journal, February 1998

    • Coronado, Eugenio; Gómez-García, Carlos J.
    • Chemical Reviews, Vol. 98, Issue 1
    • DOI: 10.1021/cr970471c

    XAFS and LIBD Investigation of the Formation and Structure of Colloidal Pu(IV) Hydrolysis Products
    journal, July 2004

    • Rothe, Jörg; Walther, Clemens; Denecke, Melissa A.
    • Inorganic Chemistry, Vol. 43, Issue 15
    • DOI: 10.1021/ic049861p

    Formation of Soluble Hexanuclear Neptunium(IV) Nanoclusters in Aqueous Solution: Growth Termination of Actinide(IV) Hydrous Oxides by Carboxylates
    journal, January 2012

    • Takao, Koichiro; Takao, Shinobu; Scheinost, Andreas C.
    • Inorganic Chemistry, Vol. 51, Issue 3
    • DOI: 10.1021/ic201482n

    Thorium(IV) Molecular Clusters with a Hexanuclear Th Core
    journal, October 2011

    • Knope, Karah E.; Wilson, Richard E.; Vasiliu, Monica
    • Inorganic Chemistry, Vol. 50, Issue 19
    • DOI: 10.1021/ic2014946

    Periodic Trends in Hexanuclear Actinide Clusters
    journal, March 2012

    • Diwu, Juan; Wang, Shuao; Albrecht-Schmitt, Thomas E.
    • Inorganic Chemistry, Vol. 51, Issue 7
    • DOI: 10.1021/ic2023242

    Plutonium(IV) Cluster with a Hexanuclear [Pu 6 (OH) 4 O 4 ] 12+ Core
    journal, May 2013

    • Knope, Karah E.; Soderholm, L.
    • Inorganic Chemistry, Vol. 52, Issue 12
    • DOI: 10.1021/ic4007185

    Local and Nanoscale Structure and Speciation in the PuO 2+ x - y (OH) 2 y · z H 2 O System
    journal, October 2004

    • Conradson, Steven D.; Begg, Bruce D.; Clark, David L.
    • Journal of the American Chemical Society, Vol. 126, Issue 41
    • DOI: 10.1021/ja049192e

    Isolation of the Large {Actinide} 38 Poly-oxo Cluster with Uranium
    journal, October 2013

    • Falaise, Clément; Volkringer, Christophe; Vigier, Jean-François
    • Journal of the American Chemical Society, Vol. 135, Issue 42
    • DOI: 10.1021/ja4067207

    Insights into the sonochemical synthesis and properties of salt-free intrinsic plutonium colloids
    journal, March 2017

    • Dalodière, Elodie; Virot, Matthieu; Morosini, Vincent
    • Scientific Reports, Vol. 7, Issue 1
    • DOI: 10.1038/srep43514

    A comprehensive comparison of transition-metal and actinyl polyoxometalates
    journal, January 2012

    • Nyman, May; Burns, Peter C.
    • Chemical Society Reviews, Vol. 41, Issue 22
    • DOI: 10.1039/c2cs35136f

    Structure and stability range of a hexanuclear Th(iv)–glycine complex
    journal, January 2012

    • Hennig, Christoph; Takao, Shinobu; Takao, Koichiro
    • Dalton Transactions, Vol. 41, Issue 41
    • DOI: 10.1039/c2dt31367g