The structure of plutonium(iv) oxide as hydrolysed clusters in aqueous suspensionsElectronic supplementary information (ESI) available. See DOI: 10.1039/c2dt32185h
The behavior of plutonium still puzzles scientists 70 years after its discovery. There are several factors making the chemistry of plutonium interesting including its ability to keep several oxidation states. Another unique property is that the oxidation states +III, +IV, +V and +VI may exist simult...
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Abstract | The behavior of plutonium still puzzles scientists 70 years after its discovery. There are several factors making the chemistry of plutonium interesting including its ability to keep several oxidation states. Another unique property is that the oxidation states +III, +IV, +V and +VI may exist simultaneously in solution. Another property plutonium shares with some other tetravalent metal ions is the ability to form stable polynuclear complexes or colloids. The structures of freshly prepared and five-year old plutonium(
iv
) colloids are compared with crystalline plutonium(
iv
) oxide using Pu L
3
-edge EXAFS. It was shown that as the plutonium colloids age they do in fact shrink in size, contrary to previous expectations. The aged colloidal particles are indeed very small with only 3-4 plutonium atoms, and with a structure very similar to solid plutonium(
iv
) oxide, but with somewhat shorter mean Pu-O bond and Pu Pu distances indicating a partial oxidation. The very small size of the colloidal particles is further supported by the fact that they do not sediment on heavy ultra-centrifugation.
At the formation of plutonium oxide colloids most particles are sufficiently large to sediment easily. However, a minor fraction is sufficiently small to form a stable suspension. The change in the size and structure of these colloidal particles has been studied over five years. |
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AbstractList | The behavior of plutonium still puzzles scientists 70 years after its discovery. There are several factors making the chemistry of plutonium interesting including its ability to keep several oxidation states. Another unique property is that the oxidation states +III, +IV, +V and +VI may exist simultaneously in solution. Another property plutonium shares with some other tetravalent metal ions is the ability to form stable polynuclear complexes or colloids. The structures of freshly prepared and five-year old plutonium(
iv
) colloids are compared with crystalline plutonium(
iv
) oxide using Pu L
3
-edge EXAFS. It was shown that as the plutonium colloids age they do in fact shrink in size, contrary to previous expectations. The aged colloidal particles are indeed very small with only 3-4 plutonium atoms, and with a structure very similar to solid plutonium(
iv
) oxide, but with somewhat shorter mean Pu-O bond and Pu Pu distances indicating a partial oxidation. The very small size of the colloidal particles is further supported by the fact that they do not sediment on heavy ultra-centrifugation.
At the formation of plutonium oxide colloids most particles are sufficiently large to sediment easily. However, a minor fraction is sufficiently small to form a stable suspension. The change in the size and structure of these colloidal particles has been studied over five years. |
Author | Persson, Ingmar Ödegaard-Jensen, Arvid Skarnemark, Gunnar Larsson, Kristian Ekberg, Christian |
AuthorAffiliation | Department of Chemistry Nuclear Chemistry/Industrial materials recycling Swedish University of Agricultural Sciences Chalmers University of Technology |
AuthorAffiliation_xml | – name: Chalmers University of Technology – name: Swedish University of Agricultural Sciences – name: Department of Chemistry – name: Nuclear Chemistry/Industrial materials recycling |
Author_xml | – sequence: 1 givenname: Christian surname: Ekberg fullname: Ekberg, Christian – sequence: 2 givenname: Kristian surname: Larsson fullname: Larsson, Kristian – sequence: 3 givenname: Gunnar surname: Skarnemark fullname: Skarnemark, Gunnar – sequence: 4 givenname: Arvid surname: Ödegaard-Jensen fullname: Ödegaard-Jensen, Arvid – sequence: 5 givenname: Ingmar surname: Persson fullname: Persson, Ingmar |
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DOI | 10.1039/c2dt32185h |
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References | 257 |
References_xml | – issn: 1970 publication-title: The Chemistry of Plutonium doi: Cleveland – issn: 2004 publication-title: The Chemistry of Plutonium Solubility doi: Nilsson – issn: 2006 publication-title: Investigation of the Behaviour of Gaseous I and RuO in Different Atmospheres doi: Holm – issn: 2003 publication-title: Update on the Chemical Thermodynamics of Uranium, Neptunium, Plutonium, Americium and Technetium, Chemical Thermodynamics doi: Guillaumont Fanghänel Fuger Grenthe Neck Palmer Rand – issn: 2006 issue: 2 end-page: 813-1203 publication-title: The Chemistry of Actinide and Transactinide Elements doi: Clark Hecker Jarvinen Neu – issn: 1988 publication-title: X-Ray Absorption Principles, Applications and Techniques of EXAFS, SEXAFS and XANES doi: Sayers Bunker – issn: 2001 publication-title: Chemical Thermodynamics of Neptunium and Plutonium, Vol. 4 of Chemical Thermodynamics doi: Lemire Fuger Nitsche Potter Rand Rydberg Spahiu Sullivan Ullman Vitorge Wanner – issn: 1978 volume-title: Technical Report TM-6365 doi: Johnson Toth – issn: 1993 publication-title: EXAFSPAK - A Suite of Computer Programs for Analysis of X-Ray Absorption Spectra doi: George Pickering – issn: 1984 issue: 44 end-page: 359-368 publication-title: Scientific Basis for Nuclear Waste Managemant VIII doi: Kim Treiber Lierse – issn: 1986 publication-title: Chemistry of the Actinide Elements doi: Katz – issn: 1987 publication-title: Chemistry: Principles and Applications doi: Chatterjee Magee – issn: 1993 issue: 294 volume-title: Scientific basis for nuclear waste management XVI end-page: 739-745 publication-title: Materials Research Society Symposia Proceedings doi: Weger Okajima Cunnane Reed – issn: 1996 doi: Ankudinov – issn: 1983 issue: 26 end-page: 867-873 publication-title: Materials Research Society Annual Meeting doi: Newton Rundberg – issn: 1949 end-page: 295 publication-title: The Transuranium Elements doi: Kasha – issn: 2008 – publication-title: Rates and Mechanisms of Radioactive Release and Retention Inside a Waste Disposal Canister – issn: 2008 publication-title: PuO and Spent Nuclear Fuel Matrix Dissolution Under Respository Conditions doi: Ödegaard-Jensen – issn: 1956 volume-title: Int. Conf. on the Peaceful Use of Atomic Energy year: 257 end-page: 245 doi: Kraus |
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Title | The structure of plutonium(iv) oxide as hydrolysed clusters in aqueous suspensionsElectronic supplementary information (ESI) available. See DOI: 10.1039/c2dt32185h |
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