The structure of plutonium(IV) oxide as hydrolysed clusters in aqueous suspensions
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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| Published in | Dalton transactions : an international journal of inorganic chemistry Vol. 42; no. 6; pp. 2035 - 2040 |
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| Main Authors | , , , , |
| Format | Journal Article |
| Language | English |
| Published |
England
01.01.2013
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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. |
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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. 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 sub(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. 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. 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. |
| Author | Persson, Ingmar Ödegaard-Jensen, Arvid Skarnemark, Gunnar Ekberg, Christian Larsson, Kristian |
| Author_xml | – sequence: 1 givenname: Christian surname: Ekberg fullname: Ekberg, Christian email: che@chalmers.se organization: Nuclear Chemistry/Industrial materials recycling, Chalmers University of Technology, SE-412 96 Göteborg, Sweden. che@chalmers.se – 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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| Cites_doi | 10.1524/ract.1978.25.34.139 10.1088/0370-1328/78/5/317 10.1002/anie.200704420 10.1524/ract.1989.48.34.145 10.1021/ja01100a011 10.1007/978-94-009-4077-2 10.1107/S0567739476001551 10.1039/jr9470001010 10.1016/0022-1902(81)80645-8 10.1103/PhysRevB.52.2995 10.1023/A:1005166517699 10.1524/ract.2009.1595 10.1016/S0022-3115(00)00392-5 10.1126/science.287.5451.285 10.1016/0925-8388(95)02122-1 10.1016/0022-1902(73)80577-9 10.1021/ic0346477 10.1107/S0365110X49001016 10.1016/S0022-3115(96)00709-X 10.1524/ract.2007.95.4.193 10.1021/ic049861p 10.1107/S0021889804022885 10.1021/ic00335a028 10.1021/ja01611a108 10.1021/ic901763s 10.1039/jr9560003358 10.1524/ract.2000.88.9-11.527 10.1557/S0883769400048703 |
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| Snippet | The behavior of plutonium still puzzles scientists 70 years after its discovery. There are several factors making the chemistry of plutonium interesting... |
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| SubjectTerms | Atomic structure behavior Bonding Clusters Colloids Colloids - chemistry Crystal structure dioxide Hydrolysis Inorganic Chemistry Oorganisk kemi Oxidation-Reduction Oxides Oxides - chemistry Plutonium Plutonium - chemistry polymerization products pu(iv) solubility spectra uo2 Valence water Water - chemistry |
| Title | The structure of plutonium(IV) oxide as hydrolysed clusters in aqueous suspensions |
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