Atomistic Simulations of Uranium Incorporation into Iron (Hydr)Oxides.
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| Title: | Atomistic Simulations of Uranium Incorporation into Iron (Hydr)Oxides. |
|---|---|
| Authors: | Kerisit, Sebastien1 sebastien.kerisit@pnl.gov, Felmy, Andrew R.1, Ilton, Eugene S.1 |
| Source: | Environmental Science & Technology. 4/1/2011, Vol. 45 Issue 7, p2770-2776. 7p. |
| Subject Terms: | *Environmental chemistry, *Iron oxides, *Oxidation-reduction reaction, Coordination compounds, Research methodology, Simulation methods & models, Migration of uranium, Radioactive waste characterization |
| Abstract: | Atomistic simulations were carried out to characterize the coordination environments of U incorporated in three Fe-(hydr)oxide minerals, goethite, magnetite, and hematite. The simulations provided information on U-O and U-Fe distances, coordination numbers, and lattice distortion for U incorporated in different sites (e.g., unoccupied versus occupied sites, octahedral versus tetrahedral) as a function of the oxidation state of U and charge compensation mechanisms (i.e., deprotonation, vacancy formation, or reduction of Fe(III) to Fe(II)). For goeshite, deprotonation of first shell hydroxyls enables substitution of U for Fe(III) with a minimal amount of lattice distortion, whereas substitution in unoccupied octahedral sites induced appreciable distortion to 7-fold coordination regardless of U oxidation states and charge compensation mechanisms. Importantly, U-Fe distances of ∼3.6A were associated with structural incorporation of U and cannot be considered diagnostic of simple adsorption to goethite surfaces. For magnetite, the octahedral site accommodates U(V) or U(VI) with little lattice distortion. U substituted for Fe(III) in hematite maintained octahedral coordination in most cases. In general, comparison of the simulations with available experimental data provides further evidence for the structural incorporation of U in iron (hydr)oxide minerals. [ABSTRACT FROM AUTHOR] |
| Copyright of Environmental Science & Technology is the property of American Chemical Society and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.) | |
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| FullText | Text: Availability: 0 |
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| Header | DbId: 8gh DbLabel: GreenFILE An: 60712446 AccessLevel: 6 PubType: Academic Journal PubTypeId: academicJournal PreciseRelevancyScore: 0 |
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| Items | – Name: Title Label: Title Group: Ti Data: Atomistic Simulations of Uranium Incorporation into Iron (Hydr)Oxides. – Name: Author Label: Authors Group: Au Data: <searchLink fieldCode="AR" term="%22Kerisit%2C+Sebastien%22">Kerisit, Sebastien</searchLink><relatesTo>1</relatesTo><i> sebastien.kerisit@pnl.gov</i><br /><searchLink fieldCode="AR" term="%22Felmy%2C+Andrew+R%2E%22">Felmy, Andrew R.</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Ilton%2C+Eugene+S%2E%22">Ilton, Eugene S.</searchLink><relatesTo>1</relatesTo> – Name: TitleSource Label: Source Group: Src Data: <searchLink fieldCode="JN" term="%22Environmental+Science+%26+Technology%22">Environmental Science & Technology</searchLink>. 4/1/2011, Vol. 45 Issue 7, p2770-2776. 7p. – Name: Subject Label: Subject Terms Group: Su Data: *<searchLink fieldCode="DE" term="%22Environmental+chemistry%22">Environmental chemistry</searchLink><br />*<searchLink fieldCode="DE" term="%22Iron+oxides%22">Iron oxides</searchLink><br />*<searchLink fieldCode="DE" term="%22Oxidation-reduction+reaction%22">Oxidation-reduction reaction</searchLink><br /><searchLink fieldCode="DE" term="%22Coordination+compounds%22">Coordination compounds</searchLink><br /><searchLink fieldCode="DE" term="%22Research+methodology%22">Research methodology</searchLink><br /><searchLink fieldCode="DE" term="%22Simulation+methods+%26+models%22">Simulation methods & models</searchLink><br /><searchLink fieldCode="DE" term="%22Migration+of+uranium%22">Migration of uranium</searchLink><br /><searchLink fieldCode="DE" term="%22Radioactive+waste+characterization%22">Radioactive waste characterization</searchLink> – Name: Abstract Label: Abstract Group: Ab Data: Atomistic simulations were carried out to characterize the coordination environments of U incorporated in three Fe-(hydr)oxide minerals, goethite, magnetite, and hematite. The simulations provided information on U-O and U-Fe distances, coordination numbers, and lattice distortion for U incorporated in different sites (e.g., unoccupied versus occupied sites, octahedral versus tetrahedral) as a function of the oxidation state of U and charge compensation mechanisms (i.e., deprotonation, vacancy formation, or reduction of Fe(III) to Fe(II)). For goeshite, deprotonation of first shell hydroxyls enables substitution of U for Fe(III) with a minimal amount of lattice distortion, whereas substitution in unoccupied octahedral sites induced appreciable distortion to 7-fold coordination regardless of U oxidation states and charge compensation mechanisms. Importantly, U-Fe distances of ∼3.6A were associated with structural incorporation of U and cannot be considered diagnostic of simple adsorption to goethite surfaces. For magnetite, the octahedral site accommodates U(V) or U(VI) with little lattice distortion. U substituted for Fe(III) in hematite maintained octahedral coordination in most cases. In general, comparison of the simulations with available experimental data provides further evidence for the structural incorporation of U in iron (hydr)oxide minerals. [ABSTRACT FROM AUTHOR] – Name: AbstractSuppliedCopyright Label: Group: Ab Data: <i>Copyright of Environmental Science & Technology is the property of American Chemical Society and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.) |
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| RecordInfo | BibRecord: BibEntity: Identifiers: – Type: doi Value: 10.1021/es1037639 Languages: – Code: eng Text: English PhysicalDescription: Pagination: PageCount: 7 StartPage: 2770 Subjects: – SubjectFull: Environmental chemistry Type: general – SubjectFull: Iron oxides Type: general – SubjectFull: Oxidation-reduction reaction Type: general – SubjectFull: Coordination compounds Type: general – SubjectFull: Research methodology Type: general – SubjectFull: Simulation methods & models Type: general – SubjectFull: Migration of uranium Type: general – SubjectFull: Radioactive waste characterization Type: general Titles: – TitleFull: Atomistic Simulations of Uranium Incorporation into Iron (Hydr)Oxides. Type: main BibRelationships: HasContributorRelationships: – PersonEntity: Name: NameFull: Kerisit, Sebastien – PersonEntity: Name: NameFull: Felmy, Andrew R. – PersonEntity: Name: NameFull: Ilton, Eugene S. IsPartOfRelationships: – BibEntity: Dates: – D: 01 M: 04 Text: 4/1/2011 Type: published Y: 2011 Identifiers: – Type: issn-print Value: 0013936X Numbering: – Type: volume Value: 45 – Type: issue Value: 7 Titles: – TitleFull: Environmental Science & Technology Type: main |
| ResultId | 1 |
