Journal article
Aqueous Speciation of Tetravalent Actinides in the Presence of Chloride and Nitrate Ligands
Inorganic chemistry, Vol.61(37), pp.14718-14725
09/19/2022
DOI: 10.1021/acs.inorgchem.2c02064
PMID: 36050286
Abstract
Speciation of hexachloride tetravalent uranium, neptunium, and plutonium species in aqueous media has been investigated using density functional theory in the presence of inner sphere ligands such as chloride, nitrate, and solvent molecules. All possible structures with the formula [AnIV(Cl)x(H2O)y(NO3)z]4-x-z (An = U, Np, and Pu; x = 0-6, y = 0-8, and z = 0-6) were considered to explore the speciation chemical space of each actinide. The nature of the mixed-ligand complexes present in solution is controlled by the concentration of free ligands in solution. A low chloride concentration is suitable to drive the speciation away from the highly thermodynamically stable hexachloride species. Furthermore, the formation of dimeric species can proceed through both olation and oxolation mechanisms. Oxolation is preferred for monomers that contain fewer water ligands, while olation becomes favorable for complexes with more water ligands.
Details
- Title: Subtitle
- Aqueous Speciation of Tetravalent Actinides in the Presence of Chloride and Nitrate Ligands
- Creators
- Rameswar Bhattacharjee - University of South DakotaPere Miro - University of South Dakota
- Resource Type
- Journal article
- Publication Details
- Inorganic chemistry, Vol.61(37), pp.14718-14725
- Publisher
- Amer Chemical Soc
- DOI
- 10.1021/acs.inorgchem.2c02064
- PMID
- 36050286
- ISSN
- 0020-1669
- eISSN
- 1520-510X
- Number of pages
- 8
- Grant note
- Competitive Research Grant Program South Dakota Board of Regents Department of Chemistry at the University of South Dakota (USD) for start-up funds OAC-1626516 / High Performance Computing Systems at the University of South Dakota - National Science Foundation MRI Award
- Language
- English
- Date published
- 09/19/2022
- Academic Unit
- Chemistry
- Record Identifier
- 9984618515302771
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