Molecular models for actinide speciation

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Much effort has been devoted to the development of sensitive spectroscopic techniques for the study of actinide speciation based on the sensitivity of f-f electronic absorption bands to oxidation state and ligation of the actinide ions. These efforts assume that data obtained in such studies will be interpretable in terms of changes in complexation of the metal center. However, the current understanding of 5f electronic structure is based on data from solid state doped single crystals. In those studies, the local coordination geometry about the central actinide ion is maintained in an almost perfect high-symmetry environment and will have little ... continued below

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32 p.

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Clark, D.L.; Watkin, J.G.; Morris, D.E. & Berg, J.M. June 1, 1994.

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Description

Much effort has been devoted to the development of sensitive spectroscopic techniques for the study of actinide speciation based on the sensitivity of f-f electronic absorption bands to oxidation state and ligation of the actinide ions. These efforts assume that data obtained in such studies will be interpretable in terms of changes in complexation of the metal center. However, the current understanding of 5f electronic structure is based on data from solid state doped single crystals. In those studies, the local coordination geometry about the central actinide ion is maintained in an almost perfect high-symmetry environment and will have little relevance for species in solution where deviations from perfect high symmetry tend to be the rule rather than the exception. The authors have developed a vigorous research program in the systematic preparation and spectroscopic characterization of synthetic actinide complexes (Th, U, Np, and Pu) in which they can control nuclearity, oxidation state, and molecular structure. These complexes have been used to determine how observable electronic transitions are perturbed in response to structural changes in the complex in solution. From the spectra obtained for these model complexes, the authors have found that the f-f transitions naturally fall into obvious groupings by coordination number and symmetry by which they can now differentiate between monomeric, dimeric, and trimeric species in solution. The study of radionuclide speciation is fundamentally important to the determination of radionuclide solubility in the groundwater at Yucca Mountain.

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32 p.

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INIS; OSTI as DE94012370

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  • Other Information: PBD: Jun 1994

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  • Other: DE94012370
  • Report No.: LA--12780-MS
  • Grant Number: W-7405-ENG-36
  • DOI: 10.2172/145191 | External Link
  • Office of Scientific & Technical Information Report Number: 145191
  • Archival Resource Key: ark:/67531/metadc620939

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Office of Scientific & Technical Information Technical Reports

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  • June 1, 1994

Added to The UNT Digital Library

  • June 16, 2015, 7:43 a.m.

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  • Feb. 29, 2016, 10:02 p.m.

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Clark, D.L.; Watkin, J.G.; Morris, D.E. & Berg, J.M. Molecular models for actinide speciation, report, June 1, 1994; New Mexico. (digital.library.unt.edu/ark:/67531/metadc620939/: accessed June 22, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.