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Title: Speciation of uranium in surface-modified, hydrothermally treated, (UO{sub 2}){sup 2+}-exchanged smectite clays

Technical Report ·
DOI:https://doi.org/10.2172/515513· OSTI ID:515513
; ; ;  [1]
  1. Argonne National Lab., IL (United States). Chemistry Div.

A successful solution to the problem of disposal and permanent storage of water soluble radioactive species must address two issues: exclusion of the radionuclides from the environment and the prevention of leaching from the storage media into the environment. Immobilization of radionuclides in clay minerals has been studied. In addition to the use of clays as potential waste forms, information about the interactions of radionuclides with clays and how such interactions affect their speciations is crucial for successful modeling of actinide-migration. X-ray absorption spectroscopy (XAS) is used to determine the uranium speciation in exchanged and surface-modified clays. The XAS data from uranyl-loaded bentonite clay are compared with those obtained after the particle surfaces have been coated with alkylsilanes. These silane films, which render the surface of the clay hydrophobic, are added in order to minimize the ability of external water to exchange with the water in the clay interlayer, thereby decreasing the release rate of the exchanged-uranium species. Mild hydrothermal conditions are used in an effort to mimic potential geologic conditions that may occur during long-term radioactive waste storage. The XAS spectra indicate that the uranyl monomer species remain unchanged in most samples, except in those samples that were both coated with an alkylsilane and hydrothermally treated. When the clay was coated with an organic film, formed by the acidic deposition of octadecyltrimethoxysilane, hydrothermal treatment results in the formation of aggregated uranium species in which the uranium is reduced from U{sup VI} to U{sup IV}.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Energy Research, Washington, DC (United States)
DOE Contract Number:
W-31109-ENG-38
OSTI ID:
515513
Report Number(s):
ANL/CHM/PP-90254; ON: DE97008256; TRN: 97:014866
Resource Relation:
Other Information: PBD: [1997]
Country of Publication:
United States
Language:
English