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Title: Uranium(VI) adsorption to ferrihydrite: Application of a surface complexation model

Journal Article · · Geochimica et Cosmochimica Acta
;  [1];  [2]; ;  [3]
  1. Australian Nuclear Science and Technology Organisation, Menai (Australia)
  2. Geological Survey, Menlo Park, CA (United States)
  3. Stanford Univ., CA (United States)

A study of U(VI) adsorption by ferrihydrite was conducted over a wide range of U(VI) concentrations, pH, and at two partial pressures of carbon dioxide. A two-site (strong- and weak-affinity sites, {triple_bond}Fe{sub s}OH and {triple_bond}Fe{sub w}OH, respectively) surface complexation model was able to describe the experimental data well over a wide range of conditions, with only one species formed with each site type: an inner-sphere, mononuclear, bidentate complex of the type ({triple_bond}FeO{sub 2})UO{sub 2}. The existence of such a surface species was supported by results of uranium EXAFS spectroscopy performed on two samples with U(VI) adsorption density in the upper range observed in this study (10 and 18% occupancy of total surface sites). Adsorption data in the alkaline pH range suggested the existence of a second surface species, modeled as a ternary surface complex with UO{sub 2}CO{sub 3}{sup 0} binding to a bidentate surface site. Previous surface complexation models for U(VI) adsorption have proposed surface species that are identical to the predominant aqueous species, e.g., multinuclear hydrolysis complexes or several U(VI)-carbonate complexes. The results demonstrate that the speciation of adsorbed U(VI) may be constrained by the coordination environment at the surface, giving rise to surface speciation for U(VI) that is significantly less complex than aqueous speciation.

OSTI ID:
28813
Journal Information:
Geochimica et Cosmochimica Acta, Vol. 58, Issue 24; Other Information: PBD: Dec 1994
Country of Publication:
United States
Language:
English