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Spectrophotometric and Calorimetric Studies of U(VI) Complexation with Sulfate at 25-70oC

Journal Article · · Journal of Chemical Thermodynamics
OSTI ID:959416
Sulfate, one of the inorganic constituents in the groundwater of nuclear waste repository, could affect the migration of radioactive materials by forming complexes. Spectrophotometric and microcalorimetric titrations were performed to identify the U(VI)/sulfate complexes and determine the equilibrium constants and enthalpy of complexation at 25-70 C. Results show that U(VI) forms moderately strong complexes with sulfate, i.e., UO{sub 2}SO{sub 4}(aq) and UO{sub 2}(SO{sub 4}){sub 2}{sup 2-}, in this temperature range and the complexes become stronger as the temperature is increased: 2-fold and 10-fold increases in the stability constants of UO{sub 2}SO{sub 4}(aq) and UO{sub 2}(SO{sub 4}{sub 2}{sup 2-}), respectively, when the temperature is increased from 25 C to 70 C. The complexation is endothermic and entropy-driven, showing typical characteristics of inner-sphere complexation and 'hard acid'/'hard base' interactions. The thermodynamic trends are discussed in terms of dehydration of both the cation (UO{sub 2}{sup 2+}) and the anion (SO{sub 4}{sup 2-}) as well as the effect of temperature on the structure of water.
Research Organization:
Ernest Orlando Lawrence Berkeley National Laboratory, Berkeley, CA (US)
Sponsoring Organization:
Chemical Sciences Division
DOE Contract Number:
AC02-05CH11231
OSTI ID:
959416
Report Number(s):
LBNL-1408E
Journal Information:
Journal of Chemical Thermodynamics, Journal Name: Journal of Chemical Thermodynamics; ISSN JCTDAF; ISSN 0021-9614
Country of Publication:
United States
Language:
English

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