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A Mechanistic Model of Spent Fuel Dissolution, Secondary Mineral Precipitation, and Np Release

Published online by Cambridge University Press:  10 February 2011

Y. Chen
Affiliation:
Duke Engineering & Services, Performance Assessment Operations, CRWMS M&O, 1261 Town Center Drive, Las Vegas, NV 89134, USA.
E. Siegmann
Affiliation:
Duke Engineering & Services, Performance Assessment Operations, CRWMS M&O, 1261 Town Center Drive, Las Vegas, NV 89134, USA.
P. Mattie
Affiliation:
Duke Engineering & Services, Performance Assessment Operations, CRWMS M&O, 1261 Town Center Drive, Las Vegas, NV 89134, USA.
J. McNeish
Affiliation:
Duke Engineering & Services, Performance Assessment Operations, CRWMS M&O, 1261 Town Center Drive, Las Vegas, NV 89134, USA.
S. D. Sevougian
Affiliation:
Duke Engineering & Services, Performance Assessment Operations, CRWMS M&O, 1261 Town Center Drive, Las Vegas, NV 89134, USA.
R. Andrews
Affiliation:
Duke Engineering & Services, Performance Assessment Operations, CRWMS M&O, 1261 Town Center Drive, Las Vegas, NV 89134, USA.
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Abstract

A mechanistic spent fuel dissolution model has been developed, based on the generalreaction-transport code of AREST-CT. It considers the dissolution of spent fuel under flow conditions. The kinetic reactions of spent fuel dissolution and precipitation of schoepite, uranophane, soddyite, and Na-boltwoodite are included in the model. The results of model prediction are compared against the results of drip-tests that simulate the conditions that may occur in the Yucca Mountain Repository. Comparison shows that the modeling results match the laboratory observations very well and no contradiction has been found. It indicates that the model is a reasonably good representation of the real system.

After validation, the model was used to investigate the release rate of Np from the dissolution of secondary uranyl minerals by examining various degrees of Np incorporation into secondary uranyl minerals. The predicted Np concentration in the aqueous phase is 3 orders of magnitude lower than the upper-bound of the Np solubility range currently used in DOE performance assessment analyses. It suggests that the Np solubility range currently used is too conservative and could be replaced with more realistic values.

Type
Research Article
Copyright
Copyright © Materials Research Society 1999

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References

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