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Modelling Experimental Results on Radiolytic Processes at the Spent Fuel Water Interface. I. Radiolysis Products and U Release

Published online by Cambridge University Press:  01 February 2011

J. Bruno ,
E. Cera ,
T. E. Eriksen ,
M. Grivé  and
S. Ripoll
J. Bruno
Affiliation:
Enviros Spain SL, Pg. de Rubí 29–31, 08197 Valldoreix (Spain)
E. Cera
Affiliation:
Enviros Spain SL, Pg. de Rubí 29–31, 08197 Valldoreix (Spain)
T. E. Eriksen
Affiliation:
Dept. Nuclear Chemistry, KTH, 100 44 Stockholm (Sweden)
M. Grivé
Affiliation:
Enviros Spain SL, Pg. de Rubí 29–31, 08197 Valldoreix (Spain)
S. Ripoll
Affiliation:
Enviros Spain SL, Pg. de Rubí 29–31, 08197 Valldoreix (Spain)
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Abstract

Experimental and modelling efforts in the last decade in the frame of nuclear waste management field have been focused on studying the role of the UO2 surfaces in poising the redox state of solid/water systems. For this purpose, an experimental programme was developed consisting on dissolution experiments with PWR spent fuel fragments in an anoxic environment and by using different solution compositions.

The collected data so far, indicate that production and fate of radiolysis products follow the same trends independently on the solution composition used in the tests. Hydrogen and oxygen concentrations show an initial increase with time until reaching a constant concentration. The trend observed for hydrogen peroxide is a decrease at short contact times to reach again a constant concentration with time. These steady-states indicate an overall balance of the generated radiolytic species.

Modelling work indicates that uranium dissolution is controlled by the oxidation of the spent fuel matrix in 10mM bicarbonate solutions while in the tests carried out at lower or without carbonate concentrations uranium in the aqueous phase is governed by the precipitation of schoepite.

These results are determinant to highlight that reducing conditions are restored in the aqueous phase in relatively short periods of time and at short distances away from the dynamic redox spent fuel/water interface.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 807: Symposium Scientific Basis for Nuclear Waste Management XXVII , 2003 , 397
Copyright
Copyright © Materials Research Society 2004

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References

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