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Modeling of the Effects of Radiolysis on UO2-dissolution Employing Recent Experimental Data

Published online by Cambridge University Press:  01 February 2011

Mats Jonsson ,
Fredrik Nielsen ,
Ella Ekeroth  and
Trygve E. Eriksen
Mats Jonsson
Affiliation:
Department of Chemistry, Nuclear Chemistry, Royal Institute of Technology, SE-100 44 Stockholm, Sweden
Fredrik Nielsen
Affiliation:
Department of Chemistry, Nuclear Chemistry, Royal Institute of Technology, SE-100 44 Stockholm, Sweden
Ella Ekeroth
Affiliation:
Department of Chemistry, Nuclear Chemistry, Royal Institute of Technology, SE-100 44 Stockholm, Sweden
Trygve E. Eriksen
Affiliation:
Department of Chemistry, Nuclear Chemistry, Royal Institute of Technology, SE-100 44 Stockholm, Sweden
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Abstract

This study examines the effect of water radiolysis on the dissolution of uranium dioxide. A model is created to describe the system of uranium dioxide fragments in water, and the production and reactions of radiolysis products (using recent kinetic data). The system is evaluated under different conditions using MAKSIMA-CHEMIST. Conditions examined include presence of carbonate in the water and effects of hydrogen. The simulations are compared to experimental results on spent fuel dissolution. Surprisingly, the simulated U(VI)-release agrees within a factor of three with the experimentally found U(VI)-release. The inhibiting effect of hydrogen is clearly demonstrated by the simulations. From the results of the simulations we are also able to conclude that the main inhibiting effect of H2 is the reaction with OH• and not the reduction of U(VI) to U(IV).

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 807: Symposium Scientific Basis for Nuclear Waste Management XXVII , 2003 , 385
Copyright
Copyright © Materials Research Society 2004

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References

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