Development and application of the Nagra/PSI Chemical Thermodynamic Data Base 01/01

Abstract

AbstractThe Nagra/PSI Chemical Thermodynamic Data Base is a critical selection of thermodynamic data used to support performance assessments for planned radioactive waste repositories in Switzerland. For this purpose, the data base is focused on actinides and fission products, but also includes additional data for major elements occurring in common groundwaters. Recently, a peer-reviewed update was carried out (from data base version 05/92 to 01/01) involving major revisions for most actinides and fission products. Altogether, more than 70% of the data base contents have been revised. Most of the thermodynamic data for U, Np, Pu, Am, and Tc were adopted from the reviews by the NEA TDB project. In contrast, data for Th, Sn, Eu, Pd, Al, as well as the solubility and metal complexation of sulphides and silicates, were extensively reviewed. Less effort was put into the review of data for Zr, Ni, and Se as these elements are currently being reviewed in Phase II of the NEA TDB project. The data for metal complexation with organic ligands from data base version 05/92 were not included in this update. They will be reconsidered in a future update, after completion of the NEA TDB Phase II review of organic ligands. The chemical consistency of the selected data was checked with empirical rules related to the periodic properties of the elements and with correlations based on charge/size relations. As a result of the update, major gaps in the data base could be identified, especially with respect to missing carbonate complexes. In some systems, for example, Th(IV)-H2O and U(IV)-H2O, conflicting experimental data cannot be described by a unique set of thermodynamic constants and a pragmatic approach closely reproducing measured solubility data was chosen for application to performance assessment. The electronic version of the Nagra/PSI Chemical Thermodynamic Data Base 01/01 and information concerning its full documentation is available on the PSI web site.