Evolution of Chemical Conditions and Estimated Plutonium Solubility in the Residual Waste Layer During Post-Closure Aging of Tank 18.

摘要

This document updates the Eh-pH transitions from grout aging simulations and the plutonium waste release model of Denham (2007, Rev. 1) based on new data. New thermodynamic data for cementitious minerals are used for the grout simulations. Newer thermodynamic data, recommended by plutonium experts (Plutonium Solubility Peer Review Report, LA-UR-12- 00079 ), are used to estimate solubilities of plutonium at various pore water compositions expected during grout aging. In addition, a new grout formula is used in the grout aging simulations and apparent solubilities of coprecipitated plutonium are estimated using data from analysis of Tank 18 residual waste. The conceptual model of waste release and the grout aging simulations are done in a manner similar to that of Denham (2007, Rev. 1). It is assumed that the pore fluid composition passing from the tank grout into the residual waste layer controls the solubility, and hence the waste release concentration of plutonium. Pore volumes of infiltrating fluid of an assumed composition are reacted with a hypothetical grout block using The Geochemists Workbench and changes in pore fluid chemistry correspond to the number of pore fluid volumes reacted. As in the earlier document, this results in three states of grout pore fluid composition throughout the simulation period that are termed Reduced Region II, Oxidized Region II, and Oxidized Region III. The one major difference from the earlier document is that pyrite is used to account for reducing capacity of the tank grout rather than pyrrhotite.