Mass transfer and transport in a geologic environment

Abstract

This report is in a continuing series of reports that present analytic solutions for the dissolution and hydrogeologic transport of radionuclides from geologic repositories of nuclear waste. Previous reports have dealt mainly with radionuclide transport in the far-field, away from the effects of the repository. In the present report, the emphasis is on near-field processes, the transfer and transport of radionuclides in the vicinity of the waste packages. The primary tool used in these analyses is mass transfer theory from chemical engineering. The thrust of our work is to develop methods for predicting the performance of geologic repositories. The subjects treated in the present report are: radionuclide transport from a spherical-equivalent waste form through a backfill; analysis of radionuclide transport through a backfill using a non-linear sorption isotherm; radionuclide transport from a prolate spheroid-equivalent waste form with a backfill; radionuclide transport from a spherical-equivalent waste form through a backfill, where the solubility, diffusivity and retardation coefficients are temperature dependent; a coupled near-field, far-field analysis where dissolution and migration rates are temperature dependent; transport of radionuclides from a point source in a three-dimensional flow field; and a general solution for the transport of radioactive chains in geologic media. There are several important results from the numerical evaluations. First, radioactive decay, higher sorption in the rock and the backfill steepens the gradient for mass transfer, and lead to higher dissolution rates. This is contrary to what was expected by some other workers, but is shown clearly in the analytical solutions. Second, the backfill serves to provide sorption sites so that there is a delay in the arrival of radionuclides in the rock, although this effect is not so important for the steady-state transport of long-lived radionuclides.