This report documents numerical flow and transport simulations performed that establish initial waste acceptance criteria for the potential waste streams that may be safely sequestered in the 221-U Building and similar canyon structures. Specifically, simulations were executed to identify the maximum loading of contaminant mass (without respect to volume) that can be emplaced within the 221-U Building with no more than 1 pCi/m2 of contaminant migrating outside the structure within a 1,000 year time period. The initial scoping simulations were executed in one dimension to assess important processes, and then two dimensions to establish waste acceptance criteria. Two monolithic conditions were assessed: (1) a grouted canyon monolith; and (2) a canyon monolith filled with sand, both assuming no cracks or fissures were present to cause preferential transport. A three-staged approach was taken to account for different processes that may impact the amount of contaminant that can be safely sequestered in canyon structure. In the first stage, flow and transport simulations established waste acceptance criteria based on a linear (Kd) isotherm approach. In the second stage, impacts on thermal loading were examined and the differences in waste acceptance criteria quantified. In the third stage of modeling, precipitation/dissolution reactions were considered on the release and transport of the contaminants, and the subsequent impact on the maximum contaminant loading. The reactive transport modeling is considered a demonstration of the reactive transport capability, and shows the importance of its use for future performance predictions once site-specific data have been obtained.