Evaporative Evolution of Carbonate-Rich Brines from Synthetic Topopah Spring Tuff Pore Water, Yucca Mountain, NV

摘要

The evaporation of a range of synthetic pore water solutions representative of the potential high-level-nuclear-waste repository at Yucca Mountain, NV is being investigated. The motivation of this work is to understand and predict the range of brine compositions that may contact the waste containers from evaporation of pore waters, because these brines could form corrosive thin films on the containers and impact their long-term integrity. A relatively complex synthetic Topopah Spring Tuff pore water was progressively concentrated by evaporation in a closed vessel, heated to 95℃ in a series of sequential experiments. Periodic samples of the evaporating solution were taken to determine the evolving water chemistry. According to chemical divide theory at 25℃ and 95℃ our starting solution should evolve towards a high pH carbonate brine. Results at 95℃ show that this solution evolves towards a complex brine that contains about 99 mol% Na~+ for the cations, and 71 mol% Cl~- 18 mol% ∑CO_2(aq), 9 mol% SO_4~(2-) for the anions. Initial modeling of the evaporating solution indicates precipitation of aragonite, halite, silica, sulfate and fluoride phases. The experiments have been used to benchmark the use of the EQ3/6 geochemical code in predicting the evolution of carbonate-rich brines during evaporation.