Title: DEGRADATION OF CEMENTITIOUS MATERIALS ASSOCIATED WITH SALTSTONE DISPOSAL UNITS

The Saltstone facilities at the DOE Savannah River Site (SRS) stabilize and dispose of low-level radioactive salt solution originating from liquid waste storage tanks at the site. The Saltstone Production Facility (SPF) receives treated salt solution and mixes the aqueous waste with dry cement, blast furnace slag, and fly ash to form a grout slurry which is mechanically pumped into concrete disposal cells that compose the Saltstone Disposal Facility (SDF). The solidified grout is termed “saltstone”. Cementitious materials play a prominent role in the design and long-term performance of the SDF. The saltstone grout exhibits low permeability and diffusivity, andmore » thus represents a physical barrier to waste release. The waste form is also reducing, which creates a chemical barrier to waste release for certain key radionuclides, notably Tc-99. Similarly, the concrete shell of an SDF disposal unit (SDU) represents an additional physical and chemical barrier to radionuclide release to the environment. Together the waste form and the SDU compose a robust containment structure at the time of facility closure. However, the physical and chemical state of cementitious materials will evolve over time through a variety of phenomena, leading to degraded barrier performance over Performance Assessment (PA) timescales of thousands to tens of thousands of years. Previous studies of cementitious material degradation in the context of low-level waste disposal have identified sulfate attack, carbonation influenced steel corrosion, and decalcification (primary constituent leaching) as the primary chemical degradation phenomena of most relevance to SRS exposure conditions. In this study, degradation time scales for each of these three degradation phenomena are estimated for saltstone and concrete associated with each SDU type under conservative, nominal, and best estimate assumptions. The nominal value (NV) is an intermediate result that is more probable than the conservative estimate (CE) and more defensible than the best estimate (BE). The combined effects of multiple phenomena are then considered to determine the most limiting degradation time scale for each cementitious material. Degradation times are estimated using a combination of analytic solutions from literature and numerical simulation codes provided through the DOE Cementitious Barriers Partnership (CBP) Software Toolbox (http://cementbarriers.org). For the SDU 2 design, the roof, wall, and floor components are projected to become fully degraded under Nominal conditions at 3866, 923, and 1413 years, respectively. For SDU 4 the roof and floor are estimated to be fully degraded under Nominal conditions after 1137 and 1407 years, respectively; the wall is assumed to be fully degraded at time zero in the most recent PA simulations. Degradation of these concrete barriers generally occurs from combined sulfate attack and corrosion of embedded steel following carbonation. Saltstone is projected to degrade very slowly by decalcification, with complete degradation occurring in excess of 200,000 years for any SDU type. Complete results are provided.« less

The Saltstone facilities at the DOE Savannah River Site (SRS) stabilize and dispose of low-level radioactive salt solution originating from liquid waste storage tanks at the site. The Saltstone Production Facility (SPF) receives treated salt solution and mixes the aqueous waste with dry cement, blast furnace slag, and fly ash to form a grout slurry which is mechanically pumped into concrete disposal cells that compose the Saltstone Disposal Facility (SDF). The solidified grout is termed “saltstone”. Cementitious materials play a prominent role in the design and long-term performance of the SDF. The saltstone grout exhibits low permeability and diffusivity, andmore » thus represents a physical barrier to waste release. The waste form is also reducing, which creates a chemical barrier to waste release for certain key radionuclides, notably Tc-99. Similarly, the concrete shell of a saltstone disposal unit (SDU) represents an additional physical and chemical barrier to radionuclide release to the environment. Together the waste form and the SDU compose a robust containment structure at the time of facility closure. However, the physical and chemical state of cementitious materials will evolve over time through a variety of phenomena, leading to degraded barrier performance over Performance Assessment (PA) timescales of thousands to tens of thousands of years. Previous studies of cementitious material degradation in the context of low-level waste disposal have identified sulfate attack, carbonation influenced steel corrosion, and decalcification (primary constituent leaching) as the primary chemical degradation phenomena of most relevance to SRS exposure conditions. In this study, degradation time scales for each of these three degradation phenomena are estimated for saltstone and concrete associated with each SDU type under conservative, nominal, and best estimate assumptions.« less

As part of the current Saltstone Disposal Facility (SDF) Performance Assessment (PA) revision, the closure cap configuration was reevaluated and closure cap degradation mechanisms and their impact upon infiltration through the closure cap was evaluated for the existing SDF concrete vaults (i.e. vaults 1 and 4) for the base case land use scenario (i.e. institutional control to pine forest scenario) and documented in Phifer and Nelson (2003). The closure cap configuration was modified from a compacted kaolin barrier layer concept to a geosynthetic clay layer (GCL) barrier layer concept. The degradation mechanisms developed included pine forest succession, erosion, and colloidalmore » clay migration. These degradation mechanisms resulted in changes in the hydraulic properties of the closure cap layers and resulting increases in infiltration through the closure cap over time.« less

The Performance Assessment (PA) for the Saltstone Disposal Facility (SDF) is currently under revision. As part of the PA revision and as documented herein, the closure cap configuration has been reevaluated and closure cap degradation mechanisms and their impact upon infiltration through the closure cap have been evaluated for the institutional control to pine forest, land use scenario. This land use scenario is considered the base case land use scenario. This scenario assumes a 100-year institutional control period following final SDF closure during which the closure cap is maintained. At the end of institutional control, it is assumed that amore » pine forest succeeds the cap's original bamboo cover. Infiltration through the upper hydraulic barrier layer of the closure cap as determined by this evaluation will be utilized as the infiltration input to subsequent PORFLOW vadose zone contaminant transport modeling, which will also be performed as part of the PA revision. The impacts of pine forest succession, erosion, and colloidal clay migration as degradation mechanisms on the hydraulic properties of the closure cap layers over time have been estimated and the resulting infiltration through the closure cap has been evaluated. The primary changes caused by the degradation mechanisms that result in increased infiltration are the formation of holes in the upper GCL by pine forest succession and the reduction in the saturated hydraulic conductivity of the drainage layers due to colloidal clay migration into the layers. Erosion can also result in significant increases in infiltration if it causes the removal of soil layers, which provide water storage for the promotion of evapotranspiration. For this scenario, infiltration through the upper GCL was estimated at approximately 0.29 inches/year under initial intact conditions, it increased to approximately 11.6 inches/year at year 1000 in nearly a linear fashion, and it approached an asymptote of around 14.1 inches/year at year 1800 and thereafter. At year 1800, it was estimated that holes covered approximately 0.3 percent of the GCL due to root penetration, and that this resulted in an infiltration near that of typical background infiltration (i.e. as though the GCL were not there at all). This demonstrated that a very small area of holes essentially controlled the hydraulic performance of the GCL.« less

As part of the current Saltstone Disposal Facility (SDF) Performance Assessment (PA) revision, Mechanically Stabilized Earth (MSE) vault closure cap degradation mechanisms and their impact upon filtration through the MSE vault closure cap were evaluated for the base case land use scenario (i.e. institutional control to pine forest). The degradation mechanisms evaluated included pine forest succession, erosion, and colloidal clay migration (Phifer 2003). Infiltration through the upper hydraulic barrier layer of the closure cap as determined by this evaluation will be utilized as the infiltration input to subsequent PORFLOW vadose zone contaminant transport modeling, which will also be performed asmore » part of the PA revision.« less