Property/composition relationships for Hanford high-level waste glasses melting at 115{degrees}C volume 1: Chapters 1-11

A Composition Variation study (CVS) is being performed within the Pacific Northwest Laboratory Vitrification Technology Development (PVTD) project in support of a future high-level nuclear waste vitrification plant at the Hanford site in Washington. From 1989 to 1994, over 120 nonradioactive glasses were melted and properties measured in five statistically-designed experimental phases. Glass composition is represented by the 10 components SiO{sub 2}, B{sub 2}O{sub 3}, Al{sub 2}O{sub 3}, Fe{sub 2}O{sub 3}, ZrO{sub 2}, Na{sub 2}O, Li{sub 2}O, CaO, MgO, and Others (all remaining components). The properties measured include viscosity ({eta}), electrical conductivity ({epsilon}), glass transition temperature (T{sub g} ), thermal expansion of solid glass ({alpha}{sub s}) and molten glass ({alpha}{sub m}), crystallinity (quenched and canister centerline cooled glasses), liquidus temperature (T{sub L}), durability based on normalized elemental releases from the Materials Characterization Center-1 28-day dissolution test (MCC-1, r{sub mi}) and the 7-day Product Consistency Test (PCT, r{sub pi}), and solution pHs from MCC-1 and PCT. Amorphous phase separation was also evaluated. Empirical first- and second-order mixture models were fit using the CVS data to relate the various properties to glass composition. Equations for calculating the uncertainty associated with property values predicted by the models were also developed. The models weremore » validated using both internal and external data. Other modeling approaches (e.g., non-bridging oxygen, free energy of hydration, phase-equilibria T{sub L}) were investigated for specific properties. A preliminary Qualified Composition Region was developed to identify glass compositions with high confidence of being processable in a melter and meeting waste form acceptance criteria. « less