Charles L. Crawford

Silicate Based Glass Formulations for Immobilization of U.S. Defense Wastes Using Cold Crucible Induction Melters

iii Acknowledgments v Acronyms and Abbreviations vii 1.0 Introduction and Background 1 2.0 Quality Assurance 2 3.0 Previous Silicate Glass Formulation Efforts for CCIM Processing of U.S. Tank Wastes 3 3.1 Hanford TWRS-P HLW 3 3.2 Hanford C-106/AY-102 Formulation for Crystal Tolerant Melters 4 3.3 Idaho Sodium Bearing Waste 6 3.4 Savannah River Sludge Batch 2 Glasses 8 3.5 Savannah River Sludge Batch 3 Glasses 9 3.6 Savannah River Sludge Batch 4 Glasses 11 3.6.1 Frit 503-R4 (SIA Radon) 12 3.6.2 Frit 503-R3 (KHNP) 13 3.6.3 Frit 503-R6 (CEA) 13 3.7 Hanford AZ-101 High Level Waste Glass 14 3.8 Hanford AN-105 Low-Activity Waste Glass Formulation 16 3.9 Hanford HLW Waste Cluster Groups 18 3.10 Summary of Key Processing Related Properties for CCIM Test Glasses 19 4.0 Glass Formulation and Testing for Hanford High-Alumina and High-Iron HLWs 23 4.1 Selection of Wastes 23 4.2 Experimental Methods 25 4.2.1 Glass Fabrication and Canister Centerline Cooling Treatment 25 4.2.2 Composition Analyses 26 4.2.3 Product Consistency Test 26 4.2.4 Viscosity 26 4.2.5 Electrical Conductivity 27 4.2.6 Equilibrium Crystal Fraction and Crystal Identification After Canister Centerline Cooling 27 4.3 Glass Formulation Approaches 28 4.4 High-Al2O3 Glass Formulation and Testing for C-102 29 4.5 High-Fe2O3 Glass Formulation and Testing for 244-TX 39 4.6 Summary of Glass Formulation Results for C-102 and 244-TX 45 5.0 Evaluation of Glass Formulations for Hanford Tank Waste Using CCIM 46 5.1 High-Level Waste Melter Study Report 47 5.2 Evaluation of Hanford HLW Vitrification Process Alternatives 47 5.3 River Protection Project System Plan (Current Baseline) 48

Plutonium Feed Impurity Testing in Lanthanide Borosilicate (LaBS) Glass

A vitrification technology utilizing a lanthanide borosilicate (LaBS) glass is a viable option for dispositioning excess weapons-useable plutonium that is not suitable for processing into mixed oxide (MOX) fuel. A significant effort to develop a glass formulation and vitrification process to immobilize plutonium was completed in the mid-1990s. The LaBS glass formulation was found to be capable of immobilizing in excess of 10 wt % Pu and to be tolerant of a range of impurities. A more detailed study is now needed to quantify the ability of the glass to accommodate the anticipated impurities associated with the Pu feeds now slated for disposition. The database of Pu feeds was reviewed to identify impurity species and concentration ranges for these impurities. Based on this review, a statistically designed test matrix of glass compositions was developed to evaluate the ability of the LaBS glass to accommodate the impurities. Sixty surrogate LaBS glass compositions were prepared in accordance with the statistically designed test matrix. The heterogeneity (e.g. degree of crystallinity) and durability (as measured by the Product Consistency Test - Method A (PCT-A)) of the glasses were used to assess the effects of impurities on glass quality.

Demonstration of the defense waste processing facility vitrification process for tank 42 radioactive sludge – glass preparation and characterization

The Defense Waste Processing Facility (DWPF) at the Savannah River Site (SRS) is currently processing and immobilizing the radioactive high level waste sludge at SRS into a durable borosilicate glass for final geological disposal. The DWPF has recently finished processing the first radioactive sludge batch, and is ready for the second batch ofradioactive sludge. The second batch is primarily sludge from Tank 42. Before processing this batch in the DWPF, the DWPF process flowsheet has to be demonstrated with a sample of Tank 42 sludge to ensure that an acceptable melter feed and glass can be made. This demonstration was recently completed in the Shielded Cells Facility at SRS. An earlier paper in these proceedings described the sludge composition and processes necessary for producing an acceptable melter feed [1]. This paper describes the preparation and characterization of the glass from that demonstration. Results substantiate that Tank 42 sludge after mixing with the proper amount of glass forming frit (Frit 200) can be processed to make an acceptable glass.