Publications

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The fillers research and development (R&D) program, mostly experimental, is part of a broader R&D program that includes new process modeling and performance assessment of criticality effects and the overall importance of criticality to repository performance (consequence screening). A literature research and consultation effort with experts by Hardin and Brady (2018) identified several potentially effective and workable filler materials including cements (primarily phosphate based), moltenmetal alloys, and low-temperature glasses. Filler attributes were defined, and the preliminary lists were compared qualitatively. Further comparative analysis will be done (e.g., cost estimates) after experimental screening has narrowed the list of alternatives. The research presented here is focused Sandia’s efforts for the development of phosphate-based cement fillers. Molten metal filler research is an ongoing activity at Oak Ridge National Laboratories and is not discussed herein. After the completion of the FY20 research effort the following cement filler compositions were selected for further experimental development work and advanced testing in FY21: 1. Aluminum phosphate cements (APCs); more specifically aluminum oxide / aluminum phosphate (Al₂O₃ / AlPO₄) cements in which Al₂O₃ serves as the filler material bound by an AlPO₄ binder formed by the reaction of Al₂O₃ with various phosphate sources; 2. Wollastonite phosphate cements (WPCs), specifically wollastonite and aluminum or calcium aluminum phosphates in which CaSiO₃ serves as the filler material bound by a calcium phosphate that serves as the binder; and 3. Calcium aluminate phosphate cements (CAPCs) specifically grossite (CaAl₄O₇) and hibonite (CaAl₁₁O₁₈) fillers bound by an aluminum phosphate that serves as the binder. This effort focused on the optimization and subsequent processing of these three cements to achieve dense and well-consolidated monolithic samples. Upon completion of the FY21 effort the aluminum phosphate cements (APCs) and the calcium aluminate phosphate cements (CAPCs) show the most promise for advanced testing and scale up. We will begin the work in FY22 focused on testing the performance of these two cements in small scale DPCs as well as advanced materials testing to evaluate cement performance under expected radiation doses and representative post-closure geochemical environments.

The US generates approximately 2,000 Metric Tons of Heavy Metal (MTHM) of commercial spent fuel (SNF) each year and currently stores ~ 85,000 MTHM of commercial SNF at 70+ reactor sites, the disposal of which is the responsibility of the US Department of Energy (DOE). SNF is initially stored in spent nuclear fueld pools (SFPs). SFPs were initially constructed by US utilities for temporary fuel storage, but with no final disposal pathway available, SFPs are reaching capacity. To allow continued operation of the nation's commercial nuclear reactor fleet, utilities started transferring SNF from SFPs (wet storage) to dry cask storage systems, typically using dual-purpose (storage and transportation) canisters (DPCs). And while DPCs were designed, licensed and loaded to meet Nuclear Regulatory Commission (NRC) requirements that preclude the possibility of a critical event during SNF storage and transport, they were not designed or loaded to preclude the possibility of a criticality event during the regulated post-closure period following disposal, which could be up to 1,000,000 years (Price, 2019). DPC filler option criteria are detailed and materials that exhibit these attributes are explored. This document is an update of the SNL Joint Workplan on Filler Investigations for DPCs.

This report represents completion of milestone deliverable M2SF-21SN010309012 “Annual Status Update for OWL and Waste Form Characteristics” that provides an annual update on status of fiscal year (FY 2020) activities for the work package SF-20SN01030901 and is due on January 29, 2021. The Online Waste Library (OWL) has been designed to contain information regarding United States (U.S.) Department of Energy (DOE)-managed (as) high-level waste (DHLW), spent nuclear fuel (SNF), and other wastes that are likely candidates for deep geologic disposal, with links to the current supporting documents for the data (when possible; note that no classified or official-use-only (OUO) data are planned to be included in OWL). There may be up to several hundred different DOE-managed wastes that are likely to require deep geologic disposal. This draft report contains versions of the OWL model architecture for vessel information (Appendix A) and an excerpt from the OWL User’s Guide (Appendix B and SNL 2020), which are for the current OWL Version 2.0 on the Sandia External Collaboration Network (ECN).

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Commercial spent nuclear fuel (SNF) is accumulating at 72 sites across the U.S., at the rate of about 2,000 metric tons of uranium (MTU) per year. There are currently more than 2,700 dualpurpose canisters (DPCs) loaded with SNF, which are designed for storage and transportation but not disposal. If current storage practices continue, about half the eventual total U.S. SNF inventory will be in about 5,500 dry storage systems by 2035, with the entire inventory stored in 10,000 or more by 2060. The quantity of SNF in DPCs is now much greater than that anticipated in the past, leading the DOE to investigate the technical feasibility of direct disposal of SNF in DPCs. Studies in 2013-2015 concluded that the main technical challenges for disposal of SNF in DPCs are thermal management, handling and emplacement of large, heavy waste packages, and postclosure criticality control (Hardin et al. 2015). Of these, postclosure criticality control is the most challenging, and the R&D needed for this aspect of DPC direct disposal is the primary focus of this report.

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This report represents completion of milestone deliverable M2SF-19SNO10309013 "Online Waste Library (OWL) and Waste Forms Characteristics Annual Report" that reports annual status on fiscal year (FY) 2019 activities for the work package SF-19SN01030901 and is due on August 2, 2019. The online waste library (OWL) has been designed to contain information regarding United States (U.S.) Department of Energy (DOE)-managed (as) high-level waste (DHLW), spent nuclear fuel (SNF), and other wastes that are likely candidates for deep geologic disposal, with links to the current supporting documents for the data (when possible; note that no classified or official-use-only (OUO) data are planned to be included in OWL). There may be up to several hundred different DOE-managed wastes that are likely to require deep geologic disposal. This annual report on FY2019 activities includes evaluations of waste form characteristics and waste form performance models, updates to the OWL development, and descriptions of the management processes for the OWL. Updates to the OWL include an updated user's guide, additions to the OWL database content for wastes and waste forms, results of the beta testing and changes implemented from it. Also added are descriptions of the management/control processes for the OWL development, version control, and archiving. These processes have been implemented as part of the full production release of OWL (i.e., OWL Version 1.0), which has been developed on, and will be hosted and managed on, Sandia National Laboratories (SNL) systems. The version control/update processes will be implemented for updates to the OWL in the future. Additionally, another process covering methods for interfacing with the DOE SNF Database (DOE 2007) at Idaho National Laboratory on the numerous entries for DOE-managed SNF (DSNF) has been pushed forward by defining data exchanges and is planned to be implemented sometime in FY2020. The INL database is also sometimes referred to as the Spent Fuel Database or the SFDB, which is the acronym that will be used in this report. Once fully implemented, this integration effort will serve as a template for interfacing with additional databases throughout the DOE complex.

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This report presents a generic (i.e., site-independent) preliminary plan for drilling, testing, sampling, and analyzing data for a deep characterization borehole drilled into crystalline basement for the purposes of assessing the suitability of a site for deep borehole disposal (DBD). This research was performed as part of the deep borehole field test (DBFT). Based on revised U.S. Department of Energy (DOE) priorities in mid-2017, the DBFT and other research related to a DBD option was discontinued; ongoing work and documentation were closed out by the end of fiscal year (FY) 2017. This report was initiated as part of the DBFT and documented as an incomplete draft at the end of FY 2017. The report was finalized by Sandia National Laboratories in FY2018 without DOE funding, subsequent to the termination of the DBFT, and published in FY2019. This report presents a possible sampling, testing, and analysis campaign that could be carried out as part of a future project to quantify geochemical, geomechanical, geothermal, and geohydrologic conditions encountered at depths up to 5 km in crystalline basement.

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This report represents completion of milestone deliverable M2SF-18SNO10309013 "Inventory and Waste Characterization Status Report and OWL Update that reports on FY2018 activities for the work package (WP) SF-18SNO1030901. This report provides the detailed final information for completed FY2018 work activities for WP SF-18SN01030901, and a summary of priorities for FY2019. This status report on FY2018 activities includes evaluations of waste form characteristics and waste form performance models, updates to the OWL development, and descriptions of the two planned management processes for the OWL. Updates to the OWL include an updated user's guide, additions to the OWL database content for wastes and waste forms, results of the Beta testing and changes implemented from it. There are two processes being planned in FY2018, which will be implemented in FY2019. One process covers methods for interfacing with the DOE SNF DB (DOE 2007) at INL on the numerous entries for DOE managed SNF, and the other process covers the management of updates to, and version control/archiving of, the OWL database. In FY2018, we have pursued three studies to evaluate/redefine waste form characteristics and/or performance models. First characteristic isotopic ratios for various waste forms included in postclosure performance studies are being evaluated to delineate isotope ratio tags that quantitatively identify each particular waste form. This evaluation arose due to questions regarding the relative contributions of radionuclides from disparate waste forms in GDSA results, particularly, radionuclide contributions of DOE-managed SNF vs HLW glass. In our second study we are evaluating the bases of glass waste degradation rate models to the HIP calcine waste form. The HIP calcine may likely be a ceramic matrix material, with multiple ceramic phases with/without a glass phase. The ceramic phases are likely to have different degradation performance from the glass portion. The distribution of radionuclides among those various phases may also be a factor in the radionuclide release rates. Additionally, we have an ongoing investigation of the performance behavior of TRISO particle fuels and are developing a stochastic model for the degradation of those fuels that accounts for simultaneous corrosion of the silicon carbide (SiC) layer and radionuclide diffusion through it. The detailed model of the TRISO particles themselves, will be merged with models of the degradation behavior(s) of the graphite matrix (either prismatic compacts or spherical "pebbles") containing the particles and the hexagonal graphite elements holding the compacts.

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This report provides an update to Sassani et al. (2016) and includes: (1) an updated set of inputs (Sections 2.3) on various additional waste forms (WF) covering both DOE-managed spent nuclear fuel (SNF) and DOE-managed (as) high-level waste (HLW) for use in the inventory represented in the geologic disposal safety analyses (GDSA); (2) summaries of evaluations initiated to refine specific characteristics of particular WF for future use (Section 2.4); (3) updated development status of the Online Waste Library (OWL) database (Section 3.1.2) and an updated user guide to OWL (Section 3.1.3); and (4) status updates (Section 3.2) for the OWL inventory content, data entry checking process, and external OWL BETA testing initiated in fiscal year 2017.

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This paper considers concepts for disposal of canistered high-level (radioactive) waste (HLW) in large diameter deep boreholes. Vitrified HLW pour canisters are limited in diameter to promote glass cooling, and constitute a large potential application for borehole disposal where diameter is constrained. The objective for disposal would be waste packages with diameter of 22 to 29 inches, which could encompass all existing and projected HLW glass inventory in the United States. Deep, large diameter boreholes of the sizes needed have been successfully drilled, and we identify other potentially effective designs. The depth of disposal boreholes would be site-specific, and need not be as deep as the 5 km being investigated in the Deep Borehole Field Test. For example, a 0.91 m (36 inch) diameter borehole drilled to 3 km could be used for disposal from 2.5 to 3 km (8, 200 to 9, 840 ft). The engineering feasibility of such boreholes is greater today than was concluded by earlier studies done in Sweden and the United States. Moreover, the disposal concept and generic safety case have evolved to a point where borehole construction need not be as elaborate as previously assumed. Each borehole in the example could accommodate approximately 100 waste packages containing canisters of vitrified HLW. Emplacement of the packages would be through a 32-inch (0.81 m) guidance casing, installed in two sections to reduce hoisting loads, and forming a continuous pathway from the surface to total depth. Above the disposal zone would be a nominal 1 km (3, 280-ft) seal interval, similar to previously published concepts. Following those concept studies, the seal system would consist of alternating lifts of swelling clay, backfill and cement. Above the seal zone the borehole would be plugged with cement in the conventional manner for oil-and-gas wells. The function of seals in deep borehole disposal is to maintain the pre-drilling hydrologic regime in the crystalline basement, where groundwater is increasingly saline, stagnant, and ancient. Seals would resist fluid movement and radionuclide transport during an early period of waste heating, but after cooling little fluid movement is expected. Thus, the function of seals could be less important with HLW that has low heat output, and sealing requirements could be limited. The safety case for deep borehole disposal relies on the prevalence of groundwater that is increasingly saline with depth, stagnant, and ancient, in crystalline basement rock that has low bulk permeability and is isolated from surface processes. The minimum depth for disposal depends on sitespecific factors, and may be less than the 2.5 km example. Rough-order-of-magnitude cost estimates show that deep borehole disposal of HLW would be cost-competitive with the lowest cost mine repository options. Thinner overburden, and shallower development of conditions favorable to waste isolation, could make drilling of large-diameter disposal boreholes even more cost effective. The dimensions of the disposal zone and seal zone would be site specific, and would be adjusted to ensure that both are situated in unaltered crystalline basement rock.

The sorption of selenite, SeO32−, by carbonate substituted hydroxylapatite was investigated using batch kinetic and equilibrium experiments. The carbonate substituted hydroxylapatite was prepared by a precipitation method and characterized by SEM, XRD, FT-IR, TGA, BET and solubility measurements. The material is poorly crystalline, contains approximately 9.4% carbonate by weight and has a surface area of 210.2 m2/g. Uptake of selenite by the carbonated hydroxylapatite was approximately an order of magnitude higher than the uptake by uncarbonated hydroxylapatite reported in the literature. Distribution coefficients, Kd, determined for the carbonated apatite in this work ranged from approximately 4200 to over 14,000 L/kg. A comparison of the results from kinetic experiments performed in this work and literature kinetic data indicates the carbonated apatite synthesized in this study sorbed selenite 23 times faster than uncarbonated hydroxylapatite based on values normalized to the surface area of each material. The results indicate carbonated apatite is a potential candidate for use as a sorbent for pump-and-treat technologies, soil amendments or for use in permeable reactive barriers for the remediation of selenium contaminated sediments and groundwaters.