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DOE OSTI2012

The Living Publication

Within the ICSTI Insights Series we offer three articles on the 'living publication' that is already available to practitioners in the important field of crystal structure determination and analysis. While the specific examples are drawn from this particular field, we invite readers to draw parallels in their own fields of interest. The first article describes the present state of the crystallographic living publication, already recognized by an ALPSP (Association of Learned and Professional Society Publishers) Award for Publishing Innovation in 2006. The second article describes the potential impact on the record of science as greater post-publication analysis becomes more common within currently accepted data deposition practices, using processed diffraction data as the starting point. The third article outlines a vision for the further improvement of crystallographic structure reports within potentially achievable enhanced data deposition practices, based upon raw (unprocessed) diffraction data. The IUCr in its Commissions and Journals has for many years emphasized the importance of publications being accompanied by data and the interpretation of the data in terms of atomic models. This has been followed as policy by numerous other journals in the field and its cognate disciplines. This practice has been well served by databases and archiving institutions such as the Protein Data Bank (PDB), the Cambridge Crystallographic Data Centre (CCDC), and the Inorganic Crystal Structure Database (ICSD). Normally the models that are archived are interpretations of the data, consisting of atomic coordinates with their displacement parameters, along with processed diffraction data from X-ray, neutron or electron diffraction studies. In our current online age, a reader can not only consult the printed word, but can display and explore the results with molecular graphics software of exceptional quality. Furthermore, the routine availability of processed diffraction data allows readers to perform direct calculations of the electron density (using X-rays and electrons as probes) or the nuclear density (using neutrons as probe) on which the molecular models are directly based. This current community practice is described in our first article. There are various ways that these data and tools can be used to further analyze the molecules that have been crystallized. Notably, once a set of results is announced via the publication, the research community can start to interact directly with the data and models. This gives the community the opportunity not only to read about the structure, but to examine it in detail, and even generate subsequent improved models. These improved models could, in principle, be archived along with the original interpretation of the data and can represent a continuously improving set of interpretations of a set of diffraction data. The models could improve both by correction of errors in the original interpretation and by the use of new representations of molecules in crystal structures that more accurately represent the contents of a crystal. These possible developments are described in our second article. A current, significant, thrust for the IUCr is whether it would be advantageous for the crystallographic community to require, rather than only encourage, the archiving of the raw (unprocessed) diffraction data images measured from a crystal, a fibre or a solution. This issue is being evaluated in detail by an IUCr Working Group (see http://forums.iucr.org). Such archived raw data would be linked to and from any associated publications. The archiving of raw diffraction data could allow as yet undeveloped processing methods to have access to the originally measured data. The debate within the community about this much larger proposed archiving effort revolves around the issue of 'cost versus benefit'. Costs can be minimized by preserving the raw data in local repositories, either at centralized synchrotron and neutron research institutes, or at research universities. Archiving raw data is also perceived as being more effective than just archiving processed data in countering scientific fraud, which exists in our field, albeit at a tiny level of occurrences. In parallel developments, sensitivities to avoiding research malpractice are encouraging Universities to establish their own data repositories for research and academic staff. These various 'raw data archives', would complement the existing processed data archives. These archives could however have gaps in their coverage arising from a lack of resources. Nevertheless we believe that a sufficiently large raw data archive, with reasonable global coverage, could be encouraged and have major benefits. These possible developments, costs and benefits, are described in our third and final article on 'The living publication'.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2012

Status Report on the Microbial Characterization of Halite and Groundwater Samples From the WIPP

This report summarizes the progress made in the ongoing task of characterizing the microbial community structures within the WIPP repository and in surrounding groundwaters. Through cultivation and DNA-based identification, the potential activity of these organisms is being inferred, thus leading to a better understanding of their impact on WIPP performance. Members of the three biological domains - Bacteria , Archaea , and Eukarya (in this case, Fungi ) - that are associated with WIPP halite have been identified. Thus far, their activity has been limited to aerobic respiration; anaerobic incubations are underway. WIPP halite constitutes the near-field microbial environment. We expect that microbial activity in this setting will proceed from aerobic respiration, through nitrate reduction to focus on sulfate reduction. This is also the current WIPP performance assessment (PA) position. Sulfate reduction can occur at extremely high ionic strengths, and sulfate is available in WIPP brines and in the anhydrite interbeds. The role of methanogenesis in the WIPP remains unclear, due to both energetic constraints imposed by a high-salt environment and substrate selectivity, and it is no longer considered in PA. Archaea identified in WIPP halite thus far fall exclusively within the family Halobacteriaceae . These include Halobacterium noricense , cultivated from both low- and high-salt media, and a Halorubrum -like species. The former has also been detected in other salt mines worldwide; the latter likely constitutes a new species. Little is known of its function, but it was prevalent in experiments investigating the biodegradation of organic complexing agents in WIPP brines. Bacterial signatures associated with WIPP halite include members of the phylum Proteobacteria - Halomonas , Pelomonas , Limnobacter , and Chromohalobacter - but only the latter has been isolated. Also detected and cultivated were Salinicoccus and Nesterenkonia spp. Fungi were also isolated from halite. Although these were most likely introduced into the WIPP as contaminants from above-ground, their survival and potential role in the WIPP (e.g., cellulose degradation) is under investigation. WIPP groundwaters comprise the far-field microbial environment. Bacteria cultivated and identified from the overlying Culebra and nearby borehole groundwater are capable of aerobic respiration, denitrification, fermentation, metal reduction, and sulfate reduction and are distributed across many different phyla. Two of the Bacteria found in groundwater were also found in WIPP halite ( Chromohalobacter sp. and Virgibacillus sp.). Archaea identified in groundwater include Halococcus saccharolyticus , Haloferax sp., and Natrinema sp. The differences in the microbial communities detected thus far in halite and groundwater suggest that there will be significant differences in the associated metabolic potential of the near- and far-field environments. Whereas the near-field is dominated by Archaea with more limited metabolic capabilities, the far-field is dominated by Bacteria with extremely broad capabilities. Because the majority of the repository's lifetime will be anoxic, ongoing and future work focuses on the presence and role of anaerobic organisms in WIPP. Further tasks on biosorption, cellulose degradation, and bioreduction are being performed using organisms obtained from this characterization work.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2012

U.S. Virgin Islands Petroleum Price-Spike Preparation

This NREL technical report details a plan for the U.S. Virgin Islands (USVI) to minimize the economic damage caused by major petroleum price increases. The assumptions for this plan are that the USVI will have very little time and money to implement it and that the population will be highly motivated to follow it because of high fuel prices. The plan's success, therefore, is highly dependent onbehavior change. This plan was derived largely from a review of the actions taken and behavior changes made by companies and commuters throughout the United States in response to the oil price spike of 2008. Many of these solutions were coordinated by or reported through the 88 local representatives of the U.S. Department of Energy's Clean Cities program. The National Renewable Energy Laboratoryprovides technical and communications support for the Clean Cities program and therefore serves as a de facto repository of these solutions. This plan is the first publication that has tapped this repository.

02 PETROLEUM↗
DOE OSTI2012

Radiolysis Process Model

Assessing the performance of spent (used) nuclear fuel in geological repository requires quantification of time-dependent phenomena that may influence its behavior on a time-scale up to millions of years. A high-level waste repository environment will be a dynamic redox system because of the time-dependent generation of radiolytic oxidants and reductants and the corrosion of Fe-bearing canister materials. One major difference between used fuel and natural analogues, including unirradiated UO 2 , is the intense radiolytic field. The radiation emitted by used fuel can produce radiolysis products in the presence of water vapor or a thin-film of water (including OH• and H• radicals, O 2 -, eaq, H 2 O 2 , H 2 , and O 2 ) that may increase the waste form degradation rate and change radionuclide behavior. H 2 O 2 is the dominant oxidant for spent nuclear fuel in an O 2 depleted water environment, the most sensitive parameters have been identified with respect to predictions of a radiolysis model under typical conditions. As compared with the full model with about 100 reactions it was found that only 30-40 of the reactions are required to determine [H 2 O 2 ] to one part in 10–5 and to preserve most of the predictions for major species. This allows a systematic approach for model simplification and offers guidance in designing experiments for validation.

Hydrogen Peroxide↗
DOE OSTI2014

Nondestructive Assay Options for Spent Fuel Encapsulation

This report describes the role that nondestructive assay (NDA) techniques and systems of NDA techniques may have in the context of an encapsulation and deep geological repository. The potential NDA needs of an encapsulation and repository facility include safeguards, heat content, and criticality. Some discussion of the facility needs is given, with the majority of the report concentrating on the capability and characteristics of individual NDA instruments and techniques currently available or under development. Particular emphasis is given to how the NDA techniques can be used to determine the heat production of an assembly, as well as meet the dual safeguards needs of 1) determining the declared parameters of initial enrichment, burn-up, and cooling time and 2) detecting defects (total, partial, and bias). The report concludes with the recommendation of three integrated systems that might meet the combined NDA needs of the encapsulation/repository facility.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2013

Microbial Characterization of Halite and Groundwater Samples from the WIPP

This report summarizes the progress made in characterizing the microbial community structures within the WIPP repository, and in surrounding groundwaters. Through cultivation and DNA-based identification, the potential activity of these organisms is being inferred, thus leading to a better understanding of their impact on WIPP performance. WIPP halite constitutes the near-field microbial environment. Microbial activity in this setting is predicted by WIPP performance assessment (PA) to proceed from aerobic respiration, through nitrate reduction, to focus on sulfate reduction. The role of methanogenesis in the WIPP remains unclear, due to both energetic constraints imposed by a high-salt environment and substrate selectivity, so this role is no longer considered in PA. Members of the three biological domains — Bacteria, Archaea, and Eukarya (in this case, Fungi) — have been found associated with WIPP halite. Thus far, their activity has been limited to aerobic respiration. Archaea identified in WIPP halite thus far fall exclusively within the family Halobacteriaceae. These include Halobacterium noricense, a Halorubrum-like species, and a Halopenitus-like species. Bacterial signatures associated with WIPP halite include members of the phylum Proteobacteria — Halomonas, Pelomonas, Limnobacter, and Chromohalobacter — but only the latter has been isolated. Also detected and cultivated were Salinicoccus and Nesterenkonia spp. Three fungal species were isolated from halite (Cladosporium, Phoma, and Engyodontium). Although these were most likely introduced into the WIPP as contaminants from above-ground, their survival and potential role in the WIPP (e.g., cellulose degradation) is under investigation. WIPP groundwaters comprise the far-field microbial environment. Bacteria cultivated and identified from the overlying Culebra and nearby borehole groundwater are capable of aerobic respiration, denitrification, fermentation, metal reduction, and sulfate reduction, and are distributed across many different phyla. Their structural and metabolic diversity is dependent upon the ionic strength of the sampled groundwater, with a decrease in both at higher strength. Two of the Bacteria found in groundwater were also found in WIPP halite (Chromohalobacter sp. and Virgibacillus sp.). Archaea identified in groundwater include Halococcus saccharolyticus, Haloferax sp., and Natrinema sp. The differences in the microbial communities detected thus far in halite and groundwater suggest that there will be significant differences in the associated metabolic potential of the near- and far-field environments. Whereas the near-field is dominated by Archaea with more limited metabolic capabilities, the far-field is dominated by Bacteria with extremely broad capabilities. The authors wish to thank Russ Patterson and Dan Ferguson (DOE-CBFO) for their support, and Washington TRU Solutions for access to sampling. All research was performed by the Los Alamos National Laboratory Actinide Chemistry & Repository Science team at the Carlsbad Environmental and Monitoring Research Center, managed by New Mexico State University (NMSU) and located in Carlsbad, NM. Funding for this research is through the Waste Isolation Pilot Plant project, managed by the Department of Energy—Carlsbad Field Office.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2013

Scoping Thermal Analysis of Alternative Dual-Purpose Canister Disposal Concepts

This report evaluates the feasibility of disposing of large DPCs in a clay/shale geologic environment. It utilizes the thermal-analytical models developed over the past two years as part of the Disposal Systems Evaluation Framework (DSEF). It evaluates waste streams representative of existing SNF waste streams (at 40-GWd/MT burnup) and potential future waste streams (at 60 GWd/MT burnup). The analyses cover ventilated (open) repository concepts in clay/shale, where backfill may or may not be added to emplacement drifts at closure. The results show that repository concepts which meet a design thermal constraint of TC = 100°C at the drift wall are feasible with large drift spacing (70 to 90 m) and large waste package (WP) spacing (20 to 40 m).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2013

Potential vertical movement of large heat-generating waste packages in salt.

With renewed interest in disposal of heat-generating waste in bedded or domal salt formations, scoping analyses were conducted to estimate rates of waste package vertical movement. Vertical movement is found to result from thermal expansion, from upward creep or heave of the near-field salt, and from downward buoyant forces on the waste package. A two-pronged analysis approach was used, with thermal-mechanical creep modeling, and coupled thermal-viscous flow modeling. The thermal-mechanical approach used well-studied salt constitutive models, while the thermal-viscous approach represented the salt as a highly viscous fluid. The Sierra suite of coupled simulation codes was used for both approaches. The waste package in all simulations was a right-circular cylinder with the density of steel, in horizontal orientation. A time-decaying heat generation function was used to represent commercial spent fuel with typical burnup and 50-year age. Results from the thermal-mechanical base case showed approximately 27 cm initial uplift of the package, followed by gradual relaxation closely following the calculated temperature history. A similar displacement history was obtained with the package density set equal to that of salt. The slight difference in these runs is attributable to buoyant displacement (sinking) and is on the order of 1 mm in 2,000 years. Without heat generation the displacement stabilizes at a fraction of millimeter after a few hundred years. Results from thermal-viscous model were similar, except that the rate of sinking was constant after cooldown, at approximately 0.15 mm per 1,000 yr. In summary, all calculations showed vertical movement on the order of 1 mm or less in 2,000 yr, including calculations using well-established constitutive models for temperature-dependent salt deformation. Based on this finding, displacement of waste packages in a salt repository is not a significant repository performance issue.

Clayton, Daniel James↗
DOE OSTI2013

Report on International Collaboration Involving the FE Heater and HG-A Tests at Mont Terri

Nuclear waste programs outside of the US have focused on different host rock types for geological disposal of high-level radioactive waste. Several countries, including France, Switzerland, Belgium, and Japan are exploring the possibility of waste disposal in shale and other clay-rich rock that fall within the general classification of argillaceous rock. This rock type is also of interest for the US program because the US has extensive sedimentary basins containing large deposits of argillaceous rock. LBNL, as part of the DOE-NE Used Fuel Disposition Campaign, is collaborating on some of the underground research laboratory (URL) activities at the Mont Terri URL near Saint-Ursanne, Switzerland. The Mont Terri project, which began in 1995, has developed a URL at a depth of about 300 m in a stiff clay formation called the Opalinus Clay. Our current collaboration efforts include two test modeling activities for the FE heater test and the HG-A leak-off test. This report documents results concerning our current modeling of these field tests. The overall objectives of these activities include an improved understanding of and advanced relevant modeling capabilities for EDZ evolution in clay repositories and the associated coupled processes, and to develop a technical basis for the maximum allowable temperature for a clay repository.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2014

Evaluation of COTS Rad Detection Apps

Mobile applications are currently under distribution to smart phones utilizing the built-in charge coupled-device (CCD) camera as a radiation detector. The CCD detector has a very low but measurable gamma interaction cross section so the mechanism is feasible, especially for higher dose rate environments. Given that in a large release of radioactive material these ‘crowd sourced’ measurements will be put forth for consideration, a testing and evaluation of the accuracy and uncertainty of the Apps is a critical endeavor. Not only is the accuracy of the reported measurement of concern to the immediate user’s safety, a quantitative uncertainty is required for a government response such as the Federal Radiological Monitoring and Assessment Center (FRMAC) to accept the values for consideration in the determination of regions exceeding protective action guidelines. Already, prompted by the Fukushima nuclear material releases, several repositories of this crowd-sourced data have been created (http://japan.failedrobot.com, http://www.stubbytour.com/nuc/index_en.asp, and http://www.rdtn.org) although the question remains as to the reliability of measurements incorporated into these repositories. In cases of conflict between the real-time published crowd-sourced data and governmental protective actions prepared literature should be on-hand documenting why the difference, if any, exists. Four applications for iOS devices were obtained along with hardware to benchmark their performance. Gamma/X-Ray Detector by Stephan Hotto, Geiger Camera by Senscare, and RadioactivityCounter App by Hotray LTD are all the applications available for distribution within the US that utilize the CCD camera sensor for detection of radiation levels. The CellRad app under development by Idaho National Laboratory for the Android platform was evaluated. In addition, iRad Geiger with the associated hardware accessory was also benchmarked. Radiation fields were generated in a Cs-137 JL Shepherd Model 89 shielded calibration range. The accuracy of the exposure rate within the box calibrator is +/- 5% of the system settings and NIST traceable. This is the same calibration unit utilized for calibration of US DOE exposure rate meters. Measurements were performed from 0.2 to 40,000 mR/hr. Included in the following sections are discussions on each of the evaluated applications and their performance in reporting radiation field measurements. Unfortunately the applications do not provide a readily identifiable quality of the measurement in order to produce error bars or even out of range conditions. In general all the CCD based applications had issues detecting consistent measurements in radiation fields less than 5 mR/hr. This is most likely attributable to the electronic noise level on the CCD’s becoming comparable to the signal level due to the ionizing radiation photons.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2014

Performance Assessment Modeling and Sensitivity Analyses of Generic Disposal System Concepts

The Used Fuel Disposition Campaign (UFDC) of the U.S. Department of Energy (DOE) Office of Nuclear Energy (NE) is conducting research and development (R&D) on generic deep geologic disposal systems (i.e., repositories) for high-activity nuclear wastes (i.e., used nuclear fuel (UNF) and high-level radioactive waste (HLW)) that exist today or that could be generated in future fuel cycles. This report describes specific activities in FY2014 toward the development of an enhanced generic disposal system modeling and analysis capability that utilizes high performance computing (HPC) environments to simulate important multi-physics phenomena and couplings associated with the potential behavior of a geologic repository for UNF and HLW.

Sevougian, S. David↗
DOE OSTI2015

Mechanical Behavior of the Near-field Host Rock Surrounding Excavations

This report is being prepared under the FY14 activity FT-14LA0818069, Mechanical and Hydrological Behavior of the Near-Field Host Rock Surrounding Excavations, and fulfills the Los Alamos National Laboratory deliverable M4FT-14LA08180610, which in PICS:NE is titled “Draft report, Test Plan for Mechanical and Hydrological Behavior of the Near-field Host Rock Surrounding Excavations.” Since the report is an intermediate deliverable intended as input to the eventual test plan for this test, rather than being an actual test plan, the activity title is used as the title of this document to avoid confusion as to the contents in the report. This report summarizes efforts to simulate mechanical processes occurring within a hypothetical high-level waste (HLW) repository in bedded salt. The report summarizes work completed since the last project deliverable, “Coupled model for heat and water transport in a high level waste repository in salt “, a Level 2 milestone submitted to DOE in September 2013 (Stauffer et al., 2013).

58 GEOSCIENCES↗
DOE OSTI2015

Generic Crystalline Disposal Reference Case

A generic reference case for disposal of spent nuclear fuel and high-level radioactive waste in crystalline rock is outlined. The generic cases are intended to support development of disposal system modeling capability by establishing relevant baseline conditions and parameters. Establishment of a generic reference case requires that the emplacement concept, waste inventory, waste form, waste package, backfill/buffer properties, EBS failure scenarios, host rock properties, and biosphere be specified. The focus in this report is on those elements that are unique to crystalline disposal, especially the geosphere representation. Three emplacement concepts are suggested for further analyses: a waste packages containing 4 PWR assemblies emplaced in boreholes in the floors of tunnels (KBS-3 concept), a 12-assembly waste package emplaced in tunnels, and a 32-assembly dual purpose canister emplaced in tunnels. In addition, three failure scenarios were suggested for future use: a nominal scenario involving corrosion of the waste package in the tunnel emplacement concepts, a manufacturing defect scenario applicable to the KBS-3 concept, and a disruptive glaciation scenario applicable to both emplacement concepts. The computational approaches required to analyze EBS failure and transport processes in a crystalline rock repository are similar to those of argillite/shale, with the most significant difference being that the EBS in a crystalline rock repository will likely experience highly heterogeneous flow rates, which should be represented in the model. The computational approaches required to analyze radionuclide transport in the natural system are very different because of the highly channelized nature of fracture flow. Computational workflows tailored to crystalline rock based on discrete transport pathways extracted from discrete fracture network models are recommended.

Environmental Protection↗
DOE OSTI2014

Thermo-hydrological and chemical (THC) modeling to support Field Test Design

This report summarizes ongoing efforts to simulate coupled thermal-hydrological-chemical (THC) processes occurring within a hypothetical high-level waste (HLW) repository in bedded salt. The report includes work completed since the last project deliverable, “Coupled model for heat and water transport in a high level waste repository in salt”, a Level 2 milestone submitted to DOE in September 2013 (Stauffer et al., 2013). Since the last deliverable, there have been code updates to improve the integration of the salt module with the pre-existing code and development of quality assurance (QA) tests of constitutive functions and precipitation/dissolution reactions. Simulations of bench-scale experiments, both historical and currently in the planning stages have been performed. Additional simulations have also been performed on the drift-scale model that incorporate new processes, such as an evaporation function to estimate water vapor removal from the crushed salt backfill and isotopic fractionation of water isotopes. Finally, a draft of a journal paper on the importance of clay dehydration on water availability is included as Appendix I.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2014

Clay Generic Disposal System Model - Sensitivity Analysis for 32 PWR Assembly Canisters (+2 associated model files).

The Used Fuel Disposition Campaign (UFDC), as part of the DOE Office of Nuclear Energy’s (DOE-NE) Fuel Cycle Technology program (FCT) is investigating the disposal of high level radioactive waste (HLW) and spent nuclear fuela (SNF) in a variety of geologic media. The feasibility of disposing SNF and HLW in clay media has been investigated and has been shown to be promising [Ref. 1]. In addition the disposal of these wastes in clay media is being investigated in Belgium, France, and Switzerland. Thus, Argillaceous media is one of the environments being considered by UFDC. As identified by researchers at Sandia National Laboratory, potentially suitable formations that may exist in the U.S. include mudstone, clay, shale, and argillite formations [Ref. 1]. These formations encompass a broad range of material properties. In this report, reference to clay media is intended to cover the full range of material properties. This report presents the status of the development of a simulation model for evaluating the performance of generic clay media. The clay Generic Disposal System Model (GDSM) repository performance simulation tool has been developed with the flexibility to evaluate not only different properties, but different waste streams/forms and different repository designs and engineered barrier configurations/ materials that could be used to dispose of these wastes.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2014

Review of Inputs Provided to Jason Associates Corporation in Support of RWEV-REP-001, the Analysis of Postclosure Groundwater Impacts Report

Report RWEV-REP-001, Analysis of Postclosure Groundwater Impacts for a Geologic Repository for the Disposal of Spent Nuclear Fuel and High Level Radioactive Waste at Yucca Mountain, Nye County, Nevada was issued by the DOE in 2009 and is currently being updated. Sandia National Laboratories (SNL) provided support for the original document, performing calculations and extracting data from the Yucca Mountain Performance Assessment Model that were used as inputs to the contaminant transport and dose calculations by Jason Associates Corporation, the primary developers of the DOE report. The inputs from SNL were documented in LSA-AR-037, Inputs to Jason Associates Corporation in Support of the Postclosure Repository Supplemental Environmental Impact Statement. To support the updating of the original Groundwater Impacts document, SNL has reviewed the inputs provided in LSA-AR-037 to verify that they are current and appropriate for use. The results of that assessment are documented here.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Technical Approach for Determining Key Parameters Needed for Modeling the Performance of Cast Stone for the Integrated Disposal Facility Performance Assessment

Washington River Protection Solutions (WRPS) and its contractors at Pacific Northwest National Laboratory (PNNL) and Savannah River National Laboratory (SRNL) are conducting a development program to develop / refine the cementitious waste form for the wastes treated at the ETF and to provide the data needed to support the IDF PA. This technical approach document is intended to provide guidance to the cementitious waste form development program with respect to the waste form characterization and testing information needed to support the IDF PA. At the time of the preparation of this technical approach document, the IDF PA effort is just getting started and the approach to analyze the performance of the cementitious waste form has not been determined. Therefore, this document looks at a number of different approaches for evaluating the waste form performance and describes the testing needed to provide data for each approach. Though the approach addresses a cementitious secondary aqueous waste form, it is applicable to other waste forms such as Cast Stone for supplemental immobilization of Hanford LAW. The performance of Cast Stone as a physical and chemical barrier to the release of contaminants of concern (COCs) from solidification of Hanford liquid low activity waste (LAW) and secondary wastes processed through the Effluent Treatment Facility (ETF) is of critical importance to the Hanford Integrated Disposal Facility (IDF) total system performance assessment (TSPA). The effectiveness of cementitious waste forms as a barrier to COC release is expected to evolve with time. PA modeling must therefore anticipate and address processes, properties, and conditions that alter the physical and chemical controls on COC transport in the cementitious waste forms over time. Most organizations responsible for disposal facility operation and their regulators support an iterative hierarchical safety/performance assessment approach with a general philosophy that modeling provides the critical link between the short-term understanding from laboratory and field tests, and the prediction of repository performance over repository time frames and scales. One common recommendation is that experiments be designed to permit the appropriate scaling in the models. There is a large contrast in the physical and chemical properties between the Cast Stone waste package and the IDF backfill and surrounding sediments. Cast Stone exhibits low permeability, high tortuosity, low carbonate, high pH, and low Eh whereas the backfill and native sediments have high permeability, low tortuosity, high carbonate, circumneutral pH, and high Eh. These contrasts have important implications for flow, transport, and reactions across the Cast Stone – backfill interface. Over time with transport across the interface and subsequent reactions, the sharp geochemical contrast will blur and there will be a range of spatially-distributed conditions. In general, COC mobility and transport will be sensitive to these geochemical variations, which also include physical changes in porosity and permeability from mineral reactions. Therefore, PA modeling must address processes, properties, and conditions that alter the physical and chemical controls on COC transport in the cementitious waste forms over time. Section 2 of this document reviews past Hanford PAs and SRS Saltstone PAs, which to date have mostly relied on the lumped parameter COC release conceptual models for TSPA predictions, and provides some details on the chosen values for the lumped parameters. Section 3 provides more details on the hierarchical modeling strategy and processes and mechanisms that control COC release. Section 4 summarizes and lists the key parameters for which numerical values are needed to perform PAs. Section 5 provides brief summaries of the methods used to measure the needed parameters and references to get more details.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗