Engineering topics

Zavarin, M.

Publications and source records attributed to Zavarin, M..

9 records

DOE OSTI2024

Area V: Waste Management and Subsurface Science (FY21-23 Final Report)

The objective of the Waste Management and Subsurface Science Topic Area V project is to evaluate the feasibility and safety of an intermediate-depth borehole for disposal of Israel Atomic Energy Commission (IAEC) nuclear waste. The IAEC nuclear waste is currently stored in above ground and/or in near-surface facilities that provide short-term radiological worker safety but do not provide long-term, full security and safeguards protection for the nuclear material. Disposal of the IAEC nuclear waste several hundred meters below the surface in a sealed borehole would provide long-term security and safeguards due to its depth underground, as well as long-term radiological safety, due to its isolation in a stable geological formation. This project supports the nuclear security and safeguards initiatives of the Science and Technology Working Group of the NNSA/IAEC Memorandum of Understanding (MOU) and addresses the Topic Area V objective and associated goals. The goals for Topic Area V are: (1) Assess the suitability of the vadose zone in the Yamin Plain of the northern Negev Desert, Israel as a host location for intermediate-depth borehole disposal of radioactive waste, (2) Define and refine the necessary characterization needs to better understand the regional climate, structure, and stratigraphy, geomechanics, geochemistry, hydrogeology, and seismicity of the stratigraphic sequence from the surface to the water table in the vicinity of the proposed host location for the disposal borehole(s), and (3) Develop a preliminary plan and schedule, including necessary resources and costs, for a borehole disposal concept and robust and transparent pre-closure and post-closure safety assessments. The safety assessments will require iteration with process level models at both site and regional scales. Upon completion, the information collected by this effort will allow the IAEC to make decisions regarding the viability and applicability of an intermediate depth (<500m) borehole for disposal in the vadose zone of the Yamin Plain. This FY21-23 final report is provided in lieu of a workshop report that was originally planned for delivery in January, 2024. Due to the conflict in Israel and associated delays, the workshop has been delayed to April 2024. The workshop will be held at LLNL but offsite and will switch to hybrid if travel restrictions remain in place. The associated workshop report will be provided as part of a new FY24-26 LCP.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Surface Complexation/Ion Exchange Hybrid Model for Radionuclide Sorption to Clay Minerals (M4SF-23LL010301062)

This progress report (Level 4 Milestone Number M4SF-23LL010301062) summarizes research conducted at Lawrence Livermore National Laboratory (LLNL) within the Argillite International Collaborations Activity Number SF-23LL01030106. The activity is focused on our long-term commitment to engaging our partners in international nuclear waste repository research. The focus of this milestone is the establishment of international collaborations for surface complexation modeling and the associated impacts of unlocking larger, community-based datasets. More specifically, we are developing a database framework for Spent Fuel and Waste and Science Technology (SFWST) that is aligned with the Helmholtz Zentrum Dresden Rossendorf (HZDR) sorption database development group in support of the database needs of the SFWST program. In our FY22 effort, we described a detailed analysis of U(VI) sorption to quartz through both traditional surface complexation modeling and through a hybrid ML framework. In FY23, effort was placed on publication of these results and expansion of the LLNL surface complexation and ion exchange database (L-SCIE) in order to assess mineral-based radionuclide retardation under a wider variety of geochemical conditions (e.g., ionic strength, varying electrolyte compositions). Efforts were initiated to expand L-SCIE to include radionuclide surface complexation and ion exchange to clays that are relevant to subsurface geochemical processes occurring at nuclear waste repositories. In particular, a large source of sorption data for clays resides at the Paul Scherrer Institute (PSI) (work primarily by Bradbury and Baeyens) and we initiated discussions on how to retrieve those data and apply FAIR principles to those datasets. In addition to L-SCIE development, two hybrid models that incorporate AI/ML were investigated and compared to discern the most promising approaches for accurate and precise estimations of radionuclide retardation. Key considerations for future model development include (1) the ability to reduce computational burden on determining retardation coefficients for PA and (2) the ability to quantify and predict radionuclide-mineral partitioning at a more efficient, rapid pace due to automated workflows. Upon the careful consideration of the most effective modeling approaches, we are identifying ways to implement these approaches into PA. Ultimately, the data science-based workflows will provide a major incentive for other institutions to adopt a FAIR-formatted, interoperable database. LLNL will play a key role in disseminating sorption data and acting as good data stewards by updating the database in a consistent format and assessing the quality of the newly assimilated data in an organized fashion. To this end, all data and workflows are open access and made available on the LLNL Seaborg research website (https://seaborg.llnl.gov/resources/geochemical-databases-modeling-codes).

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2023

Radionuclide Interaction with Hydrothermally Altered Repository Materials (M4SF-23LL010302052)

This progress report (Level 4 Milestone Number M4SF-23LL010302052) summarizes research conducted at Lawrence Livermore National Laboratory (LLNL) within the Crystalline Activity Number SF-23LL01030205. The research is focused on actinide and radionuclide sequestration in hydrothermally altered repository materials. In FY23, a manuscript was in preparation for publication summarizing our analysis of radionuclide sorption and coprecipitation into Fe oxide phases and evaluation of radionuclide partitioning values across a range of radionuclides relevant to performance assessment. We demonstrated our approach in detail using Se sorption and coprecipitation with iron oxide minerals. These data were presented in our FY22 annual report and will not be repeated here. We also initiated experiments to identify radionuclide interaction with hydrothermally altered crystalline repository and backfill materials. Recent research performed at Los Alamos National Laboratory (LANL) and Sandia National Laboratory (SNL) has provided key insights regarding the hydrothermal alteration behavior of bentonite backfill in the presence of repository materials (steel, concrete, etc.). We are now examining how mineral alteration affects retardation behavior of plutonium and a suite of other radionuclides. These experiments also allow us to test the predictive ability of our component additivity approach to surface complexation and ion exchange. Our guiding hypothesis is that a robust surface complexation/ion exchange model and associated database, developed using our L-SCIE approach, can effectively predict changes in radionuclide sorption behavior resulting from the hydrothermal alteration of mineralogy in a repository near field. A short update of results to date is presented below. A manuscript was also in preparation describing a self-consistent model and approach to simulating Se(IV) and Se(VI) sorption to 5 iron oxide phases based on our L-SCIE community database. This will be the first implementation of a multi-mineral and multi-oxidation state sorption model using our new L-SCIE database and workflow. A short summary of these results is presented below.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2023

Management and International Sorption Model Collaboration (M4SF-23LL010302062-NEA-TDB)

This progress report (Level 4 Milestone Number M4SF-23LL010302062) summarizes research conducted at Lawrence Livermore National Laboratory (LLNL) within the Crystalline International Collaborations Activity Number SF-23LL01030206. The activity is focused on our long-term commitment of engaging our partners in international nuclear waste repository research. This includes participation in the Nuclear Energy Agency Thermochemical Database (NEA-TDB) Project and development of methodologies for integrating US and international thermodynamic databases for use in SFWST Generic Disposal System Assessment (GDSA) efforts. A continuing focus for FY23 efforts has been to support the US participation in the NEA-TDB effort (Mavrik Zavarin replaced Cindy Atkins-Duffin on the NEA-TDB Management Board (MB) and Executive Group (EG)) and developing mechanisms for integration of NEA-TDB thermochemical data with LLNL’s SUPCRTNE thermodynamic database that supports the SFWST GDSA activities. This effort is coordinated with the Argillite work package SUPCRTNE database development efforts. The goal is to provide a downloadable database that will be hosted on a LLNL website which integrates NEA-TDB data into the LLNL SUPCRTNE database where appropriate. As part of our international activities, we continue our effort to integrate international sorption databases into L-SCIE (Zavarin et al., 2022b). We presented opportunities to include sorption in the next phase of NEA-TDB efforts at the April 2023 EG meeting in Paris. FY23 efforts focused on ensuring interoperable database development across multiple international database development activities. The overall goal is to produce an open source database that can be shared and integrated with multiple nuclear waste programs internationally and harness modern data science workflows and algorithms to incorporate these new approaches into reactive transport and performance assessment models. In collaboration with our Helmholtz Zentrum Dresden Rossendorf partners, we recently demonstrated the power of FAIR open source databases by fitting iron oxide (hydrous ferric oxide, goethite, hematite, and magnetite) protolysis constants to all available L-SCIE data. The results were submitted as a manuscript to J. Colloid Interface Science. This work will inform future metal sorption studies on a variety of iron oxides in order to discern the most appropriate acidity constants and surface complexation modeling constructs to account for pH-dependent mineral surface charge behavior. This work also explored automated surface complexation model development workflows in order to generate higher throughput model input files for a more facile incorporation into GDSA activities.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2023

Area V: Waste Management and Subsurface Science Q3 Report

The objective of Topic Area V is to evaluate the feasibility and safety of an intermediate-depth borehole for disposal of IAEC nuclear waste. The IAEC nuclear waste is currently stored in above ground and/or in near-surface facilities that provide short-term radiological worker safety but do not provide long-term, full security and safeguards protection for the nuclear material. Disposal of the IAEC nuclear waste several hundred meters below the surface in a sealed borehole would provide long-term security and safeguards due to its depth underground, as well as long-term radiological safety, due to its isolation in a stable geological formation.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2022

Radiolysis of Organic Solvents in the Presence of Plutonium

In this report, we describe a set of organic solvent radiolysis experiments performed at Lawrence Livermore National Laboratory. The goal of these experiments was to test for radiolytic solvent damage due to the presence of plutonium (Pu) particulates in solvent baths that are part of a materials production and cleaning workflow. The solvents (NOVEC 72DE and NOVEC 7500) were tested at a Pu activity level of ~1 microCi/mL using weapons grade Pu -- equivalent to 0.35 g Pu dispersed in a 5 gallon fluid bath filled to 4.5 gallons. Experiments were performed using fresh solvent and solvent that was 95% evaporated; the evaporated solvent was meant to represent fluids that may be in the solvent bath and subjected to evaporation and refilling without a full solvent replacement.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2022

M4SF-22LL010301062-Surface Complexation Database and Hybrid ML Model Development for GDSA

This progress report (Level 4 Milestone Number M4SF-22LL010301062) summarizes research conducted at Lawrence Livermore National Laboratory (LLNL) within the Argillite International Collaborations Activity Number Activity SF-22LL01030106. The activity is focused on our long-term commitment to engaging our partners in international nuclear waste repository research. The focus of this milestone is the establishment of international collaborations for surface complexation modeling and the associated impacts of unlocking larger, community-based datasets. More specifically, we are developing a database framework for Spent Fuel and Waste and Science Technology (SFWST) that is aligned with the Helmholtz Zentrum Dresden Rossendorf (HZDR) sorption database development group in support of the database needs of the SFWST program.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2022

M4SF-22LL010302052-Radionuclide Incorporation Model for Corrosion Products

This progress report (Level 4 Milestone Number M4SF-22LL010302052) summarizes research conducted at Lawrence Livermore National Laboratory (LLNL) within the Crystalline Activity Number SF-22LL01030205. The research is focused on actinide and radionuclide sequestration in steel corrosion products.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2022

M4SF-22LL010302062-NEA-TDB and Sorption DataBase Development

This progress report (Level 4 Milestone Number M4SF-22LL010302062) summarizes research conducted at Lawrence Livermore National Laboratory (LLNL) within the Crystalline International Collaborations Activity Number SF-22LL01030206. The activity is focused on our long-term commitment of engaging our partners in international nuclear waste repository research. This includes participation in the Nuclear Energy Agency Thermochemical Database (NEA-TDB) Project (Cindy Atkins-Duffin, Mavrik Zavarin) and development of methodologies for integrating US and international thermodynamic databases for use in SFWST Generic Disposal System Assessment (GDSA) efforts.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗