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DOE OSTI2023

Performance Assessment for the E-Area Low-Level Radioactive Waste Disposal Facility at the Savannah River Site: Chapter 8

This chapter, together with Appendix H, provides the necessary CWTS inventory limits and trigger values for every parent radionuclide not screened out in Sections 2.3.6, 2.3.7, and 2.3.8. Also provided are details associated with how generic and special waste forms are handled on a DU-specific basis, and a discussion of the conversion of preliminary inventory limits (via transport runs summarized in Chapter 5) into final inventory limits for use in the CWTS limits system. Using the final inventory limits, a projected 2065 CWTS inventory is generated for use in the PA closure analysis outlined in Chapter 9.

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DOE OSTI2023

Performance Assessment for the E-Area Low-Level Radioactive Waste Disposal Facility at the Savannah River Site: Appendix F

As a supplement to Chapter 6, Section 6.1.1.3, Table F-1 through Table F-24 provide tabular results of the sensitivity analysis calculations for waste disposal timing (Sensitivity Case S6) in NR07E (Cases 3 and 4) and NR26E (Cases 1 through 4). The title of each table identifies the DU, sensitivity case, and performance measure. Section F.1.1 (Table F-1 through Table F-8) presents results for NR07E and Section F.1.2 (Table F-9 through Table F-24) presents results for NR26E. In each table, radionuclides are sorted from highest to lowest nominal concentration or dose factor. Nominal values are when waste disposal occurs at the start of operations; timeline values are when waste disposal occurs at the end of operations. The differences (Δ values) in the last column of each table equal the timeline concentration or dose factor minus the nominal concentration or dose factor, where DF and CF are shorthand designations for dose factor and concentration factor, respectively.

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DOE OSTI2023

Performance Assessment for the E-Area Low-Level Radioactive Waste Disposal Facility at the Savannah River Site: Appendix G

This appendix contains supporting information and key data used during the IHI analysis, including the following: • A list of parent radionuclides requiring IHI inventory limits (Section G.1) • Tables of IHI acute and chronic dose factors, inventory limits, and concentration limits for all DUs (Section G.2) • IHI acute and chronic dose history time profiles for all DUs (Section G.3)

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DOE OSTI2023

Performance Assessment for the E-Area Low-Level Radioactive Waste Disposal Facility at the Savannah River Site: Appendix I

As stated in Section 9.1.2.2, a final inventory of parent radionuclides is projected for every DU at the time of facility operational closure in 2065. These final closure inventories are upper-bound estimates wherein each DU is assumed to reach its activity capacity. Composition vectors based on existing DU inventories are employed to estimate the final compositions of all existing and future DUs. Specifically, (1) the existing DU compositions are assumed to remain constant; (2) future DUs are assigned averaged existing compositions based on appropriately averaged DUs. This information is detailed in Appendix H, Section H.7. In addition, the variability in composition among existing DUs is used to generate log-normal distributions for uncertainty quantification, which is detailed in Section I.1.1.

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DOE OSTI2023

Modeling of Chemical Slurry Rheology in DWPF Sludge Batch (SB) 10 Simulants

The Defense Waste Processing Facility (DWPF) treats high-activity radionuclides from sludge through a process called vitrification. This process converts radioactive liquid waste currently stored in tank farms into a solid glass form that is suitable for long-term storage and disposal. Due to the complexities involved in vitrifying this waste within each operation of the Chemical Processing Cell (CPC), waste rheology is studied to characterize the fluid-mechanical properties as it passes through the CPC and into the Melter. To better understand the waste and validate flow behavior, slurry rheology of simulants that represents the waste was studied at various acid stoichiometry percentages and solids concentrations to determine the simulant’s yield stress and viscosity. This research work has been supported by the DOE-FIU Science & Technology Workforce Development Initiative, an innovative program developed by the U.S. Department of Energy’s Office of Environmental Management (DOE-EM) and Florida International University’s Applied Research Center (FIU-ARC). During the spring of 2022, a DOE Fellow intern, Brendon Cintas, spent 10 weeks doing a summer internship at Savannah River National Laboratory (SRS) under the supervision and guidance of Dan Lambert, Chemical Flowsheet Development. The intern’s project was initiated on June 6, 2022, and continued through August 11, 2022 with the objective of assisting scientists at SRNL’s Rheology and Grout Laboratory at Aiken Country Technology Lab (ACTL) better understand the sludge composition on the rheology of a simulant slurry using a HAAKE RheoStress 6000 rheometer and extrapolate the results to the real-waste data.

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DOE OSTI2023

2022 Long-Term Hydrologic Monitoring Program Report for the Rio Blanco, Colorado Site

This report presents the monitoring data collected by the U.S. Department of Energy (DOE) Office of Legacy Management (LM) during the 2022 sampling event at the Rio Blanco, Colorado, Site, where an underground nuclear test was conducted in 1973. The test resulted in residual radionuclide contamination at the detonation depth. The 2022 sampling event included the collection of samples from onsite groundwater wells to monitor for any potential contamination that might be attributed to the Rio Blanco nuclear tests. This report summarizes the laboratory results obtained from the sampling along with the historical results since monitoring began in the 1970s. This annual report and previous reports are available on the LM public website at https://www.energy.gov/lm/rio-blanco-colorado-site. Data collected during this and previous monitoring events are available on the Geospatial Environmental Mapping System (GEMS) website at https://gems.lm.doe.gov/#site=RBL.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Radon Survey of Los Alamos National Laboratory Buildings and Los Alamos County Residential Buildings

A radon survey of office spaces was of interest to LANL for several reasons. First, exposure to natural radon in LANL office spaces has been considered to be outside the regulatory reach of the federal regulations and the U.S. Department of Energy (U.S. DOE) orders, and thus has not been studied as extensively as occupational exposure to other radionuclides and is not subject to the same rigorous radiological controls. Second, a general survey of radon concentrations in LANL workspaces was of interest to management to ensure safe environments for workers and is in keeping with the intent of OSHA requirements. Though radon in LANL offices would not be derived from enhanced radioactive sources, radon exposure in general office spaces has the potential to significantly impact worker risk. The purpose of the 2009 radon survey was to measure and document indoor radon levels across a broad spectrum of office-type workspaces and neighboring homes. The measured concentrations were compared against those measured across the United States and across the world. The results were also compared against a wide variety of radiation protection thresholds such as (1) the action levels of 148 Bq m -3 (the U.S. EPA action level for public housing), (2) ≈1,200 Bq m -3 OSHA threshold for office spaces, (3) effective dose threshold of 1 mSv threshold for defining a radiological worker, (4) 50 mSv occupational effective dose limit, and (5) 0.1 mSv and 1 mSv limits for public exposures from the air pathway and all pathways, respectively.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2023

Effects of Mineral Impurities and Heat on Uranium(VI) Sorption onto Bentonite (Final Report)

Most nuclear waste disposal options include compacted bentonite, consisting of montmorillonite clay, as part of a barrier system to minimize contaminant mobility. Uranium (U) is the primary element in spent nuclear fuel, and from an environmental perspective, a potential contaminant of water resources. Furthermore, uranium may control nuclear fuel degradation rates and the consequent release of other radioactive contaminants based on its diffusive transport away from waste canisters. Uranium sorption onto clay and other mineral surfaces is expected to limit U(VI) mobility in these systems. However, at this point a prediction of U(VI) sorption and transport behavior in performance assessment (PA) models is complicated by a series of factors, such as: (1) the presence of various U(VI) solution species with different charges and sorption characteristics; (2) the complex microstructure of montmorillonite clay resulting in two types of clay porosities and multiple sorption sites; (3) the largely unknown effects of bentonite mineral impurities on pore water chemistry, U(VI) sorption and diffusion behavior; and (4) the potential impacts of heat, generated by the decay of spent fuel, on mineralogical and microstructural transformations, and any subsequent effects on radionuclide sorption and mobility. In this project, we investigated the effects of calcite impurities on U(VI) sorption and diffusion onto montmorillonite before and after mineral exposure to heat. Overall, our main goals were to: 1. Gain a mechanistic understanding of the effects of calcite impurities on U(VI) sorption and diffusion in montmorillonite/bentonite at variable chemical conditions, and before and after mineral exposure to heat; and to 2. Work towards the development of new surface complexation and diffusion models to predict U(VI) sorption and mobility in montmorillonite/bentonite while accounting for the impacts of calcite impurities and heat. In order to achieve these goals, we pursued the following research objectives and tasks: 1. Characterize the effects of calcite impurities on U(VI) sorption onto Na-montmorillonite, and evaluate if and how these effects change due to solids’ exposure to heat (Task 1). 2. Characterize U(VI) surface speciation in solid samples from Task 1, with a particular focus on U(VI) precipitates and co-precipitates (Task 2). 3. Test the relevance of observed changes in U(VI) sorption characteristics for U(VI) diffusive transport behavior in bentonite barriers (Task 3). 4. Evaluate the exclusion of anionic U(VI) solution complexes from clay nanopores (Task 4). 5. Building on Tasks 1-4, start the development of new surface complexation and reactive transport models that can simulate and predict U(VI) sorption and diffusion in complex bentonite systems (Task 5). A detailed description of all tasks, and their specific results and conclusions is provided in this report.

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DOE OSTI2023

Innovative Strategies for Long-Term Monitoring of Complex Groundwater Plumes at DOE’s Legacy Sites (Workshop Report)

Most remaining Department of Energy (DOE) sites will require extended periods of institutional control, especially at complex groundwater sites where attenuation-based strategies have been implemented to facilitate closure. The current practice of monitoring—obtaining and analyzing contaminant concentration in groundwater samples at numerous wells—will account for a large portion of the projected life-cycle at these DOE sites unless a new approach is adopted. State-of-the-art technologies are being developed, including in situ sensors, geophysics, radiation mapping, numerical modeling and AI/ML. These technologies can optimize monitoring strategies in space and time, provide spatially extensive information at vulnerable regions and/or provide more continuous monitoring at lower cost. As part of DOE’s Office of Environmental Management (DOE-EM’s) efforts to advance long-term monitoring systems, an in-person/virtual hybrid workshop was hosted by Savannah River National Laboratory (SRNL) on January 24 and 25, 2023, in Augusta, Georgia. Because DOE-EM’s complex sites will eventually be transferred to DOE’s Office of Legacy Management (DOE-LM), representatives of DOE-LM were important participants in the workshop. The purpose of the workshop was to identify challenges and opportunities for deploying advanced technologies for long-term monitoring at DOE sites. The key questions during the workshop were: 1) the regulatory acceptance of replacing a process that traditionally has used laboratory sampling and analysis of groundwater samples, and 2) the application of this strategy to the southwestern arid sites that include many of the remaining DOE-EM and DOE-LM complex groundwater plumes. Characteristics common to most arid sites present both limitations and opportunities for advanced technologies. DOE-EM has funded a National Laboratory team from SRNL, Lawrence Berkeley National Laboratory (LBNL), and Pacific Northwest National Laboratory (PNNL) to establish the overarching framework of long-term monitoring by systematically combining advanced hardware and software technologies. This project is titled “Advanced Long-Term Environmental Monitoring Systems (ALTEMIS)” and is sponsored by the DOE-EM Technology Development Program. The multi-laboratory team is currently developing and testing innovative monitoring strategies, including the use of in situ groundwater sensors, geophysics, drone/satellite-based remote sensing, reactive transport modeling, and artificial intelligence/machine learning (AI/ML). The project’s demonstration testbed is at the Savannah River Site (SRS) F-Area Seepage Basins, where a well-characterized complex groundwater plume composed of uranium and other radionuclides is in the latter stages of remediation. The workshop included more than 70 participants, presentations, a field visit to F-Area, breakout working groups, and large group discussion. Participants developed recommendations on five topics: in situ sensors, spatially integrative tools, challenges to regulatory acceptance, AI/ML strategies, and transitioning sites to DOE-LM.

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DOE OSTI2023

Health Hazards of Exposures to Radioiodine

Iodine is a chemical element with atomic number 53. Iodine-127 is stable (non-radioactive) and commonly found in nature. Elemental iodine is a purple-colored solid at room temperature and pressure, but spontaneously sublimates (turns into vapor). Iodine is an essential element for life, and is required for proper functioning of the thyroid. Iodine is present in many foods, and is readily absorbed by the body and concentrated in the thyroid gland. A fraction of iodine ingested or inhaled is rapidly removed by the kidneys. The rest of the inhaled or ingested iodine is absorbed the by thyroid and retained for many months. Iodine has a biological half-life of approximately 120 days in health individuals. The biological half-life can be shorter in individuals with hyperthyroidism, and longer in individuals with hypothyroidism. Iodine has a number of radioactive isotopes, most of which have relatively short half-lives (days or weeks). Short half-life iodine isotopes are useful for a variety of medical applications, including imaging and cancer therapy. For example, Iodine-123 (half-life 13 hours) is commonly used for medical imaging of the thyroid, while iodine-131 (half-life 8 days) is used for suppressing thyroid function in individuals with hyperthyroidism or ablating (killing) thyroid cells to treat thyroid cancer. Iodine-125 (half-life 59 days) is produced in nuclear reactors, and has medical uses. Although iodine-125 can be used for thyroid imaging, Iodine-123 is more commonly used for that purpose because of its shorter half-life and higher-energy emissions. Iodine-125 is more commonly used for cancer treatment, and can be processed into small metal pellets (seeds) inserted directly into a tumor. Iodine-125 emits low-energy x-rays which can kill tumor cells and generally cannot escape the tumor, sparing other tissues. Medical iodine for imaging or treatment is typically administered orally in the form a pill or liquid solution. A typical adult thyroid scan using iodine-123 involves having the patient swallow between one and four 0.1 millicuries pills, with the exact dose dependent on the patient’s weight. This results in a whole-body committed effective dose of 80 – 320 mrem, and a thyroid equivalent dose of 1443 – 5772 mrem. Note that the whole-body effective dose relates to the overall cancer risk, while the larger equivalent dose to the thyroid only indicates that most of this risk is the result of exposure to the thyroid. These doses are considered safe, although the procedure is not recommended for pregnant or breastfeeding women. In contrast, the quantities of iodine-131 used for treatment of hyperthyroidism and thyroid cancers are much higher. For treatment of hyperthyroidism, 4 – 10 millicuries are administered, while for thyroid cancer the administration can range from 50 – 150 millicuries of I-131. In addition to medical exposures, large populations were exposed to radioiodine as result of the atomic bombings of Hiroshima and Nagasaki in Japan, and the Chernobyl nuclear accident. These populations have been carefully followed for many years to assess the effect of their radiation exposures on cancer risk. As a result, a great deal is known about the cancer risks associated with radioiodine exposure. Because iodine is concentrated in the thyroid, the principal risk of exposure to radioiodine is thyroid cancer. Children have the highest risk of thyroid cancer after exposure to radioactive iodine. According to a large study of Japanese atomic bomb survivors, an effective dose of one Sievert (100,000 mrem) has been observed to increase the risk of thyroid cancer by a factor of 9.5 in children aged zero to nine years old, by a factor of 3 in children aged 10 to 19 years old, and by barely detectable amounts in adults. Another way of quantifying the risk from radioiodine exposure is from risk coefficients, which provide the risk per unit intake of radionuclides in terms of both morbidity (any cancer) and mortality (death). Both morbidity (risk of cancer) and mortality (death) risks are shown in the table below. Note that because thyroid cancer is almost never fatal, the morbidity coefficients are much larger than the mortality coefficients.

61 RADIATION PROTECTION AND DOSIMETRY↗

DOE OSTI2021

Calendar Year 2020 Post-Closure Monitoring Report for Corrective Action Unit 99: Rainier Mesa/Shoshone Mountain, Underground Test Area, Nevada National Security Site, Nevada (Rev. 1)

This report presents the results of monitoring conducted for water quality, water levels, and institutional controls in calendar year (CY) 2020 by the U.S. Department of Energy (DOE), Environmental Management (EM) Nevada Program’s Underground Test Area (UGTA) Activity at Corrective Action Unit (CAU) 99, Rainier Mesa/Shoshone Mountain (RM/SM), at the Nevada National Security Site (NNSS), Nevada. This report also presents analytical laboratory results (including results of quality assurance/quality control samples, such as field duplicates [FDs]), and verification of use restrictions (URs), institutional controls, and water usage. Groundwater samples were collected; water levels were measured; and well site surveillance was conducted in support of the Underground Test Area Closure Report (CR) for Corrective Action Unit 99: Rainier Mesa/Shoshone Mountain, Nevada National Security Site, Nevada (DOE/EMNV, 2020). Rainier Mesa (RM) was the site of 61 underground nuclear tests, and Shoshone Mountain (SM) was the site of 6 underground nuclear tests. As a result of these activities, which took place from 1957 to 1992, radionuclides (RNs) were released in the subsurface in the vicinity of the detonations. These 67 underground nuclear tests are associated with 66 specific corrective action site (CAS) numbers, as listed in the Federal Facility Agreement and Consent Order (FFACO) (1996, as amended). Two tests, HURON LANDING and DIAMOND ACE (conducted simultaneously), are included within one CAS. The CR (DOE/EMNV, 2020) establishes the regulatory boundaries and regulatory boundary objectives, monitoring program, UR boundaries and URs, and other institutional controls agreed to by EM Nevada Program and the Nevada Division of Environmental Protection (NDEP) for closure of CAU 99. Regulatory boundaries for the RM/SM CAU were established to protect receptors of groundwater from RN contamination within the three downgradient groundwater basins that receive recharge from RM. The SM regulatory boundary was established to verify that RN contamination does not reach the lower carbonate aquifer below SM. The UR boundaries were established based on contaminant simulation forecasts from the flow and transport simulations with consideration of site-specific topographical controls. The URs associated with the UR boundaries were identified to protect onsite workers and the public from inadvertent exposure to contaminated groundwater as forecasted to occur assuming current conditions. The UR is intended to restrict activities that might expose workers to contaminated groundwater within the UR area. In addition to the URs, other institutional controls are established to monitor and limit access to groundwater. These include federal ownership and management in perpetuity, controlled access of the NNSS and surrounding areas, and reporting water use on the NNSS and surrounding hydrographic basins.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

U.S. Efforts in Support of Examinations at Fukushima Daiichi - November 2022 Meeting Notes and Information Request Status

Information obtained from Fukushima Daiichi Nuclear Power Station (Daiichi) is required to inform future Decontamination and Decommissioning (D&D) activities, improving the ability of the Tokyo Electric Power Company Holdings, Incorporated (TEPCO Holdings) to characterize potential hazards and to ensure the safety of workers involved with cleanup activities. This information also has important implications for the safety and operation of U.S. commercial nuclear power plants. This document summarizes results from the Fiscal Year 2023 (FY2023) U.S. effort to review Daiichi information and extract insights to enhance the safety of existing and future nuclear power plant designs. This U.S. effort, which was initiated in 2014 by the Department of Energy Office of Nuclear Energy, is completed by a group of experts in reactor safety and plant operations that identify examination needs and evaluate recent Daiichi examination data to address these needs. Fukushima-related information and associated discussions during these meetings benefit operating, new, and advanced reactors. Significant safety insights have been and are continuing to be obtained in several areas: system and component performance, radionuclide surveys and sampling, debris end-state location, combustible gas effects, and plant operations and maintenance. In addition to reducing uncertainties related to severe accident modeling progression, these insights have and continue to be used to update guidance for severe accident prevention, mitigation, and emergency planning. Furthermore, Daiichi-related activities, such as code modeling improvements and analysis, testing, and new technology deployment efforts, have the potential to offer additional benefits to the operating fleet and new LWR and non-LWR designs. U.S. evaluations of obtained examination information and input regarding future Daiichi examinations are of interest to several organizations within Japan. Since its inception, the U.S. has provided consensus input for high priority time-sequenced examination tasks and supporting research activities. In their Mid-to-Long-term Examination Plan for 1F investigations, TEPCO included all remaining U.S. consensus information requests and additional information requests they identified. TEPCO periodically provides reports on the status of these requests (reflecting D&D priorities, new insights from investigations, and new technologies that become available). Hence, U.S. experts agreed that it was appropriate for TEPCO to track and prioritize these information requests as D&D progresses. U.S. experts will continue to review and comment on the information obtained from examinations and, as needed, provide additional details and relevant background material to support future examinations. As documented in this report, several other items, such as additional details on information requests pertaining to ex-vessel examinations, relevant references from prior research, additional documents to provide insights regarding recent investigation findings, and reviews of recently released documents, were agreed to during the FY2023 meeting.

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DOE OSTI2023

Performance Assessment for the Disposal of Low-Level Waste in the 200 East Area Burial Grounds (Annual Status Report FY 2022)

This annual review provides the projected dose estimates of radionuclide inventories disposed in the 200 East Area Low-Level Waste Burial Grounds (LLBGs) since September 26, 1988. These estimates are calculated using the original dose methodology developed in the performance assessment (PA) analysis (WHC-SD-WM-TI-730). The estimates are compared with the performance objectives defined in U.S. Department of Energy requirements (DOE O 435.1 and its companion documents DOE M 435.1-1 and DOE-STD-5002-2017). All performance objectives are currently satisfied, and operational waste acceptance criteria (HNF-EP-0063) and waste acceptance practices continue to be sufficient to maintain compliance with performance objectives. Inventory estimates and associated dose estimates from future waste disposal actions are unchanged from previous years’ evaluations that indicate potential impacts well below performance objectives; therefore, future compliance with DOE O 435.1 is expected.

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DOE OSTI2023

Performance Assessment for the Disposal of Low-Level Waste in the 200 West Area Burial Grounds (Annual Status Report FY 2022)

This annual review provides the projected dose estimates of radionuclide inventories disposed in the active 200 West Area Low-Level Waste Burial Grounds (LLBGs) since September 26, 1988. These estimates are calculated using the original dose methodology developed in the performance assessment (PA) analysis (WHC-EP-0645). The estimates are compared with the performance objectives defined in U.S. Department of Energy requirements (DOE O 435.1 and its companion documents DOE M 435.1-1 and DOE-STD-5002-2017). All performance objectives are currently satisfied, and operational waste acceptance criteria (HNF-EP-0063) and waste acceptance practices continue to be sufficient to maintain compliance with performance objectives. Inventory estimates and associated dose estimates from future waste disposal actions are unchanged from previous years’ evaluations that indicate potential impacts well below performance objectives; therefore, future compliance with DOE O 435.1 is expected. Within the active burial grounds, low-level and mixed low-level waste currently may be disposed only in two lined trenches in the 218-W-5 Burial Ground (Trenches 31 and 34) until they are either filled or a decision is made to close these trenches. Some mixed low-level waste is also disposed at the Environmental Restoration Disposal Facility in the 200 West Area (which is covered under a separate PA). During this (fiscal year 2022) reporting period (October 1, 2021, through September 30, 2022), waste was disposed to the 200 West Area LLBGs. Continued groundwater monitoring of the 200 West Area LLBGs indicates no groundwater contamination due to LLBG waste. Current assumptions about future land use at the Hanford Site are consistent with PA analysis assumptions of a postclosure facility that will not be degraded by human activity. The LLBGs are in an area identified for waste management and containment of residual contamination (DOE/EIS-0391). The current closure plan for the LLBGs (DOE/RL-2000-70) estimates that the 200 West LLBGs will be closed in the 2050 timeframe. The Disposal Authorization Statement, other technical basis documents, and the radioactive waste management basis are of continued adequacy to meet the performance objectives of DOE O 435.1. Overall, there are no substantive changes to primary PA assumptions and no changes to the PA analysis conclusion; therefore, compliance with DOE O 435.1 and the Disposal Authorization Statement is maintained. A new PA to evaluate the long-term impacts of three disposal trenches that are currently active within the 200 East and 200 West Areas (Trench 94 in the 200 East Area and Trenches 31 and 34 in the 200 West Area) was initiated in fiscal year 2019 and completed in fiscal year 2022. Corrective actions addressing 3 key issues and 31 secondary issues identified during the review process were developed and submitted to the Low-Level Waste Disposal Facility Federal Review Group Co-Chairs for review and approval. This PA provides additional technical basis for the continued adequacy of the existing Operating Disposal Authorization Statement.

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DOE OSTI2022

Performance Assessment for the Disposal of Low-Level Waste in the 200 West Area Burial Grounds (Annual Status Report FY 2021)

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DOE OSTI2023

Thermodynamics of Minerals Stable near Earth's Surface

Project “Thermodynamics of Minerals Stable Near the Earth’s Surface” uses specialized calorimetric techniques to obtain new thermochemical data for solid phases of interest in the Earth’s “critical zone”, the near surface regions of the planet most directly affecting and affected by human activity. Major activity was in three areas: manganese oxide materials, aluminum clusters which are precursors to aluminum oxyhydroxide precipitates, and zeolites. All these classes of minerals are potential carriers of heavy metals and radionuclides in the environment, both within their crystal structures and as adsorbed layers or colloids. Their thermodynamic stability, as well as the sequence of stability of competing phases, governs the aqueous solubility of contaminants (and nutrients) in soil, groundwater, and sediments. The thermodynamics of these phases is strongly affected by particle size and crystallinity, since they often occur as very fine particles which do not coarsen in the near-surface environment. Many of these materials exhibit extensive polymorphism, multicomponent solid solution, and variable hydration states. Thus, one must define and systematize important thermodynamic variables, since one cannot make measurements on each and every possible phase, particle size, and composition. A major finding of the work on manganese oxides was labile water-induced oxidation-reduction reactions. These will be studied further by a combination of thermodynamic and synchrotron-based spectroscopic methods, the latter in collaboration with Peggy O’Day at UC Merced. The adsorption of other species, including simple organics, on such redox-active surfaces will also be investigated by a combination of thermochemical and spectroscopic studies. Studies of the energetics of water adsorption on mineral surfaces will be expanded to emphasize the adsorption of CO2 and small organic molecules, relevant to soil, groundwater, and the subsurface environment. Gas adsorption calorimetry, immersion calorimetry, and solution calorimetry will be combined with appropriate analytical and spectroscopic techniques to obtain a comprehensive picture of the interactions and their energetics. The evolution of aqueous aluminum clusters to form aluminum oxyhydroxide precipitates will be studied in detail by a combination of calorimetric and structural methods applied to aqueous samples aged at room temperature. The energetics of new classes of clusters will be explored. The project addresses several common themes relevant to the broad mission of the Department of Energy. Thermochemical data for minerals stable near the Earth’s surface, though still incomplete, are essential for understanding both natural and anthropogenic processes that affect our very existence on this planet. Such data contribute to the fundamental underpinning for mitigation and management strategies for the extraction and use of energy. Fundamental thermodynamic and mechanistic understanding is required to model processes ranging from heavy metal pollution to nuclear waste disposal to climate change.

58 GEOSCIENCES↗

DOE OSTI2020

EMP, Attachment 3: Dose Assessment Guidance

This Dose Assessment Guidance (DAG) describes methods used to comply with the reporting requirements for dose to an individual member of the public receptor, collective dose, and biota dose for radionuclide air emissions under the U.S. Department of Energy, Office of Science, Pacific Northwest National Laboratory (PNNL) Environmental Monitoring Plan (EMP). The National Emission Standards for Hazardous Air Pollutants (40 CFR 61), Subpart H, is the greatest driver for the requirements. This DAG applies to public dose from radioactive material releases to the air from PNNL Richland Campus and PNNL Sequim Campus. Dose determinations from Richland Campus surveillance of ambient external dose and ambient air particulates is also briefly discussed. This guidance is Attachment 3 to PNNL’s EMP (PNNL-20919) and addresses a discrete, vital subject area of the EMP that is subject to revision independent of the main text of the EMP document.

40 CFR 61 Subpart H↗

DOE OSTI2021

EMP Attachment 3: Dose Assessment Guidance (Rev.3)

This Dose Assessment Guidance (DAG) describes methods used to comply with the reporting requirements for dose to an individual member of the public receptor, collective dose, and biota dose for radionuclide air emissions under the U.S. Department of Energy, Office of Science, Pacific Northwest National Laboratory (PNNL) Environmental Monitoring Plan (EMP). The National Emission Standards for Hazardous Air Pollutants (40 CFR 61), Subpart H, is the greatest driver for the requirements. This DAG applies to public dose from radioactive material releases to the air from PNNL-Richland Campus and PNNL Marine and Coastal Research Laboratory. Dose determinations from Richland Campus surveillance of ambient external dose and ambient air particulates is also briefly discussed. This guidance is Attachment 3 to PNNL’s EMP (PNNL-20919) and addresses a discrete, vital subject area of the EMP that is subject to revision independent of the main text of the EMP document.

40 CFR 61 Subpart H↗