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At least 217 records · Page 12

Characterization of CST Post-Processing AP-105 Hanford Tank Waste

The primary goal of the Tank Side Cesium Removal (TSCR) system, under development by Washington River Protection Solutions, LLC (WRPS), is to remove entrained solids and 137 Cs from the Hanford tank waste supernate to expedite production of low-activity waste. Ion exchange (IX) testing of 10.9 L of waste from Hanford tank 241-AP-105 (AP-105), performed by Pacific Northwest National Laboratory, used a lead-lag-polish column format, with a bed volume of 10 mL per column, to decontaminate tank waste supernate using crystalline silicotitanate (CST) as the IX media. The AP-105 Cs IX processing test, discussed elsewhere, resulted in a shorter transition zone (i.e., steeper load curve) than those defined by wastes from tanks 241-AP-107 and 241-AW-102.1 The shorter transition zone was indicative of a matrix effect retarding Cs capacity. Therefore, aliquots of spent CST from the lead, lag, and polish columns were subjected to a digestion protocol to quantify analytes retained by the CST and extrapolate the impact on Cs capacity. The spent CST was digested using a combination of 5 M HNO 3 and H 2 O 2 with vigorous heating and stirring. Due to the radiation dose accompanying the 137 Cs on the CST columns, a secondary Cs separation by ammonium molybdophosphate embedded in polyacrylonitrile (AMP-PAN) was performed to separate the 137 Cs from the CST so the samples could be contact-handled for analysis outside of a shielded facility.

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Summary of MCU Flush Sample Results

Starting in May 2021, samples from the Modular Caustic-Side Solvent Extraction Unit (MCU) were sent to the Savannah River National Laboratory (SRNL) for analysis. Samples resulting from flushes of the Strip Effluent Hold Tank (SEHT) and the Decontaminated Salt Solution Hold Tank (DSSHT) were sent on multiple dates. Over the range of samples, all had less than detectable concentrations of Isopar-L™, and there was an overall decline in 137 Cs activity.

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Organic Iodide Sorption from Dilute Gas Streams

Reprocessing used nuclear fuel releases volatile radionuclides, including 129 iodine (I), into the off-gas of a processing plant. Volatile radioiodine could be present in several forms, depending on the chemistry of the process used and the off-gas stream. Inorganic I 2 is expected to be the predominant I species in the dissolver off-gas (DOG), with minor organic iodides present. The bulk of the I is expected to volatilize into the DOG in parts-per-million-level (ppm) concentrations. In contrast, in the vessel off-gas (VOG), most of the volatile I is expected to be found as organic iodides, such as CH 3 I, C 4 H 9 I, and C 12 H 25 I. These species are expected to be present in parts-per-billion-level (ppb) concentrations but require abatement, even at low expected concentrations, to meet regulatory emissions limits in the United States. Historically, studies of I abatement by Ag-functionalized sorbents have focused on inorganic I in the DOG, but in the last few years, more research attention has been given to organic iodides, especially longer chain species, such as C 4 H 9 I, and C 12 H 25 I. This report has three main goals: (1) to present new data generated at Oak Ridge National Laboratory (ORNL) in FY21 on the sorption behavior of organic iodides on AgZ, (2) to summarize and synthesize organic iodide data produced by ORNL and Idaho National Laboratory (INL) over the last 4 years to answer questions on organic iodides behavior outlined in the 2018 joint test plan (Jubin et al. 2018), and (3) to propose a VOG abatement system design that can provide the capture efficiencies required to meet I emission limits. The 2021 ORNL experimental campaign tested the effects of organic iodide speciation and concentration in the off-gas, superficial velocity of the off-gas, and effects of aging on AgZ sorbent capacity. These studies found that the sorption rate of organic iodides by AgZ depends on the hydrocarbon chain length and the concentration in the off-gas. Higher molecular weight organic iodides adsorb to AgZ more slowly than I. At a concentration of 50 ppm concentration in the off-gas, CH 3 I loads 8% slower, C 4 H 9 I loads 20% slower, and C 12 H 25 I loads 40% slower than I. The lowest concentration loading rates calculated were in 5 ppm organic iodide gas streams in which AgZ gained on average 0.14 mg I/g sorbent/hour in the bench scale test system. Thus, longer sorbent beds might be needed to accommodate slower loading rates onto AgZ in lower concentration gas streams. Although sorption rate varies as a function of hydrocarbon chain length, the saturation concentration of the sorbent for these I-bearing species does not vary. Aging AgZ in a humid air stream for 9 months drops the overall sorbent capacity by ~35% for CH 3 I, ~50% for C 4 H 9 I, and ~40% for C 12 H 25 I. This results in a saturation capacity between 35 and 70 mg I/g sorbent for the aged AgZ. In conjunction with recent data produced by INL, these data are used to estimate the mass transfer zone (MTZ) and decontamination factor (DF) for sorbent beds of AgZ. Sorption tests performed with iodide gas concentrations of about 1 ppm and higher at a superficial gas velocity of 10 m/min, indicate that MTZ depths for these conditions tend to range between about 8-20 cm. Tests performed at lower concentrations between 50-90 ppb and at gas superficial velocities of 1, 10, and 20 m/min indicate that the MTZ depth increases with increasing superficial gas velocity. The 20 m/min test indicates that the MTZ for those conditions was at least 22 cm, and doubling the superficial gas velocity from 10 to 20 m/min could roughly double or triple the MTZ depth. Doubling and tripling the bounding MTZ depth of 20 cm for the body of MTZ estimates made at with 10 m/min superficial velocity would extend the MTZ for a superficial velocity of 20 m/min to 40-60 cm. This bounding limit applies to all of the organic iodides that have been tested. These results also indicate that the sorption rate-limiting step is not sensitive to the superficial gas velocity; otherwise the MTZ depth would not have increased approximately in proportion to the increase in the gas superficial velocity. This further suggests that the rate limiting step is not associated with mass transfer of the sorbate to the sorbent surface, or mass transfer of the reaction byproducts from the sorbent surface, but is associated with sorption or chemical reactions on the sorbent surface or in sorbent pores. Deep bed testing at INL has established DFs of >2,000 for I, CH 3 I, and C 4 H 9 I under a range of conditions (Soelberg et al. 2021, Bruffey et al. 2019). DF does not seem to be affected by the concentration of the organic iodide in the gas stream over the range of 1 to 50 ppm. Thus, if the MTZ is accommodated in sorbent bed design for the DOG and VOG, then regulatory DFs will be met. To meet the third objective outlined in this report, these experimental data were used to update an engineering evaluation of the VOG first completed in 2016. The updated VOG design can be found in an accompanying document (Welty et al., 2021; INL- LTD-21-64587). This report finds that the VOG will decrease in both size and complexity, relative to previous designs, and will still meet regulatory requirements for all iodine forms.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

CB10412: Bulk CWA Destruction

The objective of this project was to eliminate and/or render bulk agent unusable by a threat entity via neutralization and/or polymerization of the bulk agent using minimal quantities of additives. We proposed the in situ neutralization and polymerization of bulk chemical agents (CAs) by performing reactions in the existing CA storage container via wet chemical approaches using minimal quantities of chemical based materials. This approach does not require sophisticated equipment, fuel to power generators, electricity to power equipment, or large quantities of decontaminating materials. By utilizing the CA storage container as the batch reactor, the amount of logistical resources can be significantly reduced. Fewer personnel are required since no sophisticated equipment needs to be set up, configured, or operated. Employing the CA storage container as the batch reactor enables the capability to add materials to multiple containers in a short period of time as opposed to processing one container at a time for typical batch reactor approaches. In scenarios where a quick response is required, the material can be added to all the CA containers and left to react on its own without intervention. Any attempt to filter the CA plus material solution will increase the rate of reaction due to increased agitation of the solution.

36 MATERIALS SCIENCE↗

CoDCon Project (Final Report)

The co-decontamination (CoDCon) project was established in FY 2016 with the objectives of (a) evaluating the uncertainty in the uranium (U)/plutonium (Pu) ratio in a mixed U/Pu product from a tributyl phosphate (TBP)–based solvent extraction flowsheet, and (b) developing and demonstrating on-line optical spectroscopy for real-time monitoring of key components (e.g., Pu, U, and HNO 3 concentrations) in the process solutions. We were interested in assessing the accuracy and precision to which a specific uranium-to-plutonium (U/Pu) ratio can be achieved, which for the purposes of this project was set at a U/Pu mass ratio of 7/3. The uncertainty associated with achieving this specific target U/Pu ratio was investigated during five flowsheet tests using laboratory-scale solvent extraction equipment. In addition, optical spectroscopic techniques were incorporated into the CoDCon solvent extraction testing system, allowing real time monitoring of all input and output process streams. Two CoDCon flowsheet tests were performed in FY 2018 using a simple dissolved fuel simulant containing only U (~1 M) and Pu (~15 mM) in nitric acid (HNO 3 ; ~3 M). In FY 2019, two additional flowsheet tests were performed. For the first of these (CoDCon Run 3), the dissolved fuel simulant was similar to that used in the first two tests, with the inclusion of 1 mM neptunium (Np). The second test conducted in FY 2019 (CoDCon Run 4) used a more representative dissolved fuel simulant, including addition of non-radioactive fission product elements. A fifth CoDCon flowsheet test (CoDCon Run 5) was conducted in FY 2020, with the following additional objectives: (1) routing of the technetium (Tc) in the simulated dissolved fuel solution to the solvent extraction raffinate, and (2) routing of the Np in the simulated dissolved fuel solution to the U/Pu product. All tests used a bank of sixteen 2 cm centrifugal contactors. The tests involved first loading the solvent (30 vol% TBP dissolved in n-dodecane) with U and Pu (and Np, for Run 5), then the Pu (and Np) was stripped from the loaded solvent with a U(IV) solution (~50 mM) and the flowsheet conditions were adjusted such that some U partitioned into the Pu-containing product stream. The amount of U accompanying the Pu was monitored in real time using optical spectroscopic techniques coupled with chemometric modeling. Based on the real-time spectroscopic measurement of the U/Pu ratio, adjustments were made to the flowrate of the fresh TBP solvent phase used to scrub U from the aqueous Pu-containing product. This proved to be a very effective way to control the U/Pu mass ratio in the product. This report presents the results of the CoDCon Run 5 test. The flowsheet tested in Run 5 was substantially different than that run in the prior tests, especially the solvent loading section of the flowsheet. Two key changes were made. First, based on the objective to extract all the Np and route it with the U/Pu product, pentavalent vanadium [V(V)] was added to the feed and scrub solutions. The purpose of the V(V) was to convert all the Np to the +6 oxidation state, which is extractable by TBP. Second, a high acid (8 M HNO 3 ) scrub was added to the flowsheet to scrub the Tc from the solvent. This was followed by a low acid scrub (0.05 M HNO 3 ) to reduce the residual HNO 3 concentration in the solvent prior to the Pu stripping step. The output from the low acid scrub was collected separately, rather than routing towards the raffinate. The modifications to the solvent loading part of the flowsheet were only partially successful. The treatment with V(V) was effective at converting the Np to Np(VI). Only 1.3% of the Np remained in the raffinate solution. However, ~40% of the Np stripped out of the solvent in the low acid scrub step; nearly 20% of the Pu also was stripped from the solvent during the low acid scrub. For further development, either modifications to the flowsheet, or concentration and recycle of the low acid stream into the

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U.S. Efforts in Support of Examinations at Fukushima Daiichi (November 2021 Meeting Notes with Updated Information Requests)

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 2022 (FY2022) 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 forensics meetings benefit operating, new, and advanced reactors. Significant safety insights are being 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. As discussed in this document, revised operator guidance was successfully used to improve operator response during a loss of off-site power event at the Duane Arnold Energy Center plant. Reduced uncertainties in modeling the events at Daiichi improve the realism of reactor safety evaluations that inform future D&D activities. U.S. evaluations of information from Fukushima and input regarding future examinations are of interest to several organizations within Japan. Meeting presentations by Japan describe how comments and recommendations documented in prior U.S. forensics effort reports, including consensus information requests developed by forensics effort participants, are considered in future Fukushima D&D activities. As discussed in this report, TEPCO Holdings considered these information requests in their D&D planning activities. An updated list of consensus information requests is included in this FY2022 report.

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Mercury Remediation Technology Development for Lower East Fork Poplar Creek—FY 2021 Update

Mercury remediation is a high priority for the US Department of Energy (DOE) Oak Ridge Office of Environmental Management. Mercury contamination in the environment can be found at all three DOE facilities in Oak Ridge, Tennessee, but the greatest environmental risk concern relative to Hg on the Oak Ridge Reservation is likely associated with historical Hg losses at and near the Y-12 National Security Complex (Y-12). Mercury in water and fish from East Fork Poplar Creek (EFPC) downstream of Y-12 exceeds regulatory thresholds. Because of the complexities of Hg transport and fate in the aquatic environment, conventional remedial options for EFPC are highly uncertain. DOE is using a phased adaptive management approach to Hg remediation at Y-12, with a focus in the next few years on construction of the Mercury Treatment Facility (MTF) to treat the most contaminated Y-12 outfall entering EFPC (DOE 2017a; DOE 2017b). Once operational, the MTF will provide additional protection against inadvertent releases of Hg into the stream from decontamination and decommissioning of Y-12 Hg-use buildings. Although the MTF is anticipated to substantially decrease Hg water concentrations and flux in upper EFPC (UEFPC), research and technology development are needed to develop appropriate and longer-term remedial solutions for the downstream environment. Since late 2014, the Oak Ridge Office of Environmental Management and URS | CH2M Oak Ridge LLC/Restoration Services Inc. have supported DOE’s Oak Ridge National Laboratory (ORNL) Environmental Sciences Division staff in conducting field and laboratory studies to develop Hg remedial technology solutions for lower EFPC (LEFPC). Whereas previous annual reporting updates for Hg remediation technology development for LEFPC have focused on presenting detailed results from the previous fiscal year, this FY 2021 update takes a comprehensive, higher-level approach to the research and technology development activities conducted since 2014. The report is organized to be consistent with the three tasks defined in the LEFPC strategic plan

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Characterization of Tank 11H Samples from Tank Closure Cesium Removal 1A (TCCR 1A) Batch 1

Savannah River Mission Completion (SRMC) is currently operating the Tank Closure Cesium Removal 1A (TCCR 1A) process to remove 137 Cs from tank waste supernate using an ion exchange process. The TCCR 1A unit processes dissolved salt fed from Tank 10H through a series of ion exchange columns containing crystalline silicotitanate (CST, IONSIV TM R9120-B, 30x60) and the effluent is then discharged to Tank 11H. In support of the TCCR 1A program, SRNL analyzed samples taken from Tank 11H (without tank mixing) before, during, and at the completion of TCCR 1A Batch 1 processing. Tank 11H serves as the receipt tank for the filtered and cesium removed product from the TCCR 1A system. Processing of Batch 1 commenced on January 13, 2022 and completed on February 17, 2022, after processing approximately 70,100 gallons. A pre-production sample was collected from the heel remaining in Tank 11H just before Batch 1 processing began. In addition, five interim surface samples were collected from Tank 11H during processing, and both a surface and a variable depth sample (VDS, ~7” from tank bottom) were collected just after processing completed. Analysis of all samples included density and gamma spectroscopy, in addition to a more comprehensive suite of analytes for the pre- and post-production samples. The density of the pre-production sample was the highest of all samples measured and was then observed to decrease for the first two interim samples, followed by becoming fairly consistent for the remainder of the samples (~1.3 g/mL). The density of 1.3 g/mL is similar to the density measured for one of the three Tank 10H qualification samples (HTF-10-21-126). The 137 Cs activity was found to decrease as additional decontaminated effluent from the TCCR columns was added to Tank 11H during processing; however, an increase in activity was observed during periods of no processing which can be attributed to leaching of 137 Cs from the known solids in Tank 11H. The Cs isotope concentrations in the Tank 11H postproduction surface sample were determined to be 99.7-99.8% lower than the concentrations measured in the Tank 10H feed as measured by mass spectrometry.

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Environmental Monitoring Report, Calendar year 2020. Knolls Laboratory and Kesselring Site

The results of the effluent and environmental monitoring programs at the Knolls Laboratory and Kesselring Site are summarized and assessed in this report. Tables 1 - 4 summarize the major elements of the environmental monitoring programs at each site. Information regarding the U.S. Department of Energy – Office of Environmental Management (DOE-EM) Separations Process Research Unit (SPRU) Disposition Project (SPRU DP), is also included in this report; however, the project was completed in 2020 and will no longer be reported in subsequent reports. DOE-EM will be continuing to perform other Decontamination & Decommissioning (D&D) work at Knolls Laboratory and Kesselring Site, which may require environmental monitoring, and will be included in this report, as warranted. Operations at the Knolls Laboratory, which includes SPRU and other DOE-EM activities, and the Kesselring Site continue to have no adverse effect on human health and the quality of the environment.

54 ENVIRONMENTAL SCIENCES↗

An Adaptable and Comprehensive Project Assessment Tool

Most companies, agencies, and other real property owners require capital asset projects to pass some type of scrutiny before budgets and authority to expend funds for the design, construction and eventual operations are approved. This process typically involves management approval of key/critical decision(s) or a project’s passage through gates (or critical decisions). Cost, functionality, safety, and risk are just some of the factors typically considered during project assessment processes. This paper describes a tool that was developed and is used by the Department of Energy to facilitate this project assessment process. There are three versions of this tool for construction, decontamination and decommissioning (D&D), and environmental restoration/cleanup project types. The tool’s elements and associated criteria are tailored for each project type; although some elements, such as cost estimating and scheduling, are used in common. The tool is easy to use, requiring little or no training. It provides a common assessment tool for project self-appraisals and independent project reviews. It promotes efficiency and reduces disagreements and unnecessary effort. A comprehensive array of elements covers the gamut of cost, schedule, scope/technical, and safety/security ensuring that no important project attributes are overlooked. The tool is adaptable for use by any organization.

97 MATHEMATICS AND COMPUTING↗

Removal of Tc-99, Zr-95, and Nb-95, From Solutions Obtained After Dissolution of Irradiated Mo Targets

Decontamination of 99 Tc, Nb, and Zr impurities in dissolved irradiated Mo disks can be accomplished using Fe(II) precipitation. Here, we report bench-scale experiments and large-scale demonstrations on removal of 99 Tc (0.1 mM), 95 Nb, and 95 Zr from dissolved Mo disk simulant solutions. Tc removal is accomplished through the reduction and simultaneous immobilization of Tc(VII) by Fe(II), producing an insoluble, Tcincorporated Fe(II)-Fe(III) solid that is removed by filtration. Large-scale testing showed that Tc (97.6% ± 1.7%) is removed without affecting 99 Mo yields. Other important side reaction product impurities in irradiated Mo targets, namely various isotopes of Nb and Zr, are also removed (>99%) in this process. The effects of metal (Fe, Tc, Mo) concentrations, Fe(II)/Fe(III) ratio, pH, temperature, Fe addition method, and hydrogen peroxide addition were tested. The minimum amount of Fe(II) needed to remove up to 99% Tc is 10 mM and the optimal pH value for simultaneous removal of Tc, Nb, and Zr impurities is pH 13.

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User’s Manual for RESRAD-BUILD Code V.4: Vol. 1 – Methodology and Models Used in RESRAD-BUILD Code

The RESRAD-BUILD computer code models radionuclide release and transport in indoor environments and performs pathway analyses to evaluate the potential radiological dose and risk incurred by an individual who works or lives in a building contaminated with radioactive material or housing radioactively contaminated furniture or equipment. The code provides four geometries to characterize a radiation source: point, line, area, and volume, in which radionuclides are homogeneously distributed. Radionuclides contained in a source are considered to be released to the indoor air due to various processes including erosion (mechanically or weathering), diffusion (for tritium and radon in a volume source), or emanation (radon in a point, line, or area source). The release can proceed through different time phases with different rates. In RESRAD-BUILD Version 4.0, a dynamic ventilation model is implemented to simulate the fate and transport of source material particles and radionuclides after their releases. This dynamic ventilation model considers (1) air exchange between rooms in the building and between the rooms and the outdoor environment, (2) deposition from air to floor, (3) resuspension from the floor to the air, and (4) periodical vacuuming that reduces the floor deposition. The fate and transport modeling provides estimates of radionuclide concentrations in the source, in the air, and on the floor at different times, which are then integrated over the exposure duration for the calculation of radiation doses and cancer risks. A single run of the RESRAD-BUILD code can model a building with up to 9 rooms, 10 sources, and 10 receptors. The potential radiation dose and cancer risk incurred by each receptor are calculated for seven exposure pathways: (1) external radiation directly from the sources (accounting for shielding), (2) external radiation from radioactive particles deposited on the floors, (3) external radiation from airborne radionuclides, (4) inhalation of airborne radionuclides, (5) inhalation of radon and radon progenies, (6) inadvertent ingestion of radioactive particles directly from the source, and (7) ingestion of radioactive particles deposited on the floors. Various exposure scenarios can be modeled with RESRAD-BUILD, including but are not limited to, office worker, renovation worker, decontamination worker, building visitor, and resident. Both deterministic and probabilistic analyses can be performed to obtain results in both text reports and graphic displays.

61 RADIATION PROTECTION AND DOSIMETRY↗

Off-Gas Design and Testing from Advanced Chlorination Process

Chlorination of Zr alloy cladding with sulfur-chloride reagents is being considered as a means of separating the main metal from alloying elements, imbedded U, actinides, and fission and activation products to purify the Zr. This would allow the Zr to be disposed of as low-level nuclear waste or possibly be recycled. A multistage process was developed that involves several steps and waste streams. Recycling of sulfur-chloride reagents S 2 Cl 2 and SOCl 2 is planned to minimize the waste stream. The generation of off-gas and entrainment of volatiles is anticipated to be minimized. However, given the complex nature of spent nuclear fuel (SNF), some volatile components will be generated, including the solvents themselves; Cl 2 used for the regeneration of S 2 Cl 2 ; volatile fission product chlorides, such as Sb and 3 H; and chlorinated alloying components, such as Sn, Nb, Fe, and Mo. This report discusses the chemical phenomena that might give rise to volatile species and their planned capture. The volatility of the transition metals will depend on their oxidation state and the compounds that are formed, such as Zr tritide. Loading radionuclides in the process off-gas will depend on the inputs to the process. For instance, processing separated Zr to reduce waste will have a much lower loading of radionuclides than if alternative chlorination were used for decladding SNF. Much of the volatile process streams will be part of the solvent recycling, which may involve online scrubbing. Generally, a caustic scrubber should be included in the off-gas to remove acidic vapors (e.g., Cl 2 , SOCl 2 ). The decontamination procedures for removing these species could involve pretreatment (i.e., heating) options or reduction by contact with H 2 . This report discusses these options along with a framework for testing these alternatives in future experiments. Technologies for off-gas capture will leverage those developed in the Materials Recovery and Waste Forms program.

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Screening Level Ecological Exposure Assessment Work Plan

This work plan is part of an effort to complete an updated evaluation of the potential for adverse effects from miscellaneous treatment unit emissions to potential ecological receptors within and surrounding Site 200. It will address potential pathways between air emissions from the Lawrence Livermore National Laboratory’s (LLNL) Decontamination and Waste Treatment Facility (DWTF), single emission stack, and ecological receptors (i.e., plants and wildlife) present onsite and within a one-mile radius from the DWTF stack. This work plan outlines the procedures by which data collected as part of the previous investigations will be evaluated to assess risks to ecological receptors. It presents the problem formulation, initial conceptual site models, methods for characterizing exposure, toxicity, and risks that will be used if a more detailed “baseline” ecological risk assessment (BERA) is required.

54 ENVIRONMENTAL SCIENCES↗

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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Mercury Speciation During Vitrification of LAW

n this work, laboratory and engineering-scale tests were conducted that mimic the reactive environment of the Hanford Tank Waste Treatment and Immobilization Plant (WTP) low activity waste (LAW) melter and off-gas system in order to assess the speciation of mercury at select points in the processing system. The experimental protocols, test equipment, feed materials used, and rationale for testing are detailed in the Test Plan for this work. Particular attention was paid to the amount and speciation of mercury in submerged bed scrubber (SBS) solutions, which are intended to be recycled back to the melter feed at the WTP. Results are presented from detailed mercury analysis of these solutions using Environmental Protection Agency (EPA) Method 1630 and modifications to this method for dimethyl mercury and methyl mercury as well as EPA Method 1631 and modifications to this method for total, dissolved, elemental, suspended, and ionic mercury. Testing was conducted in two separate sets of experiments: (1) One set of tests (crucible-scale furnace tests) that involved heating small batches of mercury-spiked melter feed in crucibles to determine the amount of mercury retained in the glass and the species of mercury in the exhaust gases; (2) A second set of tests (DM10 melter tests) was planned that involved creating LAW melter plenum gas compositions using the DM10 melter system, injecting mercury into the off-gas stream, and passing that stream though a reactor that simulates various plenum gas conditions. Operational issues led to the need to use one of the VSL DM100 melters in place of the planned DM10 melter for these tests. The speciation of mercury after exposure to those conditions was monitored. In both sets of tests, the exhaust gases were run through a scrubber that was intended to mimic the LAW SBS in order to determine how much of the mercury exiting the melter would be retained in the primary off-gas system fluids and in what form. After passing through the SBS, the exhaust stream was analyzed to determine particulate, ionic, elemental, and total mercury passing downstream of the SBS. In tests employing gases derived from the DM100 melter that were spiked with elemental mercury, the processing system provided gas temperatures and residence times that are representative of the WTP LAW vitrification system in order to assess the effect of those conditions on mercury speciation. The Decontamination Factor (DF) across the system in the tests with mercury-spiked DM100 melter exhaust was determined using the analytical data from EPA Method 30B (Fluegas Adsorption Mercury Speciation (FAMS TM )) exhaust samples and the amount of mercury detected in the SBS solutions. Mercury species used in melter feed crucible scale tests were divalent (chloride and iodide), monovalent (chloride and fluoride), and elemental mercury. Individual tests included only a single form of mercury in the feed. The results for total mercury mass balances in the crucible tests are also presented.

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Cultural Resource Management Plan for Brookhaven National Laboratory

The Cultural Resource Management Plan (CRMP) for Brookhaven National Laboratory (BNL) provides an organized guide that describes or references the facets and interrelationships of cultural resources at BNL. Management strategies included within this CRMP are designed to adequately identify the cultural resources that BNL and DOE consider significant and to acknowledge associated management actions. A principal objective of the CRMP is to reduce the need for additional regulatory documents and to serve as the basis for a formal agreement between the DOE and the New York State Historic Preservation Officer (NYSHPO). The BNL CRMP is designed to be a “living document.” Each section includes identified gaps in the management plan, with proposed goals and actions for addressing each gap. The plan will be periodically revised to incorporate new documentation. The current (2023) update incorporates new findings and/or updated text based on completed or ongoing projects related to cultural resources at BNL since inception of the last updated CRMP in 2013. Historically, Brookhaven National Laboratory had little need for cultural resource management because many of its buildings were less than 50 years old. Most of the features that are potentially eligible for inclusion in the National Register of Historic Places were protected simply by avoiding the features. Compliance with cultural resource laws and regulations has included archeological surveys, such as those associated with the 1977 Final Environmental Impact Statement for Brookhaven National Laboratory and the 1978 Final Environmental Impact Statement for the Proton-Proton Storage Accelerator Facility (ISABELLE). In 1979, World War I trenches associated with the former Camp Upton and located near ISABELLE were determined to be eligible for inclusion in the National Register of Historic Places; however, many of these trenches had been destroyed by construction work. In 1991, the NYSHPO provided BNL with a letter indicating that only three structures and features were likely to be eligible for inclusion in the National Register of Historic Places. Between 1991 and 1999, little work associated with cultural resource management was accomplished. Beginning in 1999, awareness for the need of a program to manage cultural resources grew out of the realization that over half of the buildings at BNL were either 50 years old or were reaching that age and were, therefore, subject to the requirements in Section 106 of the National Historic Preservation Act. This fact, concomitant with the decontamination and decommissioning of the Brookhaven Graphite Research Reactor (BGRR) and the subsequent determination of BGRR’s eligibility for listing as an historical site, fueled the need for developing and implementing a more structured program for managing cultural resources at BNL.

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Low Activity Waste Tuning Feed Material Testing VSL-18R4350-1 (Final Report)

High level waste (HLW) from the Hanford tank farms will be retrieved and transferred to the Hanford Tank Waste Treatment and Immobilization Plant (WTP). The waste will be pretreated to separate the soluble chemical salts (mostly sodium nitrate/nitrite and sodium hydroxide) from the bulk of the radioactive materials. This decontaminated salt solution is the low activity waste (LAW) stream which constitutes most of the total waste volume. The remaining HLW contains most of the radioactive materials but a fraction of the volume. Each of these waste streams is directed to an independent processing facility where the waste is mixed with glass forming chemicals (mostly silica and borax or boric acid) and fed into the melters for stabilization by conversion into glass. The molten glass is poured into stainless steel containers to produce packages for disposal: local shallow burial for the LAW containers and a future geologic repository for the HLW containers. The LAW facility melters produce significant quantities of NOx-laden off-gas that require abatement in accordance with 10 CFR 830 and air emission requirements. The NOx emissions also pose a safety risk. The LAW facility commissioning sequence requires that the melters be operated and process control loops tuned prior to introducing waste or waste feed materials that produce NOx. Therefore, a temporary or permanent system architecture is needed that provides a feed supply to the melters for the purpose of melter testing and off-gas tuning that does not result in the production of significantly hazardous off-gas products.

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