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Pacific Northwest National Laboratory Annual Site Environmental Report for Calendar Year 2019 (Final Report)

The PNNL Annual Site Environmental Report is prepared to meet the requirements of DOE Order 231.1B, Environmental, Safety and Health Reporting, and DOE Order 458.1, Radiation Protection of the Public and the Environment, assuring that the public is informed of any PNNL Richland Campus or PNNL Sequim Campus event that could adversely affect the health and safety of the public, site staff, or the environment. The report provides a synopsis of ongoing environmental management performance and compliance activities for operations that occur on the PNNL Richland Campus in Richland, Washington, and at the PNNL Sequim Campus near Sequim, Washington. It describes the location of and background for each facility; addresses compliance with applicable DOE, federal, state, and local regulations and site-specific permits; documents environmental monitoring efforts and their status; presents potential radiation doses to staff and the public in the surrounding areas; and describes DOE-required data quality assurance methods used for data verification.

54 ENVIRONMENTAL SCIENCES↗

Pacific Northwest National Laboratory Facility Radionuclide Emission Points and Sampling Systems

Battelle–Pacific Northwest Division operates numerous research and development laboratories in Richland, Washington. U.S. Department of Energy (DOE) contracts to Battelle include Richland facilities on the DOE Hanford Site and the Pacific Northwest National Laboratory (PNNL) – Richland Campus that have the potential for radionuclide air emissions. The PNNL contract also includes DOE operations at the PNNL-Sequim Campus, in Sequim, Washington, where there is also the potential for radionuclide air emissions. This document is a periodic update that describes current PNNL facility emission units and sampling systems.

54 ENVIRONMENTAL SCIENCES↗

Treatment of Problematic Reactive Metal Wastes Using GeoMelt ICV - WM2020 Conference Paper

Decommissioning of sodium-cooled reactors and fast reactor technologies has generated a number of reactive metal waste configurations that are problematic to treat and typically lack cost effective treatment methods and disposition options. As a result, Veolia Nuclear Solutions, under contract with Idaho National Laboratory (owned by the U.S. Department of Energy and managed and operated by Battelle Energy Alliance, LLC) demonstrated its GeoMelt® In-Container Vitrification (ICV)™ technology to safely convert sodium metal to a non-reactive vitrified oxide form. The demonstration project, supported by glass formulation and crucible testing, consisted of a series of ICV™ melts that processed elemental sodium into stable non-reactive glass. INL is currently implementing GeoMelt® technology as a means to safely and reliably convert radioactive reactive metal residues that contaminate sodium cooled reactor components into waste forms that comply with existing disposition pathways. Reactive metal wastes require treatment in order to remove the Resource Conservation and Recovery Act (RCRA) reactivity and ignitability characteristics to comply with land disposal restrictions. GeoMelt®, which is an alternative to other potential treatment approaches, provides a robust approach that chemically converts the reactive metals to an inert oxide while also immobilizing radionuclides in a vitrified waste form with durability equal to or better than vitrified nuclear fuel reprocessing wastes (very robust and inert waste forms). Most other treatment approaches generate hydrogen gas which is problematic. In 2016, Veolia Nuclear Solutions first demonstrated the effectiveness of the GeoMelt® ICV™ process in deactivating reactive sodium metal. Crucible, bench-scale, and engineering-scale demonstrations were conducted on several surrogate waste configurations with various ratios of sodium metal and glass-formers. Each ratio and configuration demonstrated complete deactivation of the surrogate sodium metal. Follow-on work in 2017 demonstrated the deactivation of reactive sodium by GeoMelt® ICV™ at a higher waste loading relative to previously demonstrated work performed in 2016; the higher waste loading optimized glass chemistry while enhancing the economical full-scale treatment of reactive metals. Additionally, follow-on demonstration testing in 2018 and 2019 focused on more complex shapes and other reactive-metals (mocked up Experimental Breeder Reactor II [EBR-II] subassembly, sodium filled heat exchanger, and a can containing sodium potassium alloy) which were all performed at engineering-scale. Since 2018, a 10-metric ton full-scale GeoMelt unit (GeoMelt® Richland) was designed, installed, and commissioned at Perma-Fix Northwest in Richland, Washington for the treatment of reactive metal wastes. As of September 2019, over 900 55-gallon drums containing a total of around 3,500 lb of sodium with low levels of radioactivity have been treated at GeoMelt ® Richland, with resulting glass monoliths disposed at the Nevada National Security Site (NNSS). A full-scale radiological demonstration melt on an actual EBR-II subassembly has also been performed using the full-scale melter in 2019. The GeoMelt® technology is a proven radioactive waste treatment technology capable of immobilizing radioactive wastes, including bulk rubble such as drums and other steel vessels usually without pretreatment. Utilizing the GeoMelt® technology to treat reactive metals eliminates pretreatment steps resulting from having to separate the reactive metal from steel containers or jackets as GeoMelt® can easily operate at temperatures sufficient to melt the steel and expose the reactive metal for treatment. Eliminating handling steps of reactive metals is a significant safety advantage since reactive metals are pyrophoric. The results generated as a part of the 2018-2019 demonstration program are presented in the paper.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Treatment of Problematic Reactive Metal Wastes Using the GeoMelt{sup R} In-Container Vitrification (ICV{sup TM}) Process - 20326

Decommissioning of sodium-cooled reactors and fast reactor technologies has generated a number of reactive metal waste configurations that are problematic to treat and typically lack cost effective treatment methods and disposition options. As a result, Veolia Nuclear Solutions, under contract with Idaho National Laboratory (owned by the U.S. Department of Energy and managed and operated by Battelle Energy Alliance, LLC) demonstrated its GeoMelt{sup R} In-Container Vitrification (ICV){sup TM} technology to safely convert sodium metal to a non-reactive vitrified oxide form. The demonstration project, supported by glass formulation and crucible testing, consisted of a series of ICV{sup TM} melts that processed elemental sodium into stable non-reactive glass. INL is currently implementing GeoMelt{sup R} technology as a means to safely and reliably convert radioactive reactive metal residues that contaminate sodium cooled reactor components into waste forms that comply with existing disposition pathways. Reactive metal wastes require treatment in order to remove the Resource Conservation and Recovery Act (RCRA) reactivity and ignitability characteristics to comply with land disposal restrictions. GeoMelt{sup R}, which is an alternative to other potential treatment approaches, provides a robust approach that chemically converts the reactive metals to an inert oxide while also immobilizing radionuclides in a vitrified waste form with durability equal to or better than vitrified nuclear fuel reprocessing wastes (very robust and inert waste forms). Most other treatment approaches generate hydrogen gas which is problematic. In 2016, Veolia Nuclear Solutions first demonstrated the effectiveness of the GeoMelt{sup R} ICV{sup TM} process in deactivating reactive sodium metal. Crucible, bench-scale, and engineering-scale demonstrations were conducted on several surrogate waste configurations with various ratios of sodium metal and glass formers. Each ratio and configuration demonstrated complete deactivation of the surrogate sodium metal. Follow-on work in 2017 demonstrated the deactivation of reactive sodium by GeoMelt{sup R} ICV{sup TM} at a higher waste loading relative to previously demonstrated work performed in 2016; the higher waste loading optimized glass chemistry while enhancing the economical full-scale treatment of reactive metals. Additionally, follow-on demonstration testing in 2018 and 2019 focused on more complex shapes and other reactive-metals (mocked up Experimental Breeder Reactor II [EBR-II] subassembly, sodium filled heat exchanger, and a can containing sodium potassium alloy) which were all performed at engineering scale. Veolia Nuclear Solutions designed, installed, and commissioned in September 2018, at Perma-Fix Northwest in Richland Washington, a 10-metric ton full-scale GeoMelt unit (GeoMelt{sup R} Richland) for the treatment of reactive metal wastes. As of September 2019, over 900 55-gallon drums containing a total of around 3,500 lb of sodium with low levels of radioactivity have been treated at GeoMelt{sup R} Richland, with resulting glass monoliths disposed at the Nevada National Security Site (NNSS). A full-scale radiological demonstration melt on an actual EBR-II subassembly has also been performed using the full-scale melter in 2019. The GeoMelt{sup R} technology is a proven radioactive waste treatment technology capable of immobilizing radioactive wastes, including bulk rubble such as drums and other steel vessels usually without pretreatment. Utilizing the GeoMelt{sup R} technology to treat reactive metals eliminates pretreatment steps resulting from having to separate the reactive metal from steel containers or jackets as GeoMelt{sup R} can easily operate at temperatures sufficient to melt the steel and expose the reactive metal for treatment. Eliminating handling steps of reactive metals is a significant safety advantage since reactive metals are pyrophoric. The results generated as a part of the 2018-2019 demonstration program are presented in the paper. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Advanced Retrieval and Disposition Techniques for Remote Handled Mixed Low-Level Waste - 20319

Legacy waste generated by the sodium-cooled fast reactor, EBR-II, program at the Idaho National Laboratory (INL) (owned by the U.S. Department of Energy and managed and operated by Battelle Energy Alliance, LLC) is challenging to treat and disposition using conventional methods. As a result, Veolia Nuclear Solutions is under contract with the Idaho National Laboratory to demonstrate an integrated retrieval and disposition solution for Remote-Handled Mixed Low-Level Waste currently stored in underground liners at INL. Delivery of the integrated solution builds on the expertise and successes of Veolia Nuclear Solutions under its Problematic Waste Treatment Initiative with INL. This initiative focuses solely on the treatment of problematic (reactive metal containing) waste streams using the Veolia Nuclear Solutions GeoMelt{sup R} In-Container Vitrification (ICV{sup TM}) technology. Under the contract, Veolia Nuclear Solutions will provide a fully commissioned prototype remote retrieval system to semi-remotely retrieve and size-reduce problematic waste liners into a safe and consolidated package for transport. The consolidated package will be shipped to Richland, Washington for demonstration treatment using the robust GeoMelt Richland system at Perma-Fix Northwest. The treated waste will ultimately be disposed of as a vitrified Low-Level Waste glass monolith. Veolia Nuclear Solutions has delivered countless remotely operated systems globally to solve some of the industry's most challenging problems. To ensure risk is mitigated in the best possible manner, a methodical phased approach is being utilized to validate the integrated solution. This contract focuses on the delivery and deployment of the prototype retrieval system onsite and the treatment of a single liner. Following successful demonstration treatment using GeoMelt ICV, the project is planning to make prototype enhancements before retrieving and treating another liner. Establishing a new integrated approach for retrieval and disposition of waste offers many benefits to INL and the U.S. Department of Energy. It is anticipated that the integrated solution will provide significant cost and schedule savings by increasing the number of liners dispositioned per year. In addition, the complexity of the overall waste disposition process will be reduced. Remotely retrieving and size-reducing waste in the field will provide additional safety to operational personnel and allow critical resources, such as hot cells, to focus on the primary missions at hand. Vitrification (using the GeoMelt ICV technology) allows for the direct processing of metal clad waste thereby significantly reducing pretreatment steps while providing a robust waste form for long-term disposal. The results from this ongoing contract are presented in this paper. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Radiative impact of record-breaking wildfires from integrated ground-based data

The radiative effects of wildfires have been traditionally estimated by models using radiative transfer calculations. Assessment of model-predicted radiative effects commonly involves information on observation-based aerosol optical properties. However, lack or incompleteness of this information for dense plumes generated by intense wildfires reduces substantially the applicability of this assessment. Here we introduce a novel method that provides additional observational constraints for such assessments using widely available ground-based measurements of shortwave and spectrally resolved irradiances and aerosol optical depth (AOD) in the visible and near-infrared spectral ranges. We apply our method to quantify the radiative impact of the record-breaking wildfires that occurred in the Western US in September 2020. For our quantification we use integrated ground-based data collected at the Atmospheric Measurements Laboratory in Richland, Washington, USA with a location frequently downwind of wildfires in the Western US. We demonstrate that remarkably dense plumes generated by these wildfires strongly reduced the solar surface irradiance (up to 70% or 450 Wm -2 for total shortwave flux) and almost completely masked the sun from view due to extremely large AOD (above 10 at 500 nm wavelength). We also demonstrate that the plume-induced radiative impact is comparable in magnitude with those produced by a violent volcano eruption occurred in the Western US in 1980 and continental cumuli.

54 ENVIRONMENTAL SCIENCES↗

Multi-omics data resource: Data package 25 (Pck025)

This data package comprises omics datasets from human pancreatic islets treated with IL-1β + IFNγ or with estrogen (E2) for 18 h. Two RNA-seq datasets are available: the first is a discovery dataset involving human islets treated with or without IL-1β + IFNγ for 18 hours; the second is a validation dataset, where human islets are treated with or without IL-1β + IFNγ or E2 for 18 hours. DIA proteomic analysis was performed on the same validation dataset samples. Data contributors: Kiersten L. Webster, Sarah Tersey & Raghavendra G. Mirmir: Kovler Diabetes Center and Department of Medicine, The University of Chicago, Chicago, IL, 60637, USA. Soumyadeep Sarkar, Raghavendra Mirmira, Ernesto S. Nakayasu: Biological Sciences Division, Pacific Northwest National Laboratory, Richland, WA, 99354, USA. Data repository: RNA-seq: GSE310965 Proteomics: MSV000101892 Publication: PMID 41279069

Sarkar, Soumyadeep [Pacific Northwest National Lab↗

Summary Report from the 2025 Interfaces for Energy and the Environment Conference

The inaugural Interfaces for Energy and the Environment Conference (IEEC) took place on May 19-23, 2025, at Pacific Northwest National Laboratory (PNNL), Richland, Washington (USA). The aim of this first-of-its-kind interdisciplinary meeting was to provide a forum for participants to share the latest cutting edge experimental and computational advances in interfacial science across energy and environmental applications. The sessions below (elaborated further in the report summaries) highlighted fundamental and applied collaborative research aimed at understanding the interactions occurring at interfaces in aqueous environments, including, but not limited to, the fields of geochemistry, atmospheric chemistry, agriculture, environmental management, and catalysis. They were organized to stimulate and provide opportunities to create, renew, and deepen collaborations. The conference included activities such as oral and poster presentations, honoree mentoring session, and a team building exercise to support all career stages (detailed summaries of these activities are in the Appendices).

54 ENVIRONMENTAL SCIENCES↗

Geographic source attribution of honey by strontium isotope analyses: Latvia and India measurements compared to model predictions in a feasibility study

Strontium isotope ratios ( 87 Sr/ 86 Sr) can be used to determine the geographic origin of agricultural products. Here, in this study, we measured the 87 Sr/ 86 Sr of honey samples from Richland, WA, USA, Latvia, and India, and compared the results to published 87 Sr/ 86 Sr from surrounding areas and values predicted based upon a random forest isoscape model (Bataille et al., 2020). While the 87 Sr/ 86 Sr of the honey samples compared well with previously published data, the model did not accurately predict the 87 Sr/ 86 Sr of the honey samples, demonstrating that further refinement of the model would be beneficial. Because Sr cycling in terrestrial ecosystems is complex, the 87 Sr/ 86 Sr of honey is likely to reflect several sources (e.g., nectar, surface water, dust) and may change over time. In order to accurately predict the 87 Sr/ 86 Sr of honey, models must consider local geology, ecology, and bee behavior. Additional research examining how Sr is incorporated into honey is needed to inform models.

60 APPLIED LIFE SCIENCES↗

Investigating Particle Phase State Dependencies during a Historic Pacific Northwest Wildfire Event

The function and lifetime of an atmospheric particle are greatly dependent upon its phase state. Studying particle phase states from specific ambient source types is often challenging due to uncontrolled environmental conditions and multiple source contributions. However, a historic Pacific Northwest wildfire event occurred in September 2020, providing a rare opportunity to study a pseudo-single particle type ambient sample (i.e., wildfire) over time. Sampling was performed in Richland, Washington, capturing aged particles from shifting wildfire sources. In addition to source variability, temporal variation in wildfire particle phase state was observed from single particle analyses. Despite this, single particle elemental compositions were homogenous over time (=87% carbonaceous) with no significant temporal variation in organic functional group abundances within individual particles either (e.g., 4% relative standard deviation in alkene contributions). While particle composition is indeed known to affect phase state, water uptake appeared to be the most significant contributor to phase state variability amongst single particles here, as particle aspect ratios (related to phase state) linearly correlated with ambient relative humidity during sampling (R2 = 0.65). Therefore, while limited to a case study, meteorological considerations are found to convey greater comparative importance than particle composition for aged particle phase state predictions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Determining Unabated Airborne Radionuclide Emissions Monitoring Requirements Using Inventory-Based Methods

Compliance with the airborne radionuclide emission monitoring requirements in the National Emission Standards for Hazardous Air Pollutants (NESHAP; 40 CFR Part 61, Subpart H) and State requirements in Washington Administrative Code 246–247 and 173-480 were evaluated for Pacific Northwest National Laboratory (PNNL) operations. Additional guidance may be found in the U.S. Department of Energy Handbook, Environmental Radiological Effluent Monitoring and Environmental Surveillance. To meet regulatory requirements, reviews of planned or proposed projects and activities provide the basis for implementing necessary monitoring adjustments or for implementing changes to projects and activities in a timely manner. Potential unabated off-site doses were evaluated for emission locations managed by PNNL and licensed to the Department of Energy. These locations were at facilities in Richland, Washington (i.e., the Hanford Site and PNNL-Richland Campus) and in Sequim, Washington, (PNNL-Sequim Campus, which formerly was known as the Marine Sciences Laboratory). This report describes the inventory-based methods and provides the results for the NESHAP assessment performed in January 2021 for calendar year ending 2020.

40 CFR 61 Subpart H↗

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↗

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↗

EMP, Attachment 3: Dose Assessment Guidance (Rev.4)

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 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↗

Determining Unabated Airborne Radionuclide Emissions Monitoring Requirements Using Inventory-Based Methods

Compliance with the airborne radionuclide emission monitoring requirements in the National Emission Standards for Hazardous Air Pollutants (NESHAP; Title 40 of the U.S. Code of Federal Regulations Part 61, Subpart H) and State requirements in Washington Administrative Code 246–247: Radiation Protection – Air Emissions and 173-480: Ambient Air Quality Standards and Emission Limits for Radionuclides were evaluated for Pacific Northwest National Laboratory (PNNL) operations. Additional guidance may be found in the U.S. Department of Energy Handbook, Environmental Radiological Effluent Monitoring and Environmental Surveillance. To meet regulatory requirements, reviews of planned or proposed projects and activities provide the basis for implementing necessary monitoring adjustments or for implementing changes to projects and activities in a timely manner. Potential unabated off-site doses were evaluated for emission locations managed by PNNL and licensed to the Department of Energy. These locations were at facilities in Richland, Washington (i.e., the Hanford Site and PNNL–Richland campus) and in Sequim, Washington, (PNNL–Sequim campus). This report describes the inventory-based methods and provides the results for the NESHAP assessment performed in January 2024 for calendar year ending 2023.

40 CFR 61 Subpart H↗

Pacific Northwest National Laboratory Facility Radionuclide Emission Points and Sampling Systems

Battelle–Pacific Northwest Division operates numerous research and development laboratories in Washington State. The U.S. Department of Energy (DOE) contracts to Battelle at Richland facilities on both the DOE Hanford Site and the Pacific Northwest National Laboratory (PNNL)-Richland campus. These facilities have the potential for radionuclide air emissions. The PNNL contract with DOE also includes operations at the PNNL-Sequim campus in Sequim, where there is also the potential for radionuclide air emissions. This document is a periodic update that describes current PNNL facility emission units and sampling systems.

54 ENVIRONMENTAL SCIENCES↗

EMP, Attachment 1: Sampling and Analysis Plan (Rev.1)

This Sampling and Analysis Plan (SAP) is written for the Environmental Radiation Task activities related to radioactive air emissions (stack) monitoring and environmental radiological ambient air surveillance of Pacific Northwest National Laboratory (PNNL) operations at the PNNL-Richland campus and PNNL-Sequim campus. PNNL is a U.S. Department of Energy Office of Science laboratory in Richland, Washington. This plan is an attachment to PNNL’s Environmental Radiological Air Monitoring Plan (EMP) (PNNL-20919) and addresses a discrete, vital subject area that is subject to revision independent of the main text of the EMP document. This SAP provides the requirements for planning sampling events and the requirements imposed on the services provided by the analytical laboratory to the PNNL Environmental Radiation Task.

40 CFR 61 Subpart H↗

Is the red arc a good indicator of ionosphere-magnetosphere conditions

Weak red arcs were observed on the two consecutive nights of July 12-13 and July 13-14, 1969, at Richland, Washington, whereas no red arcs were detectable on the nights preceding and following the observations. Satellite (Ogo 6) data of electron temperature and density, low-frequency ac electric field, and suprathermal electron flux corresponding to the conjugate region of Richland show no significant variations during these days. The data show elevated electron temperatures and enhanced low-frequency ac noise levels at the expected red arc position in the neighborhood of the density trough, as indicated by previous observations. The data appear to indicate that the optical criterion of red arc occurrence would lead to the conclusion of significantly different ionosphere-magnetosphere conditions during these four nights, whereas the more detailed in situ data show that the conditions were very similar.

Nagy, A. F.↗