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DOE OSTI2020

Panel Session 2: Hot Topics in US DOE Environmental Management

The well-attended Panel Session was chaired by Martin Schneider. The four panelists did not provide presentations. Rather the session was a discussion focusing on pressing issues facing US DOE Environmental Management (EM) sites and how the program is moving forward. The session began by momentarily reflecting on a success: the three Tank Waste Treatment Facilities will soon be coming online. These three facilities will treat as much waste in two years as was treated in the past 30 years. That is a significant milestone in progress. Also, safety enhancements at WIPP are a big success. The panelists noted that there will be challenges with the victories of the startup of the Waste Treatment Facilities. Treating tank waste is the last EM mission and will help with the relationships with the stakeholders, regulators and Congress. One of the biggest challenges will be moving back to full operation mode. Although the operation will increase productivity of reducing/managing the tank waste, it will decrease life cycle cost and lessen years of cleanup. The challenge will be having people understand that EM will be operating 24/7 and that maintenance will be key in keeping the operations. EM will be working together with the regulators to show tangible progress that will be effective and efficient. By working together, they can find opportunities/technologies for streamlining and accelerating cleanup. Recent changes to the regulatory framework between DOE-EM Los Alamos Field Office and New Mexico Environmental Department have helped cleanup in Los Alamos. Every year EM and the agencies review progress and come to agreements on the next work priorities. At Savannah River Site, the Federal Facility Agreement among EM, South Carolina Department of Health and Environmental Control, and Environmental Protection Agency (EPA) has developed a small core team that work are shared by together in resolving issues that come up. The discussion moved on to how progress can be made by sharing lessons learned among the contractors. An example of how these learned lessons can be shared is that key representatives from projects across the EM sites participate in various forums to review/contribute to the work planned. Other opportunities can be by temporary assignments of DOE staff to gain experience and by monthly EM Headquarters report that provide the lessons learned across the EM sites. The panelists discussed how skyline changes are the best examples of tangible progress. Decontamination and Demolition (D and D) of structures are the easiest tangible progress that can be seen. Whereas tank waste cleanup is the hardest to see. Disposal of waste onsite versus offsite is another challenge, and timely discussions are necessary to get to the best value to the government.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Canonsburg, Pennsylvania, UMTRCA Title I Disposal Site 35 Years Postclosure (1985-2020) - 20288

The DOE Office of Legacy Management (LM) Canonsburg, Pennsylvania, Disposal Site is a former uranium ore-processing site located in the borough of Canonsburg and an important part of US history. For 46 years (1911-1957), the site processed ore, for vanadium, radium and then uranium. Soils and groundwater beneath the site were contaminated by the milling operations. The 15-hectare (37-acre) site is owned by the US government and managed by LM, which serves as the federal land manager and steward of cultural, historical, and natural resources at Cold War legacy sites that have been successfully cleaned up to remedial standards. In 1978 Congress directed DOE to remediate 22 inactive uranium-ore processing sites under the Uranium Mill Tailings Radiation Control Act (UMTRCA), in accordance with standards promulgated by the US Environmental Protection Agency in Title 40 CFR Part 192 (40 (CFR 192). Subpart B of 40 CFR 192 regulates the cleanup of contaminated groundwater at the processing sites. The radioactive materials were encapsulated in US Nuclear Regulatory Commission (NRC)-approved disposal cells, and the NRC general license for UMTRCA Title I sites is established in 10 CFR 40.27. Canonsburg was the first site to be remediated under UMTRCA. From 1983 to 1985, the Canonsburg site underwent cleanup under this US law that provides for the safe and environmentally sound disposal, long-term stabilization, and control of uranium mill tailings in a manner that minimizes or eliminates radiation health hazards to the public. The site is unique in that it is one of only two UMTRCA Title I sites in the eastern half of the United States, the other site being the Burrell, Pennsylvania, Title I Disposal Site, a vicinity property to the Canonsburg site. It has been 35 years since the disposal cell at the Canonsburg site was completed. This paper discusses the many efforts that have been taken to maintain the site and presents some of the lessons learned concerning the long-term care of the site. The discussion includes but is not limited to the following: (1) Preserving site history so the community can better appreciate and understand the site. (2) Community outreach efforts, and the importance of maintaining transparency of environmental monitoring results with the community. (3) Pursuing reuse opportunities that offer the potential for improving the community. (4) Remaining engaged with the local community. (5) Remaining proactive in the long-term care of the site. (authors)

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DOE OSTI2021

Molecular and Microstructural Bases for Understanding Microplastic Origin, Transport, and Fate

The formation of micro and nanoplastics from parent plastics is one of the most challenging ecological threats since plastic pollution reaches even the most desolate places on earth and is expected to double by 2030. The goal of this project is to understand physico-chemical properties on microplastics formation, transport, and fate by analyzing the microplastics found in environmentally collected samples at SRS, supported by lab-based experiments. An initial assessment found and identified microplastics and micronizing plastics in Fourmile Branch and the Savannah River. Fourmile Branch also carried trace-level radioactive contaminants associated with the Site’s legacy missions, which may incorporate into entrained microplastics.

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DOE OSTI2020

Proven Technologies for the Solidification of Complex Liquid Radioactive Waste (LRW): Global Case Studies of Applications and Disposal Options - 20424

Legacy radioactive waste streams from the Cold War still exist and newly generated waste streams from nuclear power plants and research institutes go untreated and expose environmental hazards at many nuclear sites. The nature of the waste is diverse, depending upon the source or the process from which it originated. The most problematic waste streams include complex liquids such as organic (tri-butyl-phosphate TBP) solutions contaminated with Pu and U isotopes, mixed sludge types, high acid radioactive waste, H-3 contaminated organic and aqueous streams, etc. Technological, environmental and economic challenges exist for the treatment and disposal of such waste streams. A proven technology that has been applied to LRW on a global basis provides one option as a low-cost solution to legacy streams and small volume, highly complex LRW frequently found during decommissioning at nuclear power plants and weapons sites. The engineered polymer technology from Nochar, USA, is capable of solidifying standard and highly complex LLW and ILW waste streams for interim or final storage, or for incineration. (authors)

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DOE OSTI2020

Phase Formation in Nuclear Fallout

An understanding of the physical and chemical process occurring in a nuclear explosion enables predictions of the effects of nuclear weapons, including characteristics of radioactive fallout resulting from the explosion. Near-surface nuclear explosions are of particular interest due to the potential for significant amounts of environmental material to interact with and alter the physical and chemical behavior of the fireball. Such interactions have the potential to affect the distribution of radioactive species in the fireball and subsequently become incorporated into fallout through a process known as radiochemical fractionation. Studying variations in fallout formed in different historical testing environments allows us to understand the influence of local environments on fallout formation processes. In particular, constraining variations in thermal evolution and redox conditions during the evolution of the fireball can be useful to understanding how sensitive fallout radiochemical fractionation may be to the local explosion environment. However, untangling these conditions in complex, multicomponent fallout is a challenge. Here we present one method of constraining and interpreting fallout formation conditions by relating computationally derived phase stability predictions to observations in historic fallout. Development of such approaches will help improve physics-based models of fallout formation and radiochemical fractionation in complex, near surface nuclear detonations.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Chemical and structural characterization of particulate fallout isolated from air-filters

We report particulate nuclear fallout is the radioactive byproduct of a nuclear event formed by the mixture of proximate environmental materials with vaporized bomb debris. The fallout debris can be transported into the atmosphere during cloud rise, raining out locally and dispersing globally constituting a radiation hazard and contributing to the distribution of anthropogenic radionuclides in the environment. Questions remain on how entrainment of environmental material in the fireball affects fallout formation processes and radionuclide incorporation and distribution during cooling. To inform the characterization of fallout including the development of fallout size distributions and how radionuclides are incorporated into fallout debris where entrainment plays a role, we analyzed an archived historic US air-filter collected by aircraft in the aftermath of ground interacting nuclear tests. Particulate fallout collected on the filter was isolated and analyzed using scanning electron microscopy (SEM), transmission electron microscopy (TEM) and NanoSIMS (Secondary Ion Mass Spectrometry) to determine chemistry, structure, morphology, and size of the particles. Results demonstrate that the particles isolated from the filter have spherical shape, display complex internal structures, and are mainly composed of Fe and Si oxides. In these spherical particles, Pu is preferentially associated with Fe-rich composition. The characterization of fallout particulate samples can provide information on nucleation and particle growth from the vapor phase to improve modeling and simulation of fallout hazards.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2022

Plutonium reactive transport in fractured granite: Multi-species experiments and simulations

Plutonium (Pu) in the subsurface environment can transport in different oxidation states as an aqueous solute or as colloidal particles. The transport behavior of Pu is affected by the relative abundances of these species and can be difficult to predict when they simultaneously exist. This study investigates the concurrent transport of Pu intrinsic colloids, Pu(IV) (aq) and Pu(V-VI) (aq) through a combination of controlled experiments and semi-analytical dual-porosity transport modeling. Pu transport experiments were conducted in a fractured granite at high and low flow rates to elucidate sorption processes and their scaling behavior. In the experiments, Pu(IV) (aq) was the least mobile of the Pu species, Pu(V-VI) (aq) had intermediate mobility, and the colloidal Pu, which consisted mainly of precipitated and/or hydrolyzed Pu(IV), was the most mobile. The semi-analytical modeling revealed that the sorption of each Pu species was rate-limited, as the sorption could not be described by assuming local equilibrium in the experiments. The model was able to describe the sorption of the different Pu species that occurring either on fracture surfaces, in the pores of the rock matrix, or simultaneously in both locations. While equally good fits to the data could be achieved using any of these assumptions, a fracture-dominated process was considered to be the most plausible because it provided the most reasonable estimates of sorption rate constants. Importantly, a key result of this work is that the sorption rate constant of all Pu species tends to decrease with increasing time scales, which implies that Pu will tend to be more mobile at longer time scales than observations at shorter time scales suggest. This result has important implications for predicting the environmental impacts of Pu in the safety assessments of geologic repositories for radioactive waste disposal, and we explore potential mechanistic bases for upscaling the sorption rate constants to time and distance scales that cannot be practically evaluated in experiments.

58 GEOSCIENCES↗
DOE OSTI2021

A Focused Ion Beam-Scanning Transmission Electron Microscopy with Energy-Dispersive X-ray Spectroscopy Study on Technetium Incorporation within Iron Oxides through Fe(OH) 2 (s) Mineral Transformation

Incorporation of Tc(IV) into iron oxide/hydroxide minerals has been explored and proposed as a promising pathway to preventing Tc(IV) reoxidation to environmentally mobile pertechnetate (TcO 4 - ) and improving long-term immobilization of radioactive technetium-99 (Tc). However, visual evidence evaluating the distribution of Tc(IV) incorporated within iron oxide/hydroxide phases has not been available, until now, despite potential implications on Tc(IV) stability within the host phase. For the purpose of this study Tc(IV) incorporation into iron oxide/hydroxide phases was facilitated via Fe(OH) 2 (s) oxidation and mineral transformation to magnetite (Fe 3 O 4 ). Focused ion beam - scanning transmission electron microscopy equipped with energy-dispersive X-ray spectroscopy (FIB/STEM-EDS) methods were then combined with X-ray diffraction and absorption spectroscopy techniques to characterize and visually demonstrate that, for the first time, Tc(IV) is heterogeneously incorporated into different iron oxide/hydroxide phases as Tc(IV)-incorporated magnetite and/or TcO 2 ·2H 2 O(s) via different incorporation mechanisms. Heterogeneous distribution of Tc(IV) in magnetite suggests either (i) TcO4- is reduced quickly at the magnetite surface and then encapsulated into magnetite during continued octahedral crystal growth, or (ii) Tc(IV) alternatively partitioned into multiple layers of a blocky, plate-like morphological magnetite structure showing stratified Tc. With limited Tc-hematite (Fe 2 O 3 ) incorporation, the results suggest that TcO 2 ·2H 2 O(s) is formed and mainly associated/embedded in fibrous nanometer-sized polycrystalline hematite. This work highlights the power of modern state-of-the-art FIB/STEM-EDS approach to provide essential visual insights of the Tc-iron oxide/hydroxide incorporation and generate reliable mechanism-informed designs for waste forms relying on Tc mineral incorporation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Accessibility and Reactivity of Pentavalent Plutonium under Alkaline Conditions

Plutonium exhibits a particularly complex and rich aqueous chemistry due to a dynamic redox equilibrium that can result in the coexistence of four different oxidation states in aqueous solution. Within this equilibrium, pentavalent plutonium is among the most soluble and dominant oxidation states of Pu in neutral to alkaline aqueous solutions of relevance to environmental chemistries and the extreme chemical environments encountered in high-level radioactive wastes. Despite this, the fundamental chemistry of Pu­(V) under such conditions remains poorly understood. Here, in this study, we demonstrate the redox accessibility of Pu­(V) in alkaline media based on the observations of an electrochemically reversible Pu­(VI/V) couple at E 1/2 = 0.19 V vs Hg/HgO (0.29 V vs NHE), allowing us to electrolytically generate Pu­(V) in alkaline solution. These Pu­(V) solutions remained stable under ambient conditions for at least 9 days before precipitation of crystalline Na 2 [Pu V O 2 (OH) 3 ]·2H 2 O, the first structurally characterized Pu­(V) hydroxide. The modest potential of the Pu­(VI/V) redox couple allowed us to reproduce Na 2 [Pu V O 2 (OH) 3 ]·2H 2 O synthetically as well as isolate two additional novel Pu­(V)-bearing hydroxide phases Na­[Pu V O 2 (OH) 2 (H 2 O)]·2.5H 2 O and K 2 [Pu V O 2 (OH) 3 ]·2H 2 O as single crystals from alkaline reactions under mild hydrothermal conditions (<200 °C) using Na 2 O 2 and KO 2 as reductants. This reactivity is rationalized and informed by our electrochemical measurements. The properties of the Pu­(V) solids were further characterized by using vibrational and optical spectroscopy.

Kravchuk, Dmytro V. [Argonne National Laboratory (↗
DOE OSTI2020

Model Package Report: Plateau to River Groundwater Model Version 8.3

This model package report documents the groundwater flow component of the Plateau to River Groundwater Model (P2R Model), which is a groundwater flow and contaminant fate and transport (F&T) simulation model used to support remedial activities conducted by CH2M HILL Plateau Remediation Company at the Hanford Site in Washington State. The objective of this report is to describe the modeling objectives, conceptualization, model implementation, calibration, sensitivity, uncertainty, configuration control, limitations, and future model enhancements of the groundwater flow component of the P2R Model.

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DOE OSTI2020

Safety Functions and Features, Events and Processes for the E-Area Performance Assessment

The DOE Technical Standard, “Disposal Authorization Statement and Tank Closure Documentation,” (DOE 2017) recommends the use of safety functions and features, events and processes (FEPs) to support development of conceptual models and identification of scenarios to be considered in a performance assessment (PA). The FEP process provides a means to describe how a PA considers and addresses the factors that could influence the performance of key barriers. Understanding the roles of barriers in terms of limiting migration helps to focus on how changes in the system could lead to a situation where those roles cannot be fulfilled and there is the potential for compromised performance. The FEPs screening and review process was used to identify FEPs that are relevant for the EArea Low-Level Waste Facility (LLWF) and specifically those FEPs that could have a detrimental impact on the effectiveness of a given safety function. For this PA, a default list of FEPs developed at the International Atomic Energy Agency (IAEA 2004) and an approach implemented for PAs at the Hanford and Idaho sites (Mehta et al. 2016, DOE-ID 2019) are used to identify processes and events that could influence the effectiveness of a given safety function for the E-Area LLWF (e.g., subsidence can impact the safety function of the cover system and lead to increased infiltration). The Hanford and Idaho PAs represent two of the most recent applications of this approach. The PA evaluates the potential impacts of changes in performance of different features of the system and demonstrates that the safety functions represent multiple and redundant barriers. Barrier analyses, assuming a safety function is not present, also test the robustness of the system in the event of the loss of one or more safety functions. Such evaluations also support a qualitative illustration of the concept of defense in depth. The safety concept for closure of the E-Area LLWF (generically referred to as “E-Area”) encompasses a variety of different features (i.e., administrative controls, natural site features, and engineered barriers) that reduce the potential impacts on human health and the environment from the residual waste that will remain after closure. These features can be represented as a collection of safety functions acting independently and as a system to provide for overall safety. In some applications, there have been attempts to assign numerical expectations to specific safety functions, but that is not the intent in this case. The concept of safety functions is used more qualitatively in two ways for this PA: 1. To illustrate the robustness of the E-Area design, operational practices and closure approach by documenting features that are and are not credited in different modeling cases. 2. To identify the roles of the different features and potential processes and events that could compromise the performance of safety features and need to be considered when developing the modeling approach. This report addresses both safety functions and FEPs for the E-Area PA.

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DOE OSTI2020

Comoparison of Slit Trench and Engineered Trench 3D Vadose Zone Conceptual Models

In the next revision of the E-Area Low-Level Waste Facility (ELLWF) Performance Assessment (PA), radionuclide groundwater transport from slit (ST) and engineered trenches (ET) will be simulated using 3-dimensional PORFLOW models representing the vadose zone. In total, the conceptual framework will aim to model 29 total trenches with a degree of conservatism that provides a high level of confidence in meeting performance objectives. The implementation of generic conceptual models allows for a reasonable number of simulation scenarios, thereby reducing the chances of errors and enabling a better one-to-one comparison between the results, while still capturing the most important features of each trench. The current investigation seeks to understand if a generic trench model based on the general ET footprint can justifiably be used for representing both STs and ETs while maintaining a reasonable degree of conservatism. In this process, the groundwater transport of several key radionuclides was simulated for both ET and ST geometries and the flux-to-the-water-table profiles were compared. For all radionuclides simulated, the ET geometry is shown to be conservative (i.e., produces the highest peak flux to the water table).

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DOE OSTI2020

Chemical Waste Landfill Annual Post-Closure Care Report, Calendar Year 2019

The Chemical Waste Landfill (CWL) at Sandia National Laboratories/New Mexico (SNL/NM) is a remediated hazardous waste landfill that underwent closure in accordance with Title 20, Chapter 4, Part 1 of the New Mexico Administrative Code (20.4.1.600 NMAC), incorporating Title 40, Code of Federal Regulations (CFR), Part 265, (40 CFR § 265) Subpart G, and the CWL Final Closure Plan (SNL/NM December 1992 and subsequent revisions). The CWL Post- Closure Care Permit (PCCP) (NMED October 2009), which became effective June 2, 2011 (Kieling June 2011) and as modified, defines all post-closure requirements. This ninth CWL Annual Post-Closure Care Report documents all activities and results as required by the PCCP Attachment 1, Section 1.12.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Performance Assessment for the Disposal of Low Level Waste in the 200 East Area Burial Grounds (FY2019 Annual Status Report)

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) and are compared with U.S. Department of Energy requirements (DOE O 435.1 and performance objectives defined in companion documents DOE M 435.1 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, indicating that potential impacts are well below performance objectives; therefore, future compliance with DOE O 435.1 is expected. A new PA study has been initiated in this fiscal year (FY) 2019 for evaluation of active disposal sites within the 200 West and East Areas (Trenches 31 and 34 in 200 West; Trench 94 in 200 East) because extended time has elapsed between the current annual status report and the original PA (WHC-SD-WM-TI-370) for the active disposal sites. The new PA for the active disposal sites is expected to be completed in FY 2021.

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DOE OSTI2020

Composite Analysis for Low Level Waste Disposal in the Central Plateau of the Hanford Site (FY2019 Annual Status Report)

In accordance with DOE M 435.1-1 requirements and as implemented by DOE/RL-2000-29, the U.S. Department of Energy (DOE), Richland Operations Office has prepared this annual summary for fiscal year (FY) 2019. Originally reported in PNNL-11800 and PNNL-11800, Addendum 1, the Hanford Site Composite Analysis was approved through issuance of a 2002 memorandum. As required by DOE/RL-2000-29, an annual evaluation of new information and data developed by a number of onsite programs was completed. The reporting period for this annual evaluation is FY 2019 (October 1, 2018, through September 30, 2019). The information provided in this evaluation includes activities performed in FY 2019 that are considered pertinent to the Hanford Site Composite Analysis - information that could change source terms considered, and monitoring, research, and development results.

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DOE OSTI2020

Performance Assessment for the Disposal of Low Level Waste in the 200 West Area Burial Grounds (FY2019 Annual Statius Report)

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) and are compared with 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, indicating that potential impacts are well below performance objectives; therefore, future compliance with DOE O 435.1 is expected.

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