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At least 523 records · Page 29

A comparative techno-economic analysis of renewable methanol synthesis from biomass and CO 2 : Opportunities and barriers to commercialization

Global demand for methanol as both a chemical precursor and a fuel additive is rising. At the same time, numerous renewable methanol production pathways are under development, which, if commercialized, could provide significant environmental benefits over traditional methanol synthesis pathways. However, it is difficult to compare technologies at different maturity levels, with differing feedstocks, and with significant differences in overall process design. Thus, there is a need to harmonize the analyses of renewable pathways using a consistent techno-economic approach to evaluate the potential for commercialization of various pathways. This analysis uses a novel cross-comparison method to assess near-term and long-term viability of both low- and high-maturity level technologies. Furthermore, the techno-economic assessment considers cost factors critical to market acceptance combined with carbon- and energy-efficiency assessments of three renewable pathways compared with a commercial baseline. We find that biomass gasification to methanol represents a near-term viable pathway with a high technology readiness level and commercially competitive market price. If cost-reducing technological improvements can be realized and scaled up in the CO 2 electrolysis pathways, the potential for higher carbon efficiencies may help drive market adoption of these more modular, direct conversion pathways in future markets as they present an opportunity to better support global decarbonization efforts through efficient waste carbon utilization.

09 BIOMASS FUELS↗

2021 Annual Site Environmental Report

This report provides the U.S. Department of Energy (DOE) and the public with information on the level of radioactive and non-radioactive pollutants (if any) that are added to the environment as a result of Princeton Plasma Physics Laboratory’s (PPPL) operations. The results of PPPL’s 2021 environmental surveillance and monitoring program are presented and discussed. The report also summarizes environmental initiatives, assessments, and community involvement programs that were undertaken in 2021. PPPL’s on-site operations were significantly curtailed in 2021 due to the global coronavirus pandemic. PPPL has engaged in fusion energy research since 1951. The Laboratory’s mission is to develop the scientific knowledge and advanced engineering to enable fusion to power the U.S. and the world, and to developing the understanding of plasmas from the nano- to the astrophysical scale. PPPL’s primary experiment, the National Spherical Torus Experiment-Upgrade (NSTX-U) is a collaboration among national laboratories, universities, and national and international research institutions and is a major element in the US Fusion Energy Sciences Program. Its design tests the physics principles of spherical torus (ST) plasmas, playing an important role in the development of smaller, more economical fusion reactors. Due to previous operational issues, NSTX-U did not operate in 2021. PPPL is engaged in a project to replace key NSTX-U components and systems to enable operation of this international fusion user facility. In 2021, PPPL’s radiological environmental monitoring program measured tritium in the air at the NSTX-U Stack and at onsite sampling stations. Using highly sensitive air monitors, PPPL is capable of detecting small changes in the ambient levels of tritium. The operation of an in-stack monitor located on D-site is used to demonstrate compliance with the National Emission Standard for Hazardous Air Pollutants (NESHAPs) regulations. Also included in PPPL’s radiological environmental monitoring program, are water monitoring – ground, surface, and waste waters. PPPL’s radiological monitoring program characterized the background levels of tritium in the environment and those data are presented in this report. Ground water monitoring continued under New Jersey Department of Environmental Protection’s (NJDEP) Site Remediation Program regulations. PPPL monitored for non-radiological contaminants, mainly volatile organic compounds (components of common degreasing solvents). In 2021, PPPL complied with permit limits for surface and sanitary discharges. PPPL was honored with awards for EPEAT-certified electronics purchasing and use of peracetic acid as an alternative water treatment chemical in its non-potable process water systems an NJDEP recycling award.

54 ENVIRONMENTAL SCIENCES↗

Sister Rod Destructive Examinations (FY23) Appendix E2: Four-Point Bend Fractured Specimen Images

This report documents work performed under the Spent Fuel and Waste Disposition’s Spent Fuel and Waste Science and Technology program for the US Department of Energy (DOE) Office of Nuclear Energy (NE). This work was performed to fulfill Level 2 Milestone M2SF-24OR010201024, “FY23 ORNL Testing on Sibling Pins,” within work package SF-24OR01020102 and is an update to the work reported in M2SF-23OR010201024, M2SF-22OR010201047, M2SF-21OR010201032, M2SF-19ORO010201026, and M2SF-19OR010201028. As a part of the DOE NE High Burnup Spent Fuel Data Project, Oak Ridge National Laboratory (ORNL) is performing destructive examinations (DEs) of high burnup (HBU) (>45 GWd/MTU) spent nuclear fuel (SNF) rods from the North Anna Nuclear Power Station operated by Dominion Energy. The SNF rods, called sister rods or sibling rods, are all HBU and include four different kinds of fuel rod cladding: standard Zircaloy-4 (Zirc-4), low-tin Zirc-4, ZIRLO, and M5. The DEs are being conducted to obtain a baseline of the HBU rods’ condition before they are sent to dry storage and are focused on gaining an understanding of overall SNF rod strength and durability. Composite fuel and defueled cladding will be tested to derive material properties. Although the data generated can be used for multiple purposes, one primary goal for obtaining the post-irradiation examination data and the associated measured mechanical properties is to support SNF dry storage licensing and relicensing activities by (1) addressing identified knowledge gaps and (2) enhancing the technical basis for post-storage transportation, handling, and subsequent disposition. This report documents the status of the ORNL Phase 1 DE activities related to the mechanical testing of selected sister rods in Phase 1 of the sister rod test program. This appendix provides images of the segments broken in four-point bending (4PB).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Role of Bifunctional Ru/Acid Catalysts in the Selective Hydrocracking of Polyethylene and Polypropylene Waste to Liquid Hydrocarbons

Hydrogenolysis of C–C bonds over Ru-based catalysts has emerged as a deconstruction strategy to convert single-use polyolefin waste to liquid alkanes at relatively mild conditions, but this approach exhibits limitations, including methane formation resulting from terminal C–C bond scission. In this study, a variety of catalysts were investigated for the reductive deconstruction of polyethylene (PE) and polypropylene (PP) to identify supports that promote nonterminal C–C bond scission. We found that Ru nanoparticles supported on Brønsted-acidic zeolites with the faujasite (FAU) and Beta (BEA) topologies were highly active for the cleavage of C–C bonds in PE and PP, exhibiting improved liquid yields and suppressed methane formation. For the deconstruction of PE, supporting ruthenium nanoparticles (5 wt %) on FAU increased the yields of liquid alkanes to 67% compared to 33% over an inert silica support (5 wt % Ru/SiO 2 ) at 200 °C, 16 h, under 30 bar of H2. A dramatic selectivity enhancement toward liquid hydrocarbons was also observed for PP over Ru/FAU and Ru/BEA compared to Ru/SiO 2 . To understand the origin of this selectivity improvement, a combination of ex situ and operando characterization techniques were used to reveal that both catalyst structure and acidity play key roles in PE and PP conversion. Operando X-ray absorption spectroscopy studies with model polyolefins over Ru-supported catalysts with varying acidity levels revealed that the local chemical environment of Ru [0] during the reaction is consistent across multiple acidic supports, although the onset of reduction during synthesis of the nanoparticles varies across different supports. These results, combined with reactivity data, demonstrate the importance of the acid-noble metal cooperativity in promoting selective C–C bond scission toward liquid alkanes that shifts the mechanism from hydrogenolysis to ideal hydrocracking.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Long-term sinking of nuclear waste canisters in salt formations by low-stress creep at high temperature

Abstract Rock salt has a self-sealing capacity, low permeability, and high thermal conductivity, making it a potential host for heat-generating nuclear waste. The feasibility of nuclear waste disposal within salt formations has been investigated mostly for small-sized canisters. Geologic disposal of larger-sized canisters originally designed for spent fuel storage and transportation has lately been examined as a cost-effective alternative. This raises questions about their long-term vertical movement due to their weight and high decay heat. Low-stress creep governs this movement; however, most salt constitutive models do not incorporate it. In this paper, the Norton and the WIPP creep models are compared with the Lux/Wolters/Lerche (LWL) model and a simpler model that combines linear and Norton creep laws (named combined creep model). The LWL and combined creep models consider pressure solution creep, though all incorporate dislocation creep. The models are first applied to creep tests under various stress levels. The LWL and the combined creep models results fit the experimental data well in both high and low stress ranges, whereas the Norton and WIPP models results only fit in higher-stress ranges. The different models are further applied for analyzing long-term canister movement. A sinking rate of $$-4.4\times 10^{-7}$$ - 4.4 × 10 - 7 mm/year was predicted using the Norton and WIPP models versus $$-2.1\times 10^{-2}$$ - 2.1 × 10 - 2 mm/year and $$-3.1\times 10^{-2}$$ - 3.1 × 10 - 2 mm/year using the LWL and the combined creep models, respectively. This comparative study confirms that creep models calibrated exclusively against high-deviatoric stress data might result in an inaccurate estimation of waste packages sinking rate in salt formations.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Automated Data Review of Analytical Laboratory Results at Los Alamos National Laboratory - 20299

Newport News Nuclear BWXT-Los Alamos, LLC (N3B) collects samples in support of the U.S. Department of Energy's (DOE) Office of Environmental Management (EM) Los Alamos Legacy Cleanup Contract (LLCC). N3B receives and reviews over 1.6 million sample data points annually in support of various ongoing environmental monitoring and remediation projects of the LLCC. N3B must demonstrate and document that reported external analytical laboratory data produced for the LLCC are of sufficient quality to fulfill their intended purpose and to support defensible decision making as described in EPA QA/G4 Guidance for the Data Quality Objectives Process 1994. In 2018, N3B assumed management of the LLCC along with the Environmental Information Management (EIM) database that contains all historical and current environmental data associated with the LLCC. The entire EIM database is shared between N3B, Triad National Security, LLC (Triad), and New Mexico Environment Department (NMED). These three parties jointly manage the database, its configuration, and changes / updates. All environmental data that are entered into EIM are updated and available, on a daily basis, in the linked public database Intellus New Mexico (Intellus). The quality and defensibility of the environmental data generated from sampling activities is a key component of an effective remediation process. Providing quality data is accomplished through a data assessment process that includes examination, verification, and validation. Examination is the assessment of completeness of the deliverables, identification of any reporting errors, and determining the usability of the data based on the laboratory's evaluation of its data as described in the case narrative received with the data. Verification consists of an evaluation of the Electronic Data Deliverables (EDD) data report to determine the extent to which the external analytical laboratories met method and contract-specific quality control and reporting requirements. Validation consists of determining the data quality and the extent to which the external analytical laboratories accurately and completely reported all sample and quality control results and satisfied all contract requirements. EIM contains an automatic Data Validation Module which performs automated data review (DVM ADR). DVM ADR is a tool to assist in the validation process. When DVM ADR is used in conjunction with manual examination of sample data packages, the combination of the two will meet and exceed the requirements of verification. N3B recognized an opportunity for process improvement, focusing on DVM ADR configuration and enhancements in EIM. Testing EIM's configuration provided proof of the DVM ADR's capabilities and flexibility to accurately perform routine data checks based on analytical methods and regulatory requirements. In addition, the DVM ADR module was improved through enhancements for all analytes, particularly upgrades for radiochemistry data. Extensive testing of the DVM ADR module occurred using EDDs from actual laboratory analyses on the EIM testing site. During this process, N3B manipulated EDD information to verify that the actual outcomes matched the expected outcomes. The results of this testing were shared with the database architects, and configuration improvements were identified to address these results. During this process, N3B identified that the radiochemical DVM ADR capabilities were underutilized, and so enhanced the DVM ADR functionality with respect to radioanalytical assessment. N3B environmental data uploads to Intellus on a daily basis from EIM, once the analytical data undergoes examination and verification. As such, it is important to have a high level of confidence in the quality and defensibility of the data. The process of manual examination, along with the DVM ADR, in conjunction with full validation of a percentage the data specified through the Data Quality Objectives greatly increases efficiency of data review and confidence level of the quality of the data, and gives the project managers, governmental offices, and the public expedited access to high-quality data. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Analysis of Ionic Mercury Species in SRR Samples Measured by SRNL and Eurofins FGS

Savannah River Remediation (SRR) requested the development of mercury speciation capabilities at the Savannah River National Laboratory (SRNL) to support the Liquid Waste Operations at SRS. As part of that method development, SRR requested that SRNL Analytical Development (AD) compare their results with those obtained from their outside contract laboratory, Eurofins Frontier Global Sciences (FGS). This document reports on this method development work performed at SRNL as well as the comparative analyses conducted between the two laboratories. Development, optimization, and validation were undertaken at SRNL to produce a method for the species-specific analysis of ionic mercury. This method was developed as a secondary step to an existing method, L16.1-ADS-1579 Purgeable Mercury Cold Vapor Atomic Fluorescence Spectrophotometry. As such, much of the development and validation were performed in service of development of L16.1-ADS-1579. Six samples, representing two consecutive quarterly Tank 50 batches, were tested for ionic mercury by SRNL-AD and Eurofins FGS. The mean values reported by each lab for ionic mercury differed by less than one standard deviation, therefore the values reported by both labs were considered to be in agreement. SRNL-AD reported values for the six samples that differed by -5.56 mean percent, relative to Eurofins FGS. Together with comparable quality control data reported by each laboratory, these data represent a high level of agreement among both laboratories. With a viable method for ionic mercury that matches the data quality provided by outside commercial laboratories, SRNL-AD has demonstrated competency in measuring methylmercury, ethylmercury, total mercury, soluble & particulate mercury, purgeable mercury, and ionic mercury species in a variety of radioactive tank samples.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

The Importance of Inventory for Informing Waste Strategy - 20280

A waste inventory aims to present the best available information about the nature, quantity and location of radioactive wastes and materials at a facility, site or in a country. Quality inventory data is necessary for developing appropriate strategies and plans for managing radioactive wastes and materials, with high standards of protection for people and the environment. The inventory of wastes will change over time due to a wide range of technical, commercial or policy reasons, for example, if reactor lifetimes are extended, if decommissioning strategies change or if new technologies are introduced for managing waste. Inventory information can also improve as better waste characterisation data becomes available. At a facility or site level, good quality inventory data are needed to underpin decision making about the waste management options and to demonstrate compliance with the chosen treatment or disposal route. At a site and country level, knowledge of the inventory can drive the improvement to waste strategy; waste management asset and service planning; and implementation. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Sister Rod Destructive Examinations (FY23) Appendix I: SNF Aerosols Released During Rod Fracture

This report documents work performed under the Spent Fuel and Waste Disposition’s Spent Fuel and Waste Science and Technology program for the US Department of Energy (DOE) Office of Nuclear Energy (NE). This work was performed to fulfill Level 3 Milestone M3SF-23OR010201026, “FY23 M3 draft report on results from testing in FY23,” within work package SF-23OR01020102 and is an updated to the work reported in M2SF-23OR010201024, M2SF-22OR010201047, M2SF-21OR010201032, M2SF-19ORO010201026, and M2SF-19OR010201028. As a part of the DOE NE High Burnup Spent Fuel Data Project, Oak Ridge National Laboratory (ORNL) is performing destructive examinations (DEs) of high burnup (HBU) (>45 GWd/MTU) spent nuclear fuel (SNF) rods from the North Anna Nuclear Power Station operated by Dominion Energy. The SNF rods, called sister rods or sibling rods, are all HBU and include four different kinds of fuel rod cladding: standard Zircaloy-4 (Zirc-4), low-tin Zirc-4, ZIRLO, and M5. The DEs are being conducted to obtain a baseline of the HBU rods’ condition before dry storage and are focused on understanding overall SNF rod strength and durability. Fuel rods and defueled cladding will be tested to derive material properties. Although the data generated can be used for multiple purposes, one primary goal for obtaining the post-irradiation examination data and the associated measured mechanical properties is to support SNF dry storage licensing and relicensing activities by (1) addressing identified knowledge gaps and (2) enhancing the technical basis for post-storage transportation, handling, and subsequent disposition.This report documents the status of the ORNL Phase 1 DE activities related to the collection of SNF aerosol particles released during fuel rod fracture in 4-point bending in Phase 1 of the sister rod test program.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Cost Competitive Process of Battery Grade Oxides Preparation from Aged LIBs

The increasing demand for lithium-ion batteries (LIBs) is driving development of advanced recycling and refining methods. In this project, new cathode active materials are prepared from recycled lithium battery materials and subsequently electrochemically evaluated in coin cells. In detail, scrap LIBs were mechanically processed into a metal rich black mass, then reductive acid leached into an aqueous metal solution, and finally high-purity metal hydroxide precursor materials were prepared by selective electrochemical flow precipitation. Closed-loop LIB recycling into active electrode materials will enable US manufacturers to break their reliance on foreign sources of critical materials. For example, electroextraction process used here has potential to significantly reduce chemical & water use as well as waste production as compared to traditional metallurgic techniques. To this end, electroextracted materials refined from used batteries were collected and processed to be tested as precursor cathode active material (pCAM). For this project, two samples of high purity recycled NMC hydroxide (~1 kg each) were received from N th Cycle’s Ohio demonstration facility. The NMC compositions of the two materials are similar, and the levels of impurities have been confirmed. Indeed, impurities like copper, boron and sodium are present in quantities that could negatively impact battery performance. However, some studies have demonstrated that the control of the quantity of elements like copper or boron may improve the electrochemistry properties of Lithium-NMC batteries. The principal objective is to determine the electrochemical performance of these 2 NMC hydroxide batches and clearly determine the effect of the impurities on the performance.

25 ENERGY STORAGE↗

Alpha-Imaging Detector System Development for Large Area Monitoring

Effective management and disposal of legacy nuclear waste are essential for ensuring safe work environments and minimizing environmental impacts. Monitoring airborne actinide contamination is particularly critical due to the high internal dose potential of alpha-emitting radionuclides. Traditional continuous air monitoring systems (CAMs) used in the industry are limited in the volume of air they can sample, potentially leading to inaccurate radiation detection over large areas. For example, in 2018, elevated levels of airborne Plutonium-239 were detected beyond the controlled areas of the Hanford Plutonium Finishing Plant, highlighting the potential risks to both plant workers and nearby residents. To address these challenges, high-efficiency particulate absorbing (HEPA) air purifiers can enhance air flow by up to 1.5 orders of magnitude, thereby increasing monitoring efficiency and providing a cost-effective solution for large-area surveillance. To quantify the activities of alpha-emitting radionuclides on HEPA filters, the Savannah River National Laboratory is developing an advanced alpha-imaging detection system. This system includes scintillating materials combined with a digital scientific camera. A significant concern in operating such a large-area airborne monitoring system is the handling of HEPA filters, which may be contaminated with radioactive particles. To mitigate these hazards, it is crucial to ensure that any contamination is securely fixed onto the filters. Efforts have been made to optimize the sensitivity of scintillator-epoxy composites and apply them to HEPA filters. These materials were characterized using fluoroscence spectroscopy. These techniques confirmed the purity of the raw materials, the dispersion of scintillators in the epoxy matrix, and the stability of their optical and structural properties post-modification. The optimal scintillator-epoxy composite was selected for use on alpha-spiked HEPA filters to evaluate the efficiency of the sprayer. HEPA filters, embedded with alpha particles collected by an air purifier deployed in an airborne radiation area, have been tested to assess detection efficiency. Future work will focus on employing multiple imaging sensors simultaneously to enhance sensitivity across different regions of the HEPA filter.

Pham, Phuong [Savannah River National Laboratory (↗

Bundling measures for food systems transformation: a global, multimodel assessment

Background Current food systems leave one in ten individuals at risk of hunger while driving unsustainable environmental impacts. Inaction risks further exacerbating negative impacts on both human and planetary health. These challenges emerge from complex system interactions, requiring approaches that engage with this complexity and consider how transformation measures interact across food systems. We aimed to quantify the magnitude and uncertainty of the impacts of key food systems transformation measures both individually and in a bundle using an ensemble of global economic models. Methods In this global multimodel assessment, we applied an ensemble of ten state-of-the-art global economic models to evaluate the potential of four key measures in transforming food systems: increasing agricultural productivity, halving food loss and waste, shifting towards healthier diets, and economy-wide climate mitigation policies aligned with limiting warming to 1·5°C. The scenarios used a middle-of-the-road shared socioeconomic pathway for population and gross domestic product growth, climate impact data from Jägermeyr and colleagues, Thornton and colleagues, and Nelson and colleagues, and dietary targets based on the EAT–Lancet healthy reference diet, with model simulations conducted from 2020 to 2050. We then assessed the effect of these measures in isolation and in combination in a bundled scenario. To further understand the interactions between these measures, we conducted a decomposition analysis that distinguishes between the individual effects of a measure (effect when implemented alone), total effects (its contribution within the bundle), and interaction effects (the difference between total and individual effects). This approach aimed to show complementarities and trade-offs that emerge when multiple measures are implemented simultaneously. Findings Our analysis showed that individual measures in isolation are insufficient to achieve high-level environmental objectives and might generate unintended consequences. In contrast, bundling measures produces co-benefits: avoiding 50% of projected agricultural greenhouse gas emissions by 2050 and almost 20% of anticipated land conversion, while moderating food price increases associated with ambitious climate change mitigation policies. Our decomposition analysis further shows that measures can have varying effects across different dimensions. Although dietary shifts and climate mitigation policies are the largest drivers of environmental benefits (each contributing to a median decline of >10 percentage points in non-CO 2 emissions and 5 percentage points in agricultural land use globally), productivity improvements and reducing food loss and waste play essential roles in moderating price increases (each contributing to a median decline of >5 percentage points in average prices). Interpretation This study highlights the importance of implementing coordinated approaches to food system transformation and climate change mitigation rather than relying on isolated interventions. Comprehensive transformation requires understanding how supply-side and demand-side changes can interact with climate mitigation policies, enabling policy makers to design intervention packages that maximise benefits while minimising trade-offs across environmental, economic, and social dimensions.

Sundiang, Marina [Cornell Univ., Ithaca, NY (Unite↗

Planning decentralized urban renewable energy systems using algal cultivation for closed-loop and resilient communities

To tackle climate challenges, communities need to harvest renewable energy and resources on site locally to close the loops for enhancing the resilience of communities facing unpredictable and uncertain future changes. A decentralization planning of urban renewable energy systems is proposed by treating urban waste streams and producing biomass through applying algal biotechnology. When applying algal technology as a renewable and decentralized energy source in urban systems, the overall performance can vary by levels of urban nutrients, solar and CO 2 resources, and the transportation cost when considering its application to different urban densities, urban form, and the spatial scale of urban settings. This research explores three potential impacts on the algal system’s energy performance: (1) urban density, (2) urban form in different contexts, and (3) spatial scale. The research examines the impacts by testing urban settings given in actual contexts in Atlanta, Georgia, USA. Four neighborhoods representing the high-density urban, mid-density urban, mixed suburban, and typical suburban areas are investigated. The density-scale–performance relationships are explored through testing different urban forms of neighborhoods in both hypothetical and actual neighborhood settings. A GIS-based model is developed to estimate the overall energy performance of the decentralized renewable energy system in urban environments. Results show that the energy performance is positive mainly for high-density urban neighborhoods with small-to-medium scales, up to 0.36 MJ per ton of municipal solid wastes for actual settings and 0.37 MJ for hypothetical cases. Neighborhoods with higher density have higher energy performance while up scaling has negative effects on the energy performance with a low degree of significance. Optimal scales are found as a 1-km radius in real test beds and 1.3 km in hypothetical settings, in which the results show trade-offs between scaling effects in the system efficiency gain and the transportation cost increase.

Quan, Steven Jige↗

The energetics and dynamics of confinement in flexible frameworks and molecular confinement

This project is part of an ongoing and long-term collaboration among Alexandra Navrotsky (who moved recently from UC Davis to Arizona State University), Nancy Ross at Virginia Tech, and Brian Woodfield at Brigham Young University (BYU) on the thermodynamics and lattice dynamics of nanophase and porous materials. Navrotsky emphasizes energetics of formation and guest molecule sorption by ambient and high temperature calorimetry, Woodfield contributes cryogenic heat capacity measurements, and Ross uses inelastic neutron scattering, X-ray and neutron diffraction, and high pressure studies to probe lattice dynamics and phase transitions. Porous frameworks form the chemical and structural basis for critical technologies in separations, catalysis, nuclear waste containment and biomedical applications. Hundreds of zeolites and metal organic frameworks (MOFs) have been synthesized, and their ability to separate and store hydrogen, methane and carbon dioxide has been investigated both experimentally and theoretically. Nevertheless, a fundamental and systematic molecular-level understanding of the thermodynamic and structural factors governing the stability and guest-host interactions in these materials lags behind focused studies of specific systems. Because the guest molecules interact with each other and with the host framework, molecular confinement is a finely balanced and complex phenomenon. The ability of the guest molecules to bind and diffuse through the pores is determined by the nature of the host framework which, in turn, responds to the nature and concentration of guest molecules and to pressure and temperature. The work explores how framework flexibility, tailored by structure, composition, temperature and pressure, is a general phenomenon, similar in nature but variable in extent, in both zeolites and MOFs and is part of a free energy landscape in which framework-guest interactions, pressure, and temperature result in changes in framework geometry and, in some cases, phase transitions. These subtle and/or pronounced changes in lattice geometry, energetics, and dynamics can play a decisive role in confinement and in differentiating the binding of molecules of similar size.

36 MATERIALS SCIENCE↗

Use of Unmanned Aerial Systems for Post-closure Waste Site Maintenance and Surveillance - 20143

The P- and R-Area Reactor buildings, located at SRS near Aiken, SC, were in-situ decommissioned by grouting below-grade portions of the buildings and demolishing some above-grade structures to grade level. Other reactor building structures were left above-grade and sealed to prevent human or animal access. Because the above grade-structures are expected to continue in their present state for hundreds of years, the condition of the building roofs is critical to mitigate rainwater intrusion. For this reason, building roof areas were strengthened with high strength concrete to ensure the long-term integrity of the roof structure. Periodic inspections of the roof structures are required to ensure that the roofs are functioning properly and to identify damage areas. The traditional method of inspecting closed reactor buildings requires the use of a helicopter and photographer to generate photographs and videos for review. This method proved sufficient but lacked the resolution and clarity that is required for a thorough inspection of the building structure. Fortunately, the Savannah River National Laboratory (SRNL) has established a Small Unmanned Aircraft System (sUAS) program using commercially available and custom-built remote-controlled aircraft. EC and ACP contacted the SRNL program to evaluate whether the sUAS technology could be employed for periodic reactor building inspections. The sUAS can fly within a few meters of the reactor buildings and hover, allowing for a more thorough aerial inspection. The initial sUAS inspection of the P-Area Reactor building was completed in February 2018 and at the R-Area Reactor building in August 2018 and were successful in providing higher resolution photos and videos. The sUAS inspections also revealed that vegetation had begun to grow on the roofs that could potentially damage the structure integrity. SRNL partnered with Virginia Polytechnic Institute and State University to build a custom heavy lift sUAS that could be equipped with herbicides to remotely treat the vegetative growth. Herbicides were successfully applied to the R-Area Reactor building roof using the custom sUAS in September 2018. The use of unmanned aircraft systems at SRS to perform aerial inspections and herbicide treatment in otherwise inaccessible areas has proven to be an efficient and cost-effective technology that provides high value, increases knowledge of facility conditions, and provides for early detection of damage. Periodic inspections of the reactor building roofs using sUAS technology are performed safely, efficiently, and at a significant cost and schedule savings while reducing emissions, noise, and fossil fuel use. The use of sUAS equipment for building inspections and herbicide application at SRS is unique within the DOE complex. The goal of SRS is to apply this remote technology to other waste unit operations and maintenance activities in the future. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Synthesis Roadmap for Actinide Chloride Salts

Molten salt reactors (MSRs) are among the main advanced nuclear reactor types at the forefront of development by industry, with the support of the US government, for the next fleet of nuclear reactors to support the demand for energy in the coming decades. MSRs are highly unique because they are cooled and typically also fueled by molten salt. This quality brings about safety benefits such as low-pressure operation and self-stabilization of the neutron flux, operational benefits such as high-temperature operation and the ability for online refueling, and fuel and waste management benefits thanks to the flexibility of post-processing of molten salts and reprocessing options that involve removal of fission products and actinide separation. In fact, domestic deployment of molten salt (or molten salt–cooled) reactors is an approaching reality: a handful of molten salt reactor developers are planning to operate demonstration-scale reactors, as a step toward commercial-scale power reactors, within the decade. For example, Natura Resources received a construction permit in September 2024 for the deployment of MSR-1, which is a graphite-moderated thermal spectrum reactor, at Abilene Christian University. Also, TerraPower, in a collaborative effort with Southern Company and Idaho National Laboratory (INL), received approval from DOE in 2023 to proceed with the construction of the Molten Chloride Reactor Experiment (MCRE), a homogeneous chloride fast reactor at INL, and has begun assembly of system components. There are several other examples of developers at different stages of development of their own unique MSR designs (Jenet et al., 2025). As developers are in the process of obtaining approvals for their designs, deploying demonstration-scale reactors, and planning for their commercial-scale power reactors, there is a critical supply chain need for the synthesis of fuel for these reactors that must be addressed. The challenge generally is three-fold: (1) the quantity of fueled salt needed for these reactors is extraordinarily high (>100s of kilograms), but demonstrations of scaled-up techniques for fueled salt synthesis are significantly more limited than demonstrations of lab-scale syntheses; (2) each developer has a unique reactor design, which means different actinide halide elements in different carrier salts must be synthesized; and (3) there is a need for particularly high-purity salt so as to ensure the long-term operability of these reactors with minimal degradation to salt-wetted components, which necessitates synthesis techniques with high levels of quality control, repeatability, and well-characterized precursor and reactant materials. It is crucial that this supply chain challenge be addressed by demonstrating synthesis techniques that are scalable, de-risked, and well-documented so that these technologies may be adopted and utilized by industry to support the fueling needs of MSRs that are to come online within the next 10 years. With this supply chain challenge clearly defined for the developing MSR industry, it is important to consider that addressing such a challenge is oftentimes complex and context-dependent. There is not necessarily a single synthesis technique that can be scaled up and adopted to address the needs of all MSR developers; the synthesis approach that may be viable for producing a desired fuel salt will be entirely dependent on the exact salt composition needed, the quantity needed, purity needed, the refueling and waste plans, and the availability of a carrier salt for the fuel. Therefore, it is important to consider more broadly what synthesis techniques are available and have been demonstrated to understand the benefits, challenges, and general nuances that should be considered when evaluating a particular route for efficient production of high-purity fuel salts at scale.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Initial Testing of Alkaline Earth Metal Ion Absorption on Crystalline Silicotitanate - 20440

The Tank Closure Cesium Removal process at the Savannah River Site (SRS) has processed aqueous tank waste using the inorganic ion exchange media IONSIV{sup TM} R9120-Ba (which is also known as Crystalline Silicotitanate (CST)). Salt-cake in Tank 10H at SRS was dissolved and processed through filters and ion exchange columns. The primary purpose of the process is to remove Cs-137 from the aqueous waste so that it can be disposed as low level waste. It is known that this inorganic media also absorbs strontium from solution, and that strontium competes with cesium ions for absorption sites. The strontium ion is actually more strongly absorbed than the cesium ion from typical tank waste. However, strontium is typically present in low concentrations so does not normally cause a significant impact. Strontium is present as both non-radioactive isotopes and the radioactive Sr-90 isotope; with the non-radioactive isotopes being much more abundant. Although the total strontium solubility is usually much lower than cesium, some tank waste compositions can have a high enough soluble strontium concentration to decrease the cesium absorption. Relatedly, some testing at SRS suggested that another alkaline earth metal, calcium, may also absorb onto CST and may decrease cesium absorption. Barium is also an important species in treatment of tank waste, but is also usually present at low concentrations. However, after the Cs-137 is absorbed onto CST, it emits a beta particle and converts to Ba-137m, which then decays to non-radioactive Ba-137 by emission of a gamma ray. If the Ba-137m were to desorb quickly, it could impact the dose rate in down-stream equipment. In order to understand the impact of these alkaline earth metals on CST, SRNL performed testing using simulants of SRS tank waste that contain soluble barium, strontium, and calcium. Testing examined both removal of the alkaline earth metals and their impact on removal of cesium. Testing involved first developing realistic waste simulant formulations and dissolving the alkaline earth metals to high enough concentrations to potentially impact the Cs absorption. Once the formulations were developed and prepared, computer modeling was used to calculate the expected Cs absorption behavior to determine if the alkaline earth metals impact the performance. Measurements of the alkaline earth metals absorption by the media is also important for disposition of spent media because of the added radionuclide inventory from the Sr-90. These initial tests are examining the general impact and will be used to determine if further testing or measurements are needed. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Thermoeconomic analysis of a multigeneration system using waste heat from a triple power cycle

Multigeneration systems represent an appealing concept, due to their multiple benefits compared to standalone systems, which has motivated researchers to develop different types of multigeneration systems for several applications. Considering their significance, in this study, a novel multigeneration is proposed that uses the waste heat of a thermodynamically efficient triple power cycle with a 100 MWe capacity. The proposed system, which can generate power, freshwater, cooling, and domestic hot water concurrently, is evaluated using detailed thermodynamic and economic analyses. The triple cycle includes a simple Brayton cycle coupled with a supercritical carbon dioxide recompression cycle and a high-temperature organic Rankine cycle. The waste energy of the recompression and organic Rankine cycles is recovered by a half effect absorption chiller, a multi-effect distillation unit, and two heat exchangers. The results show that for an optimized triple cycle, up to 1,804 kW cooling and 8,472 m 3 /day of hot water can be generated from the hot supercritical carbon dioxide stream with a levelized cost of cooling and hot water of 0.0362/ton-hr and $0.6823/MWth, respectively. The integration of a multi-effect distillation unit with 7 effects can generate 4,167 m 3 /day freshwater with a levelized cost of water of $1.142/m 3 . Finally, the proposed multigeneration system offers a very promising application and a number of benefits such as a generating multiple useful products with no adverse effect on the thermodynamic efficiency of the triple power cycle.

Thermoeconomic analysis↗