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At least 379 records · Page 21

Elucidating Arsenic and Selenium Speciation in Coal Fly Ashes

Coal fly ash (CFA) is produced during the coal combustion process and contains trace elements (<100 ppm) including selenium (Se) and arsenic (As), both detrimental for environmental and human health. Existing management strategies for CFAs involve disposal in landfills and ash ponds, as well as beneficial usage in other applications such as in concrete. Both the direct disposal and beneficial usage of CFA raise concerns for environmental hazards due to the potential leaching of Se and As. CFAs were classified as reusable material by the U.S. Environmental Protection Agency (EPA) with the first federal regulation (Disposal of Coal Combustion Residuals from Electric Utilities, CCR) for its disposal established six years ago. During coal combustion process, parameters such as furnace firing type, emissions controls, coal rank, use of additives, and particulate matter controls, could contribute to significant variability in As/Se concentrations and their speciation. Although there have been a handful of studies on As/Se speciation on small sets of samples, they do not fully represent the current state of coal-fired electrical generating units. Little information exists on the detailed speciation (e.g. oxidation state, complexation state) of As/Se in large set of fly ash samples. To better investigate the role of the potential contributing parameters, a large-scale survey study with representative samples of typical coal source and combustion conditions is highly desired. The overall goal of this research is to systematically characterize As and Se speciation of representative coal fly ash samples using state-of-the-art synchrotron based spectroscopic and microscopic techniques, in order to develop a correlation between coal source/type, operation condition, As/Se speciation, and As/Se mobility. A detailed survey study was conducted documenting the current state-of-knowledge on fossil power generating units as a function of coal type/source, operating conditions, environmental control systems, additive use, and fly ash handling methods. Based on this survey, a matrix of fly ash samples representing a range of conditions were chosen and collected. The collected ash samples were analyzed for bulk characteristics such as elemental composition, microstructure, chemical and mineralogical composition, surface area, and particle size distribution. State-of-the-art synchrotron X-ray microscopy and spectroscopy techniques were applied to reveal the molecular scale speciation information of As and Se, such as oxidation state, association with other elements/minerals, and complexation states.

01 COAL, LIGNITE, AND PEAT↗

Utilization of Unmanned Aircraft Systems for Environmental Purposes at the Savannah River Site – 26578

Born in the 1950s, the Savannah River Plant was constructed as a plutonium and tritium production plant. As the Cold War era came and went, a change of direction was signaled when the name of the facility changed from Savannah River Plant to Savannah River Site (1989) – the main mission at Savannah River shifted from “production” to “cleanup.” The Department of Energy is responsible for managing the 310 square miles of land that is the Savannah River Site and the cleanup/remediation activities that occur. The Savannah River National Laboratory utilizes unmanned aircraft systems to assist with some of those environmental monitoring and remediation activities. One function of unmanned aircraft systems at the Savannah River National Laboratory is conducting aerial photography and videography. Various infrastructure evaluations have been performed with unmanned aircraft – facility rooftop inspections, water tower lock verifications, earthen dam surveys, etc. An unmanned aircraft system has been used for progress footage of remediation projects – Dunbarton Bay remediation, Saltstone Disposal Unit construction, etc. Thermal cameras on an unmanned aircraft system are used to help identify cracks/leaks in structures from vantage points not readily accessible by personnel. Virtual tours of different waste units are conducted with unmanned aircraft systems for Site groups and federal/state regulators to save costs and travel time. Additionally, advanced remote sensing technologies are used on unmanned aircraft systems at the Savannah River Site. Light Detection and Ranging uses laser pulses to measure distances to the Earth's surface or other targets to create highly detailed topographic maps that accurately portray terrain (e.g., elevation changes, slopes, and contours). Data collection with a Light Detection and Ranging unit mounted on an unmanned aircraft system is quick and efficient – large-area surveys are conducted in shorter time frames. Because Light Detection and Ranging can penetrate through foliage and vegetation to ground level, it is being used in conjunction with a watershed model to study the General Separations Area of the Site to determine stormwater flow volume and direction, monitor stream stability, and forecast river flow behavior. A hyperspectral camera captures a wide spectrum of electromagnetic wavelengths across numerous narrow bands, beyond what the human eye can see. It provides detailed spectral information about the objects or surfaces in an image, which can be used to identify and analyze materials based on their spectral signatures. A hyperspectral camera mounted on an unmanned aircraft system has been used at the Savannah River Site for non-destructive evaluation of concrete and concrete structures. Unmanned aircraft systems at the Savannah River Site are also used for the application of herbicide on identified rooftops. P-Reactor and R-Reactor are entombed nuclear reactors at the Savannah River Site. Unwanted vegetation is often present on these rooftops – over time roots can penetrate seams, cracks, and joints of the general roof and concrete caps, leading to water ingress and deterioration of the structural components. For time and cost efficiencies as well as in the interest of personnel safety, an unmanned aircraft is used to dispense herbicide on rooftop areas where vegetation is noticed to help alleviate the issues/hazards.

Lorier, Troy [Savannah River National Laboratory (↗

INL Alpha Background Radiation Study

Radiological emergencies that result in the dispersion of radioactive materials to the environment require the deployment of field monitoring teams to determine the quantity and location of the dispersed radioactive material. This information is utilized by the emergency operations center to aid in determining the appropriate protective action recommendations. The background alpha emission rates from normal environmental surfaces of soil, concrete and asphalt as measured by portable instrumentation used by field monitoring teams are not well documented. Idaho National Laboratory conducted a study of the alpha radiation background levels of the environmental surfaces in eastern Idaho to determine the normal background rates. Results for normal dry surfaces and those wetted by precipitation were measured and reported.

61 RADIATION PROTECTION AND DOSIMETRY↗

Trash to Treasure: Waste Carbon into Construction Materials

Mineralization of industrial waste and earth-abundant CO2 into value-added products is a powerful method of utilizing domestic resources to produce value from waste. Carbonate minerals formed from Ca and Mg rich waste streams are key constituents in cement and concrete, which are in demand at the gigaton-scale every year. While thermodynamically favorable, CO2 mineralization is hindered by slow kinetics, and traditional thermochemical routes are too expensive to scale. Here, we demonstrate the advantages of an electrochemical method of waste valorization, which eliminates this limitation and improves kinetics. We highlight this method's ability to initiate crystallization under favorable local conditions, producing carbonates from mining waste at mildly acidic pH. We highlight the effects of key constituents in mining waste on the mineralization process.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

Theory of a continuous bandwidth-tuned Wigner-Mott transition

Here we develop a theory for a continuous bandwidth-tuned transition at fixed fractional electron filling from a metal with a generic Fermi surface to a “Wigner-Mott” insulator that spontaneously breaks crystalline space-group symmetries. Across the quantum critical point, (i) the entire electronic Fermi surface disappears abruptly upon approaching from the metallic side, and (ii) the insulating charge gap and various order parameters associated with the spontaneously broken space-group symmetries vanish continuously upon approaching from the insulating side. Additionally, the insulating side hosts a Fermi surface of neutral spinons. We present a framework for describing such continuous metal-insulator transitions (MITs) and analyze the example of a bandwidth-tuned transition at a filling, $v$=1/6, for spinful electrons on the triangular lattice. By extending the theory to a certain large-$N$ limit, we provide a concrete example of such a continuous MIT and discuss numerous experimental signatures near the critical point. We place our results in the context of recent experiments in moiré transition metal dichalcogenide materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Full Scale HEPA Filter Encapsulation in Ultra-High-Performance Grout - Proof of Concept

The Hanford Tank Waste Treatment and Immobilization Plant (WTP) currently being constructed to treat radioactive waste, includes vitrification facilities for both the high-level waste (HLW) and low activity waste (LAW) fractions. Operation of the WTP will produce contaminated high-efficiency particulate air filters (HEPA), as part of the solid secondary waste (SSW) stream. The HEPA filters receive off-gas from the vessel vent header and primary off-gas treatment system in LAW Facility and remove particulate contaminants including 99 Tc and 129 I salts. The current disposal method for HEPA filters is encapsulation in metal containers using cementitious material (CM) and disposal in the Integrated Disposal Facility (IDF). Results from the 2017 IDF Performance Assessment (PA) WRPS (2018) demonstrated that while compliance is maintained for the 1000 year compliance period mandated by DOE O 435.1 and its accompanying manual, release of constituents from the HEPA filters result in exceedance of the performance objective imposed as the groundwater regulatory limit at later times. For example, at about 1500 years post-closure, solid secondary waste (SSW), including HEPA filters is predicted to become a dominant contributor to 99 Tc release and over the 10,000-year sensitivity analysis period, SSW is the dominant contributor of 129 I release to the groundwater. The estimated release could potentially be reduced if the HEPA filters are not compacted and waste containers could be distributed throughout a large space, thereby diluting the contaminant release. Additionally, a better cementitious material could be used to encapsulate the HEPA filters. One alternative method for disposal of contaminated HEPA filters is encapsulation of the filters in ultra high-performance grout (UHPG). UHPG is a variation of ultra-high-performance concrete (UHPC) is commonly used in the prestressed concrete industry for large structural members. Recent studies of UHPG show it has excellent properties for containing radionuclides such as 99 Tc and 129 I Nichols and Kaplan (2021). This report presents the results of the first attempt to encapsulate a clean, full-size HEPA filter in UHPG and evaluate the effectiveness of the immobilization process and final waste form. A full-scale proof-of-concept simulated waste form was prepared by encapsulating a HEPA filter in a 110-gallon stainless steel (SS) drum using UHPG. A change from Type I/II PC to Type 1L PLC was made after American Rock Products informed the team that they would no longer be using Type I/II by the end of 2024 and the northwest was phasing out Type I/II PC overall. Type I/II PC used in previous studies of UHPG for encapsulation (Nichols and Kaplan 2021). After the UHPG was cured both the scaled mockup and the full-scale simulated waste forms were sectioned for visual examination. UHPG completely encapsulated the filters and bonded to the external surfaces of materials comprising the filters. No cracks were observed in the sectioned waste forms.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Low-Temperature Architected Cementation Agents (LAMINAE)

The cement industry contributes 5-9% of all anthropogenic CO 2 . At the same time, current concrete curing processes are passive, with little-to-no control over microstructure. The LAMINAE process offers the potential for a low-temperature pathway for producing cementitious aluminosilicate hydrate (zeolite) structures which: (a) reduces the energy burden of cement production by 30%, (b) reduces CO 2 emissions by 60%, and (c) offers microstructure control as was implicitly ensured in Roman concrete. This project generated data and engineering correlations to support further scale up and design of initial commercial processes.

36 MATERIALS SCIENCE↗

Tailoring Cementitious Materials Towards Value-Added Use of Large CO 2 Volumes

Hydraulic cements with alternative chemistries were developed for large-volume and value-added use of carbon dioxide. The hydraulic cements were processed using the energy-efficient mechanochemical technique at room temperature and atmospheric pressure. Carbon dioxide was captured directly from combustion emissions during processing. For this purpose, mechanochemical processing of hydraulic cements was accomplished under a flow of combustion emissions prior to the release of emissions to the atmosphere. The process removed a significant fraction of carbon dioxide from combustion emissions. The hydraulic cements captured carbon dioxide at about 10% of their weight. Two hydraulic cement chemistries were developed, and their mechanochemical processing was successfully scaled-up. The characteristic feature of one chemistry was its relatively low (near-neutral) pH where the integration of carbon dioxide yielded clear value. The second cement chemistry was based on alkali activation of industrial wastes. This chemistry could make value-added use of carbon dioxide, but it had to be refined to control the pH drop caused by CO 2 integration. These two cements render binding effects upon hydration by forming a combination of stable carbonates and aluminosilicates or phosphates. Efforts to develop cement chemistries based solely on carbonates were not successful. The mechanochemical process was found to integrate carbon dioxide into the alternative cement chemistries in the form of disordered and metastable carbonates. During hydration reactions, the disordered/metastable carbonates are either transformed into stable carbonate phases with desired binding efforts, or carbonates get integrated into the primary inorganic binders (hydrates). When compared with mechanochemical processing in pure carbon dioxide, mechanochemical processing in combustion emissions produced hydraulic cements with improved engineering properties. The mechanochemical process was scaled-up, and its variables as well as the raw materials formulations were optimized for implementation at pilot scale. Scale-up was found to enhance the carbon capture potential and the engineering qualities of the resulting hydraulic cements. This was because scale-up raises the intensity of mechanical energy input to raw materials. Certain mechanochemical phenomena cannot be induced, irrespective of the cumulative mechanical energy input, unless the intensity of impact is raised above a minimum level that cannot be achieved in laboratory-scale implementation of the process. Due to this effect, the duration of the mechanochemical process as well as its energy demand could be reduced significantly (by an order of magnitude) upon transition from laboratory to pilot scale, with the hydraulic cements produced at pilot scale offering engineering properties that were superior to those realized in laboratory-scale mechanochemical processing. The hydraulic cements produced at pilot scale via mechanochemical processing under a flow of combustion emissions were thoroughly characterized. They were found to meet standard requirements for ‘General Use’ hydraulic cements. They were compatible with the industrial-scale concrete production and construction practices that are used with the currently prevalent hydraulic cements. The new hydraulic cements with integrated carbon dioxide were found to offer distinct advantages over the currently prevalent Portland cement in terms of net carbon footprint and energy content. The combined raw materials and energy costs of the new hydraulic cements are competitive, and major cost savings can be realized because of the simplified production process that significantly lowers the capital investment in cement production plants. Mechanochemical processing of the new hydraulic cements under a flow of combustion emissions can be implemented using some existing components of cement manufacturing plants; this facilitates adoption of the technology by the cement industry.

36 MATERIALS SCIENCE↗

A Perspective on Scalable AI on High-Performance Computing and Leadership Class Supercomputing Facilities [Industrial and Governmental Activities]

Many scientific applications that support the mission of the US Department of Energy (US-DoE) require modeling complex engineering and/or physical systems. Here, examples of such complex systems arise from: (a) materials science to develop new compounds with exceptional mechanical and thermodynamical properties (e.g., resistance to mechanical stresses and high temperatures), (b) structural and nuclear engineering to model the temporal evolution of the structural damage of concrete shields exposed to continuous neutron and gamma radiations emitted by the nuclear reactor core, (c) urban sciences (e.g., transportation and smart buildings), and (d) power grid systems.

97 MATHEMATICS AND COMPUTING↗

Montana Community-Scale Solar Strategy Project (Final Technical Report)

Grid-tied solar photovoltaic (PV) development began gradually in Montana, initially taking root in the early 2000s, largely in the form of small residential systems, rarely larger than two kilowatts. Utility support for solar technology through public benefit funding triggered the installation of the state’s first solar PV installations on community-owned facilities including schools, libraries, fire stations and local government buildings in the mid-2000s. By 2016, solar PV installations totaled approximately 28 megawatts of installed capacity, generating less than 0.05% of electricity sold in Montana. Montana’s solar fleet in 2016 included 17 megawatts of utility-scale solar farms, and three shared solar projects developed by rural electric cooperatives that ranged from 25 to 50 kilowatts in size. However, with only 3,000 households utilizing solar PV, either through an on-site installation or participation in a shared solar project, the potential benefits and reach of solar technology was limited. The Montana Solar Community Project (MSCP) was developed by the Montana Energy Office (MEO) at the Department of Environmental Quality in order to implement a “community-scale” solar energy strategy for the state that would cost-effectively expand Montanans’ access to solar PV. This project defines three types of community-scale solar projects: shared solar, community-sited solar, and group purchasing programs. The MSCP project conducted research and stakeholder engagement that helped to inform and develop model community-scale initiatives and an overarching community-scale solar strategy for Montana. Specifically, the project included a solar market assessment, stakeholder meetings across Montana, development of a menu of community-scale solar options, a study of solar potential on schools, community solar market research, and community-scale project implementation support. MSCP activities were successful in implementing solar projects and supporting solar development in communities across Montana. Project activities realized 280 kW of newly installed solar from two solarize programs, a shared solar array at a rural electric cooperative, and a solar array atop a Bozeman high school. The community-scale project implementation support and Solar on Schools components of the project resulted directly in the analysis and design of nearly 2 MW of distributed solar systems across the state. The Solar on Schools analysis alone produced solar designs for 25 schools, representing 920.8 kW of solar potential. Many of the deliverables from this project provide guidance on future development of community-scale solar in Montana, and resulted in a number of important conclusions about community-scale solar in Montana. There is strong interest in community-scale solar in Montana, as noted during stakeholder meetings, in response to solar market research surveys, and as seen by applications for implementation support grants provided by MEO. Project activities also suggest that Montanans demonstrated a desire and need for more information about solar energy technology, solar financing options, and the state’s policy and regulatory framework. Additionally, the project found that schools will be key partners for future community-scale solar programs. In addition to being excellent hosts for solar arrays, schools have the opportunity to use the installation of a solar array to develop educational materials and curricula to educate Montana’s future leaders about these technologies, which can be shared and replicated across the state. Project activities laid a clear path forward for solar energy in Montana. Certain activities have concrete next steps. For example, numerous solar arrays were designed for schools and other public buildings around the state. Many of those designs will be used as soon as funding becomes available. Other activities have less developed next steps, though lay the foundation for future work. The solar market assessment, solar market research, and community stakeholder meetings are good examples. These documents can be used as stepping stones to increase renewable energy education, increase stakeholder outreach, and support communities as they seek to develop community-scale solar projects.

14 SOLAR ENERGY↗

Discontinuous micro-fibers as intrinsic reinforcement for ductile Engineered Cementitious Composites (ECC)

Engineered Cementitious Composites (ECC) have demonstrated superior mechanical and durability performance than conventional concrete. In the micromechanical reinforcing system of ECC, fibers play a pivotal role in establishing the ultrahigh tensile ductility and autogenous crack width control. This article reviews the state-of-the-art of discontinuous micro-fibers as intrinsic reinforcement of ECC regarding technical performance as well as environmental and economic impacts. Mechanical properties of ECC made with different micro-fibers, man-made or natural, and their embodied energy, emissions and material cost, are comprehensively surveyed. Further, studies on fiber hybridization are discussed regarding the combination of different types of fibers to form synergetic reinforcements that mitigate total material cost, and potentially enhance the composite performance. Lastly, recommendations on fiber selections are highlighted and directions for future research are suggested.

42 ENGINEERING↗

Eco-Friendly High-Performance Carbon Building Material Development from Coal

The development of eco-friendly high-performance building materials based on coal-derived materials is greatly beneficial for promoting environmental sustainability and the coal industry. This project focused on advancing technology to create innovative and scalable construction materials from two domestic sources: (1) coal-derived pyrolyzed char (PC), and (2) solvent-extracted coal deposit, extracts, and residue (CDER). It aimed to simultaneously develop and produce two types of coal-derived building products: (1) char-based concrete bricks (CCB) for wall construction in buildings, and (2) carbon-based structural units (CSU) intended as alternatives to traditional wood, concrete, or steel framing structures. The project team has successfully developed methods for manufacturing CCB samples. Extensive experiments were conducted to assess various manufacturing techniques for these samples. This included measuring their physical properties such as thermal conductivity (ranging from 0.26 to 0.38 W/mK) and bulk density (ranging from 0.85 to 1.15 g/cm 3 ), along with their mechanical properties (e.g., compressive strength ranging from 14 to 16 MPa at 28 days) for samples with a PC composition of 70%. Quality assurance and quality control tests, focusing on density and compressive strength, were also performed on samples selected randomly from pilot-scale production, and cured for a long term (over three months). The average long-term compressive strength of two randomly selected CCB samples was measured as 15.1 MPa, which was higher than the required target strength of 14 MPa. This indicates that the manufactured CCB samples from the preliminary pilot scale production run have good quality control and long-term strength performance.

01 COAL, LIGNITE, AND PEAT↗

Sulfuric Acid Improves the Reactivity of Zeolites via Dealumination

The demand for supplementary cementitious materials (SCMs), like fly ash, slag, and silica fume, is projected to rise over the next few decades. However, global decarbonization efforts, such as decommissioning of coal-fired power plants, will limit the supply of SCMs. Therefore, alternative SCM sources are a critical need for the cement and concrete industry. However, the high crystallinity of zeolites limits their pozzolanic reactivity. The goal of this work was to improve the reactivity of two common zeolites, namely clinoptilolite and SSZ-13, by treating them with sulfuric acid. The treatment enhanced zeolite reactivity via dealumination and decreased particle sizes, which led to increased reactivity with calcium hydroxide, as indicated by a 42.0% increase in reaction heat measured by isothermal calorimetry. Here, we elucidate mechanistic understanding that smaller particle sizes induced by acid treatment accelerated peak heat evolution, while free aluminates from dealumination increased heat via direct reaction with aqueous Ca 2+ .

36 MATERIALS SCIENCE↗

Biodegradable Biocomposite Development for Large Scale Additive Manufacturing

Oak Ridge National Laboratory (ORNL) worked with Mitsubishi Chemical America, Inc. to develop a highly biodegradable ~100% biobased feedstock for large format additive manufacturing (AM). Together, they developed a AM feedstock based on the biobased polyester, polybutylene succinate (PBS), that is typically used in agriculture and packaging projects. The motivation for this work was to leverage the high degradability of this polymer in AM to create a new avenue for end-of-life disposal of the product. A composite feedstock was developed from PBS, polylactic acid (PLA), and wood flour (WF). While WF improves printability, reduces feedstock cost, and can improve stiffness, it also often results in a loss in tensile strength which can inhibit/limit application of the material. To recover the loss in tensile strength suffered by including large quantities, up to 30 wt%, WF in the composite a chain extender was used to compatibilze the different composite constituents with each other. The feedstock was used to 3D-print demonstration mold for precast concrete catch basins and was tested by casting 750 lbs of concrete. The mold survived the demonstration. Aerobic degradation testing of the composite feedstock showed that it was highly degradable, 40% biodegradation after 90 days, compared to other incumbent biobased feedstocks.

36 MATERIALS SCIENCE↗

Magnetic dynamics with Weyl fermions

Transport of charge and valley (axial) degrees of freedom coupled to order-parameter dynamics in magnetic Weyl semimetals is studied in the framework of nonequilibrium thermodynamics. In addition to the established valley-related transport anomalies that are rooted in band-structure topology, we construct dissipative couplings between the three dynamic constituents of the system driven out of equilibrium by electromagnetic perturbations. We show how the valley degree of freedom mediates an effective coupling between the charge and magnetic sectors of the system, through a combination of the chiral anomaly, on the electric side, and the Onsager-paired valley torque and pumping, on the magnetic side. This work complements previous studies of magnetic Weyl semimetals by a more systematic analysis of collective dissipation. We discuss several concrete examples of the valley-mediated current-driven magnetic instabilities and charge pumping, and extend the theory to the antiferromagnetic case.

36 MATERIALS SCIENCE↗