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DOE OSTI2024

Method Development and Implementation for Characterizing Uncertainties in Tank Leak Volumes for Composite Analysis.

The purpose of this environmental calculation file (ECF) is to provide a summary of methodology, inputs, assumptions, and results of a Special Analysis (SA) titled “Method Development and Implementation for Characterizing Uncertainties in Tank Leak Volumes for the Updated Composite Analysis.” This SA is one of the three SAs conducted in Fiscal Year (FY) 2024 for the Composite Analysis (CA) for the Hanford Site (DOE/RL-2019-52, Composite Analysis for Low-Level Waste Disposal in the Hanford Site Central Plateau (FY 2020)), and it is performed following the Unreviewed Composite Analysis Question Evaluation procedure, UCAQ-24-01-E (UCAQ-24-01-E, Rev. 0).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2024

Composite Analysis for Low-Level Waste Disposal in the Central Plateau of the Hanford Site (Annual Summary Report (FY 2023))

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) 2023 for maintenance of the Hanford Site Composite Analysis reported in DOE/RL-2019-52 (hereinafter referred to as the updated Hanford Site Composite Analysis). This is the first annual summary report to transition from maintenance of the initial Hanford Site Composite Analysis reported in PNNL-11800 and PNNL-11800, Addendum 1 to maintenance of the updated Hanford Site Composite Analysis following DOE approval of that update.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2026

Annual Summary Report (FY 2025) Composite Analysis for Low-Level Waste Disposal in the Central Plateau of the Hanford Site

In accordance with DOE M 435.1-1, Radioactive Waste Management Manual, requirements, the U.S. Department of Energy (DOE) Hanford Field Office (HFO) prepared this Annual Summary Report (ASR) for fiscal year (FY) 2025 for the Hanford Site Composite Analysis (CA) reported in DOE/RL-2019-52, Composite Analysis for Low-Level Waste Disposal in the Hanford Site Central Plateau (FY 2020) (hereinafter referred to as the Hanford Site Composite Analysis). The preparation of this ASR follows the technical specifications provided in DOE-STD-5002-2017, Disposal Authorization Statement and Tank Closure Documentation.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2023

Composite Analysis for Low-Level Waste Disposal in the Hanford Site Central Plateau (FY 2020) (Rev. 2)

This document provides an updated Hanford Site composite analysis (CA). A Hanford Site CA was prepared and issued in 1998 (PNNL-11800) with an addendum provided in 2002 (PNNL-11800 Addendum 1). The CA was approved in 2002 (Frei, 2002) and has been maintained (DOE/RL-2000-29 and subsequent revisions) to support low-level waste disposal performance assessments (PAs) and disposal authorizations for facilities at the Hanford Site, including the following: Continued operation of the Environmental Restoration Disposal Facility (ERDF) and the 200 East and 200 West Low-Level Burial Grounds; Construction of the Integrated Disposal Facility (IDF); Forthcoming closure of tank residual waste systems such as Waste Management Area (WMA) C. The CA maintenance program resulted in a determination in 2015 (DOE/RL-2015-66) that the Hanford Site CA needed an update for the following reasons: While the initial Hanford Site CA has been maintained since 2001, the accumulation of basis changes reported in the annual summary reports over the succeeding 14 years merit evaluation in an updated analysis; The U.S. Department of Energy (DOE) Headquarters requested in a memorandum in 2015 (Gilbertson and Marcinowski, 2015) that “as soon as the relevant PAs are complete, the CA will be revised to account for all of the new information.” This updated Hanford Site CA accounts for the following new information: 1. Inclusion of a detailed Hanford Site baseline disposition that projects remedial activities through site closure. There have been significant changes through decision making in the Comprehensive Environmental Response, Compensation, and Liability Act of 1980 (CERCLA) process that were not available when the original CA was produced; 2. Inclusion of an updated inventory basis, new modeling capabilities, and new decisions reached in the associated record of decision (ROD) that was provided by issuance of DOE/EIS-0391 in fiscal year (FY) 2013. Development of a Hanford Site groundwater model from the baseline provided in a technical transfer of models for the Final Tank Closure and Waste Management Environmental Impact Statement (DOE/EIS-0391) commenced in FY 2014 and resulted in the plateau-to-river (P2R) groundwater flow model that is used in this updated Hanford Site CA; 3. Accounting for pump and treat systems, which were not evaluated in the initial CA. Pump and treat systems have had significant impact on groundwater flow system behavior, contaminant transport, and contaminant removal from Hanford Site groundwater. This process is accounted for in the use of the P2R model for this updated Hanford Site CA; 4. Inclusion of water-level data collected since the initial CA was completed. Data collected as the unconfined aquifer water levels continue to recede since the cessation of large liquid discharges in the late 1990s have led to marked improvement in understanding of the flow system for future conditions, particularly regarding northward flow potential in the critical Gable Gap area. The calibration in the latest version of the P2R model accounts for this information; 5. Inclusion of results from the revised ERDF PA completed in 2013 (WCH-5209) that account for updated inventory and expansion of the ERDF facility to about twice the size that was evaluated in the original CA; 6. Use of updated geoframeworks to provide the structural basis for numerical fate and transport models in the groundwater pathway of this updated CA. The geologic basis for groundwater models has continued to improve with additional data collection and interpretation with the creation and maintenance of the Hanford South Geoframework and the Central Plateau Vadose Zone Geoframework tools; 7. Incorporation of updated tank residual inventory estimates. Tank residual inventory estimates have improved with the incorporation of tank retrieval inventory data for those tanks that have completed retrieval. The CA inventory data package includes this updated information; 8. Incorporation of WMA C PA results. Two additional PAs for tank farm closure decisions are in preparation during the period required to prepare an updated Hanford Site CA: WMA C (FY 2016) and WMA A-AX (in preparation). The WMA C PA results are incorporated into the updated Hanford Site CA, and its grouted residuals model is used as the basis for a release model to account for the other tank farm systems modeling in this updated CA; 9. An update to the IDF PA was submitted in FY 2017 and has been reviewed and approved. The results of the IDF PA are incorporated into this updated CA; 10. Updated risk assessment scenarios. The risk assessment scenarios currently in use for Hanford Site CERCLA and Resource Conservation and Recovery Act of 1976 (RCRA) analyses differ from those evaluated in the initial Hanford Site CA. The representative person exposure scenario evaluated in this updated Hanford Site CA is consistent with recent PAs and CERCLA and RCRA analyses as the Hanford Site. This updated Hanford Site CA provides the following: A comparison of the updated Hanford Site CA all-pathway dose results with the performance measures during the compliance period, which is assumed to begin with site closure in calendar 2070 with the last scheduled disposal action and continue for 1,000 years postclosure (to calendar year 3069); A comparison of Hanford Site CA all-pathway dose results with the performance measures during the postcompliance period to address potential peaks beyond the compliance period. This is accomplished by evaluating dose in the period for 9,000 years following the compliance period (i.e., from calendar year 3070 to 12070).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2024

Maintenance Plan for the Composite Analysis of the Hanford Site, Southeast Washington

The objective of this document is to provide a maintenance plan (MP) that supports the Hanford Site composite analysis (CA). Maintenance consists of four activities: compliance and performance monitoring; research and development; planned reviews and analysis; and revisions to the CA. This MP will be reviewed annually by the site and updated as needed to address priorities based upon new information or proposed changes, the status of any disposal authorization statement (DAS) conditions/limitations and Low-Level Waste Disposal Facility Federal Review Group (LFRG) issues. This revision supersedes Revision 4.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2023

Updates to Composite Analysis Base Case and Null Space Monte Carlo Sensitivity Based on New Unit Dose Factors

This environmental calculation file (ECF) presents the results of the exposure route-specific and total radiological dose assessments for the groundwater exposure pathway as a part of the updated Composite Analysis for Low-Level Waste Disposal in the Hanford Site Central Plateau (FY 2022), based on revised unit dose factors (UDFs) published in CA Special Studies: Updates to the Groundwater Pathway Radiological Dose. The reason for these radiological dose assessments is to estimate the cumulative radiological impacts from all screened sources of ionizing radiation and exposure routes that could potentially contribute to the projected dose to a hypothetical member of the public. Sources of ionizing radiation can include existing or future disposal facilities and other sources including past-practice discharge sites. Additionally, the results of the exposure route-specific and total radiological dose assessments have been revised for the groundwater pathway based on the null space Monte Carlo (NSMC) groundwater concentrations and the most recent updates to the UDFs as a part an uncertainty analysis for the updated Hanford Site CA.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2025

Hanford Composite Analysis Special Studies FY2025 - Groundwater Flow Simulation for use in a Comparison of Simulated Concentrations in the Saturated Zone Estimated by the Plateau-to-River Model Versions 8.3 and 9.1

In order to meet the requirements of U.S. Department of Energy (DOE) in DOE O 435.1, Radioactive Waste Management, a composite analysis (CA) must be completed for the Central Plateau at the Hanford Site. The CA requires estimates of fate and transport of radionuclides in the groundwater from multiple sources within the modeling domain. This Environmental Calculation File (ECF) details the application of the Plateau-to-River (P2R) Model (CP-57037, Rev. 3, Model Package Report for the P2R Model: Version 9.1) to predict the flow of groundwater on the Central Plateau for the 10,000-year simulation to support a special analysis associated with the Hanford Site CA. The simulated flow field will support the simulation of fate and transport of contaminants for comparison to the results obtained as part of the CA to evaluate impact of the updated version of the P2R Model.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2023

Tropical Red Macroalgae Cultivation with a Focus on Compositional Analysis

To create carbon efficient sources of bioenergy feedstocks and feedstuff for aquaculture and terrestrial livestock, it is critical to develop and commercialize the most efficient seaweed cultivation approach with a sustainable nutrient input supply. Here, we present data for a novel, onshore tropical macroalgae cultivation system, based on influent deep seawater as the nutrient and carbon sources. Two red algal species were selected, Agardhiella subulata and Halymenia hawaiiana, as the basis for growth optimization. Highest productivity in small-scale cultivation was demonstrated with A. subulata in the 10% deep seawater (64.7 µg N L−1) treatment, growing at up to 26% specific growth rate day−1 with highest yields observed at 247.5 g m−2 day−1 fresh weight. The highest yields for H. hawaiiana were measured with the addition of 10% deep seawater up to 8.8% specific growth rate day−1 and yields at 63.3 g fresh weight m−2 day−1 equivalent. Biomass should be culled weekly or biweekly to avoid density limitations, which likely contributed to a decrease in SGR over time. With a measured 30–40% carbon content of the ash-free dry weight (20–30% of the dry weight) biomass, this translates to an almost 1:1 CO2 capture to biomass ratio. The compositional fingerprint of the high carbohydrate content of both Agardhiella and Halymenia makes for an attractive feedstock for downstream biorefinery applications. By focusing on scaling and optimizing seaweed farming technologies for large-scale onshore farms, the opportunities for yield potential, adaptability to cultivation conditions, and meeting global sustainability goals through novel, carbon-negative biomass sources such as seaweed can be realized.

09 BIOMASS FUELS↗
DOE OSTI2024

Biomass yields, reproductive fertility, compositional analysis, and genetic diversity of newly developed triploid giant miscanthus hybrids

Abstract Miscanthus × giganteus (giant miscanthus), first found as a naturally occurring hybrid, has shown promise as a bioenergy/biomass crop throughout much of the temperate world. This allotriploid (2 n = 3 x = 57) hybrid resulted from a cross between tetraploid Miscanthus sacchariflorus (2 n = 4 x = 76) and diploid Miscanthus sinensis (2 n = 2 x = 38) and is particularly desirable due to its low fertility that minimizes reseeding and potential invasiveness. However, there is limited genetic diversity in commonly grown cultivars of triploid M. × giganteus and breeding and development efforts to improve and domesticate this crop have been minimal. Here, we report on newly developed M. × giganteus hybrids compared with the industry standard M. × giganteus '1993‐1780'. Dry biomass yields of new hybrids ranged from 19.5 to 32.4 Mg/ha/year for the fourth growing season, compared with 21.0 Mg/ha/year for M. × giganteus '1993‐1780'. Plant reproductive fertility remained low for all accessions with overall fertility [(seed set × seed germination)/100] ranging from 0.3% to 4.5% for new hybrids compared to 0.4% for M. × giganteus '1993‐1780'. Culm density and height varied among accessions and were positively correlated with increased biomass. Based on compositional analyses, theoretical ethanol yields ranged from 9, 740 to 16,278 L/ha/year for new hybrids compared to 10,406 L/ha/year for M. × giganteus '1993‐1780'. Relative feed value indices were low overall and ranged between 66.0 and 72.8 for new hybrids compared to M. × giganteus '1993‐1780' with 71.3. The genetic diversity of new hybrids, compared with existing cultivars, was characterized using whole genome sequences. Based on pair‐wise distances, cluster analysis clearly showed increased diversity of new hybrids compared with earlier selections. These results document new triploid hybrids of M. × giganteus with enhanced biomass and theoretical ethanol yields in combination with broader genetic diversity and lowreproductive fertility.

Touchell, Darren H.↗
DOE OSTI2025

Feasibility of fusion plasma burn control via real-time, sub-divertor neutral gas isotopic and compositional analysis

The ability to provide fusion burn control without requiring physical access through the first wall and fuel breeding blankets, would be vital for any future, magnetically confined fusion power reactor. A multi-sensor, fusion fuel cycle exhaust, neutral gas analysis system on JET, capable of delivering real time data, and accessing only the sub-divertor region, provides an excellent example of such capability. Optimized for and operated during the deuterium–tritium experimental campaigns 2 and 3 (DTE2, DTE3), it is proving valuable for planning to explore fusion reactor burn control in ITER with a comparable diagnostic system called the Diagnostic Residual Gas Analyzer (DRGA). This paper aims to show feasibility of developing model-based controllers for ITER and next generation, reactor-relevant devices, by building both on the empirical experience in JET-DTE2, and on the already emerging experience on developing such models specifically for ITER. The paper begins with a specific use-case from JET-DTE2, pertaining to the observed sensitivity of the fusion neutron yield on the concentration of isotopic helium-3 ( 3 He), with data from one of the high-performance DT shots exhibited with emphasis on the 3 He measurement via the sub-divertor. Then, a first model is developed and then explored with simulations that aim to discover how well the controllers in the model react to either insufficient levels of 3 He or excessive levels of 3 He. The simulations then explore potential impact from a delay in the measurement (or the response) that would be comparable to the ∼1 s, conductance limited response for the ITER DRGA system, currently in its final design. The simulations show that control is feasible, and that its effectiveness is not significantly impacted by such delay.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

Evaluation of Hypotheses for the Fate of Historical Discharges from Hanford Site BC Cribs and Trenches

A preliminary review of declassified reports and historical documents from the 1950s and 1960s indicated they may contain valuable information regarding potential impacts to groundwater from liquid waste discharged to the 216-BC Cribs and Trenches during the late 1950s. Transport of contaminants in the vadose zone beneath the BC Cribs area is simulated by a vadose zone model developed for the Composite Analysis (DOE/RL-2019-52, Composite Analysis for Low-Level Waste Disposal in the Hanford Site Central Plateau ). Results from this model indicate there has been no substantial breakthrough of contaminants (particularly technetium-99) to groundwater from the vadose zone up to the present day. However, there is uncertainty in the anisotropy and other model input parameters as well as acknowledged sparseness of sampling data for this area. In this study, historical documents and other information were reviewed to evaluate the possibility that contaminant breakthrough to groundwater occurred during or shortly after operation of the BC Cribs sites, and whether refinements of the vadose zone model parametrization should be considered.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2026

Feedstock/Pretreatment Screening for Bioconversion of Sugars and Lignin Residues

This project will conduct biomass deconstruction (pretreatment and enzymatic saccharification) on two representative biomass feedstocks and four different pretreatment processes, including three high temperature steam/chemical pretreatments and one low temperature chemical/mechanical pretreatment. A third biomass feedstock will undergo biomass deconstruction with three different pretreatment processes, including two high temperature chemical pretreatments and one low temperature chemical/mechanical pretreatment. Several pretreatment conditions will be performed in a screening study using NLR pilot-scale pretreatment equipment to generate a range of pretreated biomass substrates. A selected number of these substrates will be chosen for enzymatic saccharification evaluation, based on standard compositional analysis of the pretreated substrates as a primary indicator of pretreatment efficacy. Resulting enzymatic hydrolysis slurries will be analyzed to determine overall biomass sugar yields. Additional compositional analysis will be performed to determine oligomeric sugar composition and structure, to analyze structural characteristics of solids fractions on native, pretreated, and enzymatically saccharified biomass residues for one of the biomass feedstocks, corn stover. The enzymatically saccharified materials will undergo 2,3-butanediol fermentation in a shaker flask as bench scale. Using relevant process performance data collected in these various conversion steps, technoeconomic analysis activities will be performed to compare the economic potential of the various biomass feedstock and pretreatment processes and to identify key economic drivers and sustainability metrics.

09 BIOMASS FUELS↗
DOE OSTI2024

Techno-economic analysis of biomass value-added processing informed by pilot scale de-ashing of paper sludge feedstock

Paper sludge biomass represents an underutilized feedstock rich in pulped and processed cellulose which is currently a waste stream with significant disposal cost to industry for landfilling services. Effective fractionation of the cellulose from paper sludge presents an opportunity to yield cellulose as feedstock for value-added processes. A novel approach to cellulose fractionation is the sidehill screening system, herein studied at the pilot-plant scale. Composition analysis determined ash removal and carbohydrate retention of both sidehill and high-performance benchtop screening systems. Sidehill screening resulted in greater carbohydrates retention relative to benchtop screening (90% vs 66%) and similar ash removal (95% vs 98%). Techno-economic analysis for production of sugar syrup yielded a minimum selling price of $331/metric ton of sugar syrup including disposal savings, significantly less than a commercial sugar syrup without fractionation. Furthermore, sensitivity analysis showed that screening conditions played a significant role in economic feasibility for cellulosic yield and downstream processes.

09 BIOMASS FUELS↗
DOE OSTI2025

Impact of Storage Conditions on the Quality and Viability of Switchgrass as a Bioenergy Crop

With growing energy demands and climate concerns, advancements in bioenergy have become imperative. Biofuels promote energy independence, reduce fossil fuel reliance, and cut greenhouse gas emissions. Switchgrass (Panicum virgatumis) is an ideal bioenergy crop due to its ability to thrive on marginal lands unsuitable for food crops and its drought tolerance, rendering it a low-maintenance, high-yield option. In the bioenergy industry, energy crops are typically stored to facilitate supply chain management and ensure a continuous supply despite seasonal availability. However, the effective utilization of bioenergy crops is typically contingent upon addressing the challenges associated with biomass storage. These challenges include high moisture content that promotes biological degradation of the biomass leading to increased risk of pathogenic microbes, and chemical degradation that increases the ratio of inconvertible, inorganic materials. These issues lead to a reduction of feedstock value, diminishing the biomass-to-biofuel conversion efficacy, making switchgrass and other bioenergy crops less effective as fuel sources. This project aims to improve the storage of purpose-grown energy crops. Aerobic storage trials were conducted under varying moisture contents to stimulate real-world environmental exposure. Switchgrass samples were rewetted to 30% or 35% and stored in a bioreactor for approximately one month, or until cellular respiration ceased. Degradation indicators, such as dry matter loss, temperature changes, and cellular respiration, were measured throughout this process. Samples for compositional analysis, 16S, and ITS were taken at three different time points: before, during, and after storage, to monitor changes in biomass, microbial communities, and metabolites over time. Preliminary data indicate that dry matter loss is proportional to cellular respiration, with higher moisture content (35%) leading to higher temperatures and elevated dry matter loss. Compositional analysis and microbial community analysis are in progress. This research will provide a comprehensive understanding of storage, helping to identify stability factors in energy crops and improve best management practices for biomass producers.

09 - BIOMASS FUELS↗
DOE OSTI2026

Opportunities and Limitations of Nuclear Magnetic Resonance Spectroscopy in Astrobiology

For decades, Nuclear Magnetic Resonance (NMR) spectroscopy has been utilized as a powerful tool in various scientific disciplines, most prominently in chemistry, to determine molecular structures or monitor reactions. While well established in various fields, NMR applications in astrobiology are still unclear. This work aims to explore the potential of NMR in astrobiology, highlighting strengths but also weaknesses. We illustrate capabilities of NMR with two applications: (1) recently developed methods for position-specific carbon isotope analysis of complex organics; and (2) well-established tools for performing quantitative compositional analysis of complex organic mixtures. By utilizing samples relevant to astrobiology, specifically the amino acid valine and analogue mixtures of organics, we showcase that molecules retain a source dependent and distinct intramolecular carbon isotope fingerprint. We demonstrate that compositional sample analysis provides an independent and complementary line of evidence pointing towards the origin of a molecule or mixture. Together, these NMR tools have the potential to support life detection efforts, and aid in distinguishing between biotic and abiotic samples. Finally, we discuss sensitivity, detection limits, the portability of NMR, and propose how integration with mass-spectrometry techniques will be imperative to enable more targeted and comprehensive analyses relevant to astrobiology, including in-situ analysis but also sample return missions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Rapid AI-based Dissection of Ashes using Raman and XRF Spectroscopy (RADAR-X)

Waste-to-energy (WTE) facilities incinerate ~35 million tons of municipal solid waste annually in the United States. The incineration process reduces the mass and the volume of the waste fraction by over 75 and 95%, respectively. The fraction left after incineration remains as ash residues and is referred to as WTE ash, compromising of bottom and fly ash. In the United States, ~10 million tons of WTE ashes are generated annually and predominantly landfilled because of the lack of secondary end-use pathways. This incurs a significant financial burden (landfilling costs) on U.S. WTE facilities and also results in the loss of materials to the landfill. The primary objective of this research is to understand better the elemental and mineralogical composition of WTE ashes from diverse origins and find composition dependent upcycling pathways for diverting these ashes from landfills. This primary objective was addressed through three research tasks –(Task I) An AI-led Multi-Modal Approach for Compositional Analysis, (Task II) Developing a Dissolution-Based Test for Real Time Analysis, and (Task III) Establishing composition-dependent end uses. The chemical composition of WTE ash is dependent on two factors, i.e., the input waste composition and the operational parameters of a WTE facility (combustion conditions). Amongst these two factors, the input waste composition will likely show spatial and temporal variation. As a result, the chemical composition of WTE ash will also fluctuate. To understand the spatial and temporal variation in WTE ash composition, in Task I, we collected 128 ash samples (62 bottom ash and 66 fly ash samples) from 11 WTE facilities located in 11 U.S. states and characterized them via X-ray Fluorescence, powder X-ray Diffraction, and Raman Spectroscopy. The findings from this extensive characterization work indicated that the key elements in WTE fly ashes are Ca, Cl (greater than 10 wt. %), Si, S, K, Zn ( between 1 and 10 wt. %), Mg, Al, P, Ti, Fe, Cu, Br, and Pb (between 0.1 and 1 wt. %). Similarly, the key elements in WTE bottom ash fraction finer than 45μm are Ca (greater than 10 wt. %), Mg, Al, Si, S, Cl, K, Ti, Fe, Zn (between 1 and 10 wt. %), P, V, Cr, Mn, Cu, Br, and Pb (between 0.1 and 1 wt. %). Here, we note that the dominant fraction of WTE bottom ash is the coarse fraction. The coarse WTE bottom ash fraction (rich in silicon) was not characterized in this study because of excessive grinding requirements and their unsuitability as a supplementary cementitious material due to their coarse nature. The elements in WTE bottom ashes are present as calcite, anhydrite, vaterite, hydroxyapatite, quartz, bassanite, gehlenite, akermanite, hydrocalumite, and portlandite. Similarly, the mineralogical species present in WTE fly ashes are calcium chloride hydroxide, halite, calcite, anhydrite, sylvite, hydrocalumite, vaterite, hannebachite, quartz, and bassanite. Temporal variation in ash composition may also result in significant fluctuations in chemical compositions. Therefore, a WTE facility may need to monitor the ash composition (elemental and mineralogical composition) in real time. In Task I, we evaluated the possibility of using a portable X-ray fluorescence (XRF) spectrometer to monitor the elemental composition in real-time. Specifically, we collected XRF data on identical specimens via a portable XRF spectrometer (low-end) and a lab-based benchtop XRF spectrometer (high-end). The collected data was used to train an A.I. algorithm (portable XRF data as an input and benchtop XRF data as an output) to predict accurate elemental composition using portable XRF data. Finally, we developed a 2-minute photobleaching protocol to monitor the mineralogical characteristics of WTE ashes via Raman spectroscopy. Overall, the activities in Task I improved our understanding of ash composition and developed techniques to monitor elemental and mineralogical composition in near real-time. Based on the findings of Task I, we find that WTE ashes exhibit wide variability in mineralogy. For ICP-based elemental analysis, all the mineralogical species in WTE ashes must be brought into solution. This is traditionally accomplished with acid digestion using a combination of multiple acids. However, acid digestion with multiple acids is time-consuming and often fails to ensure complete digestion of the ash matrix. To address this limitation, in Task II, we developed an alkali-fusion-based digestion protocol using a combination of lithium tetraborate, lithium metaborate, and their combinations as possible alkali fluxes for digesting WTE ashes entirely and rapidly. The validity of the developed method was evaluated on two standard ash specimens, i.e., SRM 1633c coal fly ash and BCR-176R incineration fly ash specimen. The findings suggest that the developed protocol can ensure complete digestion of elements such as Al, Ba, Ca, Cr, Cu, Mg, Mn, P, Sr, V, Zn, Be, K, and rare earth elements. The recent changes in the energy market towards renewables and increased metal recycling have resulted in reduced supplies of supplementary cementitious materials (coal fly ash and slag). Therefore, in Task III, we evaluated the possibility of employing WTE ashes as SCMs. As the chemical composition of WTE ashes varies temporally (on an hourly basis), there was also a need to develop tests that can evaluate the suitability of material to act as supplementary cementitious material rapidly, i.e., in a few minutes. Therefore, in Task II, we also developed a rapid test to assess the suitability of a material to act as an SCM in 5 minutes. This represents a significant advance over the state-of-the-art R 3 test, which takes ~144 hours. This test was initially validated on amorphous aluminosilicates, such as calcined clays, and could be extended to evaluate other industrial by-products, such as WTE ashes. In Task III, we evaluated the possibility of employing WTE ashes for two applications, i.e., as an SCM and a lime substitute for clay stabilization. The findings from Task I indicated that WTE ashes are enriched in chlorine and, therefore, cannot be used directly as an SCM due to corrosion-related risks and altered hydration kinetics. Accordingly, we developed an ash treatment protocol to reduce the solubility of chlorine-containing species in WTE ashes. The developed treatment protocol also immobilized lead in certain mineral forms. As a result of the treatment, WTE ashes can be used as SCMs without any corrosion or heavy metal leaching concerns. The second application examined in this study was clay stabilization. WTE ashes are calcium-rich and can be an adequate lime replacement for clay stabilization. Our findings reveal that the sum of the concentrations of Ca(OH) 2 and CaClOH controls the clay stabilization capability of WTE ashes. In summary, in this work, we evaluated the elemental and mineralogical characteristics of U.S. WTE ashes from diverse origins and developed tests to evaluate the chemical characteristics of these ashes in real time through a portable XRF and a benchtop Raman spectrometer. Based on the chemical characteristics of these ashes, we developed an ash treatment process to enable the use of WTE ashes as an SCM and also evaluated the possibility of employing these ashes for clay stabilization. Overall, the findings from this work enables the diversion of WTE ashes from landfills for multiple end-uses, i.e., as an SCM or a lime substitute for clay stabilization.

36 MATERIALS SCIENCE↗