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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Surface Modified Fly Ash for Value Added Products (SuMo Fly Ash)

The objective of this project is to develop a technology to encapsulate coal fly ash particles in sulfurized vegetable oil, enhancing physical and mechanical properties of the fly ash as a filler material when applied in commercial products. This project significantly advances the knowledge base and technology for synthesizing coated fly ash particles for application in different polymer matrices to increase cross-linking, compatibility, air-entrainment and to decrease the leaching potential of metals of concern. Specifically, the project focuses on (a) collection, and characterization of fly ash material from coal power plants; (b) development of Sulfurized Vegetable Oil (SVO) modified (SuMo) fly ash and their detailed characterization; (c) evaluation of the mechanical properties of the SuMo fly ash incorporated plastic and rubber composites for potential replacement of CaCO 3 or carbon black as filler materials with SuMo fly ash in plastic and rubber composites; (d) leaching potential of SuMo fly ash and SuMo fly ash-incorporated plastic and rubber composites to determine the rate of release of trace metals. The major findings of this project are: i) Sulfurized Vegetable Oil coated fly ash (SuMo fly ash) was successfully prepared with a particle size of ≤ 45 micron which exhibited hydrophobicity of contact angle > 90°; ii) the coating reduces leaching of metals (e.g., B, Cr) from fly ash when exposed to water; iii) incorporation of SuMo fly ash increases thermal stability and yield strength of plastics; iv) SuMo coating helps disperse fly ash particles into cured rubbers, natural rubber; (v) SuMo fly ash-incorporated plastic/cured rubbers compounds protects against leaching of toxic elements.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2022

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↗
DOE OSTI2021

Distribution of rare earth elements in the pilot-scale processing of fly ashes derived from eastern Kentucky coals: Comparisons of the feed and processed ashes

Beneficiated fly ash from the combustion of Central Appalachian high volatile bituminous coals was extracted with HNO 3 in a pilot-scale processing plant. Several major oxides (notably CaO and SO 3 , but also including Fe 2 O 3 , MgO, K 2 O, and P 2 O 5 ) and minor elements (Mn, As, Sr, Ba, and Pb) are depleted in the post-HNO 3 -extraction spent ash. The total lanthanides, Y, and Sc concentration is reduced by about 20% in the spent ash, with Gd showing the greatest decrease. Along with Gd, Nd and Dy are also well differentiated between the feed and spent ashes, with La and Sm showing minimal partitioning. The Gd decrease is correlated with the depletion of Fe 2 O 3 . The heavy rare earth elements (REE heavier than Eu) and Y are disproportionately concentrated in the HNO 3 -leachate compared to the light REE. For the ashes studied, Sc did not partition between the feed and spent ashes. Pozzolanicity tests show that the compressive strength and strength activity indices of the spent ash + ordinary Portland cement (OPC) mixes are comparable to 100% OPC, indicating that the spent ashes produced in the pilot-scale runs have the potential to be sold as a Class F fly ash. Finally, the beneficiated ash chemistry influences the chemistry of the post-HNO 3 -extraction spent ash and the HNO 3 -leachate. A 500-ppm-REE fly ash will presumably be a more economically favorable feedstock than an ash with a significantly lesser concentration.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2025

Probing the Critical Element Chemistry of Coal-Combustion Fly Ash: Examination of Zircon and Associated Minerals from a Beneficiated Kentucky Fly Ash

Along with the principal rare earth (REE) minerals such as monazite, xenotime, and bastnasite, Y-and REE-bearing zircon and associated minerals survive the combustion process and are found in coal-combustion fly ash. Beneficiated fly ash from a power plant burning an eastern-Kentucky-sourced coal blend was found to have zircon (ZrSiO4), baddeleyite (ZrO2), fergusonite (YNbO4), yttriaite (Y2O3), and xenotime (YPO4). Previous studies of the same fly had also identified monazite with a broad REE suite. Scanning electron microscopy–electron dispersive spectroscopy (EDS) and transmission electron microscopy (TEM)–EDS as well as other TEM-based techniques revealed a variety of zircon associations, including heavy-REE suites with Y, Nb, and Hf. Hafnium is a common accessory element in zircons and the Y and Nb may be present as fergusonite (YNbO4) intermixed with zircon.

Berti, Debora (ORCID:0000000311237794)↗
DOE OSTI2022

High-Resolution Transmission Electron Microscopy Study of a Powder River Basin Coal-Derived Fly Ash

Examination of a fly ash derived from the combustion of a low-S, subbituminous Powder River Basin coal by Scanning Electron Microscopy (SEM) and High-resolution Transmission Electron Microscopy (HRTEM), both supplemented by Energy-dispersive X-ray spectroscopy (EDS), showed that the fly ashes were dominated by amorphous phases, Ca-rich plagioclase feldspars, Mg-rich phases, complex Ca-Mg-Al-Si-Ti-Fe grains, and trace amounts of REE-rich particles. Many of the particles were rimmed by a Ca-S, possibly a sulfate. HRTEM-EDS examination of a REE-rich particle proved it to be a mix of light- and heavy-rare earth minerals mixed with amorphous phases.

58 GEOSCIENCES↗
DOE OSTI2024

On the Flow of a Cement Suspension: The Effects of Nano-Silica and Fly Ash Particles

Additives such as nano-silica and fly ash are widely used in cement and concrete materials to improve the rheology of fresh cement and concrete and the performance of hardened materials and increase the sustainability of the cement and concrete industry by reducing the usage of Portland cement. Therefore, it is important to study the effect of these additives on the rheological behavior of fresh cement. In this paper, we study the pulsating Poiseuille flow of fresh cement in a horizontal pipe by considering two different additives and when they are combined (nano-silica, fly ash, combined nano-silica, and fly ash). To model the fresh cement suspension, we used a modified form of the power-law model to demonstrate the dependency of the cement viscosity on the shear rate and volume fraction of cement and the additive particles. The convection–diffusion equation was used to solve for the volume fraction. After solving the equations in the dimensionless forms, we conducted a parametric study to analyze the effects of nano-silica, fly ash, and combined nano-silica and fly ash additives on the velocity and volume fraction profiles of the cement suspension. According to the parametric study presented here, larger nano-silica content results in lower centerline velocity of the cement suspension and larger non-uniformity of the volume fraction. Compared to nano-silica, fly ash exhibits an opposite effect on the velocity. Larger fly ash content results in higher centerline velocity, while the effect of the fly ash on the volume fraction is not obvious. For cement suspension containing combined nano-silica and fly ash additives, nano-silica plays a dominant role in the flow behavior of the suspension. The findings of the study can help the design and operation of the pulsating flow of fresh cement mortars and concrete in the 3D printing industry.

36 MATERIALS SCIENCE↗
DOE OSTI2021

A new hypothesis for air loss in cement systems containing fly ash

Although there are many benefits gained from incorporating fly ash into concrete, carbon contamination in the fly ash has been shown to interfere with the efficacy of organic additives in an unpredictable manner. This work uses surface tension measurements to quantify the adsorption of air-entraining agents (AEA) onto cement and fly ash. Both the adsorption capacity of the adsorbents and the adsorption isotherms indicate that the fly ash particles, rather than the carbon itself, dominate adsorption in a carbon-contaminated ash in cement pore solution. We propose that adsorption onto fly ash particles and cement actually improve air entrainment via Pickering stabilization. While the carbon is still expected to contribute to air loss via hydrophobic adsorption of the surfactants, we suggest that the primary way in which the carbon interferes is by shielding surfactant-coated fly ash particles from participating in air development and Pickering stabilization during mixing.

36 MATERIALS SCIENCE↗
DOE OSTI2023

From ash to oxides: Recovery of rare-earth elements as a step towards valorization of coal fly ash waste

Coal fly ash (CFA) is both a valuable waste material and a potential source of environmental contamination. The inclusion of metals such as rare-earth elements offer a possible incentive towards waste valorization if the metals can be extracted and recovered in an economical manner. Rare-earth elements (REEs) have many technological applications and are critically important in the manufacture of electric vehicles, communication devices, and industrial magnets. However, the global supply of rare-earth elements has faced shortages and price shocks. Current methods for separating and isolating individual rare-earth elements use large amounts of energy and organic solvents, raising concerns over environmental impacts. These factors have led to the investigation of nontraditional sources and separation techniques for these elements. Here, we describe a column-based system that uses a newly developed ligand-associated organosilica sorbent to concentrate and separate rare-earth elements from fly ash leachate. The fly ash used in this study originally contained 0.024 wt% rare-earth elements and the final oxide powder after enrichment contained > 10 wt% rare-earth elements, which is a enrichment of > 400 times. This process requires no additional organic solvents after the sorbent media has been synthesized, offering an alternative to the current standard using solvent extraction for rare-earth element recovery.

42 ENGINEERING↗
DOE OSTI2025

Characterization of Arsenic and Selenium in Coal Fly Ash to Improve Evaluations for Disposal and Reuse Potential (Final Technical Report)

Coal fly ash is a high volume waste material that is discarded in landfills and surface water impoundments across the U.S. and is also widely recycled for a variety of applications. The leaching of potential of contaminants of concern, such as arsenic (As) and selenium (Se), is often the driver of risk assessments for coal ash disposal and reuse. The extent of leachable As and Se depends on several factors related to environmental conditions and fly ash characteristics. Previous studies employed various methods to delineate the concentration, chemical form, and distribution of As and Se in fly ash materials. However, few studies have attempted to directly correlate these properties to mobilization parameters relevant to disposal and reuse. Instead, the coal residuals industries often rely upon standardized leaching protocols that can be laborious or involve hazardous chemicals. The goals of the project were to: 1) Develop and evaluate a characterization protocol that can be used to screen fly ash samples for leachability of As and Se; 2) Characterize As, Se, and associated constituents of fly ash particles at multiple length scales (nanometer to micrometer) to determine if elemental associations differ as a function of the resolution of characterization; and 3) Establish a predictive model for the chemical composition of coal ash produced annually at major U.S. coal fired power facilities on 50-year national coal supply records. For the first objective, we performed leaching experiments with 52 fly ash samples collected from 15 different U.S. power plants and representing coal feedstocks from the three major domestic coal regions. For this work, we assessed the mobilization potential of As and Se in fly ash based on standardized leaching protocols and performed multivariate and lasso regression analyses to explore correlations of leachable As and Se contents with characteristics such as major element contents, loss on ignition (LOI) and pH. The results of regression models indicated that major elements (Fe, Ca, Al) for a wide range of fly ashes can serve as predictor variables for the leaching potential of As, but not for Se. LOI and pH were not important predictive variables in the models. Both regression approaches resulted in relatively strong fits for leachable As (correlation coefficient R 2 = 0.78 for both models) compared to models for leachable Se (R 2 = 0.49). Overall, these results suggest that correlation models combined with on-site elemental analysis with portable analyzers may enable a screening method for leachable As in coal ash. For the second objective, we utilized nanoscale 2-D imaging (30-50 nm spot size) with the Hard X-ray Nanoprobe (HXN) in combination with microprobe X-ray capabilities (~5 µm resolution) to determine As and Se elemental associations in fly ash particles. Speciation of As and Se was also measured at the nano- to microscale with X-ray absorption spectroscopy. The enhanced resolution of HXN showed As and Se that were diffusely located around or comingled with Ca- and Fe-rich particles. The results also showed nanoparticles of Se attached to the surface of fly ash grains. Overall, a comparison of As and Se species across scales highlights the heterogeneity and complexity of chemical associations for these trace elements of concern in coal fly ash. For the final objective, we developed a predictive model for major element composition of coal ash in reserve at disposal sites of major U.S. coal fired power plants. This model was constructed from coal purchase records of 705 power stations from 1973-2022 and was trained on coal ash composition data showing that coal ash elemental composition is strongly associated with the source of feedstock coal. The model showed regional shifts in the major element contents of ash produced by power plants in the last 50 years, particularly for calcium and iron (expressed as %CaO and %Fe 2 O 3 ), as coal-fired power stations changed their source of coal over this time frame. Our approach enables an estimation of coal ash chemical composition that is stored in waste impoundments at individual power stations. Such information can help delineate the regional market potential for material applications that would utilize coal ash harvested from disposal sites across the U.S.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2023

Early age hydration behavior of portland cement-based binders incorporating fly ash contaminated with flue gas desulfurization products

Fly ash co-mingled with flue gas desulfurization (FGD) products are currently discarded as off-specification materials based on their high SO3 content. However, previous studies have shown that performance of these fly ashes varies significantly based on FGD product type and as such they may be viable for use in low-CO2 concrete as supplementary cementitious materials (SCMs). In this study, fly ashes with three different types of FGD products including calcium sulfite hemihydrate, calcium sulfate (with some unreacted lime), and sodium sulfate (with some unreacted sodium carbonate) were evaluated. The early age hydration behavior in blended cementitious systems at 20% cement replacement level was studied using Vicat setting time tests, isothermal calorimetry, in-situ quantitative X-ray diffraction, and pore solution analysis. The cause of the setting time retardation and flash setting observed in fly ashes with calcium sulfite hemihydrate and sodium carbonate, respectively, were identified and suitable beneficiation options were suggested for the valorized use of these materials in low-CO 2 concrete.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Method for sulfur removal from coal fly ash

A method of reducing sulfur concentration in fly ash, flue gas desulfurization (FGD) ash, and mixtures thereof by contacting the fly ash, FGD ash, or mixtures thereof with an aqueous acidic solution, for a time, at a temperature, and at a liquid-to-solid ratio wherein the sulfur concentration within the fly ash, FGD ash, or mixture thereof is reduced to no more than 5 wt % SO.sub.3 based on the total weight of dry fly ash, FGD ash, or mixture thereof so treated.

Wang, Bu↗
DOE OSTI2022

Evaluation and beneficiation of high sulfur and high alkali fly ashes for use as supplementary cementitious materials in concrete

Coal-fuel power plants with semi-dry or dry flue gas desulfurization (FGD) systems produce high sulfur and/or high alkali fly ashes due to comingling of fly ash with FGD products. Such fly ashes do not meet the SO 3 content limit (5.0% max.) of ASTM C618 or are unable to mitigate the alkali-silica reaction. The mineralogy of the sulfur present in these ashes can vary significantly (e.g., CaSO 4 , CaSO 3 , Na2SO 4 ) based on the FGD technology used and this affects the performance of these fly ashes in concrete. Thus, the single SO 3 % limit of ASTM C618 is unable to capture the complexity and performance of fly ash, and this results in elimination of potentially viable pozzolans for concrete. Here this study performs a systematic investigation of the effect of SO 3 type and content in fly ash on various performance parameters of cement-fly ash pastes and mortars, including workability (flow and flow retention), pore fluid pH, setting time, strength development, and potential for deleterious expansion. To better quantify and understand these effects, the study considers both real and doped fly ashes (i.e., a blend of specification-compliant fly ash with target sulfur compounds). The poor performance observed in the case of setting time and pore fluid pH was successfully mitigated using chemical admixtures.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Distribution of Lanthanides, Yttrium, and Scandium in the Pilot-Scale Beneficiation of Fly Ashes Derived from Eastern Kentucky Coals

In this study, Central Appalachian coal-derived fly ashes from two power plants were beneficiated in a pilot-scale facility in order to produce a product with a relatively consistent concentration of rare earth elements (REE). The <200-mesh final fly ash product was produced by removing the carbon- and Fe-rich particles prior to screening at 200 mesh (75 µm). The Plant D fly ash had high concentrations of CaO and SO3, which were diminished through the two months when the ash was being beneficiated, representing a consequence of the heat, humidity, and excessive rainfall in the Kentucky summer. The high CaO and SO3 concentrations through the early runs likely contributed to the lower REE in the <200-mesh products of those runs. Of the non-REE minor elements, Ba, V, Mn, Zn, and As showed the greatest between-run variations within the runs for each plant. The overall REE concentrations proved to be similar, both on a between-run basis for the individual fly ash sources and on a between-plant basis. Variations in fly ash quality will occur in larger-scale operations, so on-going attention to the fly ash quality and the response of the fly ash to beneficiation is necessary. Changes in the Plant D fly ash with time imply that both the freshness of the original ash and the length and conditions of its storage at the site of beneficiation could be factors in the quality and consistency of the processed fly ash.

58 GEOSCIENCES↗
DOE OSTI2024

ASSESSMENT OF HIGH-VOLUME HARVESTED FLY ASH BLENDS FOR USE IN PRECAST CONSTRUCTION

Declining supplies of fresh fly ashes in some regions have further driven the importance of using harvested fly ash as a supplementary cementitious material and thus replacement for more energy-intensive ordinary Portland cement (OPC). Higher replacement rates of OPC with fly ash in general has traditionally been limited in precast operations due to stringent early-age strength requirements necessitated by initial prestress and lifting/handling of hardened components – often well within 24 hours after fresh concrete placement. Therefore, a series of mix designs were developed, as part of a larger framework for reassessing high-volume fly ash (HVFA) use in the context of precast construction, to demonstrate the feasibility of using larger fractions of harvested fly ash in concrete formulations suitable for precast fabrication demands. More specifically, a target minimum 24-hour compressive strength of 24.1 MPa (3500 psi) was set, in accordance with conventional precast structural design checks, while increasing the fly ash content to 40% replacement of OPC – at least a 15% increase above the traditional limit of 25%. The effect of using more sustainable Type IL cement in contrast to conventional Type III Portland cement (the traditional standard for precast use) – both in conjunction with HVFA use – was also examined. Early-age mechanical properties including compressive strength, modulus of rupture, and modulus of elasticity were evaluated within the aforementioned early-age window. Lastly, corresponding design equations were then reassessed for their applicability with respect to the high-early strength HVFA mixes examined herein.

Gombeda, Matthew J.↗
DOE OSTI2020

Distribution of rare earth elements in fly ash derived from the combustion of Illinois Basin coals

This study examined rare earth element (REE) trends for Illinois Basin coal-sourced fly ashes, with the goal of understanding the elemental composition and resource potential for various fly ash fractions. Illinois Basin coals have a high volatile C through A bituminous rank with a moderate ash content (slightly>12% ash (dry basis)), about 3% sulfur, and, in general, lower concentrations of hazardous and other trace elements than many Central Appalachian coals. Fly ash from the combustion of Illinois Basin coals tends to have a high Fe 2 O 3 content owing to the amount of pyrite in the feed coals. The rare earth element (REE) concentrations in Illinois Basin coal-sourced fly ashes are less than that for fly ashes from the combustion of Central Appalachian coals. The Upper continental crust-corrected fly ashes show an H-type enrichment, a positive Eu N /Eu N * , and, in some cases, a sharp Gd peak. For comparison, a suite of fly ashes from the combustion of a blend of eastern Kentucky coals had an H-type enrichment, a positive Eu N /Eu N * , but only a minimal Gd peak. In contrast, fly ash from the combustion of the Fire Clay coal, a REE-rich coal, had a negative Eu N /Eu N * and a sharp Gd peak. Finally, these results highlight the importance of feed coal composition on trace element contents of respective combustion fly ash fractions and also the unique REE enrichment patterns of the Illinois Basin fly ashes relative to the better studied fly ashes of eastern Kentucky and Central Appalachia.

01 COAL, LIGNITE, AND PEAT↗