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NASA NTRS2024

Inverse Modeling of the Initial Stage of the 1991 Pinatubo Volcanic Cloud Accounting for Radiative Feedback of Volcanic Ash

The way volcanic clouds evolve is very sensitive to the initial spatial 3D distributions of volcanic materials, which are often unknown. In this study, we conducted inverse modeling of the Mt. Pinatubo cloud using TOMS 2D mapping of Aerosol Index and SO 2 loading during the first three post-eruption days to estimate the time-dependent emissions profiles and initial 3D spatial distributions of volcanic ash and SO 2 . We account for aerosol radiative feedback and dynamic lofting of volcanic ash in the inversion calculations for the first time. This resulted in a lower ash injection height (by 1.5 km for ash) than without ash radiative feedback. The Pinatubo eruption ejected ≈77% of fine ash at 12 to 23 km, ≈65% of SO 2 at 18–25 km. In contrast with previous studies, which suggested that all volcanic materials were emitted above the tropopause, a significant fraction of SO 2 (5.1 of 15.5 Mt) and fine ash (37.2 of 66.5 Mt) were ejected in the troposphere, where SO 2 quickly oxidized into sulfate aerosol that is short-lived in the troposphere. This explains the early presence of sulfate aerosols in the plume and why the models can reproduce the observed volcanic aerosols' optical depth (AOD), assuming lower-than-observed SO 2 emission in the stratosphere. Despite the quicker than in observations build-up of sulfate AOD, in a month after the eruption, the evolution of the Pinatubo AOD simulated using the obtained ash and SO 2 initial distributions converges with the available stratospheric aerosol and gas experiment (SAGE) observations.

Pinatubo volcanic ash and SO2 emissions↗

DOE OSTI2014

Assessing ecological risks to the fish community from residual coal fly ash in Watts Bar Reservoir, Tennessee

For this research, extensive site-specific biological and environmental data were collected to support an evaluation of risks to the fish community in Watts Bar Reservoir from residual ash from the December 2008 Tennessee Valley Authority (TVA) Kingston ash release. This paper describes the approach used and results of the risk assessment for the fish community, which consists of multiple measurement endpoints (measures of exposure and effects) for fish. The lines of evidence included 1) comparing postspill annual fish community assessments with nearby prespill data and data from other TVA reservoirs, 2) evaluating possible effects of exposures of fish eggs and larval fish to ash in controlled laboratory toxicity tests, 3) evaluating reproductive competence of field-exposed fish, 4) assessing individual fish health through physical examination, histopathology, and blood chemistry, 5) comparing fish tissue concentrations with literature-based critical body residues, and 6) comparing concentrations of ash-related contaminants in surface waters with US Environmental Protection Agency's (USEPA) Ambient Water Quality Standards for Fish and Aquatic Life. These measurement endpoints were treated as independent lines of evidence that were integrated into an overall weight-of-evidence estimate of risk to the fish community. Collectively, the data and analysis presented here indicate that ash and ash-related constituents pose negligible risks to the fish communities in Watts Bar Reservoir. This conclusion contradicts the predictions by some researchers immediately following the ash release of devastating effects on the aquatic ecology of Watts Bar Reservoir. The information presented in this article reaffirms the wisdom of carefully evaluating the evidence before predicting probable ecological effects of a major event such as the TVA Kingston ash release. Lastly, this study demonstrates that a thorough and detailed investigation using multiple measurement endpoints is needed to properly evaluate ecological effects.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2011

The effect of oxygen-to-fuel stoichiometry on coal ash fine-fragmentation mode formation mechanisms.

Ash particles smaller than 2.5 {micro}m in diameter generated during pulverized coal combustion are difficult to capture and may pose greater harm to the environment and human health than the discharge of larger particles. Recent research efforts on coal ash formation have revealed a middle fine-fragment mode centered around 2 {micro}m. Formation of this middle or fine-fragment mode (FFM) is less well understood compared to larger coarse and smaller ultrafine ash. This study is part of an overall effort aimed at determining the key factors that impact the formation of FFM. This work examined the effects of oxygen-to-fuel stoichiometry (OFS). Pulverized Illinois No.6 bituminous coal was combusted and the ash generated was size segregated in a Dekati low pressure inertial impactor. The mass of each fraction was measured and the ash was analyzed using scanning electron microscopy (SEM) and X-ray microanalysis. The FFM ash types were classified based on the SEM images to evaluate the significant fine-fragment ash formation mechanisms and determine any possible link between stoichiometry and formation mechanism. From the particle size distributions (PSDs), the coarse mode appears unaffected by the change in OFS, however, the OFS 1.05 lowered the fraction of ultrafine ash in relation to the higher OFS settings, and appears to increase the portion of the FFM. An intermediate minimum was found in the FFM at 1.3 {micro}m for the 1.20 and 1.35 OFS tests but was not observed in the 1.05 OFS. SEM analysis also suggests that OFS may contribute to changing formation mechanisms.

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2022

Leaching of lanthanide and yttrium from a Central Appalachian coal and the ashes obtained at 550–950 °C

Here in this work, we investigated leaching of lanthanide and yttrium (REY) from a Central Appalachian coal and its ashes obtained at 550–950 °C with the main purpose of understanding the impact of ashing temperature on REY leachability in water, ammonium sulfate, and hydrochloric acid. It is found that the coal contains a negligible amount of water-soluble REY, less than 1% ion-exchangeable REY, and about 28% of HCl-soluble REY. Ashing leads to dramatic changes in REY leachability in both ammonium sulfate and hydrochloric acid solutions, which is believed to be related to transformation and redistribution of organically-associated REY in coal during the ashing process. Ashing temperature significantly affects REY leaching from coal ashes; higher ashing temperature results in lower REY leachability in both solutions. Clay minerals may play a significant role in changing the leachability of REY after ashing. In addition, the results also suggest that the organic matter in the coal is relatively enriched in heavy REY.

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2020

Persisting volcanic ash particles impact stratospheric SO 2 lifetime and aerosol optical properties

Volcanic ash is often neglected in climate simulations because ash particles are assumed to have a short atmospheric lifetime, and to not participate in sulfur chemistry. After the Mt. Kelut eruption in 2014, stratospheric ash-rich aerosols were observed for months. Here we show that the persistence of super-micron ash is consistent with a density near 0.5 g cm -3 , close to pumice. Ash-rich particles dominate the volcanic cloud optical properties for the first 60 days. We also find that the initial SO 2 lifetime is determined by SO 2 uptake on ash, rather than by reaction with OH as commonly assumed. About 43% more volcanic sulfur is removed from the stratosphere in 2 months with the SO 2 heterogeneous chemistry on ash particles than without. This research suggests the need for re-evaluation of factors controlling SO 2 lifetime in climate model simulations, and of the impact of volcanic ash on stratospheric chemistry and radiation.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2012

Chemical Imaging Analysis of Environmental Particles Using the Focused Ion Beam/Scanning Electron Microscopy Technique. Microanalysis Insights into Atmospheric Chemistry of Fly Ash

Airborne fly ash from coal combustion may represent a source of bioavailable iron (Fe) in the open ocean. However, few studies have been made focusing on Fe speciation and distribution in coal fly ash. In this study, chemical imaging of fly ash has been performed using a dual-beam FIB/SEM (focused ion beam/scanning electron microscope) system for a better understanding of how simulated atmospheric processing modify the morphology, chemical compositions and element distributions of individual particles. A novel approach has been applied for cross-sectioning of fly ash specimen with a FIB in order to explore element distribution within the interior of individual particles. Our results indicate that simulated atmospheric processing causes disintegration of aluminosilicate glass, a dominant material in fly ash particles. Aluminosilicate-phase Fe in the inner core of fly ash particles is more easily mobilized compared with oxide-phase Fe present as surface aggregates on fly ash spheres. Fe release behavior depends strongly on Fe speciation in aerosol particles. The approach for preparation of cross-sectioned specimen described here opens new opportunities for particle microanalysis, particular with respect to inorganic refractive materials like fly ash and mineral dust.

Environmental Molecular Sciences Laboratory↗

DOE OSTI2024

Ash Fouling Free Regenerative Air Preheater for Deep Cyclic Operation

The University of Kentucky (UKy) project titled “Ash Fouling Free Regenerative Air Preheater for Deep Cyclic Operation”, DE-FE0031757, was conducted from 8/15/2019 to 8/14/2024 in two Budget Periods. Other participants included PPL Corporation and Black Dragon Double Boiler. The overall goal was to investigate the proposed self-cleaning technology to achieve ash fouling free air preheater operation in a coal-fired power plant, especially during deep cycling. All project deliverables, milestones, and success criteria were met. UKy obtained the following scientific findings. • Temporary and periodic high temperature of heating elements (450 ~ 500 °F) can prevent ash accumulation and maintain air preheater free of clogging. • The ash samples analysis and unit operation provide solid evidence of ABS formed during low load with SCR ammonia slip being the major cause of ash accumulation, and air preheater clogging can be prevented by raising the heating element temperature up to 450 °F~ 500 °F at which ABS is decomposed. • In-situ self-cleaning can be controlled by monitoring temperature and/or presetting fixed number of cleanings per day. Both approaches in pilot testing show positive results for maintaining an ash free state for the air preheater. • Temperature criteria (cold end or gas outlet temperature) for entering self-cleaning service is critical to balance the number of cleaning cycles with maintaining the ash level. • Temperature criteria (cold end or gas outlet temperature) for exiting self-cleaning service is critical to balance the duration of the cleaning cycles with maintaining the ash level.

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2023

Measurements and Prediction of Ash Deposition in a Cyclone-Fired Boiler Operating under Variable Load Conditions

Measurements of ash deposition rates were made between the secondary superheater and reheater sections of a 450 MW cyclone-fired lignite boiler as the operational load varied from 33 to 100%. Significant reductions in deposition rates with a decrease in operational load were observed. To uncover the causative mechanisms behind these observations, operational data from the power plant were used to carry out computational fluid dynamic (CFD) simulations of the boiler. After ascertaining that the gas temperatures and velocities at various sections within the boiler were being represented adequately, decoupled simulations of the ash deposition process on the deposit probe were carried out using a finely resolved boundary layer mesh. Fly ash particle size distribution (PSD) and its concentration for the decoupled calculations were determined from stand-alone cyclone barrel simulations. The ash partitioning (mass %) between the fly ash and slag was found to be ~50:50, which was in line with previous field observations, and it did not vary significantly across different cyclone loads. The predicted PSD of the deposit ash was concentrated in the size range 10–30 microns, which was in agreement with cross-sectional images of the deposit obtained from the measurements. At lower loads, sharp variations in the deposition rates were predicted in the gas temperature range 950–1150 K. The particle kinetic energy—particle viscosity-based capture methodology utilized in this study in conjunction with appropriate ash compositions, ash viscosity models and gas temperature estimates can help estimate slagging propensities at different loads reasonably well in these systems.

Krishnamoorthy, Gautham (ORCID:0000000255205092)↗

NASA NTRS1989

Energy efficient continuous flow ash lockhopper

The invention relates to an energy efficient continuous flow ash lockhopper, or other lockhopper for reactor product or byproduct. The invention includes an ash hopper at the outlet of a high temperature, high pressure reactor vessel containing heated high pressure gas, a fluidics control chamber having an input port connected to the ash hopper's output port and an output port connected to the input port of a pressure letdown means, and a control fluid supply for regulating the pressure in the control chamber to be equal to or greater than the internal gas pressure of the reactor vessel, whereby the reactor gas is contained while ash is permitted to continuously flow from the ash hopper's output port, impelled by gravity. The main novelty resides in the use of a control chamber to so control pressure under the lockhopper that gases will not exit from the reactor vessel, and to also regulate the ash flow rate. There is also novelty in the design of the ash lockhopper shown in two figures. The novelty there is the use of annular passages of progressively greater diameter, and rotating the center parts on a shaft, with the center part of each slightly offset from adjacent ones to better assure ash flow through the opening.

Collins, Earl R., Jr.↗

NASA NTRS2013

Multi-Partner Experiment to Test Volcanic-Ash Ingestion by a Jet Engine

A research team of U.S. Government agencies and engine manufacturers are designing an experiment to test volcanic-ash ingestion by a NASA owned F117 engine that was donated by the U.S. Air Force. The experiment is being conducted under the auspices of NASA s Vehicle Integrated Propulsion Research (VIPR) Program and will take place in early 2014 at Edwards AFB in California as an on-ground, on-wing test. The primary objectives are to determine the effect on the engine of several hours of exposure to low to moderate ash concentrations, currently proposed at 1 and 10 mg/m3 and to evaluate the capability of engine health management technologies for detecting these effects. A natural volcanic ash will be used that is representative of distal ash clouds many 100's to approximately 1000 km from a volcanic source i.e., the ash should be composed of fresh glassy particles a few tens of microns in size. The glassy ash particles are expected to soften and become less viscous when exposed to the high temperatures of the combustion chamber, then stick to the nozzle guide vanes of the high-pressure turbine. Numerous observations and measurements of the engine s performance and degradation will be made during the course of the experiment, including borescope and tear-down inspections. While not intended to be sufficient for rigorous certification of engine performance when ash is ingested, the experiment should provide useful information to aircraft manufacturers, airline operators, and military and civil regulators in their efforts to evaluate the range of risks that ash hazards pose to aviation.

Lekki, John↗

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 OSTI2017

Two-Step Procedure of Fly Ash Modification as an Alternative Method for Creation of Functional Composite

An appropriate filler is a key component required to achieve an useful composite with expected properties. Not only sophisticated types of filler, like graphene are popular, but also more common ones, like silica flour or fly ash because of their low costs. Besides production costs, adequate size and possibility of functionalization of particles surface to create stable bonds with a matrix are essential in filler selection. To create an useful filler for epoxy resin based composites with use of a waste material, namely fly ash, two-step procedure was proposed. In the first part, raw material was sieved and five different ranges of the filler size were obtained. After mechanical tests with fracture toughness, tensile strength and Young Modulus, as well thermal conductivity, the best size of the fly ash was chosen for further modification. During the second step, filler was modified with coupling agent [3-(2-aminoethylamino)propyl]trimethoxysilane in order to enhance the coupling between particular components of composite. Presence of the silane layer was confirmed with infrared spectroscopy and scanning electron microscopy measurements, whilst prepared epoxy composite filled with silanized fly ash was examined similarly as previous composites. Obtained results have proved the significant influence of size of a filler and bonding to the matrix on mechanical and thermal properties of fly ash-epoxy resin composite. Proposed simple method of fly ash modification is an environmentally friendly way for utilization of the fly ash. Moreover, it creates an alternative material applicable in electrical devices as functional composite.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Characterization of morphology and hydration products of high-volume fly ash paste by monochromatic scanning x-ray micro-diffraction (μ-SXRD)

The present study focuses on identification and micro-structural characterization of the hydration products formed in high-volume fly ash (HVFA)/portland cement (PC) systems using monochromatic scanning x-ray micro-diffraction (μ-SXRD) and SEM-EDS. Pastes with up to 80% fly ash replacement were studied. Phase maps for HVFA samples using μ-SXRD patterns prove that μ-SXRD is an effective method to identify and visualize the distribution of phases in the matrix. μ-SXRD and SEM-EDS analysis shows that the C-S-H formed in HVFA system containing 50% or more of fly ash has a similar structure as C-S-H(I) with comparatively lower Ca/Si ratio than the one produced in PC system. Moreover, coexistence of C-S-H(I) and strätlingite is observed in the system containing 80% of fly ash, confirming that the amount of alumina and silicate phases provided by the fly ash is a major factor for the formation of C-S-H(I) and strätlingite in HVFA system. - Highlights: • High-volume fly ash (HVFA) paste was studied by scanning x-ray micro-diffraction. • Coexistence of C-S-H(I) and strätlingite in the HVFA system is clearly shown. • The distribution of minor phases in the HVFA system is shown. • Differences between inner and outer products of fly ash are observed by SEM-EDS.

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

Enhancing phase identification in waste-to-energy fly ashes: Role of Raman spectroscopy, background fluorescence, and photobleaching

Waste-to-Energy (WTE) facilities incinerate ~11% (~ 222 Mt) of global solid waste, generating bottom and fly ashes. Landfilling these ashes is costly, and risks releasing contaminants into the environment. Instead, using WTE ashes in secondary industrial applications can circumvent such environmental risks. However, their secondary use is restricted by their inconsistent mineralogy, which may vary due to fluctuating waste composition and combustion conditions. Therefore, there is a need for rapid and reliable monitoring of WTE fly ash mineralogy. Here, we evaluate the employment of Raman spectroscopy for that purpose. Our initial investigation of 12 unique WTE fly ashes resulted in excessive fluorescence, rendering key Raman peaks obscure. To address this issue, we report that a mere 2 minutes of photobleaching can significantly reduce this fluorescence, facilitating the detection of calcite, calcium sulfate, zincite, and carbon – phases previously undetectable in original spectra. Furthermore, these results show the potential of Raman spectroscopy for rapid monitoring of WTE fly ash mineralogy, which could be beneficial in diverting these ashes from landfill.

36 MATERIALS SCIENCE↗

DOE OSTI2013

Thermal and hydrometallurgical recovery methods of heavy metals from municipal solid waste fly ash

Highlights: • MSW fly ash was thermally and hydrometallurgically treated to remove heavy metals. • More than 90% of easy volatile heavy metals (Cd and Pb) were removed thermally. • More than 90% of Cd, Cr, Cu an Zn were removed by alkaline – acid leaching. • The best results were obtained for the solution of 3 M NaOH and 2 M H{sub 2}SO{sub 4}. - Abstract: Heavy metals in fly ash from municipal solid waste incinerators are present in high concentrations. Therefore fly ash must be treated as a hazardous material. On the other hand, it may be a potential source of heavy metals. Zinc, lead, cadmium, and copper can be relatively easily removed during the thermal treatment of fly ash, e.g. in the form of chlorides. In return, wet extraction methods could provide promising results for these elements including chromium and nickel. The aim of this study was to investigate and compare thermal and hydrometallurgical treatment of municipal solid waste fly ash. Thermal treatment of fly ash was performed in a rotary reactor at temperatures between 950 and 1050 °C and in a muffle oven at temperatures from 500 to 1200 °C. The removal more than 90% was reached by easy volatile heavy metals such as cadmium and lead and also by copper, however at higher temperature in the muffle oven. The alkaline (sodium hydroxide) and acid (sulphuric acid) leaching of the fly ash was carried out while the influence of temperature, time, concentration, and liquid/solid ratio were investigated. The combination of alkaline-acidic leaching enhanced the removal of, namely, zinc, chromium and nickel.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2022

Fine Ash-Bearing Particles as a Major Aerosol Component in Biomass Burning Smoke

Biomass burning (BB) events are occurring globally with increasing frequency, and their emissions are having more impacts on human health and climate. Large ash particles are recognized as a BB product with major influences on soil and water environments. However, fine-ash particles, which have diameters smaller than several microns and characteristic morphologies and compositions (mainly Ca and Mg carbonates), have not yet been explicitly considered as a major BB aerosol component either in field observations or climate models. This study measured BB aerosol samples using transmission electron microscopy (TEM) and ion chromatography during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign. We show that significant amounts of fine ash-bearing particles are transported >100 km from their fire sources. Our environmental chamber experiments suggest that they can act as cloud condensation and ice nuclei. We also found considerable amounts of fine ash-bearing particles in the TEM samples collected during previous campaigns (Biomass Burning Observation Project and Megacity Initiative: Local and Global Research Observations). These ash particles are commonly mixed with organic matter and make up ~8% and 5% of BB smoke by number and mass, respectively, in samples collected during the FIREX-AQ campaign. The measured ash-mass concentrations are approximately five times and six times greater than those of BB black carbon and potassium, respectively, scaling to an estimated global emission of 11.6 Tg yr -1 with a range of 8.8–16.3 Tg yr -1 . Better characterization and constraints on these fine ash-bearing particles will improve BB aerosol measurements and strengthen assessments of BB impacts on human health and climate.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2012

Fish Health Studies Associated with the Kingston Fly Ash Spill, Spring 2009 – Fall 2010

On December 22, 2008, over 4 million cubic meters of fly ash slurry was released into the Emory River when a dike surrounding a solid waste containment area at the Tennessee Valley Authority's (TVA) Kingston Fossil Plant ruptured. One component of TVA's response to the spill is a biological monitoring program to assess short- and long-term ecological responses to the ash and associated chemicals, including studies on fish health and contaminant bioaccumulation. These studies were initiated in early Spring 2009 for the purposes of: (1) documenting the levels of fly ash-associated metals in various tissues of representative sentinel fish species in the area of the fly ash spill, (2) determining if exposure to fly ash-associated metals causes short, intermediate, or long-term health effects on these sentinel fish species, (3) assessing if there are causal relationships between exposure to metals and health effects on fish, (4) evaluating, along with information from other ecological and physicochemical studies, the nature and route of contaminant transfer though food chains into higher level consumers, (5) providing important information for the Ecological Risk Assessment (ERA) for the Kingston fly ash project, and (6) serving as an important technology information transfer or model study focused on how to best evaluate the environmental effects of fly ash (and related environmental stressors), not only at the Kingston site, but also at sites on other aquatic systems where coal-fired generating stations are located. This report presents the results of the first two years of the fish health study. To date, fish health and bioaccumulation studies have been conducted from Spring 2009 though Fall 2011 and includes 6 seasonal studies: Spring 2009, Fall 2009, Spring 2010, Fall 2010, Spring 2011, and Fall 2011. Both the Spring and Fall studies have focused on 3-4 sentinel fish species that represent different feeding habits, behaviors, and home ranges. In addition to fish health and bioaccumulation, the Spring investigations also included reproductive integrity studies on the same fish used for bioaccumulation and fish health. In this report, results of the fish health studies from Spring 2009 through Fall 2010 are presented while an associated report will present the fish reproductive studies conducted during Spring 2009 and Spring 2010. A report on fish bioaccumulation was submitted to TVA in June 2011. The fish health study conducted in conjunction with the bioaccumulation and reproductive study is critical for assessing and evaluating possible causal relationships between contaminant exposure (bioaccumulation) and the response of fish to exposure as reflected by the various measurements of fish health.

20 FOSSIL-FUELED POWER PLANTS↗