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NASA NTRSDate not supplied

22 N HPGP Thruster Life Testing

In the ever-changing paradigm of efficient and capable spacecraft design, scientific missions continue pushing the envelope enabling spacecraft subsystems to deliver effective solutions to meet challenging new mission/spacecraft needs. From an in-space storable liquid chemical propulsion perspective, monopropellant hydrazine has been, and continues to be, a dependable propellant with considerable flight heritage, a variety of engine thrust classes available from multiple vendors, with repeatable and reliable performance. Additionally, the space propulsion industry has learned to successfully handle hydrazine, its regulations, the safety protocols, the personnel protective equipment, and the unique training standards–all requisite for loading spacecraft propulsion systems with toxic hypergolic hydrazine. The question now arises as to “what is next for in-space chemical propulsion?” Further, with the evolution and concrete advancements in innovative in-space green propellant technologies, capable of providing realizable benefits to scientific missions, concern over the reliability and availability of this higher performing and safer to handle class of propellants is waning. As science missions move forward with the potential flight in fusion of High Performance Green Propulsion (HPGP), NASA and its industry partners are working to address any gaps in system reliability, performance, or unique operational considerations. Propellant technology that offers both higher performance and significant reduction in personnel hazards compared to hydrazine presents an attractive propulsion subsystem design opportunity. Increased propulsion subsystem performance can result in lower spacecraft launch mass, larger scientific payloads, or extended on-orbit lifetimes. Mission trades using green propulsion technologies have been documented on multiple NASA Goddard Space Flight Center (GSFC) mission classes, examining various parameters and requirements to support mission architectures in Low Earth Orbit (LEO), High Earth Orbit (HEO), geostationary, lunar, planetary, and Quasi-halo orbit around Sun-Earth Lagrange point (L2). The results of these trade studies show promising, attainable benefits. The perceived programmatic risk of flying a newer propulsion technology has, unfortunately, not outweighed the benefits to date. To take advantage of the improved performance and mitigate programmatic risk, HPGP engines must demonstrate life testing at higher propellant throughputs than have currently been demonstrated. In an effort to proactively address the challenges with technology infusion into a risk-averse community, NASA and the Swedish National Space Agency (SNSA) outlined a collaborative Implementing Arrangement (IA) for the respective agencies to pursue increased HPGP technology maturation. This initial IA effort began in 2013, fresh off the heels of the successful PRISMA HPGP technology demonstration mission. The IA targeted objective is to reduce risk to potential future HPGP missions and fully characterize the LMP-103S propellant and associated engine performance. Over the past eight years, HPGP has flown in propulsion systems on twenty-five(25) spacecraft from seven(7) different Launch Ranges around the globe and on seven (7) different Launch Vehicles. Six(6) of these launches involved multiple loading operations for multiple spacecraft. For U.S. Range operations, nine (9) HPGP systems have been processed at Vandenberg Space Force Base(VSFB):six(6) in 2017, and three (3) in 2018. Six (6) more have been processed at Cape Canaveral Air Force Station (CCAFS)in May 2020, with three (3) systems launched in June 2020 and the remaining three (3) system were left loaded and ready until their launch in August of 2020. Three (3) more systems have been processed at Wallops Flight Facility(WFF)and launched in June 2021. In addition, these propulsion subsystems employed heritage propulsion subsystem component such as valves, filters, and pressure transducers, and have further demonstrated nominal functionality in both diaphragm and Propellant Management Device (PDM) propellant tanks. Based on these successes, HPGP technology continues to be considered for NASA Science Mission Directorate missions at GSFC. The work presented herein represents many years of development and collaborative efforts to successfully align higher performance, low toxicity hydrazine alternatives into scientific missions. NASA GSFC Propulsion Engineering, in collaboration with Bradford ECAPS, has developed mission specific thruster design and testing requirements to establish GSFC’s desired test conditions and firing sequences.In2017, the first flight-like 22N HPGP thruster Engineering Qualification Model (EQM-1)was designed and built by Bradford ECAPS to prove out the thruster design, materials, build process, and test campaign with respect to NASA GSFC critical component and mission requirements. This test program was developed to comprehensively test the thruster, the technology, and ultimately increase the 22N HPGP Technology Readiness Level(TRL). EQM-1was tested to environmental qualification levels prior to hot fire performance testing to represent the relevant end-to-end environment (launch to on-orbit operation)with required margin. This thruster demonstrated steady-state and pulse mode operational capability with propellant thruster throughput up to~53kg.At this throughput level, the EQM-1 engine began to present off-nominal performance and the test campaign was halted to allow for non-destructive testing and identify the root cause for the an omalous performance. Capitalizing on the successful elements of the EQM-1 campaign, an upgraded 22N HPGP EQM-2 has been manufactured by Bradford ECAPS to meet the complete GSFC requirements. The EQM-2 thruster’s test campaign has further demonstrated the robustness of the HPGP propulsion technology and increased the Technology Readiness Level (TRL) by undergoing a full acceptance test program, then proceeding into qualification, including environmental testing (vibration and shock to qualification levels),as well as hot-fire life testing, operating at steady-state and pulse modes with increased propellant thruster throughput to~150kg. The HPGP thruster performance testing enables effective HPGP thruster readiness evaluation to meet NASA candidate mission requirements in the future.

High↗
NASA NTRSDate not supplied

Design, Analysis, Testing, and Flight Activities for A Green Propulsion Dual Mode (Gpdm) Technology Demonstration Mission

NASA’s Strategic Plan (2022) outlines specific technology development objectives which direct the Agency to “innovate and advance transformational space technologies.” An example of these potentially high-impact space technologies is the low-toxicity or “green” rocket propellant known as ASCENT (or Advanced Spacecraft Energetic Non-Toxic Propellant). Developed in the 2010’s by the Air Force Research Lab (AFRL), ASCENT (formerly AF-315E) has shown improved specific impulse density (50% higher) vs. hydrazine in addition to its favorable in-space storability and ease of handling capability. The chemical propulsion capability of ASCENT has been demonstrated on several missions including the Green Propulsion Infusion Mission (GPIM) in 2019 and most recently, the Lunar Flashlight mission. ASCENT is an ionic liquid, which lends itself as both a chemical and an electrospray propellant. The capability to use the same propellants in multiple modes using the same propellant tank and feed system has yet to be demonstrated in orbit. This capability, if proven successful has the potential to reduce system weight and complexity, while taking advantage of both high thrust and high propellant efficiency in electrospray mode. The GPDM Project, managed by the Marshall Space Flight Center is seeking to develop a dual-mode propulsion system as the payload on a small spacecraft (6U CubeSat) and subsequent in-space demonstration. This paper will summarize the concept, ground testing as well as mission operations plan for demonstrating green “dual-mode” propulsion.

Nehemiah J. Williams↗
NASA NTRSDate not supplied

A Green Propulsion Dual Mode (GPDM) In-Space Technology Demonstration on a 6U CubeSat

Over the past decade there has been an increase in the launch and operations of small spacecraft. Small spacecraft (defined as having a total vehicle mass of < 180 kg) provide an opportunity for low-cost, high impact technology demonstrations on a small scale. They also create opportunities for government, industry, and academic to engage, transfer knowledge, and extend partnerships with non-traditional partners. NASA’s Marshall Space Flight Center (MSFC) is leading a collaborative effort to demonstrate a dual-mode (chemical and electrospray) propulsion system using a common propellant system as a payload on a 6U CubeSat. The novel feature in the propulsion system is the interfacing of propulsion technologies requiring dramatically different operating conditions and support hardware. GPDM will use a low toxicity or “green” propellant known as Advanced Spacecraft Energetic Non-Toxic (ASCENT) to demonstrate using a chemical thruster for translation burns and electrospray propulsion for both attitude control and translational burns on the spacecraft. Specific mission activities could include demonstration of collision avoidance during frequent altitude adjustment maneuvers to validate thruster performance and managing extended duration thruster burns of at least 24 hours with limited vehicle contact times. This paper will summarize the ground testing, spacecraft development, mission objectives, and mission planning activities to achieve some of GPDM’s technical objectives.

Nehemiah Joel Williams↗
NASA NTRS2025

Potential Health Impacts, Treatments, and Countermeasures of Martian Dust on Future Human Space Exploration

The challenges of human space exploration produce some of humanity’s greatest technological and scientific advances, not excluding innovations in medicine. The microgravity environment causes a whole host of physiological changes, and exposure to dust on the Moon caused considerable pulmonary distress to astronauts during the Apollo missions. As the National Aeronautics and Space Administration (NASA)and other space organizations prepare for long duration exploration missions to Mars, the hazards and consequences of the Martian surface need to be accounted for. This review investigates how substances analogous to the hazardous components of Martian dust have caused disease in people on Earth. Because of the small grain size of Martian dust, dust on Mars is more likely to cause lung irritation, absorb into the bloodstream, and lead to diseases in astronauts. Toxic components of Martian dust to astronaut health include perchlorates, silica, nanophase iron oxides, and gypsum in addition to trace amounts of toxic metals whose abundances are debated: chromium, beryllium, arsenic, and cadmium. Predicted effects of dust exposure ranges from asymptomatic to life threatening, with many substances being carcinogenic and most damage impacting the pulmonary system. The longer transit time for astronauts to return home makes the operations of performing emergency medical treatment more difficult and increases both the likelihood and consequences of developing chronic disease. Exposure mitigation needs to be prioritized; however, supplements may be taken to prevent disease from breakthrough exposures and treatment regimens could lessen morbidity and mortality. Treatments and equipment need to be carefully thought out and transported with the astronauts to be prepared for all possible scenarios.

Justin L Wang↗
DOE OSTI2020

Homopiperazine-based catalysts for neutralization of organophosphorus-based compounds

Novel compositions of matter based on homopiperazine precursor materials and forming a homopiperazine-based ligand are disclosed, along with suitable techniques and materials for the synthesis and utilization thereof. In particular various synthetic schemes and techniques for applying the disclosed compositions of matter as a decontaminating agent. The decontaminating agents include homopiperazine-based ligand-metal complexes that are particularly effective at neutralizing toxicity of nerve agents, pesticides, and other toxic organophosphorus-based compounds. In preferred approaches, the homopiperazine-based ligand-metal complexes act as catalysts to facilitate substitution of a leaving group of the organophosphorus-based compound with a functional group that does not permit the organophosphorus-based compound to inactivate acetylcholinesterase upon introduction of the organophosphorus-based compound to a living organism such as insects and mammals. Advantageously, the catalytic homopiperazine-based ligand-metal complexes are formed using inexpensive, readily-available precursor materials, and may be utilized to neutralize toxins without relying on damaging caustic reactants or environmentally unfriendly organic solvents.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Biocatalysts for conversion of thermochemical waste streams

Disclosed herein are microorganisms that have enhanced tolerance to toxic compounds found in thermochemical waste streams. Methods of utilizing carbon found in waste streams are also disclosed. Also presented herein are methods for detoxifying waste streams and methods of bioconversion of toxic waste stream materials into useful products.

Jayakody, Thelhawadigedara Lahiru Niroshan↗
DOE OSTI2021

BETO 2021 Peer Review - Cell Free and Immobilization Technologies (CFIT)

Today, several key factors negatively impact the production of fuels and chemicals from renewable sources. Common hindrances in the biological production of biochemicals are: (1) end-product or intermediate toxicity to the microbial biocatalyst, (2) the diversion of carbon to biomass formation, and (3) co-production of undesired byproducts. A particularly attractive alternative is to eliminate the biocatalyst entirely and instead operate the desired metabolic pathways in isolation, thus circumventing the roadblocks of biological toxicity, lower yields, and lack of specificity. However, cell-free enzyme systems still suffer from low productivities owing in part to the effects of free diffusion of intermediates, lack of long term enzyme stability, cofactor cost or inefficient recycling rates, and finally, the cost of enzyme production/purification. This project represents a new effort to propose innovative and cost competitive routes to producing biochemicals from a variety of feedstocks using cell free approaches. These routes will help reduce the current risk and cost associated with classical cell free production. Cell free technologies show promise for application to the production of toxic/inhibitory products or products difficult to separate from microbial growth media and can help reduce the production barriers in multiple areas of biological conversion of feedstocks to biochemicals.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2020

Chapter 22 - Chlorine. In: “Handbook of Toxicology of Chemical Warfare Agents, Third Edition”, Editor: Ramesh C. Gupta.

Chlorine gas is used widely by industry and as a disinfectant and bleach, and, due to its toxicity and ease of procurement, has been used as a chemical warfare agent. Chlorine is a strong oxidizer that hydrolyzes in water to form hydrochloric and hypochlorous acid. Upon chlorine inhalation, the respiratory tract is the predominant target organ in humans and animals as chlorine is a contact irritant. Exposure causes sensory irritation and pulmonary dysfunction, and at sufficiently high concentrations results in lung lesions and injury to other internal organs including the heart. Human and animal studies have shown that chlorine toxicity is influenced more by exposure concentration than duration, is gender-independent, and increases with age, cigarette smoking, and preexisting respiratory conditions such as asthma and airway hyperreactivity. Treatment is largely supportive, although animal studies are examining the utility of various compounds for chlorine-specific treatment based on its mechanism of action.

Milanez, Sylvia↗
DOE OSTI2021

Environmentally-Friendly Fixatives with Embedded Intelligence for Dust Management at Contaminated Sites – 21266

Wind or rain can potentially spread loose hazardous contaminants from piles of rubble and soil waiting to be trucked to a landfill site for disposal. Water, which is plentiful near remediation sites, is the traditional dust suppressant during demolition, post-demolition sizing and encapsulation as well as soil trucking activities. However, water can mobilize the toxic metal contaminants in the soil into the ground water. Ground water is highly regulated and contaminant removal is costly. InnoSense LLC (ISL) is developing DustSafe™ as a cost-effective alternative to water for various decontamination & decommissioning (D&D) applications. It is a sprayable dust abatement solution designed to actively trap, remediate, and aid in visualizing hazardous materials while preventing their dispersion by wind, water or impact. Aside from application as a dust suppressant to trap airborne toxic and radiological hazards during demolition activities, with customization DustSafe can be used to locate/characterize and remediate hazards prior to D&D activities.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Bioconversion of Thermochemical Intermediates

Thermochemical (TC) biofuels production via both pyrolysis and hydrothermal liquefaction produces aqueous waste streams, typically with organic compounds at concentrations of -50-100 g/L. These streams represent a wastewater treatment cost and carbon loss for the TC biorefinery, but the concentration range for these compounds is ideal for bioconversion. To that end, the Bioconversion of Thermochemical Intermediates (BTI) project is developing advanced analytics and engineered microbes to convert these waste streams to co-products, with the overall aim of improving the economics and carbon conversion efficiency of TC biorefining. To date, we have primarily focused on development of advanced analytical chemistry approaches to fully characterize TC aqueous streams and engineering of Pseudomonas putida for conversion of non-conventional substrates, including methylated phenolics, cyclic ketones, furans, and C1-C3 light oxygenates, into atom-efficient products. Two primary challenges are the rapid deployment of aqueous-compatible analytics to changing upstream conditions and dealing with the toxicity of the feed streams to engineered microbes. The project efforts have resulted in engineered strains of P. putida able to consume 90% of the organic compounds in aqueous waste streams from catalytic fast pyrolysis, more than 300-fold toxicity tolerance improvements in P. putida, and carbon closures exceeding 90% for TC wastewater streams across multiple processing technologies.

BASIC BIOLOGICAL SCIENCES,BIOMASS FUELS↗
DOE OSTI2022

Biological Lignin Valorization

Given lignin's heterogeneity, catalytic depolymerization results in aromatic compound mixtures, and conversion of this complex substrate to a single product is challenging. To that end, the Biological Lignin Valorization (BLV) project is pursuing biological funneling, wherein aromatic catabolic microbes are engineered to convert a mixture of lignin-derived compounds to a single product. Namely, we employ Pseudomonas putida and pursue atom-efficient products, such as muconic acid, which can be further converted to direct replacements or used in performance-advantaged bioproducts. Overall, biological lignin conversion can make major contributions to reduce the minimum fuel selling price of the integrated biorefinery. Early industrial efforts in this area are also leading to value-added products, including in collaboration with the BLV project. Primary challenges associated with BLV efforts include accessing bio-available monomers from lignin (with the Lignin Utilization project), enabling commercial titers, rates, and yields of bioproducts from lignin-derived compounds, and overcoming substrate and product toxicity. To date, we have 1) demonstrated 49 g/L of muconate from aromatic compounds and 4 g/L of muconate from lignin, 2) improved the toxicity tolerance of P. putida to key aromatic substrates, 3) debottlenecked biological funneling for higher rates, and 4) engineered P. putida to convert S, G, and H-type lignin-derived compounds to a single product.

BIOMASS FUELS,INORGANIC, ORGANIC, PHYSICAL, AND AN↗
DOE OSTI2023

Functional Predictor Variables for the Leaching Potential of Arsenic and Selenium from Coal Fly Ash

The release of leachates from intact coal ash impoundments is a concern due to the enrichment and mobilization of toxic elements such as arsenic (As) and selenium (Se). This study aims to explore the intrinsic properties of coal fly ash that correlate with the relative leachability of As and Se. 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 regions. 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, and pH. The results of regression models indicated that major elements (Fe, Ca, and 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.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2020

Countermeasures for Preventing and Treating Opioid Overdose

The only medication available currently to prevent and treat opioid overdose (naloxone) was approved by the US Food and Drug Administration (FDA) nearly 50 years ago. Due to its pharmacokinetic and pharmacodynamic properties, naloxone has limited utility under some conditions and would not be effective to counteract mass casualties involving large-scale deployment of weaponized synthetic opioids. To address shortcomings of current medical countermeasures for opioid toxicity, a trans-agency scientific meeting was convened by the US National Institute of Allergy and Infectious Diseases/National Institutes of Health (NIAID/NIH) on August 6 and 7, 2019, to explore emerging alternative approaches for treating opioid overdose in the event of weaponization of synthetic opioids. The meeting was initiated by the Chemical Countermeasures Research Program (CCRP), was organized by NIAID, and was a collaboration with the National Institute on Drug Abuse/NIH (NIDA/NIH), the FDA, the Defense Threat Reduction Agency (DTRA), and the Biomedical Advanced Research and Development Authority (BARDA). This paper provides an overview of several presentations at that meeting that discussed emerging new approaches for treating opioid overdose, including the following: (1) intranasal nalmefene, a competitive, reversible opioid receptor antagonist with a longer duration of action than naloxone; (2) methocinnamox, a novel opioid receptor antagonist; (3) covalent naloxone nanoparticles; (4) serotonin (5-HT)1A receptor agonists; (5) fentanyl-binding cyclodextrin scaffolds; (6) detoxifying biomimetic “nanosponge” decoy receptors; and (7) antibody-based strategies. These approaches could also be applied to treat opioid use disorder.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2020

Toward Validation of Toxicological Interpretation of Diffusive Gradients in Thin Films in Marine Waters Impacted by Copper

Determination of Mytilus galloprovincialis larvae median effect concentration (EC50), of Cu in coastal marine waters by diffusive gradient in thin-films (DGT), has been shown to effectively reduce the need to consider dissolved organic carbon (DOC) concentration and quality. West coast marine and estuarine organisms’ chronic toxicity test protocol was used to validate previously modelled protective effects, afforded to highly sensitive marine larvae by ligand competition, in five diverse site waters. The results demonstrate significant narrowing of toxicological endpoints, where EC50s ranged from 3.74 – 6.67 µg/L as CDGT Cu versus 8.76 – 26.8 µg/L as CuDISS over a DOC range of 0.74 – 3.11 mg/L. Additionally, DOC quality (characterized by fluorescence excitation and emission matrices) indicates that the heterogeneity of competing Cu binding ligands, in common marine waters, minimizes the need for class determinations toward explaining the degree of protection, when assumptions in criterion maximum concentration (CMC) setting are conservative. A CDGT Cu EC50 of 3.7 µg/L, and corresponding CMC CDGT Cu of 1.8 µg/L, for universal application by regulatory compliance-monitoring programs, are proposed as a superior approach toward both integration of dynamic water quality over effective exposure periods and quantification of biologically-relevant trace Cu speciation and are demonstrated by in situ data.

Diffusive Gradients in Thin-films, copper, seawate↗
DOE OSTI2019

Synthesis and anticancer effects of conjugates of doxorubicin and unsaturated fatty acids (LNA and DHA)

Doxorubicin (DOX) is a leading cytostatic drug with many adverse effects in use. We are still looking for methods that will allow us to preserve the therapeutic effect against the tumor cells and reduce the toxicity to the normal cells. In our work, we obtained amide derivatives of DOX by reaction of the amino group with α-linolenic (LNA) and docosahexaenoic (DHA) acids (2, 3), as well as double-substituted derivatives via amide and ester linkages (4, 5). The structures of the compounds were confirmed by Proton Nuclear Magnetic Resonance (1H NMR), Carbon-13 Nuclear Magnetic Resonance (13C NMR), and High Resolution Mass Spectrometry (HRMS) analyses. For all compounds 3-(4,5-dimethylthiazolyl-2)-2,5-diphenyltetrazolium bromide (MTT) assay was used to determine the cytotoxic effect on human cancer cell lines (SW480, SW620, and PC3) and Chinese hamster lung fibroblasts (V79) that were used as a control. The cytotoxic activity was established by calculation of the inhibitory concentration IC{sub 50}. In addition, a cytotoxic capacity against tumor cells for tested compounds was expressed as a selectivity factor (selectivity index, SI). Lactate dehydrogenase (LDH) assay was performed for all compounds to assess the level of cell damage. To explain the basic mechanism of cell death induction the Annexin V-FITC/IP flow cytometry analysis was investigated. We found that all studied conjugates exhibit lower cytotoxicity but higher selectivity than DOX. Among the all derivatives, the conjugates formed by the amide and ester linkages (4, 5) were found to be more promising compared with conjugates (2, 3) formed only by the amide linkage. They show high cytotoxicity toward the tumor cell lines and moderate cytotoxicity towards the normal cell line.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2019

Cancer Treatment-Associated Pericardial Disease: Epidemiology, Clinical Presentation, Diagnosis, and Management

Purpose of Review: Cancer therapeutics have seen tremendous growth in the last decade and have been effective in the treatment of several cancer types. However, with advanced therapies like kinase inhibitors and immunotherapies, there have been unintended consequences of cardiotoxicities. While traditional chemotherapy and radiation-induced cardiotoxicity have been well studied, further research is needed to understand the adverse effects of newer regimens. Recent Findings: Both immune-mediated and non-immune-medicated cytotoxicity have been noted with targeted therapies such as tyrosine kinase inhibitors and immune checkpoint inhibitors. In this manuscript, we describe the pericardial syndromes associated with cancer therapies and propose management strategies. Pericardial effusion and pericarditis are common presentations in cancer patients and often difficult to diagnose. Concomitant myocarditis may also present with pericardial toxicity, especially with immunotherapies. In addition to proper history and physical, additional testing such as cardiovascular imaging and tissue histology need to be obtained as appropriate. Holding the offending oncology drug, and institution of anti-inflammatory medications, and immunosuppressants such as steroids are indicated. Summary: A high index of suspicion, use of standardized definitions, and comprehensive evaluation are needed for early identification, appropriate treatment, and better outcomes for patients with cancer treatment-associated pericardial disease. Further research is needed to understand the pathophysiology and to evaluate how the management of pericardial conditions in these patients differ from traditional management and also evaluate new therapies.

62 RADIOLOGY AND NUCLEAR MEDICINE↗
DOE OSTI2024

A survey study on arsenic speciation in coal fly ash and insights into the role of coal combustion conditions

Coal fly ashes (CFAs) are the low-density byproducts of the coal combustion process. Improper or uncontrolled CFA disposal poses significant environmental and health concerns due to the potential leaching of toxic heavy metals such as arsenic (As). Previous studies have investigated the content and speciation of As in different CFA samples, yet systematic information on As speciation in CFA with representative coal source and combustion conditions is still missing. Based on a recent survey study on the typical coal sources and combustion conditions across the U.S., this study selected 19 representative CFA samples to systematically investigate As speciation and potential correlations with these parameters. The composition, morphology, mineralogy, and As speciation of these CFA samples were characterized by complementary analytical, microscopic, and spectroscopic techniques. Synchrotron X-ray spectroscopy and microscopy analyses revealed the dominant As oxidation state to be As(V) and with strong associations to Ca, with the exception of 3 samples that had 19–51% As(III), likely due to the use of selective catalytic reduction (SCR) process. Principal component analysis was conducted to identify potential correlations of As concentration and oxidation state with parameters such as major element content, loss on ignition (LOI), average particle size, coal source, and combustion condition. Al 2 O 3 and FeO content were found to capture a majority of the variability. Further, results from this study provide fundamental basis for understanding the correlations between coal source, combustion conditions, CFA characteristics, and As speciation, and providing insights for downstream beneficial utilization or disposal management.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2020

Manganese: The overlooked contaminant in the world largest mine tailings dam collapse

Manganese (Mn) is an abundant element in terrestrial and coastal ecosystems and an essential micronutrient in the metabolic processes of plants and animals. Mn is generally not considered a potentially toxic element due to its low content in both soil and water. However, in coastal ecosystems, the Mn dynamic (commonly associated with the Fe cycle) is mostly controlled by redox processes. Here, we assessed the potential contamination of the Rio Doce estuary (SE Brazil) by Mn after the world’s largest mine tailings dam collapse, potentially resulting in chronic exposure to local wildlife and humans. Estuarine soils, water, and fish were collected and analyzed seven days after the arrival of the tailings in 2015 and again two years after the dam collapse in 2017. Using a suite of solid-phase analyses including X-ray absorption spectroscopy and sequential extractions, our results indicated that a large quantity of Mn II arrived in the estuary in 2015 bound to Fe oxyhydroxides. Over time, dissolved Mn and Fe were released from soils when Fe III oxyhydroxides underwent reductive dissolution. Due to seasonal redox oscillations, both Fe and Mn were then re-oxidized to Fe III , Mn III , and Mn IV and re-precipitated as poorly crystalline Fe oxyhydroxides and poorly crystalline Mn oxides. In 2017, redox conditions (Eh: -47 ± 83 mV; pH: 6.7 ± 0.5) favorable to both Fe and Mn reduction led to an increase (~880%) of dissolved Mn (average for 2015: 66 ± 130 μg L -1 ; 2017: 582 ± 626 μg L -1 ) in water and a decrease (~75%, 2015: 547 ± 498 mg kg -1 ; 2017: 135 ± 80 mg kg -1 ) in the total Mn content in soils. The crystalline Fe oxyhydroxides content significantly decreased while the fraction of poorly ordered Fe oxides increased in the soils limiting the role of Fe in Mn retention. The high concentration of dissolved Mn found within the estuary two years after the arrival of mine tailings indicates a possible chronic contamination scenario, which is supported by the high levels of Mn in two species of fish living in the estuary. Our work suggests a high risk to estuarine biota and human health due to the rapid Fe and Mn biogeochemical dynamic within the impacted estuary.

54 ENVIRONMENTAL SCIENCES↗