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At least 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Molecular speciation controls arsenic and lead bioaccessibility in fugitive dusts from sulfidic mine tailings

Communities nearby mine wastes in arid and semi-arid regions are potentially exposed to high concentrations of toxic metal(loid)s from fugitive dusts deriving from impoundments. To assess the relation between potentially lofted particles and human health risk, we studied the relationship between pharmacokinetic bioaccessibility and metal(loid) molecular speciation for mine tailings dust particulate matter (PM), with elevated levels of arsenic and lead (up to 59 and 34 mmol kg -1 , respectively), by coupling in vitro bioassay (IVBA) with X-ray absorption spectroscopy (XAS). Mine tailing efflorescent salts (PM ES ) and PM from the surface crust (0–1 cm, PM SC ) and near surface (0–25 cm) were isolated to <10 μm and <150 μm effective spherical diameter (PM 10 and PM 150 ) and reacted with synthetic gastric and lung fluid for 30 s to 100 h to investigate toxic metal(loid) release kinetics. Bioaccessible (BAc) fractions of arsenic and lead were about 10 and 100 times greater in gastric than in lung fluid simulant, respectively, and 10–100% of the maximum gastric BAc from PM 10 and PM 150 occurred within 30 s, with parabolic dissolution of fine, highly-reactive particles followed by slower release from less soluble sources. Evaporite salts were almost completely solubilized in gastric-fluid simulants. Arsenate within jarosite and sorbed to ferrihydrite, and lead from anglesite, were identified by XAS as the principal contaminant sources in the near surface tailings. In the synthetic lung fluid, arsenic was released continuously to 100 h, suggesting that residence time in vivo must be considered for risk determination. Analysis of pre- and post-IVBA PM indicated the release of arsenic in lung fluid was principally from arsenic-substituted jarosite, whereas in synthetic gastric fluid arsenic complexed on ferrihydrite surfaces was preferentially released and subsequently repartitioned to jarosite-like coordination at extended exposures. Lead dissolved at 30 s was subsequently repartitioned back to the solid phase as pyromorphite in phosphate rich lung fluid. The bioaccessibility of lead in surface tailings PM was limited due to robust sequestration in plumbojarosite. Kinetic release of toxic elements in both synthetic biofluids indicated that a single IVBA interval may not adequately describe release dynamics.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗
NASA NTRS2012

Experimental Investigation into the Radar Anomalies on the Surface of Venus

Radar mapping of thc surface of Venus shows areas of high reflectivity (low emissivity) in the Venusian highlands at altitudes between 2.5-4.75 kilometers. The origin of the radar anomalies found in the Venusian highlands remains unclear. Most explanations of the potential causes for these radar anomalies come from theoretical work. Previous studies suggest increased surface roughness or materials with higher dielectric constants as well as surface atmospheric interactions. Several possible candidates of high-dielectric materials are tellurium) ferroelectric materials, and lead or bismuth sulfides. While previous studies have been influential in determining possible sources for the Venus anomalies, only a very few hypotheses have been verified via experimentation. This work intends to experimentally constrain the source of the radar anomalies on Venus. This study proposes to investigate four possible materials that could potentially cause the high reflectivities on the surface of Venus and tests their behavior under simulated Venusian conditions.

Kohler, E.↗
DOE OSTI2021

Analysis Report documenting the Assessment of the Solubility of Lead, EDTA and other Organic Ligands in non-Sulfide systems performed under TP 08-02 and under TP 20-01

The objective of this report is to accept or reject the hypothesis that the experiments conducted under TP 08-02 Revision 0 (Ismail et al., 2008) were affected by CO 2 (g) intrusion and sample contamination. The test of the hypothesis is accomplished by comparing the experimental data collected under the protocols of TP 08-02 Revision O and TP 20-01 Revision O (Kirkes and Zhang, 2020). The protocols of TP 20-01 Revision 0 minimize the possibilities of CO 2 (g) intrusion and sample contamination. The experimental data sets obtained under both TPs will be assessed statistically to see if they are identical or not.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2006

Thermal Constraints from Siderophile Trace Elements in Acapulcoite-Lodranite Metals

A fundamental process in the formation of differentiated bodies is the segregation of metal-sulfide and silicate phases, leading to the formation of a metallic core. The only known direct record of this process is preserved in some primitive achondrites, such as the acapulcoite-lodranites. Meteorites of this clan are the products of thermal metamorphism of a chondritic parent. Most acapulcoites have experienced significant partial melting of the metal-sulfide system but not of silicates, while lodranites have experienced partial melting and melt extraction of both. The clan has experienced a continuum of temperatures relevant to the onset of metal mobility in asteroidal bodies and thus could yield insight into the earliest stages of core formation. Acapulcoite GRA 98028 contains relict chondrules, high modal sulfide/metal, has the lowest 2-pyroxene closure temperature, and represents the least metamorphosed state of the parent body among the samples examined. Comparison of the metal-sulfide component of other clan members to GRA 98028 can give an idea of the effects of metamorphism.

Herrin, Jason S.↗
NASA NTRS2006

Tracking the Early Thermal History of Asteroids with Trace Siderophiles in Meteorite Metals

A fundamental process in the formation of differentiated bodies is the segregation of metal-sulfide and silicate phases, leading to the formation of a metallic core. The only known direct record of this process is preserved in some primitive achondrites, such as the acapulcoites and lodranites. These meteorites, thought to originate from the same parent asteroid, are the products of thermal metamorphism and igneous processing of a chondritic precursor. Collectively, they have experienced a range of peak metamorphic temperatures relevant to the onset of metal-sulfide partial melting and melt migration. We assessed the siderophile element composition of their metals in an effort to determine the conditions and extent of metal-sulfide melt extraction and thereby gain insight into the earliest stages of core formation.

Herrin, J. S.↗
DOE OSTI2020

The Geochemistry and Microbial Ecology of Produced Waters from Three Different Unconventional Oil and Gas Regions

One of the most significant challenges associated with predicting reservoir fluid properties is accounting for the effect of microbial activity, which catalyzes chemical reactions that lead to corrosion and sulfide release during or after hydraulic fracturing operations. The current understanding of microbial populations living in hydraulic fracturing systems is based on a limited number of samples and well sites, necessitating additional research efforts to confirm preliminary findings and identify factors driving the microbial ecology. The project objective is to profile the geochemistry and microbiology of three different oil and gas basins to order increase the understanding of how microbial activity affects reservoir fluids.

Lipus, Daniel↗
NASA NTRS2006

Metal-Silicate Segregation in Asteroidal Meteorites

A fundamental process of planetary differentiation is the segregation of metal-sulfide and silicate phases, leading eventually to the formation of a metallic core. Asteroidal meteorites provide a glimpse of this process frozen in time from the early solar system. While chondrites represent starting materials, iron meteorites provide an end product where metal has been completely concentrated in a region of the parent asteroid. A complimentary end product is seen in metal-poor achondrites that have undergone significant igneous processing, such as angrites, HED's and the majority of aubrites. Metal-rich achondrites such as acapulcoite/lodranites, winonaites, ureilites, and metal-rich aubrites may represent intermediate stages in the metal segregation process. Among these, acapulcoite-lodranites and ureilites are examples of primary metal-bearing mantle restites, and therefore provide an opportunity to observe the metal segregation process that was captured in progress. In this study we use bulk trace element compositions of acapulcoites-lodranites and ureilites for this purpose.

Herrin, Jason S.↗
NASA NTRSDate not supplied

Assimilation of Fossil Hydrothermal Sulfide by Early Amazonian Martian Magmas: Implications for Ore Mineralization on Mars

Martian magmas would interact with any hydrosphere present, whether a global ocean [e.g., 1] or an icy (subterranean) hydrosphere [2] creating hydrothermal systems. Volcanogenic massive sulfide (VMS) ores, with Fe-Zn-Pb sulfides, created by hydrothermal deposition associated with a wide range of volcanism would be expected on Mars [3]. Similar to terrestrial komatiites, martian igneous rocks could generate orthomagmatic Ni-sulfide ore deposits by immiscible sulfide liquid segregation [4]. For this to occur, a martian magma would need to flow over (or intrude into) a pre-existing sulfur-rich formation. Here, we elaborate on the first evidence [5-6] of potential orthomagmatic mineralization in two Early Amazonian (2.4 Ga) igneous meteorites [7-8] involving a threestep process: i) formation of Fe-Zn-Pb sulfides, (ii) assimilated by the 2.4 Ga magmas leading to (iii) formation of orthomagmatic Ni-sulfide deposits. These deposits may remain on Mars, but the telltale signs of Zn-Pb enrichment and Ni-Co depletion in the two meteorites provide important insights into martian geology.

M Humayun↗
DOE OSTI2025

Mineralogical evidence for hydrothermal alteration of Bennu samples

Samples of asteroid (101955) Bennu delivered by the OSIRIS-REx mission offer the opportunity to study pristine planetary materials unchanged by exposure to the terrestrial environment. Here we use a combination of X-ray diffraction and various electron microscopy techniques to explore the detailed mineralogy of Bennu samples and determine the alteration history of the planetesimal protolith from which they originated. The samples consist largely of hydrated sheet-silicate minerals, namely nanoscale serpentine and saponite of varied grain size, which are decorated with micro- to nanoscale Fe-sulfides, magnetite and carbonates. We observe sheet silicates parallel and normal to sulfide surfaces and as inclusions in sulfides; sulfur-rich veins transecting the sheet-silicate matrix; zoned carbonates and phosphates and sulfide and magnetite grains exhibiting embayment. The mineralogical evidence indicates alteration of accreted minerals by a fluid that evolved with time, leading to etching, dissolution and reprecipitation. Sulfide compositions indicate alteration at ~25 °C, similar to conditions inferred for asteroid (162173) Ryugu and Ivuna-type (CI) chondrite meteorites. The fluid probably evolved from neutral to alkaline, culminating with the precipitation of highly soluble salts. We conclude that Bennu’s protolith comprised mainly nanometre to micrometre silicates, with fewer chondrules and calcium–aluminium-rich inclusions than those of most chondrite groups.

Zega, T J↗
NASA NTRS1983

The isotopic composition of silver and lead in two iron meteorites - Cape York and Grant

Anomalies in silver isotope composition in the metal phases of the Cape York (IIIA) and Grant (IIIB) iron meteorites are studied together with the lead isotopic composition of both the metal and sulfide phases of Cape York. Following extensive surface cleaning, the Ag-107/Ag-109 ratio in the metal phases of the meteorites is found to be in excess of the terrestrial ratio, and of that found in the sulfide phases. A definite correlation between the Ag-107/Ag-109 and Pd-108/Ag-109 ratios is observed for these meteorites, indicating the in situ decay of Pd-107 and supporting the widespread presence of Pd in the early universe. Lead, determined after cleaning and with chemical separations using low blank levels, is found to exist in variable proportions in the metal and sulfide phases. The sulfides appear to be dominated by radiogenic modern lead, which may be explained by terrestrial contamination or by late metamorphism in the meteorite parent body.

Chen, J. H.↗
NASA NTRS1995

Investigation of the Prebiotic Synthesis of Amino Acids and RNA Bases from CO2 Using FeS/H2S As a Reducing Agent

An autotrophic theory of the origin of metabolism and life has been proposed in which carbon dioxide is reduced by ferrous sulfide and hydrogen sulfide by means of a reversed citric acid cycle, leading to the production of amino acids. Similar processes have been proposed for purine synthesis. Ferrous sulfide is a strong reducing agent in the presence of hydrogen sulfide and can produce hydrogen as well as reduce alkenes, alkynes, and thiols to saturated hydrocarbons and reduce ketones to thiols. However, the reduction of carbon dioxide has not been demonstrated. We show here that no amino acids, purities, or pyrimidines are produced from carbon dioxide with the ferrous sulfide and hydrogen sulfide system. Furthermore, this system does not produce amino acids from carboxylic acids by reductive amination and carboxylation. Thus, the proposed autotrophic theory, using carbon dioxide, ferrous sulfide, and hydrogen sulfide, lacks the robustness needed to be a geological process and is, therefore, unlikely to have played a role In the origin of metabolism or the origin of life.

Keefe, Anthony D.↗
NASA NTRS1995

Investigation of the Prebiotic Synthesis of Amino Acids and RNA Bases from CO2 using FeS/H2S as a Reducing Agent

An autotrophic theory of the origin of metabolism and life has been proposed in which carbon dioxide is reduced by ferrous sulfide and hydrogen sulfide by means of a reversed citric acid cycle, leading to the production of amino acids. Similar processes have been proposed for purine synthesis. Ferrous sulfide is a strong reducing agent in the presence of hydrogen sulfide and can produce hydrogen as well as reduce alkenes, alkynes, and thiols to saturated hydrocarbons and reduce ketones to thiols. However, the reduction of carbon dioxide has not been demonstrated. We show here that no amino acids, purines, or pyrimidines are produced from carbon dioxide with the ferrous sulfide and hydrogen sulfide system. Furthermore, this system does not produce amino acids from carboxylic acids by reductive amination and carboxylation. Thus, the proposed autotrophic theory, using carbon dioxide, ferrous sulfide, and hydrogen sulfide, lacks the robustness needed to be a geological process and is, therefore, unlikely to have played a role in the origin of metabolism or the origin of life.

Keefe, Anthony D.↗
NASA NTRS1986

Theoretical studies of the low-lying states of ScO, ScS, VO, and VS

Bonding in the low-lying states of ScO, ScS, VO, and VS is theoretically studied. Excellent agreement is obtained with experimental spectroscopic constants for the low-lying states of ScO and VO. The results for VS and ScS show that the bonding in the oxides and sulfides is similar, but that the smaller electronegativity in S leads to a smaller ionic component in the bonding. The computed D0 of the sulfides are about 86 percent of the corresponding oxides, and the low-lying excited states are lower in the sulfides than in the corresponding oxides. The CPF method is shown to be an accurate and cost-effective method for obtaining reliable spectroscopic constants for these systems.

Bauschlicher, Charles W., Jr.↗
DOE OSTI2024

Vapor Infiltration Synthesis of Indium Sulfide Magic Size Cluster

The energetically favorable formation of atomically precise clusters, known as magic size clusters, in the solution phase enables a precision nanoscale synthesis with exquisite uniformity. Here, we report the synthesis of magic size clusters via vapor infiltration of atomic layer deposition precursors directly in a polymer thin film. Sequential infiltration of trimethylindium vapor and hydrogen sulfide gas into poly(methyl methacrylate) leads to the formation of clusters with uniform properties consistent with a magic size cluster-In 6 S 6 (CH 3 ) 6 . While an increase in cluster size might be expected with additional sequential infiltration cycles of the reactive In and S precursors, uniform properties consistent with magic size clusters form in multiple polymers under a range of processing conditions. Ultraviolet-visible absorption spectra of In 6 S 6 (CH 3 ) 6 are largely independent of the number of sequential infiltration cycles and exhibit air stability, both of which are attributed to an energetically favorable synthetic pathway that is evaluated with density functional theory.

atomic layer deposition↗
NASA NTRS2018

Aubrite and Enstatite Chondrite Impact Melt Meteorites: Analogs to Mercury?

New data obtained during the MESSENGER mission has allowed us to better contrain the composition and mineralogy of the mercurian surface. One unique feature of Mercury is its extremely low oxygen fugacity (ƒO2) (Iron Wustite (IW) -7.3 to IW-2.6). At such extreme conditions, elements that exhibit lithophile behavior on Earth can exhibit chalcophile or siderophile behavior, leading to the formation of exotic sulfides and metals. As no samples have been returned from Mercury, it is critical to study meteorite analogs to better under-stand the formation conditions of the minerals present at the mercurian surface, as well as mercurian magmatic processes. Given the low fO2 on Mercury, we have selected to investigate potential meteoritic analogs for Mercury among the most reduced meteorite types, including the aubrites and enstatite chondrite impact melts. The aubrites are differentiated meteorites that show varying degrees of brecciation, have a similar ƒO2 to the mercurian surface and interior, and contain exotic sulfides that have been inferred to be present on the mercurian surface. The enstatite chondrite impact melts are from undifferentiated parent bodies, have a similar ƒO2 to the mercurian surface and interior, and contain exotic sulfides that have been inferred to be present on the mercurian surface. In this study, we present a comprehensive analysis of a representative suite of aubrites and enstatite chondrite impact melts and assess their relevance to under-standing magmatic processes on Mercury.

Wilbur, Z. E.↗
DOE OSTI2021

Classification of Semiconductors Using Photoluminescence Spectroscopy and Machine Learning

Photoluminescence spectroscopy is a nondestructive optical method that is widely used to characterize semiconductors. In the photoluminescence process, a substance absorbs photons and emits light with longer wavelengths via electronic transitions. This paper discusses a method for identifying substances from their photoluminescence spectra using machine learning, a technique that is efficient in making classifications. Neural networks were constructed by taking simulated photoluminescence spectra as the input and the identity of the substance as the output. Here, six different semiconductors were chosen as categories: gallium oxide (Ga 2 O 3 ), zinc oxide (ZnO), gallium nitride (GaN), cadmium sulfide (CdS), tungsten disulfide (WS 2 ), and cesium lead bromide (CsPbBr 3 ). The developed algorithm has a high accuracy (>90%) for assigning a substance to one of these six categories from its photoluminescence spectrum and correctly identified a mixed Ga 2 O 3 /ZnO sample.

47 OTHER INSTRUMENTATION↗
NASA NTRS1997

Phase Equilibrium Investigations of Planetary Materials

This grant provided funds to carry out experimental studies designed to illuminate the conditions of melting and chemical differentiation that has occurred in planetary interiors. Studies focused on the conditions of mare basalt generation in the moon's interior and on processes that led to core formation in the Shergottite Parent Body (Mars). Studies also examined physical processes that could lead to the segregation of metal-rich sulfide melts in an olivine-rich solid matrix. The major results of each paper are discussed below and copies of the papers are attached as Appendix I.

Grove, T. L.↗