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DOE OSTI2024

Modeling and Optimization of Zeolites for Contaminant Removal from Coal Combustion Impoundment Leachates

Coal Combustion Residual (CCR) landfills in the U.S. can lead to elevated contaminant concentrations in groundwater and runoff, particularly of arsenic, boron, and selenium. Zeolites can be readily synthesized from materials contained within the coal combustion ash impoundments and can be cation-exchanged to enhance adsorption capacity, selectivity, and reactivity. However, the optimization of zeolites becomes a daunting task when accounting for the variety of Si:Al ratios, the species of extra-framework cations present, and the zeolite pore structure. Molecular simulations provide methods to study and guide the design of zeolites for the sorption of contaminants from aqueous solution. In this work, models that predict the sorption of arsenic, boron, and selenium from water using cation-exchanged zeolites. Because of the lack of experimental adsorption data for these species of contaminants, models were parametrized to reproduce the results of first-principles calculations and then used to predict sorption for zeolites for a dataset containing 6000 combinations of zeolites and sorption conditions. Machine learning was used to train a model to predict sorption for materials in this database based on the results of the molecular simulations. Next, a genetic algorithm was used to optimize zeolites for the removal of each contaminant from aqueous solution for individual impoundment sites based on contaminant concentrations reported by the Electric Power Research Institute.

Findley, John↗

DOE OSTI2024

Editorial: Water supply sustainability and challenges in Asian megadeltas under global change

Globally, riverine deltas comprise barely 1% of land area, but they support the livelihoods of more than 500 million people (Moorhouse et al., 2021). The Asian megadeltas (e.g., Indus, Bengal, Mekong, Red River, and Yangtze) and their riverine floodplains are the most dynamic economic and environmental systems in the world. These low-lying coastal landforms support surface water bodies and highly productive aquifer systems. However, water resources of the Asian megadeltas are extremely vulnerable to geogenic (e.g., arsenic) and anthropogenic (e.g., bacteria) contamination, increased water salinisation from rising sea levels (Figure 1), and chemicals (e.g., fertilizers, pesticides) from land-use practices (Mukherjee et al., 2024) – all of which are threatening the sustainability of water supply and food security in the region. This Research Topic collection features five original articles that explore water chemistry including arsenic and bacteriological contamination, water salinisation, water-energy-food nexus in irrigated agriculture, and groundwater depletion resulting from irrigation, rapid urbanization, and climate change. Although the Research Topic collection does not include case studies from all the Asian Megadeltas shown in Figure 1, the relevance of multi-hazard driven water risks to all deltaic and river floodplain environments around the world is well-illustrated.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1973

Trace element analysis of coal by neutron activation

The irradiation, counting, and data reduction scheme is described for an analysis capability of 1000 samples per year. Up to 56 elements are reported on each sample. The precision and accuracy of the method are shown for 25 elements designated as hazardous by the Environmental Protection Agency (EPA). The interference corrections for selenium and ytterbium on mercury and ytterbium on selenium are described. The effect of bromine and antimony on the determination of arsenic is also mentioned. The use of factorial design techniques to evaluate interferences in the determination of mercury, selenium, and arsenic is shown. Some typical trace element results for coal, fly ash, and bottom ash are given.

Sheibley, D. W.↗

NASA NTRS1973

Trace element analysis of coal by neutron activation.

Sheibley, D. W.↗

NASA NTRS1977

Technology of GaAs metal-oxide-semiconductor solar cells

The growth of an oxide interfacial layer was recently found to increase the open-circuit voltage (OCV) and efficiency by up to 60 per cent in GaAs metal-semiconductor solar cells. Details of oxidation techniques to provide the necessary oxide thickness and chemical structure and using ozone, water-vapor-saturated oxygen, or oxygen gas discharges are described, as well as apparent crystallographic orientation effects. Preliminary results of the oxide chemistry obtained from X-ray, photoelectron spectroscopy are given. Ratios of arsenic oxide to gallium oxide of unity or less seem to be preferable. Samples with the highest OVC predominantly have As(+3) in the arsenic oxide rather than As(+5). A major difficulty at this time is a reduction in OCV by 100-200 mV when the antireflection coating is vacuum deposited.

Stirn, R. J.↗

NASA NTRS1981

Chemical and morphological characteristics of lithium electrode surfaces

Lithium electrode surfaces were analyzed for chemical and morphological characteristics, using electron spectroscopy chemical analysis (ESCA) and scanning electron microscopy (SEM). Samples included lithium metal and lithium electrodes which were cycled in a 1.5 M lithium arsenic hexafluoride/two-methyl tetrahydrofuran electrolyte. Results show that the surface of the as-received lithium metal was already covered by a film composed of LiO2 and an Li2O/CO2 adduct with a thickness of approximately 100-200 A. No evidence of Ni3 was found. Upon exposure of the lithium electrode to a 1.5 M LiAsF6/2-Me-THF electrochemical environment, a second film was observed to form on the surface, consisting primarily of As, Si, and F, possibly in the form of lithium arsenic oxyfluorides or lithium fluorosilicates. It is suggested that the film formation may be attributed to salt degradation.

Yen, S. P. S.↗

NASA NTRS1983

El Chichon - Composition of plume gases and particles

Aircraft measurements were made of trace gases, atmospheric particles, and condensed acid volatiles in the plume of El Chichon volcano, Chiapas, Mexico, in November 1982. Hydrogen sulfide was the primary gaseous sulfur species in the plume at the time of collection. Concentrations of 28 elements were determined by neutron activation analysis of particulate material from the plume. The volatile elements sulfur, chlorine, arsenic, selenium, bromine, antimony, iodine, tungsten, and mercury were enriched relative to bulk pyroclastic material by factors of 60 to 20,000. Arsenic, antimony, and selenium were associated predominantly with small (not greater than 3 micrometer) particles. Calcium and sodium were present almost exclusively on larger particles and aluminum and manganese were bimodally distributed. Ashladen particulate material injected into the stratosphere during the early violent eruptions was enriched by factors of 10 to 30 relative to ash in some of the same elements observed in the quiescent plume.

Kotra, J. P.↗

NASA NTRS1989

Arsine in Saturn and Jupiter

New spectra of Saturn and Jupiter are reported that show a prominent, heretofore unidentified absorption near 2126/cm. The observation is interpreted as unambiguous evidence for the presence of arsine, AsH3. The abundance of AsH3 appears to be almost a factor of two higher in Saturn than in Jupiter. The observed enrichments are consistent with the core instability model for the formation of giant planets. Models of arsenic chemistry that predict strong depletions of AsH3 at temperatures below 370 K are not consistent with the observations, suggesting that vertical convection or perhaps some other mechanism inhibits depletion. Arsenic is the first new element identified in a planetary atmosphere since germanium was found in Jupiter a decade ago.

Noll, Keith S.↗

NASA NTRS1997

Development of 256 x 256 Element Impurity Band Conduction Infrared Detector Arrays for Astronomy

This report describes the work performed on a one and a half year advance technology program to develop Impurity Band Conduction (IBC) detectors with very low dark current, high quantum efficiency, and with good repeatable processes. The program fabricated several epitaxial growths of Si:As detecting layers from 15 to 35 microns thick and analyzed the performance versus the thickness and the Arsenic concentration of these epitaxial layers. Some of the epitaxial runs did not yield because of excessive residual impurities. The thicker epitaxial layers and the ones with higher Arsenic concentration resulted in good detectors with low dark currents and good quantum efficiency. The program hybridized six detector die from the best detector wafers to a low noise, 256 x 256 readout array and delivered the hybrids to NASA Ames for a more detailed study of the performance of the detectors.

Domingo, George↗

NASA NTRS2001

Synthesis of ZnO:As Films Using Off-Axis Sputtering Deposition

As a novel oxide semiconductor material, ZnO is interesting for use in many applications. For fabricating electronic devices, it is important to have n- and p- type ZnO materials. Arsenic has been proven to be one of the p-type dopants for ZnO materials. However, information in studying the ZnAsO ternary compound films has been scarce. In order to investigate the morphology, structure and electrical properties of ZnAsO ternary compounds, ZnO:As films have been synthesized using off-axis sputtering deposition on various substrates including (100) Si and (0001) sapphire crystals. Films are grown under various growth conditions. ZnO:As targets with the atomic weight ratios of arsenic to zinc from 0.01 to 0.10 are used for film synthesis. The growth temperatures and pressures range from 350 to 550C and 5 to 150 mTorr, respectively. Argon to oxygen gas ratio for film growth is varied to examine the film quality as well. Film surface morphology, crystal structure, and compositions, are characterized using atomic force microscopy, x-ray diffraction, and energy dispersive spectroscopy, respectively. The compositions of target material and ZnO:As films grown under various conditions are then assessed. The electrical properties were also measured. The detail of these measurements will be discussed in the presentation.

Zhu, Shen↗

NASA NTRS2007

Aerospace Toxicology and Microbiology

Toxicology dates to the very earliest history of humanity with various poisons and venom being recognized as a method of hunting or waging war with the earliest documentation in the Evers papyrus (circa 1500 BCE). The Greeks identified specific poisons such as hemlock, a method of state execution, and the Greek word toxos (arrow) became the root of our modern science. The first scientific approach to the understanding of poisons and toxicology was the work during the late middle ages of Paracelsus. He formulated what were then revolutionary views that a specific toxic agent or "toxicon" caused specific dose-related effects. His principles have established the basis of modern pharmacology and toxicology. In 1700, Bernardo Ramazzini published the book De Morbis Artificum Diatriba (The Diseases of Workers) describing specific illnesses associated with certain labor, particularly metal workers exposed to mercury, lead, arsenic, and rock dust. Modern toxicology dates from development of the modern industrial chemical processes, the earliest involving an analytical method for arsenic by Marsh in 1836. Industrial organic chemicals were synthesized in the late 1800 s along with anesthetics and disinfectants. In 1908, Hamilton began the long study of occupational toxicology issues, and by WW I the scientific use of toxicants saw Haber creating war gases and defining time-dosage relationships that are used even today.

James, John T.↗

NASA NTRS2016

Growth Mechanism of Nanowires: Ternary Chalcogenides

In the past two decades there has been a large rise in the investment and expectations for nanotechnology use. Almost every area of research has projected improvements in sensors, or even a promise for the emergence of some novel device technologies. For these applications major focuses of research are in the areas of nanoparticles and graphene. Although there are some near term applications with nanowires in photodetectors and other low light detectors, there are few papers on the growth mechanism and fabrication of nanowire-based devices. Semiconductor nanowires exhibit very favorable and promising optical properties, including high transparency and a several order of magnitude better photocurrent than thin film and bulk materials. We present here an overview of the mechanism of nanowire growth from the melt, and some preliminary results for the thallium arsenic selenide material system. Thallium arsenic selenide (TAS) is a multifunctional material combining excellent acousto-optical, nonlinear and radiation detection properties. We observed that small units of (TAS) nanocubes arrange and rearrange at moderate melt undercooling to form the building block of a nanowire. In some cases very long wires (less than mm) are formed. Since we avoided the catalyst, we observed self-nucleation and uncontrolled growth of wires from different places.

Singh, N. B.↗

NASA NTRS2016

Stellar Laboratories

For the spectral analysis of high-resolution and high signal-to-noise (SN) spectra of hot stars, state-of-the-art non-local thermodynamic equilibrium (NLTE) model atmospheres are mandatory. These are strongly dependent on the reliability of the atomic data that is used for their calculation. Aims: To identify molybdenum lines in the ultraviolet (UV) spectra of the DA-type white dwarf G191B2B and the DO-type white dwarf RE 0503289 and, to determine their photospheric Mo abundances, reliable Mo iv-vii oscillator strengths are used. Methods: We newly calculated Mo iv-vii oscillator strengths to consider their radiative and collisional bound-bound transitions indetail in our NLTE stellar-atmosphere models for the analysis of Mo lines exhibited in high-resolution and high SN UV observations of RE 0503289.Results. We identified 12 Mo v and nine Mo vi lines in the UV spectrum of RE 0503289 and measured a photospheric Mo abundance of 1.2 3.0 104(mass fraction, 22 500 56 400 times the solar abundance). In addition, from the As v and Sn iv resonance lines,we measured mass fractions of arsenic (0.51.3 105, about 300 1200 times solar) and tin (1.33.2 104, about 14 300 35 200 times solar). For G191B2B, upper limits were determined for the abundances of Mo (5.3 107, 100 times solar) and, in addition, for Kr (1.1106, 10 times solar) and Xe (1.7107, 10 times solar). The arsenic abundance was determined (2.35.9 107, about 21 53 times solar). A new, registered German Astrophysical Virtual Observatory (GAVO) service, TOSS, has been constructed to provide weighted oscillator strengths and transition probabilities.Conclusions. Reliable measurements and calculations of atomic data are a prerequisite for stellar-atmosphere modeling. Observed Mo v-vi line profiles in the UV spectrum of the white dwarf RE 0503289 were well reproduced with our newly calculated oscillator strengths. For the first time, this allowed the photospheric Mo abundance in a white dwarf to be determined.

Rauch, T.↗

NASA NTRS2022

Un-Numbered Operational Areas PRL 229 Railroad Tie Disposal Area Pond Confirmation Sampling Report

This Confirmatory Sampling (CS) Report (CSR) was prepared for the National Aeronautics and Space Administration (NASA), Kennedy Space Center (KSC), Florida in accordance with the CS Work Plan (CSWP) (HGL, 2022a). The CSR summarizes investigation activities performed on the Railroad Tie Disposal Area (RTDA) of the Un-Numbered Operational Areas (UNOA), Potential Release Location (PRL) 229 located at KSC. HydroGeoLogic, Inc. (HGL) prepared this report under Contract Number 80KSC019D0012. The purpose of the CSR is to provide information to evaluate the level of potential contamination in surface water and sediment samples collected from the RTDA PRL 229 Pond and determine if contaminants pose unacceptable risks to ecological receptors. The CSR provides analytical data of 10 sets of surface water and sediment samples collected in 2021. Surface water samples were analyzed for volatile organic compounds (VOCs), semi-volatile organic compounds (SVOCs), polynuclear aromatic hydrocarbon (PAHs), metals, hardness, and salinity, while sediment samples were analyzed for metals, total organic carbon (TOC), SVOCs, PAHs, and total petroleum hydrocarbons (TPH). The CSR includes a Screening Level Ecological Risk Assessment (SLERA) conducted under KSC’s Resource Conservation and Recovery Act (RCRA) Corrective Action Program to determine if unacceptable risks to ecological receptors exist at PRL 229 Pond. Metals and PAHs were detected in surface water samples, including detections of antimony, arsenic, barium, calcium, copper, lead, magnesium, thallium, zinc, anthracene, benzo(a)anthracene, benzo(a)pyrene, benzo(b)fluoranthene, benzo(g,h,i)perylene, benzo(k)fluoranthene, chrysene, dibenzo(a,h)anthracene, fluoranthene, indeno(1,2,3-c,d)pyrene and pyrene. Based on measured salinity (1.03 to 1.21 parts per thousand), the pond was identified as freshwater. Sediment analytical results also contained detections of metals and PAHs, including antimony, arsenic, barium, beryllium, cadmium, chromium, copper, lead, mercury, nickel, selenium, thallium, zinc, anthracene benzo(a)anthracene, benzo(a)pyrene, benzo(b)fluoranthene, benzo(g,h,i)perylene, benzo(k)fluoranthene, chrysene, dibenzo(a,h)anthracene, fluoranthene, indeno(1,2,3-c,d)pyrene and pyrene. Potential risks to ecological receptors were evaluated in accordance with the SLERA Work Plan and the Decision Process Document for the Resource Conservation and Recovery Act (RCRA) Corrective Action Program at KSC (DPD) (Geosyntec, 2019), and using the 2021 sediment and surface water analytical results. Potential ecological receptors evaluated in the SLERA include the aquatic community, benthic invertebrates, aquatic birds, and aquatic mammals. The SLERA included Steps 2a through 2c of the Ecological Risk Assessment (ERA) process in accordance with the DPD. Using multiple lines of evidence, the SLERA concluded that many of the detected analytes are present at concentrations similar to those in background or reference locations at KSC, and/or at concentrations that would not pose a significant risk to ecological communities. There are no screening values available for the avian community, and PAHs are bioaccumulative compounds. For this reason, food web modeling was completed as a supplement to Step 2c to provide a quantitative evaluation of this exposure pathway. Food web modeling indicates that PAHs are unlikely to pose a risk to birds exposed to site sediment and surface water. Based on the results of the SLERA, the contaminants in sediment and surface water pose no to minimal risk to the ecological communities that could live or forage at the site. Based on the results of the SLERA, no further study is recommended for the RTDA Pond at PRL 229.

Confirmation Sampling↗

DOE OSTI2022

Rice husk and charred husk amendments increase porewater and plant Si but water management determines grain As and Cd concentration

Abstract Purpose Rice is a staple crop worldwide and a silicon (Si) hyperaccumulator with Si levels reaching 5–10% of its mass; this can result in desilication and Si-deficiency if plant residues are not managed correctly. Rice is also uniquely subject to arsenic (As) and cadmium (Cd) contamination depending on soil conditions. Our goal is to quantify the effects of rice husk (a Si-rich milling byproduct) amendments and different water management strategies on rice uptake of Si, As, and Cd. Methods We employed 4 husk amendment treatments: Control (no husk), Husk (untreated husk), Biochar (husk pyrolyzed at 450 °C), and CharSil (husk combusted at > 1000 °C). Each of these amendments was studied under nonflooded, alternate wetting and drying (AWD), and flooded water management in a pot study. Porewater chemistry and mature plant elemental composition were measured. Results Husk and Biochar treatments, along with flooding, increased porewater and plant Si. Vegetative tissue As decreased with increasing porewater Si, but grain As and plant Cd were primarily controlled by water management. Grain As and Cd were inversely correlated and are simultaneously minimized in a redox potential (Eh) range of 225–275 mV in the studied soil. Ferrihydrite in root iron plaque decreased As translocation from porewater to grain, but amendments were not able to increase plaque ferrihydrite content. Conclusion We conclude moderate husk amendment rates (i.e., 4 years’ worth) with minimal pretreatment strongly increases rice Si content but may not be sufficient to decrease grain As in low Si and As soil.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Measurement of the 70 Ge( d , n ) 71 As cross section from 2.1 MeV to 10 MeV

This work reports experimental 70 Ge(d,n) 71 As cross sections producing Arsenic-71 (t 1/2 = 65.3 h, 28% β + ), a potentially useful diagnostic radionuclide. Target stacks containing two nat Ge foils, a nat Ni monitor foil, and an Al degrader were irradiated with 5.5–10 MeV deuterons using an FN Tandem Van de Graaff accelerator. 71 As and 61 Cu, 56 Co, and 58 Co (from nat Ni(d,x)) were quantified in the foils by high purity germanium gamma spectrometry. Furthermore, the measured cross sections are larger than previously reported and suitable for producing preclinical quantities of diagnostic radiopharmaceuticals.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2024

Angle-resolved polarized Raman study of layered b-As x P x-1 alloys: Identification of As-P vibrational modes

In this study, the polarization-resolved Raman spectra of b-As x P x-1 flakes with varying arsenic concentration (x = 0, 0.4, and 0.8) are systematically investigated. A clear polarization dependence is observed in the Raman intensity of all the P-P, As-P, and As-As modes and confirmed by the first-principles calculations. The observed angle-dependence can be related to the structure of the Raman tensors of each peak. In particular, the Raman intensities corresponding to As-P vibration modes are studied in detail. The out of plane As-P mode ($A$$^{1}_{g}$) is clearly identified, but the butterfly-shaped behavior observed in the polar plot around 350 cm -1 is interpreted as the combination of the two in-plane vibrations, one along the armchair and the other along the zigzag direction. This work allows unambiguous assignment of the $A$$^{1}_{g}$, B 2g , and $A$$^{2}_{g}$ modes of the As-P vibrational modes and the importance of the consideration of the superposition of the in-plane B 2g and $A$$^{2}_{g}$ modes. Such study can be utilized to further characterize the anisotropic structural properties and analyze the local distribution of the As and P in b-As x P x-1 alloys which will play key roles in electronic and optical properties. Furthermore, this methodology can be further extended to alloyed two-dimensional material systems with in-plane anisotropy in general.

2D materials↗

DOE OSTI2021

The adsorption of As(V) on poorly crystalline Fe oxyhydroxides, revisited: Effect of the reaction media and the drying treatment

Arsenic (As) adsorbed on Fe oxyhydroxides (adsorbent) is widely occurring in many environmental settings such as in acid mine drainage systems or in the hydrometallurgical operations to form Fe-As coprecipitates. However, the influence of the reaction media and the drying treatment on the microstructure of the directly formed adsorbents at various pHs was still not fully understood. In this work, As adsorption behaviors on various forms of Fe oxyhydroxides were systematically investigated by using XRD, FTIR, Raman, XANES, and HRTEM. Overall, the results revealed that at weak acidic pH, more As could adsorbed on the suspension adsorbent formed in sulfate and chloride media than that in nitrate media, possibly due to the microstructure alteration of the adsorbent in the presence of sulfate and chloride. Besides, the increasing crystallinity of the Fe oxyhydroxides and the aggregation effect after drying were the major reasons why less As could be hold by the dried adsorbents than that of the corresponding suspension adsorbents. These findings could shed more light on the nature of the Fe oxyhydroxides which may be helpful for more precisely predicting the fate of some toxic metal(loid)s in the environment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗