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DOE OSTI2025

Phosphate-modulated transformation of Sb(V)-bearing ferrihydrite under microbial iron- and sulfate-reducing conditions

Antimony (Sb) is a toxic metalloid that poses environmental risks in terrestrial and aquatic systems. The fate of the Sb(V) oxyanion, Sb(OH) 6 − , is governed by complex biogeochemical processes, including immobilization by ferric (Fe(III)) oxides, reduction by sulfide, and the less-explored competitive adsorption with other anions such as phosphate (PO 4 3− ). Here, this study investigates the interplay between such mechanisms in controlling the behavior of Sb(V) associated with ferrihydrite (Fh) under Fe(III)- and sulfate-reducing conditions, with a particular emphasis on the role of phosphate in influencing Sb(V) mobility and transformation. Anoxic reactors that contained Sb(V)-coprecipitated Fh, varying PO 4 3− concentrations (0, 0.2, and 2 mM), and sulfate, were inoculated with a microbial community sourced from Sb-contaminated soil. Additionally, abiotic reactors with either Sb(V)-adsorbed or Sb(V)-coprecipitated Fh and different PO 4 3− loadings (0–100 mM) were created to investigate the competitive adsorption mechanisms in the absence of microbial activity. Results from the abiotic reactors suggest that Sb(V) is likely incorporated into the Fh structure, with only minor amounts remaining surface-bound and extractable by PO 4 3− . In the biotic reactors, microbial Fe(III) and sulfate reduction were more extensive in the presence of PO 4 3− . At 0.2 mM PO 4 3− , microbial activity transformed Fh into siderite and led to the complete reduction of Sb(V) to Sb(III) as stibnite (Sb 2 S 3 ). At 2 mM PO 4 3− , the greater coverage by PO 4 3− stabilized Fh and decreased the extent of both Fe(III) and Sb(V) reduction, and shifted the reduced products to mackinawite and Sb(III) adsorbed onto Fh, in addition to stibnite formation. This study demonstrates that while PO 4 3− may not directly compete with Sb(V) for sorption sites, it can influence Sb mobility in Fe(III)- and sulfate-reducing environments by enhancing microbial activity and altering the mineralization pathways.

Microbial Fe(III) and sulfate reduction↗

DOE OSTI2025

Surface Phase Stability of Fe 2 O 3 (001) in Hydrogen Reducing Environments: A DFT and XPS Analysis

Here, this study combines density functional theory (DFT) and ab initio thermodynamics calculations with X-ray photoelectron spectroscopy (XPS) investigations to identify the reduction properties of the Fe 2 O 3 (001) surface with implications for corrosion resistance, hydrogen transport, and energy safety. Ab initio thermodynamics modeling predicts fully hydroxylated surface stability across a broad range of pressures (1 × 10 –23 to 1 × 10 5 mbar) and temperatures below 700 K, consistent with previous experimental studies. Above 800 K, exposures to 1 × 10 –4 mbar H 2 , 1 × 10 –4 mbar O 2 , or 1 × 10 –4 mbar H 2 + 1 × 10 –4 mbar O 2 each yield unique XPS signals indicating a loss of −OH coverage, aligning with DFT predictions. Insight into the mechanism of reduction as a function of H 2 exposure is provided, as well as conditions that promote further reduction toward Fe 3 O 4 . Theoretical and experimental investigations indicate the ability to maintain the Fe 2 O 3 protective layer of iron oxides that have been exposed to H 2 environments by including trace amounts of aqueous O2.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

NASA NTRS1975

Holographic flow visualization within a rotating compressor blade row

Rapid double-pulsed holographic techniques were used to visualize the shock configurations in the tip region of a lightly loaded, high tip speed fan stage. The holograms showed the passage shock emanating from the blade leading edge, a moderately strong conical shock originating at the intersection of the part span shroud leading edge and the blade suction surface, and a second conical shock originating at the intersection of the part span shroud and the blade pressure surface. Due to a limited viewing angle, the bow waves upstream of the rotor could not be observed, and only limited details of the trailing edge shocks were obtained. Reasonable details of the shock patterns were obtained from holograms which were made without extensive rig modifications. Results indicate that larger viewing windows and and holographic plates would permit a wider viewing angle and give much more coverage of the regions of interest. Also, shorter time delay for double-pulsed holograms is also desirable, and would minimize blade movement and give clearer holograms.

Benser, W. A.↗

NASA NTRS1979

Lunar magnetic anomalies detected by the Apollo subsatellite magnetometers

Properties of lunar crustal magnetization thus far deduced from Apollo subsatellite magnetometer data are reviewed using two of the most accurate available magnetic anomaly maps, one covering a portion of the lunar near side and the other a part of the far side. The largest single anomaly found within the region of coverage on the near-side map correlates exactly with a conspicuous light-colored marking in western Oceanus Procellarum called Reiner Gamma. This feature is interpreted as an unusual deposit of ejecta from secondary craters of the large nearby primary impact crater Cavalerius. The mean altitude of the far-side anomaly gap is much higher than that of the near side map and the surface geology is more complex; individual anomaly sources have therefore not yet been identified. The mechanism of magnetization and the origin of the magnetizing field remain unresolved, but the uniformity with which the Reiner Gamma deposit is apparently magnetized, and the north-south depletion of magnetization intensity across a substantial portion of the far side, seem to require the existence of an ambient field, perhaps of global or larger extent.

Hood, L. L.↗

NASA NTRS1983

A preliminary global oceanic cloud climatology from satellite albedo observations

A predictive relationship is developed between over-ocean cloud system albedo and the cloud amount present, using as a data base ERB satellite microwave readings at 0.5-0.7 micron and the USAF three-dimensional nephanalysis archive. The ERB data provided global coverage at a resolution of 2.5 x 2.5 deg during the 1974-78 period. Regression analyses were performed on the amounts and albedos for several years of data for one month in order to detect seasonal variations. A logarithmic relationship was found between the cloud system albedo and cloud amount over the oceans, with negligible seasonal variance. The analysis is noted to apply only where low surface albedos are encountered, and further work to extend the study to continental vegetated areas is indicated.

Hughes, N. A.↗

NASA NTRS1992

Gravitational microlensing - The effect of a single lens and the impact of sparse sampling

Topics in gravitational microlensing are examined. One issue is that even in cases in which the surface mass density is quite low, microlensing events cannot be considered as caused by individual stars. Whenever a high-magnification event occurs, the quasar has crossed a caustic. These caustics, however, are complex structures even for low surface-mass densities. This is illustrated by removing a single low-mass star from an ensemble of microlenses. The magnification patterns and light curves are compared with and without this star. The differences are striking and much more complex than expected. The effect of sparse sampling on the perception of microlensed light curves is examined, and attention is given to the influence of poor time coverage on simulated light curves. A regular monitoring program for microlensing candidates (especially 2237 + 0305) with a dedicated telescope is needed to make observations in different wavebands each night.

Wambsganss, Joachim↗

NASA NTRS2008

Retrieval with Infrared Atmospheric Sounding Interferometer and Validation during JAIVEx

A state-of-the-art IR-only retrieval algorithm has been developed with an all-season-global EOF Physical Regression and followed by 1-D Var. Physical Iterative Retrieval for IASI, AIRS, and NAST-I. The benefits of this retrieval are to produce atmospheric structure with a single FOV horizontal resolution (approx. 15 km for IASI and AIRS), accurate profiles above the cloud (at least) or down to the surface, surface parameters, and/or cloud microphysical parameters. Initial case study and validation indicates that surface, cloud, and atmospheric structure (include TBL) are well captured by IASI and AIRS measurements. Coincident dropsondes during the IASI and AIRS overpasses are used to validate atmospheric conditions, and accurate retrievals are obtained with an expected vertical resolution. JAIVEx has provided the data needed to validate the retrieval algorithm and its products which allows us to assess the instrument ability and/or performance. Retrievals with global coverage are under investigation for detailed retrieval assessment. It is greatly desired that these products be used for testing the impact on Atmospheric Data Assimilation and/or Numerical Weather Prediction.

Zhou, Daniel K.↗

NASA NTRS2010

Updates of Land Surface and Air Quality Products in NASA MAIRS and NEESPI Data Portals

Following successful support of the Northern Eurasia Earth Sciences Partner Initiative (NEESPI) project with NASA satellite remote sensing data, from Spring 2009 the NASA GES DISC (Goddard Earth Sciences Data and Information Services Center) has been working on collecting more satellite and model data to support the Monsoon Asia Integrated Regional Study (MAIRS) project. The established data management and service infrastructure developed for NEESPI has been used and improved for MAIRS support.Data search, subsetting, and download functions are available through a single system. A customized Giovanni system has been created for MAIRS.The Web-based on line data analysis and visualization system, Giovanni (Goddard Interactive Online Visualization ANd aNalysis Infrastructure) allows scientists to explore, quickly analyze, and download data easily without learning the original data structure and format. Giovanni MAIRS includes satellite observations from multiple sensors and model output from the NASA Global Land Data Assimilation System (GLDAS), and from the NASA atmospheric reanalysis project, MERRA. Currently, we are working on processing and integrating higher resolution land data in to Giovanni, such as vegetation index, land surface temperature, and active fire at 5km or 1km from the standard MODIS products. For data that are not archived at the GESDISC,a product metadata portal is under development to serve as a gateway for providing product level information and data access links, which include both satellite, model products and ground-based measurements information collected from MAIRS scientists.Due to the large overlap of geographic coverage and many similar scientific interests of NEESPI and MAIRS, these data and tools will serve both projects.

Shen, Suhung↗

NASA NTRSDate not supplied

Assessment of Cloud Fraction Derived from a New Geostationary Satellite Cloud Retrieval Algorithm for CERES and Progress Towards Cross-platform Continuity

For over two decades The Clouds and the Earth’s Radiant Energy System (CERES) project has produced long-term records of top-of-atmosphere (TOA) and surface irradiances for detecting changes in the Earth’s radiation budget and advancing understanding of how clouds contribute to those changes. Accurate characterization of the spatial and temporal distributions of clouds are a critical component for producing CERES datasets. The CERES Cloud Working Group (CWG) derives cloud properties from both geostationary (GEO) and low-Earth orbit (LEO) satellite sensors in order to provide complete global coverage at hourly temporal resolution. However, the use of multiple sensors to provide this spatiotemporal coverage throughout a long-term record presents some challenges, because the various sensors generally have different spectral band characteristics (e.g., spectral band width and response) and spatial resolution. These differences can result in spatial artifacts at the coverage boundary between two sensors or temporal artifacts when one sensor replaces another in the record. For the upcoming Edition 5 release of CERES products, the CWG is developing cloud retrieval algorithms which utilize only spectral bands common to most modern passive satellite radiometers and account for differences in spectral width and response. The goal with this approach is to provide global cloud properties for CERES with greater cross-platform consistency than the previous Edition 4 products and thus mitigate artifacts which are evident at the interface of two sensors. This study focuses on retrieval of total cloud fraction from various GEO sensors, and we use Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) observations to assess the accuracy of total cloud fraction derived from the various sensors. The Edition 5 cloud mask algorithm depends on estimates of cloud-free TOA spectral radiances to differentiate clear and cloudy conditions, and CALIOP is used to assess the accuracy of those estimates when cloud-free conditions are indeed observed.

CALIOP↗

DOE OSTI2020

Critical Hydrogen Coverage Effect on the Hydrogenation of Ethylene Catalyzed by δ-MoC(001): An Ab Initio Thermodynamic and Kinetic Study

Highly selective oxidation of methane to methanol has long been challenging in catalysis. Here, we reveal key steps for the promotion by water when tuning the selectivity of a well-defined CeO 2 /Cu 2 O/Cu(111) catalyst from CO and CO 2 to methanol under a reaction environment with methane, oxygen, and water. Ambient-pressure x-ray photoelectron spectroscopy showed that water added to CH 4 and O 2 led to surface CH 3 O and accelerated methanol production. These results were consistent with density functional theory calculations and kinetic Monte Carlo simulations which showed that water preferentially dissociates over the active Ce ions at the CeO 2 -Cu 2 O/Cu(111) interface. The adsorbed OH blocked O-O bond cleavage that would dehydrogenate CH 3 O to CO and CO 2 , and it directly converted this species to methanol, while O 2 now reoxidized the reduced surface. Water adsorption also displaced the produced methanol into the gas phase.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Facet-Dependent Water Inhibition of Alkanol Dehydration on TiO2 via Distinct Water–Alkanol Complexes

Water is ubiquitous in biomass-derived feeds, yet its molecular impact on oxygen-elimination reactions remains poorly understood, particularly for catalysts exposing different facets. Here, we utilize well-defined TiO2 nanocrystals with dominant (101) and (001) facets to reveal a pronounced facet-dependent effect of water, where inhibition for dehydration of isopropanol (IPA) on the TiO2(001) surface is about four times more severe than TiO2(101). Through a combination of in situ solid state NMR, in situ infrared spectroscopy, kinetics studies, and theoretical calculations, we demonstrate that this disparity arises from the formation of distinct alkanol-water complex intermediates. On TiO2(001), IPA undergoes dissociative adsorption to form an isopropoxide-H2O complex that readily drives the surface into a complex-dominated regime. This pathway increases the activation barrier for C–H cleavage by 40 kJ mol-1 by inducing a disordered transition state. In contrast, TiO2(101) favors molecular IPA adsorption with weak hydrogen bonding to water, resulting in a smaller complex formation constant and a much smaller activation barrier increase (25 kJ mol-1). By quantitatively linking facet-dependent complex coverage to transition-state destabilization, this work moves beyond simple site-blocking models and provides a conceptual framework for designing catalysts that remain active in water-containing environments

Hu, Wenda↗

DOE OSTI2025

From Micro-environments to Macroscopic Effects: How the Alkaline Hydrogen Evolution Reaction Drives Cu Cathodic Corrosion

Cathodic corrosion of copper (Cu) has posed a significant challenge for over a century, impeding various technological progresses such as electrochemical conversion of CO 2 (eCO 2 RR) into fuels and other value-added carbon products. Here, in this study, employing a combined Density Functional Theory (DFT) and kinetic Monte Carlo (kMC) simulation approach, we delve into the atomistic level mechanism driving this phenomenon in Cu. Our hypothesis posits the pivotal role of alkaline hydrogen evolution reaction (HER) in facilitating cathodic corrosion in Cu. We rigorously develop a pH-dependent hydroxide (OH) adsorption mechanism and calculate the equilibrium OH coverage (𝜃 OH ) at varying pH levels, the thermodynamic stability of subsurface oxygen (O sub ), as well as the Cu-vacancy mediated diffusion of subsurface oxygens (O sub ). Through comprehensive analysis, we establish correlation among various microenvironments, including oxygen diffusion in subsurface layers, pH-dependent OH adsorption, and Cu dissolution into the electrolyte as (Cu-OH) complexes. Furthermore, our investigation explores the correlation between surface coordination environment of active sites and cathodic corrosion of Cu. Finally, by integrating DFT-derived thermodynamic data into a kMC model, we successfully predict the formation of experimentally observed corrosion pits on Cu-surfaces. This combined approach not only advances our fundamental understanding of Cu cathodic corrosion but also offers insights crucial for developing effective corrosion mitigation strategies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1999

GPS Altimetry

The advent of satellite altimetry has greatly improved our ability to observe global ocean circulation. However, the swath of a single, nadir-viewing satellite altimeter is only a few km and the track spacing is several hundred km to resolve the two-dimensional structure of ocean eddies. Our goal is to increase spatial and temporal coverage by monitoring Global Positioning System (GPS) signals reflected from the ocean. A constellation of spacecraft would each carry a GPS receiver capable of recording 8 reflections simultaneously. The reflections are well distributed in azimuth and elevation and can be tracked continuously while the satellite is in view, and another is then acquired, as illustrated below. The diagram depicts a new approach at altimetry measurements where ocean surface reflected GPS signals are simultaneously tracked and processed in a GPS flight receiver in space. The reflected GPS signals from the ocean must be compared precisely with the direct GPS signals in order to infer the characteristics of the ocean from the combined data set. Understanding the features and accuracy of GPS altimetry measurement is crucial to establishing its suitability for oceanography. Preliminary work has enabled us to theoretically model the signal output of the correlator for a variety of system parameters such as wind speed (sea roughness), receiver height, incidence angle, receiver range and Doppler filter bandwidth and antenna gain. Expected signal-to-noise ratio has been estimated from which we have inferred, to a first approximation, the basic receiver gain requirements for a space-based altimeter and the expected range raw error. In 1998, work on a different task led to the extraction of the first reflected GPS signal observed from a spaceborne receiver during the 1995 Space Transportation System-68 (STS-68) Shuttle Radar Laboratory-2 (SRL-2) high resolution synthetic aperture radar mission. Good comparisons with our signal models have been obtained. Having established that only modest signal-to-noise ratios are obtainable unless very high gain antennas are used, we expect that single measurements might not provide an estimate of sea state parameters as accurate as that obtainable with traditional remote sensing instruments, if costs are limited. Therefore spatial and temporal averaging of many measurements is required. Since the receiving satellite tracks do not repeat, measurements in a given area will be used to refine the local solution as a function of time, and will define the spatial resolution. In order to make this instrument viable in space, we need to detect and process many scattered signals. In 1998 we made a first step at understanding what configurations of antenna gain and orientations capture the largest number of viable signals to be used in the subsequent spatial/temporal averaging process. Additional information is contained in the original.

Lichten, Stephen M.↗

NASA NTRS2010

Far-IR Measurements at Cerro Toco, Chile: FIRST, REFIR, and AERI

In mid-2009, the Radiative Heating in the Underexplored Bands Campaign II (RHUBC-II) was conducted from Cerro Toco, Chile, a high, dry, remote mountain plateau, 23degS , 67.8degW at 5.4km, in the Atacama Desert of Northern Chile. From this site, dominant IR water vapor absorption bands and continuum, saturated when viewed from the surface at lower altitudes, or in less dry locales, were investigated in detail, elucidating IR absorption and emission in the atmosphere. Three FTIR instruments were at the site, the Far-Infrared Spectroscopy of the Troposphere (FIRST), the Radiation Explorer in the Far Infrared (REFIR), and the Atmospheric Emitted Radiance Interferometer (AERI). In a side-by-side comparison, these measured atmospheric downwelling radiation, with overlapping spectral coverage from 5 to100um (2000 to 100/cm), and instrument spectral resolutions from 0.5 to 0.64/cm, unapodized. In addition to the FTIR and other ground-based IR and microwave instrumentation, pressure/temperature/relative humidity measuring sondes, for atmospheric profiles to 18km, were launched from the site several times a day. The derived water vapor profiles, determined at times matching the FTIR measurement times, were used to model atmospheric radiative transfer. Comparison of instrument data, all at the same spectral resolution, and model calculations, are presented along with a technique for determining adjustments to line-by-line calculation continuum models. This was a major objective of the campaign.

Cageao, Richard P.↗

DOE OSTI2024

iButton snow-ground interface temperature measurements in Los Alamos, New Mexico from 2023-2024

Snow/ground interface temperature measurements were collected at two sites in Los Alamos, New Mexico. Data were collected from November 29, 2023 to April 8, 2024 using iButton Link DS1921G-F5# Thermochron miniature temperature sensors (https://www.ibuttonlink.com/products/ds1921g). These sensors are a cost-efficient way to collect snowpack temperatures at a higher spatial resolution than what is normally achieved. iButton data were collected every 3 hours from a total of 19 iButtons. iButtons were placed in pairs, with one iButton placed at the ground surface and another buried 1 - 5 cm below the ground surface. One buried iButton did not successfully collect data, and therefore was excluded from this dataset. Data were collected throughout the snow cover season so that snowpack characteristics could be derived using the temperature data. Specifically, this dataset was used as a validation source for a novel machine learning approach to estimating snow depth (see related publication). Sensors were placed in areas with bare ground or minimal grass coverage, located away from any large vegetation. At Site A (TA51), manual snow depths were collected as validation data. These measurements were taken next to iButtons periodically throughout the winter, and notes on other precipitation types were also recorded. At Site B (TA6 Meteorological Station), a nearby sensor collected snow depths throughout the winter. This dataset contains one *.csv file of snow/ground interface temperatures at two sites, one *.csv file of manually collected snow depths, and one *.kml file of sensor locations. The Next-Generation Ecosystem Experiments: Arctic (NGEE Arctic) was a 15-year research effort (2012-2027) to reduce uncertainty in Earth System Models by developing a predictive understanding of carbon-rich Arctic ecosystems and feedbacks to climate. NGEE Arctic was supported by the Department of Energy’s Office of Biological and Environmental Research.The NGEE Arctic project had two field research sites: 1) located within the Arctic polygonal tundra coastal region on the Barrow Environmental Observatory (BEO) and the North Slope near Utqiagvik (Barrow), Alaska and 2) multiple areas on the discontinuous permafrost region of the Seward Peninsula north of Nome, Alaska.Through observations, experiments, and synthesis with existing datasets, NGEE Arctic provided an enhanced knowledge base for multi-scale modeling and contributed to improved process representation at global pan-Arctic scales within the Department of Energy’s Earth system Model (the Energy Exascale Earth System Model, or E3SM), and specifically within the E3SM Land Model component (ELM).

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Towards Realistic Models of Heterogeneous Catalysis: Simulations of Oxidation Catalysis from First Principles

Among the most significant developments in heterogeneous catalysis in the last 20 years is the emergence of microkinetic models, often parameterized from density functional theory (DFT) calculations, used to quantify observed catalyst performance and to guide the discovery of new catalytic materials. While DFT directly reports binding energies and elementary step activation energies, the free energies that enter into microkinetic models must be computed from additional approximations. Frequently these free energy approximations assume ideal behavior—that adsorbates do not interact with one another, or that adsorbates are immobile or vibrate harmonically about a binding site. These assumptions can and do have an impact on predicted catalyst performance and potentially even on predicted trends. Our work relates to three categories of non-idealities, explored in the context of nitrogen oxidation and reduction catalysis on metal surfaces. One component relates to adsorbate translational free energy, the contribution least well described by conventional models, in which we develop modeling approaches that improve accuracy with limited increase in computational expense. A second component relates adsorbate-adsorbate interactions, in which we develop benchmark on-lattice interaction models and compare kinetic predictions with conventional mean-field models, in an effort to develop more robust coverage-dependent mean field modeling approaches. The last relates the most fundamental assumption of all—that of energy equipartition—in an effort to rationalize and guide plasma-enhanced catalysis.

99 GENERAL AND MISCELLANEOUS↗

NASA NTRS1978

The Earth Radiation Budget Satellite System

The scientific objectives of an Earth Radiation Budget Satellite System (ERBSS) are discussed along with the associated data analysis methods, mission analysis, and the instrument systems. High resolution data on the scale of about 250 km over the entire globe are essential to gain insight into such features as the development of sea-surface temperature anomalies, radiation effects of ice and snow cover on the atmospheric circulation, albedo variation in the desert-vegetation boundaries, and major long-period circulation phenomena. The ERBSS experiment is also viewed as a precursor of an operational satellite system for monitoring the earth's radiation budget. Various numbers of satellites and orbit inclinations have been analyzed to define the satellite combination which provides sufficient coverage of the earth for spatial and temporal radiation sampling.

Woerner, C. V.↗

NASA NTRS1989

Sampling characteristics of satellite orbits

The irregular space-time sampling of any finite region by an orbiting satellite raises difficult questions as to which frequencies and wavenumbers can be determined and which will alias into others. Conventional sampling theorems must be extended to account for both irregular data distributions and observational noise - the sampling irregularity making the system much more susceptible to noise than in regularly sampled cases. The problem is formulated here in terms of least-squares and applied to spacecraft in 10-day and 17-day repeating orbits. The 'diamond-pattern' laid down spatially in such repeating orbits means that either repeat period adequately samples the spatial variables, but the slow overall temporal coverage in the 17-day pattern leads to much greater uncertainty than in the shorter repeat cycle. The result is not definitive and it is not concluded that a 10-day orbit repeat is the most appropriate one. A major conclusion, however, is that different orbital choices have potentially quite different sampling characteristics which need to be analyzed in terms of the spectral characteristics of the moving sea surface.

Wunsch, Carl↗