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DOE OSTI2021

Exploring the Potential of Using Carbonyl Sulfide to Track the Urban Biosphere Signal

Abstract Cities are implementing additional urban green as a means to capture CO 2 and become more carbon neutral. However, cities are complex systems where anthropogenic and natural components of the CO 2 budget interact with each other, and the ability to measure the efficacy of such measures is still not properly addressed. There is still a high degree of uncertainty in determining the contribution of the vegetation signal, which furthermore confounds the use of CO 2 mole fraction measurements for inferring anthropogenic emissions of CO 2 . Carbonyl sulfide (OCS) is a tracer of photosynthesis which can aid in constraining the biosphere signal. This study explores the potential of using OCS to track the urban biosphere signal. We used the Sulfur Transport and dEposition Model (STEM) to simulate the OCS concentrations and the Carnegie Ames Stanford Approach ecosystem model to simulate global CO 2 fluxes over the Bay Area of San Francisco during March 2015. Two observation towers provided measurements of OCS and CO 2 : The Sutro tower in San Francisco (upwind from the area of study providing background observations), and a tower located at Sandia National Laboratories in Livermore (downwind of the highly urbanized San Francisco region). Our results show that the STEM model works better under stable marine influence, and that the boundary layer height and entrainment are driving the diurnal changes in OCS and CO 2 at the downwind Sandia site. However, the STEM model needs to better represent the transport and boundary layer variability, and improved estimates of gross primary productivity for characterizing the urban biosphere signal are needed.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

BioRT‐HBV 1.0: A Biogeochemical Reactive Transport Model at the Watershed Scale

Abstract Reactive Transport Models (RTMs) are essential tools for understanding and predicting intertwined ecohydrological and biogeochemical processes on land and in rivers. While traditional RTMs have focused primarily on subsurface processes, recent watershed‐scale RTMs have integrated ecohydrological and biogeochemical interactions between surface and subsurface. These emergent, watershed‐scale RTMs are often spatially explicit and require extensive data, computational power, and computational expertise. There is however a pressing need to create parsimonious models that require minimal data and are accessible to scientists with limited computational background. To that end, we have developed BioRT‐HBV 1.0, a watershed‐scale, hydro‐biogeochemical RTM that builds upon the widely used, bucket‐type HBV model known for its simplicity and minimal data requirements. BioRT‐HBV uses the conceptual structure and hydrology output of HBV to simulate processes including advective solute transport and biogeochemical reactions that depend on reaction thermodynamics and kinetics. These reactions include, for example, chemical weathering, soil respiration, and nutrient transformation. The model uses time series of weather (air temperature, precipitation, and potential evapotranspiration) and initial biogeochemical conditions of subsurface water, soils, and rocks as input, and output times series of reaction rates and solute concentrations in subsurface waters and rivers. This paper presents the model structure and governing equations and demonstrates its utility with examples simulating carbon and nitrogen processes in a headwater catchment. As shown in the examples, BioRT‐HBV can be used to illuminate the dynamics of biogeochemical reactions in the invisible, arduous‐to‐measure subsurface, and their influence on the observed stream or river chemistry and solute export. With its parsimonious structure and easy‐to‐use graphical user interface, BioRT‐HBV can be a useful research tool for users without in‐depth computational training. It can additionally serve as an educational tool that promotes pollination of ideas across disciplines and foster a diverse, equal, and inclusive user community.

Sadayappan, Kayalvizhi↗

DOE OSTI2022

Potential use of engineered nanoparticles in ocean fertilization for large-scale atmospheric carbon dioxide removal

Artificial ocean fertilization (AOF) aims to safely stimulate phytoplankton growth in the ocean and enhance carbon sequestration. AOF carbon sequestration efficiency appears lower than natural ocean fertilization processes due mainly to the low bioavailability of added nutrients, along with low export rates of AOF-produced biomass to the deep ocean. Here we explore the potential application of engineered nanoparticles (ENPs) to overcome these issues. Data from 123 studies show that some ENPs may enhance phytoplankton growth at concentrations below those likely to be toxic in marine ecosystems. ENPs may also increase bloom lifetime, boost phytoplankton aggregation and carbon export, and address secondary limiting factors in AOF. Life-cycle assessment and cost analyses suggest that net CO 2 capture is possible for iron, SiO 2 and Al 2 O 3 ENPs with costs of 2–5 times that of conventional AOF, whereas boosting AOF efficiency by ENPs should substantially enhance net CO 2 capture and reduce these costs. Therefore, ENP-based AOF can be an important component of the mitigation strategy to limit global warming.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Sulfide electrolyte additive enables multi-ionic transfer pathways in alkaline iron redox

Traditional alkaline iron (Fe) batteries rely on the conversion reaction between Fe and Fe(OH) 2 but suffer from hydrogen generation upon Fe formation on charging. Fe 2+ /Fe 3+ redox is a promising anode reaction for alkaline Fe batteries, as it alleviates the formation of hydrogen gas during charging. However, achieving complete Fe 2+ /Fe 3+ redox with a one-electron transfer reaction is challenging due to the formation of electrochemically inert Fe 3 O 4 materials. Here, we demonstrate that an alkaline sulfide-containing electrolyte facilitates the reversible multi-ion transfer and transport pathways within (and beyond) the Fe 2+ /Fe 3+ redox system, including Fe(OH) 2 /Fe 3 O 4 conversion, intercalation of hydrosulfide into layered Fe(OH) 2 , and hydrogen deposition, mediated by hydroxyl ions, hydrosulfide anions, and protons, respectively. This multi-ionic charge storage mechanism delivers a compelling discharge capacity of up to 330 mA h g −1 , as determined by chronopotentiometry measurements at a current density of 0.1 A g −1 , exceeding the theoretical iron redox capacity solely relying on Fe 2+ /Fe 3+ redox (∼299 mA h g −1 ). Our study will highlight the potential of alkaline iron redox as a green anode reaction for various aqueous energy storage systems by utilizing a scalable and low-concentration hydrosulfide electrolyte additive.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Spontaneous emulsification induced by nanoparticle surfactants

Microemulsions, mixtures of oil, water, and surfactant, are thermodynamically stable. Unlike conventional emulsions, microemulsions form spontaneously, have a monodisperse droplet size that can be controlled by adjusting the surfactant concentration, and do not degrade with time. To make microemulsions, a judicious choice of surfactant molecules must be made, which significantly limits their potential use. Nanoparticle surfactants, on the other hand, are a promising alternative because the surface chemistry needed to make them bind to a liquid-liquid interface is both well flexible and understood. Here, we derive a thermodynamic model predicting the conditions in which nanoparticle surfactants drive spontaneous emulsification that agrees quantitatively with experiments using Noria nanoparticles. This new class of microemulsions inherits the mechanical, chemical, and optical properties of the nanoparticles used to form them, leading to novel applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Detecting low-mass perturbers in cluster lenses using curved arc bases

ABSTRACT Strong gravitationally lensed arcs produced by galaxy clusters have been observationally detected for several decades now. These strong lensing constraints provided high-fidelity mass models for cluster lenses that include substructure down to $10^{9{-}10}\, \mathrm{M}_\odot$. Optimizing lens models, where the cluster mass distribution is modelled by a smooth component and subhaloes associated with the locations of individual cluster galaxies, has enabled deriving the subhalo mass function, providing important constraints on the nature and granularity of dark matter. In this work, we explore and present a novel method to detect and measure individual perturbers (subhaloes, line-of-sight haloes, and wandering supermassive black holes) by exploiting their proximity to highly distorted lensed arcs in galaxy clusters, and by modelling the local lensing distortions with curved arc bases. This method offers the possibility of detecting individual low-mass perturber subhaloes in clusters and haloes along the line of sight down to a mass resolution of $10^8\, \mathrm{M}_\odot$. We quantify our sensitivity to low-mass perturbers ($M\sim 10^{7{-}9}\, \mathrm{M}_\odot$) in clusters (M ∼ 1014–15 M⊙), by creating realistic mock data. Using three lensed images of a background galaxy in the cluster SMACS J0723, taken by JWST, we study the retrieval of the properties of potential perturbers with masses $M=10^{7{-}9}\, \mathrm{M}_\odot$. From the derived posterior probability distributions for the perturber, we constrain its concentration, redshift, and ellipticity. By allowing us to probe lower mass substructures, the use of curved arc bases can lead to powerful constraints on the nature of dark matter as discrimination between dark matter models appears on smaller scales.

Astronomy & Astrophysics↗

DOE OSTI2020

A Predictive Model for Survival of Escherichia coli O157:H7 and Generic E. coli in Soil Amended with Untreated Animal Manure

Abstract This study aimed at developing a predictive model that captures the influences of a variety of agricultural and environmental variables and is able to predict the concentrations of enteric bacteria in soil amended with untreated Biological Soil Amendments of Animal Origin (BSAAO) under dynamic conditions. We developed and validated a Random Forest model using data from a longitudinal field study conducted in mid‐Atlantic United States investigating the survival of Escherichia coli O157:H7 and generic E. coli in soils amended with untreated dairy manure, horse manure, or poultry litter. Amendment type, days of rain since the previous sampling day, and soil moisture content were identified as the most influential agricultural and environmental variables impacting concentrations of viable E. coli O157:H7 and generic E. coli recovered from amended soils. Our model results also indicated that E. coli O157:H7 and generic E. coli declined at similar rates in amended soils under dynamic field conditions.The Random Forest model accurately predicted changes in viable E. coli concentrations over time under different agricultural and environmental conditions. Our model also accurately characterized the variability of E. coli concentration in amended soil over time by providing upper and lower prediction bound estimates. Cross‐validation results indicated that our model can be potentially generalized to other geographic regions and incorporated into a risk assessment for evaluating the risks associated with application of untreated BSAAO. Our model can be validated for other regions and predictive performance also can be enhanced when data sets from additional geographic regions become available.

Pang, Hao↗

DOE OSTI2025

Stable, Efficient Iron Electrodeposition via Anion-Directed Control of Fe(II) Coordination

Traditional steelmaking processes consume about 7% of the world’s energy supply, with reduction of iron oxides into iron via blast furnaces representing the most energy-demanding and capital-intensive step. To economize and modularize iron reduction processes, we aim to develop an electrodeposition technique to reduce aqueous iron ions to metallic iron. However, the hydrogen reduction reaction (HER) occurs at a more positive standard reduction potential than the iron reduction reaction. In addition, aqueous Fe(II) cations easily precipitate at mildly acidic conditions (pH ≥ 3), which limits the deposition efficiency and degrades deposit quality. To address these challenges, we first search for anions that have intermediate coordination strength with Fe(II) based on the hard-soft acid-base theory, trading a slightly more negative Fe(II) reduction potential for a considerably broader pH stability range. We select citrate with predicted intermediate coordination strength, in combination with more weakly coordinating anions (e.g., SO 4 2- , Cl - ) to control the coordination structure of Fe 2+ for improved electrolyte stability and electrodeposition behavior. We find that citrate coordination stabilizes Fe 2+ -based electrolytes at higher pH conditions (4.8–5.5), significantly extending their shelf life while also suppressing HER during Fe electrodeposition by orders of magnitude. To measure Faradaic efficiencies (FE), we developed a straightforward, titration-based methodology to quantify the amount of deposited iron regardless of the rate of concurrent HER. Although coordination between citrate and Fe 2+ decreases the reduction potential of Fe(II), high FE (≥98%) was achieved at 10 mA cm -2 . FE and achievable deposition rates are tunable by both concentration and the ratio of Fe 2+ to citrate. In all cases, Raman spectroscopy and X-ray diffraction (XRD) reveal that iron deposition in citrate-containing electrolytes suppresses iron oxide/hydroxide precipitation, in contrast to deposits generated in citrate-free electrolytes. Altogether, this work demonstrates that citrate-mediated anion coordination enables high-purity iron electrodeposition with increased FE, high current density, and improved electrolyte stability. This multi-anion coordination strategy provides a versatile framework for designing stable electrolyte and efficient metal electrodeposition.

coordination↗

DOE OSTI2022

Quantifying the inhibitory impact of soluble phenolics on anaerobic carbon mineralization in a thawing permafrost peatland

The mechanisms controlling the extraordinarily slow carbon (C) mineralization rates characteristic of Sphagnum -rich peatlands (“bogs”) are not fully understood, despite decades of research on this topic. Soluble phenolic compounds have been invoked as potentially significant contributors to bog peat recalcitrance due to their affinity to slow microbial metabolism and cell growth. Despite this potentially significant role, the effects of soluble phenolic compounds on bog peat C mineralization remain unclear. We analyzed this effect by manipulating the concentration of free soluble phenolics in anaerobic bog and fen peat incubations using water-soluble polyvinylpyrrolidone (“PVP”), a compound that binds with and inactivates phenolics, preventing phenolic-enzyme interactions. CO 2 and CH 4 production rates (end-products of anaerobic C mineralization) generally correlated positively with PVP concentration following Michaelis-Menten (M.M.) saturation functions. Using M.M. parameters, we estimated that the extent to which phenolics inhibit anaerobic CO 2 production was significantly higher in the bog—62 ± 16%—than the fen—14 ± 4%. This difference was found to be more substantial with regards to methane production—wherein phenolic inhibition for the bog was estimated at 54 ± 19%, while the fen demonstrated no apparent inhibition. Consistent with this habitat difference, we observed significantly higher soluble phenolic content in bog vs. fen pore-water. Together, these findings suggest that soluble phenolics could contribute to bogs’ extraordinary recalcitrance and high (relative to other peatland habitats) CO 2 :CH 4 production ratios.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2023

Resolving intragranular stress fields in plastically deformed titanium using point-focused high-energy diffraction microscopy

Abstract The response of a polycrystalline material to a mechanical load depends not only on the response of each individual grain, but also on the interaction with its neighbors. These interactions lead to local, intragranular stress concentrations that often dictate the initiation of plastic deformation and consequently the macroscopic stress–strain behavior. However, very few experimental studies have quantified intragranular stresses across bulk, three-dimensional volumes. In this work, a synchrotron X-ray diffraction technique called point-focused high-energy diffraction microscopy (pf-HEDM) is used to characterize intragranular deformation across a bulk, plastically deformed, polycrystalline titanium specimen. The results reveal the heterogenous stress distributions within individual grains and across grain boundaries, a stress concentration between a low and high Schmid factor grain pair, and a stress gradient near an extension twinning boundary. This work demonstrates the potential for the future use of pf-HEDM for understanding the local deformation associated with networks of grains and informing mesoscale models. Graphical abstract

36 MATERIALS SCIENCE↗

DOE OSTI2020

Experimental Investigation on Separation Behavior of Heavy-Oil Emulsion for Polymer Flooding on Alaska North Slope

The first-ever field pilot on Alaska North Slope (ANS) to validate using polymer floods for heavy-oil enhanced oil recovery is currently ongoing. One of the major concerns of the operator is the effect of polymer on oil/water-separation efficiency after polymer breakthrough. This work investigates the influence of polymer on the separation behavior of heavy-oil emulsions and evaluates the performance of emulsion breakers (EBs). In this study, two types of heavy-oil emulsions were prepared and tested at 20 and 50% water cut (WC), respectively. The bottle test method was used in the experiments, in which the separated water volume with time, the separated water quality, and the volume fraction of phases were recorded. Results showed that polymer accelerated the oil/water separation acting as an emulsion inhibitor at 20% WC but tended to impede the water separation at 50% WC. Regardless of WC, polymer resulted in poor water quality and the formation of a stable intermediate oil in water (o/w) emulsion, because of the increased viscosity of the water phase. The performance of EBs showed a complex dependency on the WC, the type of demulsifier and dosage, and the polymer concentration. Despite the varied conditions encountered in the heavy-oil/water/polymer/demulsifier system, a compound EB achieved satisfactory demulsification performance, showing the highest potential for deployment in the current ANS polymer flooding pilot. Here, we systematically studied the potential influence of polymer breakthrough on the separation behavior of heavy-oil emulsion on ANS for the first time. The findings of this study will provide practical guidance in advance for produced fluid treatment of the ongoing first-ever polymer flooding pilot on ANS.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Design Methods, Tools, and Data for Ceramic Solar Receivers Year 1 Continuation Report

This report describes the first year of work on a project to develop the methods, tools, and data required to analyze high temperature ceramic Concentrating Solar Power (CSP) components. This first year focused on developing the methods and data required for a time-independent assessment of potential components, focusing in particular on ceramic solar receivers. The report describes both model development and testing work focused on accomplishing this goal. Our overall conclusion is that high temperature ceramic CSP components are viable and could provide a means to overcome the expected low reliability and short service life for equivalent components constructed from Ni-based superalloys. Based on the results reported here, we recommend the project continue to Phase II which will develop more sophisticated, realistic models for time-dependent failure of ceramics operating in expected CSP component conditions and develop the time-dependent ceramic test data needed to parameterize these models, using commercial SiC as a reference material.

14 SOLAR ENERGY↗

DOE OSTI2023

Identification and Characterization of ten Escherichia coli Strains Encoding Novel Shiga Toxin 2 Subtypes, Stx2n as Well as Stx2j, Stx2m, and Stx2o, in the United States

The sharing of genome sequences in online data repositories allows for large scale analyses of specific genes or gene families. This can result in the detection of novel gene subtypes as well as the development of improved detection methods. Here, we used publicly available WGS data to detect a novel Stx subtype, Stx2n in two clinical E. coli strains isolated in the USA. During this process, additional Stx2 subtypes were detected; six Stx2j, one Stx2m strain, and one Stx2o, were all analyzed for variability from the originally described subtypes. Complete genome sequences were assembled from short- or long-read sequencing and analyzed for serotype, and ST types. The WGS data from Stx2n- and Stx2o-producing STEC strains were further analyzed for virulence genes pro-phage analysis and phage insertion sites. Nucleotide and amino acid maximum parsimony trees showed expected clustering of the previously described subtypes and a clear separation of the novel Stx2n subtype. WGS data were used to design OMNI PCR primers for the detection of all known stx1 (283 bp amplicon), stx2 (400 bp amplicon), intimin encoded by eae (221 bp amplicon), and stx2f (438 bp amplicon) subtypes. These primers were tested in three different laboratories, using standard reference strains. An analysis of the complete genome sequence showed variability in serogroup, virulence genes, and ST type, and Stx2 pro-phages showed variability in size, gene composition, and phage insertion sites. The strains with Stx2j, Stx2m, Stx2n, and Stx2o showed toxicity to Vero cells. Stx2j carrying strain, 2012C-4221, was induced when grown with sub-inhibitory concentrations of ciprofloxacin, and toxicity was detected. Taken together, these data highlight the need to reinforce genomic surveillance to identify the emergence of potential new Stx2 or Stx1 variants. The importance of this surveillance has a paramount impact on public health. Per our description in this study, we suggest that 2017C-4317 be designated as the Stx2n type-strain.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2020

Structure and Stability of Iron Fluoride at High Pressure–Temperature and Implication for a New Reservoir of Fluorine in the Deep Earth

Fluorine (F) is the most abundant halogen in the bulk silicate Earth. F plays an important role in geochemical and biological systems, but its abundance and distribution in the terrestrial mantle are still unclear. Recent studies suggested that F reservoirs in the deep mantle are potentially hosted in terrestrial oxide minerals, especially in aluminous bridgmanite. However, the knowledge about the formation and stability field of fluoride in the Earth’s interior is rare. In this study, we combine in situ laser-heated diamond anvil cell, synchrotron X-ray diffraction, and first-principles structure search to show that a new tetragonal structure of FeF 3 is stable at pressures of 78–130 GPa and temperatures up to ~1900 K. Simulation predicted the tetragonal phase takes a much denser structure due to the rotation of FeF 6 octahedral units. The equations of states of tetragonal FeF3 are determined by experiment and verified by simulation. Our results indicate that FeF 3 can be a potential key phase for storing F in the Earth’s lower mantle and may explain some mantle-derived magma with high F concentration.

58 GEOSCIENCES↗

DOE OSTI2025

Water Column Respiration in the Yakima River Basin is Explained by Temperature, Nutrients and Suspended Solids

Understanding aquatic ecosystem metabolism involves the study of two key processes: carbon fixation via primary production and organic C mineralization as total ecosystem respiration (ERtot). In streams and rivers, ERtot includes respiration in the water column (ERwc) and in the sediments (ERsed). While literature surveys suggest that ERsed is often a dominant contributor to ERtot, recent studies indicate that the relative influence of sediment-associated processes versus water column processes can fluctuate along the river continuum. Still, a comprehensive understanding of the factors contributing to these shifts within basins and across stream orders is needed. Here we contribute to this need by measuring ERwc and collecting water samples across 47 sites in the Yakima River basin, Washington, USA. We found that ERwc rates varied throughout the basin during baseflow conditions, ranging from –7.38 to 0.36 g O2 m?3 d?1, and encompassed the range of ERwc literature values. Additionally, by comparing to ERtot estimates for rivers across the contiguous United States, we suggest that the contribution of ERwc rates to reach-scale ERtot rates across the Yakima River was likely highly variable, but we did not test this directly. We observed that temperature, nutrient concentrations (dissolved organic carbon, total dissolved nitrogen), and total suspended solids explained 41% of ERwc variability across the basin. Our findings highlight the potential relevance of water column processes in aquatic ecosystem metabolism, with the Yakima River basin serving as an environmentally diverse river network representative of the larger Columbia River basin that spans much of the Pacific Northwest region of the United States. Our results are generally congruent with previous work, suggesting that the observed variability and suite of associated environmental factors influencing ERwc are potentially transferable across basins.

Laan, Maggi M.↗

NASA NTRS1981

Ni partitioning between diopside and silicate melt - A redetermination by ion microprobe and recognition of an experimental complication

The capabilities of and potential problems with ion microprobe analysis are illustrated in the determination of Ni distribution between silicate melt and diopside as a function of concentration. Samples of diopside and a melt in the albite-anorthite-diopside system were doped with Ni to levels of 5.22 and 1.08 wt % and 1060, 138, 42 and 30 ppm, and with 3 ppm of Ni-63, and characterized by both electron and ion microprobe techniques. Measurements of Ni-62 distribution by the ion probe method give a ratio of 1.87 for the ratio of count rates in the diopsides with the glass, which is slightly lower than the value of 2.05 obtained from beta-track mapping. The measurements required the secondary ion signal to be linear with concentration in the range measured, and a calibration to correct for differential secondary ion yields from different phases. It is found, however, that partition coefficients measured for Ni-58 and Ni-60 are not constant with Ni concentration, probably due to Ni migration during crystallization. The results thus show ion microprobe analyses to be feasible for simultaneous measurements of distributions of more than one element, and of elements inappropriate for beta-track mapping or electron probe analysis.

Steele, I. M.↗

NASA NTRS1983

Phosphine photochemistry in Saturn's atmosphere

The phosphine photochemistry on Saturn is studied with a 1D photochemical model. The PH3 concentration is rapidly depleted with height (scale height 3.5 km) in the upper troposphere. Formation of P, a probable precursor of P4, (a potential red chromophore in the atmosphere), is highly improbable unless the rate constant for the recombination reaction PH + H2 + M yields PH3 + M is less than 10 to the -41st cm exp 6/molecule-squared sec. Coupling of PH3 and hydrocarbon photochemistry, specifically the C2H2 catalyzed photodissociation of CH, is important. Column production rates of the organophosphorus compounds CH3PH2 and HCP of 3 x 10 to the 8th/sq cm sec are predicted, with potentially observable column densities of greater than 1 x 10 to the 17th/sq cm.

Kaye, J. A.↗

NASA NTRS1983

Meteorological and dynamical requirements for MST radar networks: Waves

Studies of wave motions using the MST radar have concentrated on single station time series analyses of gravity waves and tides. Since these radars collect high time resolution data they have the potential to become a significant tool for mesoscale research. In addition, radars are operated almost continuously unattended and, consequently, data sets are available for analyzing longer period wave motions such as tides and planetary scale waves. Although there is much to learn from single station data, the possibilities of new knowledge from a network of radars is exciting. The scales of wave motions in the atmosphere cover a broad range. Consequently the choice of a radar network depends to a large extent on the types of wave motions that are studied. There are many outstanding research problems that would benefit from observations from a MST radar network. In particular, there is a strong need for measurements of gravity wave parameters and equatorial wave motions. Some of the current problems in wave dynamics are discussed.

Avery, S. K.↗