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DOE OSTI2020

Assessment of Impurities in Neptunium Metal Using Double-Focusing SF-ICP-MS

In the transmutation process, minor actinides such as neptunium, americium and curium obtained from spent nuclear fuel are incorporated into new fuel that can be placed into a fast reactor, where these elements fission into products with shorter half-lives which reduces the health and safety hazards. In order to better understand the all the involved processes, fundamental physical properties of actinides should be investigated, and for that reason, high-purity materials need to be produced. One of the main challenges in characterizing these materials is the lack of pure metal available for study, and lack of analytical methods to determine the purity. Trans-uranic elements are challenging to study because of the need to be handled in specialized facilities, safeguards concerns and they are not easily purchased and/or produced. High-purity Np metal is being produced at the Materials and Fuels Complex (MFC) of Idaho National Laboratory (INL), in a process of direct oxide reduction developed by Squires and Lessing, with a target purity of 99.999%. The goal of this research is to develop methods to determine the impurities in the Np metal, with detection limits low enough to achieve this purity level. In this work, we have used several ICP-MS and ICP OES techniques, but the focus was the method development using a recently acquired Double-Focusing Sector Field Inductively Coupled Plasma Mass Spectrometer (SF-ICP-MS). To produce the Np metal, approximately 20 g of the neptunium oxide powder was calcined at 800 oC for 6 h in a magnesium oxide crucible, which is placed inside a stainless steel crucible, that goes into the Hot Uniaxial Press (HUP) furnace insert. After the calcining step, the Np oxide was mixed with approximately 9 g of calcium metal and 100 g of ultra-dry calcium chloride. The HUP furnace was heated in a ramp rate of 50 oC min -1 up to 1000 oC. When the reaction mixture reached 850 oC, a tantalum stirrer was activated at 100 rpm. After the tantalum stirrer was removed and the mixture cooled overnight, the MgO crucible was opened with a hammer and chisel to retrieve the Np metal button at the bottom of the reaction mixture. Prior to the dissolution process, the surface contaminants of the sample were removed. The Np button was washed in 10 mL of ultra-pure water for 1 min, with a faint reaction observed on the surface, indicating the presence of Ca metal. The water-washed sample was placed in a tube with 2 M HCl for only 3 s, as a vigorous reaction in the button surface was observed. The leachates were saved for further analysis. The sample was then rinsed with ultra-pure water and air-dried prior to dissolution. The cleaned sample was placed in a PTFE beaker and 25 mL of 6 M HCl and 150 µL of 24 M HF were added. After 10 minutes of reaction, the beaker was placed on a hot plate for 1 h and 30 min, followed by the addition of 1 mL of 16 M HNO3 and allowed to react for a further 1 h and 20 min. The sample was removed from heat and 10 mL of HNO3 16 M was added to react with the HCl. The beaker was covered and left for overnight reaction, producing a solution with approximately 20 mL of final volume. A Quadrupole Inductively Coupled Plasma Mass Spectrometer (Q-ICP-MS, Perkin Elmer ELAN DRC II Q-ICP-MS) was used to obtain qualitative mass spectra for the dissolution blank, each of the leachates and the dissolved sample. In the water leachate spectrum mainly Ca and Mg were observed, while the acid wash had a similar peak pattern to the one observed for the Np metal sample, indicating that the process not only removed surface contamination, but also reacted with the sample itself. In the Np material spectrum, Ta and actinides were identified as candidates for major contaminants, as the most intense peaks corresponded to the mass-to-charge ratios of these elements. Minor contaminants included Al, Au, Ca, Cr, Fe, I, Na, Nb, Pb, Sn, Ti, Tl, V, Y. The presence of impurities in the material could have originated from several sources, such as the materials used for the casting process, the use of impure NpO2 or contamination of reagents and materials used for the analysis. Some of the isotopes listed as potential contaminants are susceptible to spectral interferences, so Double-Focusing SF-ICP-MS (Nu Instruments Attom ES HR-ICP-MS) was used for the quantitative analysis. For each isotope determined, several items were evaluated: raw signal of a blank solution, sensitivity and determination coefficient of calibration curves, possibility of interferences and comparison of results obtained for at least two resolving powers (RP): 300 and 4000. The evaluation of the signal in a blank solution can indicate if a spectral interference from the plasma gas and/or the solvent was successfully resolved (commonly observed for 52Cr+/40Ar12C+, for example). It is important to highlight that a signal reduction is expected when a higher RP is used, as the ion beam transmission is decreased by the use of narrower slits

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Impact of Salinity on Ground Ice Distribution Across an Arctic Coastal Polygonal Tundra Environment

The heterogeneous distribution of ground ice in the Arctic is a key driver of uneven ground subsidence as permafrost thaws, significantly impacting infrastructure and surface/subsurface hydrology. These topographic and hydrological changes contribute to major uncertainties in energy and carbon fluxes and storage in a warming Arctic. This study aims to improve our understanding of the controls on ground ice and organic matter distribution within the top 3 m of permafrost in coastal polygonal tundra near Utqiagvik, Alaska. To this end, we apply a neural network approach to bulk density distributions derived from nondestructive X-ray tomography of soil cores, trained with laboratory analyses, to improve the resolution and spatial coverage of estimates of dry bulk density, ice content, and organic matter content. In addition, we use capacitively coupled geophysical imaging to map soil electrical conductivity and salinity variations. The results show that sedimentary deposits from ocean transgressions, along with subsequent ice wedge polygon geomorphological processes, jointly influence the distribution of ice content at various scales. The impact of the latter decreases with depth, whereas the influence of salinity and sedimentary history increases. Although the controls on the distribution of soil organic matter content (g/cm 3 ) remain unclear, the pronounced heterogeneity in bulk density strongly influences its calculation from laboratory mass fraction measurements (g/g). From a methodological perspective, the interdependencies among soil components and the need for increased data coverage underscore the value of high-resolution density measurements, such as using X-ray tomography. Overall, this study emphasizes the importance of considering salinity constraints on ice content distribution in coastal permafrost regions. The results are expected to aid in the development of data products and process representations in geomorphological and ecosystem models.

Dafflon, Baptiste [Lawrence Berkeley National Labo↗

DOE OSTI2026

Postanaerobic Digestion Manure Fibers as a Renewable Source of Lignin-Derived Aromatic Compounds for Microbial Upgrading

Abstract Postanaerobic digestion manure fibers are an abundant solid residue that remains underutilized. The substantial lignocellulosic content of digested manure opens the possibility of using it as a renewable resource for producing valuable products. In this study, we performed compositional and nuclear magnetic resonance analyses to determine lignin content and aromatic composition of these fibers. Additionally, alkaline-based treatment and reductive catalytic fractionation were evaluated as two different processes to produce aromatic-rich streams. The liquor from the alkaline treatment was subsequently utilized for microbial upgrading to produce 2-pyrone-4,6-dicarboxylic acid (PDC). The results showed that lignin in manure fibers represents 30% of the biomass (dry weight basis), with a ∼26% abundance of β-ether-linked aromatics and ∼13% p-coumarate moieties, indicating that the amount of lignin in the postanaerobic biomass is comparable to a moderately pretreated plant biomass. The alkaline treatment released 5.6 g aromatics/kg fibers, while reductive catalytic fractionation produced 14.0 g aromatics/kg fibers. A bioreactor operated in fed-batch mode produced a yield of ∼1 mol of PDC/mol measured aromatics at a rate of 0.2 g PDC/L·h and a titer of 2.6 g PDC/L. This study demonstrates how postanaerobic digestion manure fibers could be used in a circular bioeconomy by harnessing their lignocellulosic content to extract aromatic compounds and use them for obtaining valuable chemicals via microbial upgrading.

Riascos, Brayan D. [University of Wisconsin-Madiso↗

DOE OSTI2022

The Role of Groundwater Withdrawals on River Regulation: Example From the Columbia River Basin

The Columbia River Basin (CRB) is heavily regulated by more than 250 dams on its river system while depending significantly on groundwater withdrawals in certain sub-basins. Neglecting groundwater withdrawals in hydrologic models of the basin could result in inaccurate predictions of its water budget and thus mislead water management decisions in the basin. This work aims to understand the impacts of groundwater pumping on the spatiotemporal patterns of modeling regulated streamflow in the CRB using a modified version of the Variable Infiltration Capacity (VIC) model integrated with a water management component that accounts for groundwater withdrawals, irrigation demands, and reservoir operation (VIC-GIRR). The VIC-GIRR simulations showed that considering additional groundwater withdrawals would alleviate the stress of irrigation water deficit in the Snake River Basin with an average reduction of 10 km 3 /year. Such a reduction in water deficit resulted in slight streamflow increase over the CRB with maximum increase up to 40% during dry period in certain locations. We also note that the implementation of groundwater withdrawal does not, however, improve the overall model performance in long-term averaged streamflow and storage predictions. Our results highlight the efforts needed to examine additional important processes in representing the interactions between water withdrawals and reservoir operations. Such efforts will aid in better simulation of multi-reservoir system and improve effectiveness for agricultural productivity, power generation, flood control, and navigation purposes.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Permafrost thaw driven changes in hydrology and vegetation cover increase trace gas emissions and climate forcing in Stordalen Mire from 1970 to 2014

Permafrost thaw increases active layer thickness, changes landscape hydrology and influences vegetation species composition. These changes alter belowground microbial and geochemical processes, affecting production, consumption and net emission rates of climate forcing trace gases. Net carbon dioxide (CO 2 ) and methane (CH 4 ) fluxes determine the radiative forcing contribution from these climate-sensitive ecosystems. Permafrost peatlands may be a mosaic of dry frozen hummocks, semi-thawed or perched sphagnum dominated areas, wet permafrost-free sedge dominated sites and open water ponds. We revisited estimates of climate forcing made for 1970 and 2000 for Stordalen Mire in northern Sweden and found the trend of increasing forcing continued into 2014. The Mire continued to transition from dry permafrost to sedge and open water areas, increasing by 100% and 35%, respectively, over the 45-year period, causing the net radiative forcing of Stordalen Mire to shift from negative to positive. This trend is driven by transitioning vegetation community composition, improved estimates of annual CO 2 and CH 4 exchange and a 22% increase in the IPCC's 100-year global warming potential (GWP_100) value for CH 4 . These results indicate that discontinuous permafrost ecosystems, while still remaining a net overall sink of C, can become a positive feedback to climate change on decadal timescales.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1992

Resin transfer molding of textile preforms for aircraft structural applications

The NASA LaRC is conducting and supporting research to develop cost-effective fabrication methods that are applicable to primary composite aircraft structures. One of the most promising fabrication methods that has evolved is resin transfer molding (RTM) of dry textile material forms. RTM has been used for many years for secondary structures, but has received increased emphasis because it is an excellent method for applying resin to damage-tolerant textile preforms at low cost. Textile preforms based on processes such as weaving, braiding, knitting, stitching, and combinations of these have been shown to offer significant improvements in damage tolerance compared to laminated tape composites. The use of low-cost resins combined with textile preforms could provide a major breakthrough in achieving cost-effective composite aircraft structures. RTM uses resin in its lowest cost form, and storage and spoilage costs are minimal. Near net shape textile preforms are expected to be cost-effective because automated machines can be used to produce the preforms, post-cure operations such as machining and fastening are minimized, and material scrap rate may be reduced in comparison with traditional prepreg molding. The purpose of this paper is to discuss experimental and analytical techniques that are under development at NASA Langley to aid the engineer in developing RTM processes for airframe structural elements. Included are experimental techniques to characterize preform and resin behavior and analytical methods that were developed to predict resin flow and cure kinetics.

Hasko, Gregory H.↗

NASA NTRS1997

Spatial Distribution and Pattern Persistence of Surface Soil Moisture and Temperature Over Prairie from Remote Sensing

Images remotely sensed aboard aircraft during FIFE, namely, PBMR (microwave) soil moisture and NS001 thermal infrared surface temperature, were mapped on the same coordinate system covering the 20 km x 20 km experimental site. For both kinds of image data, the frequency distributions were close to symmetric, and the area average compared reasonably well with the ground based measurements. For any image on any given day, the correlation between the remotely sensed values and collocated ground based measurements over the area was usually high in the case of NS001 surface temperature but low in the case of PBMR soil moisture. On the other hand, at any given flux station the correlation between the PBMR and gravimetric soil moisture over all available days was usually high. The correlation pixel by pixel between images of PBMR on different days was generally high. The preservation of the spatial patterns of soil moisture was also evaluated by considering the correlation station by station between ground-based soil moisture measurements on different days; no persistence of spatial pattern was apparent during wet periods, but a definite pattern gradually established itself toward the end of each drying episode. The spatial patterns of surface temperature revealed by NS001 were not preserved even within a single day. The cross-correlations among the two kinds of images and the vegetation index NDVI were normally poor. This suggests that different processes of vegetation growth, and of the near-surface soil water and energy budgets.

Chen, Daoyi↗

NASA NTRS2000

Marangoni Effects on Near-Bubble Microscale Transport During Boiling of Binary Fluid Mixtures

In earlier investigations, Marangoni effects were observed to be the dominant mechanism of boiling transport in 2-propanol/water mixtures under reduced gravity conditions. In this investigation we have examined the mechanisms of binary mixture boiling by exploring the transport near a single bubble generated in a binary mixture between a heated surface and cold surface. The temperature field created in the liquid around the bubble produces vaporization over the portion of its interface near the heated surface and condensation over portions of its interface near the cold surface. Experiments were conducted using different mixtures of water and 2-propanol under 1g conditions and under reduced gravity conditions aboard the KC135 aircraft. Since 2-propanol is more volatile than water, there is a lower concentration of 2-propanol near the hot surface and a higher concentration of 2-propanol near the cold plate relative to the bulk quantity. This difference in interface concentration gives rise to strong Marangoni effects that move liquid toward the hot plate in the near bubble region for 2-propanol and water mixtures. In the experiments in this study, the pressure of the test system was maintained at about 5 kPa to achieve the full spectrum of boiling behavior (nucleate boiling, critical heat flux and film boiling) at low temperature and heat flux levels. Heat transfer data and visual documentation of the bubble shape were extracted from the experimental results. In the 1-g experiments at moderate to high heat flux levels, the bubble was observed to grow into a mushroom shape with a larger top portion near the cold plate due to the buoyancy effect. The shape of the bubble was somewhat affected by the cold plate subcooling and the superheat of the heated surface. At low superheat levels for the heated surface, several active nucleation sites were observed, and the vapor stems from them merged to form a larger bubble. The generation rate of vapor is moderate in this regime and the bubble shape is cylindrical in appearance. In some instances, the bubble interface appeared to oscillate. At higher applied heat flux levels, the top of the bubble became larger, apparently to provide more condensing interface area adjacent to the cold plate. Increasing the applied heat flux ultimately led to dry-out of the heated surface, with conditions just prior to dryout corresponding to the maximum heat flux (CHF). A more stable bubble was observed when the system attained the minimum heat flux (for film boiling). In this regime, most of the surface under the bottom of the bubble was dry with nucleate boiling sometimes occuring around the contact perimeter of the bubble at heated surface. Different variations (e.g. gap between two plates, molar concentration of the liquid mixture) of the experiments were examined to determine parametric effects on the boiling process and to determine the best conditions for the KC135 reduced gravity tests. Variation of the gap was found to have a minor impact on the CHF. However, reducing the gap between the hot and cold surface was observed to significantly reduce the minimum heat flux for fixed molar concentration of 2-propanol. In the reduced gravity experiments aboard the KC135 aircraft, the bubble formed in the 6.4 mm gap was generally cylindrical or barrel shaped and it increased its extent laterally as the surface superheat increased. In reduced gravity experiments, dryout of the heated surface under the bubble was observed to occur at a lower superheated temperature than for 1g conditions. Observed features of the boiling process and heat transfer data under reduced gravity will be discussed in detail. The results of the reduced gravity experiments will also be compared to those obtained in comparable 1g experiments. In tandem with the experiments we are also developing a computational model of the transport in the liquid surrounding the bubble during the boiling process. The computational model uses a level set method to model motion of the interface. It will incorporate a macroscale treatment of the transport in the liquid gap between the surfaces and a microscale treatment of transport in the regions between the bubble interface and the solid surfaces. The features of the model will be described in detail. Future research directions suggested by the results to date will also be discussed.

V. Carey↗

NASA NTRS2009

Treating Fibrous Insulation to Reduce Thermal Conductivity

A chemical treatment reduces the convective and radiative contributions to the effective thermal conductivity of porous fibrous thermal-insulation tile. The net effect of the treatment is to coat the surfaces of fibers with a mixture of transition-metal oxides (TMOs) without filling the pores. The TMO coats reduce the cross-sectional areas available for convection while absorbing and scattering thermal radiation in the pores, thereby rendering the tile largely opaque to thermal radiation. The treatment involves a sol-gel process: A solution containing a mixture of transition-metal-oxide-precursor salts plus a gelling agent (e.g., tetraethylorthosilicate) is partially cured, then, before it visibly gels, is used to impregnate the tile. The solution in the tile is gelled, then dried, and then the tile is fired to convert the precursor salts to the desired mixed TMO phases. The amounts of the various TMOs ultimately incorporated into the tile can be tailored via the concentrations of salts in the solution, and the impregnation depth can be tailored via the viscosity of the solution and/or the volume of the solution relative to that of the tile. The amounts of the TMOs determine the absorption and scattering spectra.

Zinn, Alfred↗

NASA NTRS2009

Sequential Imaging of Earth by Astronauts: 50 Years of Global Change

For nearly 50 years, astronauts have collected sequential imagery of the Earth. In fact, the collection of astronaut photography comprises one of the earliest sets of data (1961 to present) available to scientists to study the regional context of the Earth s surface and how it changes. While today s availability of global high resolution satellite imagery enables anyone with an internet connection to examine specific features on the Earth s surface with a regional context, historical satellite imagery adds another dimension (time) that provides researchers and students insight about the features and processes of a region. For example, one of the geographic areas with the longest length of record contained within the astronaut photography database is the lower Nile River. The database contains images that document the flooding of Lake Nasser (an analog to today s flooding behind China s Three Gorges Dam), the changing levels of Lake Nasser s water with multiyear cycles of flood and drought, the recent flooding and drying of the Toshka Lakes, as well as urban growth, changes in agriculture and coastal subsidence. The imagery database allows investigations using different time scales (hours to decades) and spatial scales (resolutions and fields of view) as variables. To continue the imagery collection, the astronauts on the International Space Station are trained to understand basic the Earth Sciences and look for and photograph major events such as tropical storms, landslides, and volcanic eruptions, and document landscapes undergoing change (e.g., coastal systems, cities, changing forest cover). We present examples of selected sequences of astronaut imagery that illustrate the interdependence of geological processes, climate cycles, human geography and development, and prompt additional questions about the underlying elements of change.

Evans, Cynthia A.↗

DOE OSTI2024

Cellulose molecular weight of corn stover with cotreatment

Here we present a dataset of cellulose molecular weights from corn stover after a cotreatment process. The corn stover sample was subjected to a combination of mechanical disruption (ball milling) and consolidated bioprocessing (CBP) process using the bacterium C. thermocellum at 60 grams/L solids loadings. Cellulose was isolated from control, no cotreatment control, and cotreatment corn stover. Cellulose was then derivatized using anhydrous pyridine and phenyl isocyanate over 48 h at 70 ºC. The reaction was quenched by anhydrous methanol. Methanol and water mixture (7:3, v/v) was added dropwise to promote precipitation of the cellulose derivative. The solids were collected by filtration and thoroughly washed with the methanol and water mixture followed by water. The cellulose derivative was dried overnight under vacuum at 40°C. The obtained cellulose tricarbanilates was then dissolved in tetrahydrofuran (THF) at 1.0 mg/mL and the solution was filtered through a 0.45 µm PTFE filter and placed in an auto-sampler vial. The molecular weight of cellulose was measured by Agilent GPC SECurity 1200 system equipped with four Waters Styragel columns (i.e., HR0.5, HR2, HR4, and HR6) and a UV detector (270 nm). THF was used as the mobile phase. Data collection and processing was performed by Polymer Standards Service WinGPC Unity software (Build 6807). The molecular weight was calculated relative to the polystyrene calibration curve. The data on molecular weights provided information about the effects of cotreatment on corn stover cellulose molecular changes.

Cellulose, molecular weights, corn stover, cotreat↗

NASA NTRS2006

Effects of Vegetation and of Heat and Vapor Fluxes from Soil on Snowpack Evolution and Radiobrightness

The radiobrightness of a snowpack is strongly linked to the snow moisture content profile, to the point that the only operational inversion algorithms require dry snow. Forward dynamic models do not include the effects of freezing and thawing of the soil beneath the snowpack and the effect of vegetation within the snow or above the snow. To get a more realistic description of the evolution of the snowpack, we reported an addition to the Snow-Soil-Vegetation-Atmosphere- Transfer (SSVAT) model, wherein we coupled soil processes of the Land Surface Process (LSP) model with the snow model SNTHERM. In the near future we will be adding a radiobrightness prediction based on the modeled moisture, temperature and snow grain size profiles. The initial investigations with this SSVAT for a late winter and early spring snow pack indicate that soil processes warm the snowpack and the soil. Vapor diffusion needs to be considered whenever the ground is thawed. In the early spring, heat flow from the ground into a snow and a strong temperature gradient across the snow lead to thermal convection. The buried vegetation can be ignored for a late winter snow pack. The warmer surface snow temperature will affect radiobrightness since it is most sensitive to snow surface characteristics. Comparison to data shows that SSVAT provides a more realistic representation of the temperature and moisture profiles in the snowpack and its underlying soil than SNTHERM. The radiobrightness module will be optimized for the prediction of brightness when the snow is moist. The liquid water content of snow causes considerable absorption compared to dry snow, and so longer wavelengths are likely to be most revealing as to the state of a moist snowpack. For volumetric moisture contents below about 7% (the pendular regime), the water forms rings around the contact points between snow grains. Electrostatic modeling of these pendular rings shows that the absorption of these rings is significantly higher than a sphere of the same volume. The first implementation of the radiobrightness module will therefore be a simple radiative transfer model without scattering.

soil↗

DOE OSTI2024

Laboratory time series moisture manipulative experiment from sediment across the contiguous US: time series aerobic respiration and geochemistry (v2)

This dataset supports a broader study examining the effects of wetting and drying on hyporheic zone respiration across the contiguous United States (CONUS). The dataset provides data generated from a laboratory moisture manipulation experiment. The contents include time series aerobic respiration and moisture; dissolved oxygen; sediment geochemistry data; and field metadata (including qualitative information on instream and river corridor characteristics). Samples were collected as part of the WHONDRS CONUS-Scale Model-Sample Study (CM). This study was designed following ICON (integrated, coordinated, open, and networked) principles to facilitate a model-experiment (ModEx) iteration approach, leveraging crowdsourced sampling across the CONUS. The data package associated with the CM study is available at https://data.ess-dive.lbl.gov/view/doi:10.15485/1923689. CM sampling began in April 2022 and ended in October 2023. This study uses subsamples from a subset of CM samples collected between June 2022 and June 2023. The original field samples were labeled as CM_###. Subsequent subsamples for this study were labeled as EC_###. The labels from the field samples and the EC subsamples can be mapped directly based on the digits following the prefix and underscore (i.e., EC_001 is a subsample from CM_001). See the critical details section below for more details on sample naming. This data package was originally published in August 2024. It was updated in February 2026 (v2; new and modified files). See the change history section in the readme for more details. For details on how to navigate this data package, see this infographic from the River Corridor SFA https://data.ess-dive.lbl.gov/portals/PNNLRiverCorridorSFA/About. This dataset is comprised of one folder of raw Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS) data and one main data folder containing (1) file-level metadata; (2) data dictionary; (3) field metadata; (4) readme; (5) field protocol; and a (6) a subfolder with sediment sample data from the incubation experiment. The sample data subfolder contains (1) dissolved organic carbon (DOC, measured as non-purgeable organic carbon, NPOC); (2) total nitrogen (TN); (3) adenosine triphosphate (ATP); (4) percent carbon and nitrogen; (5) effect size; (6) iron (II); (7) gravimetric moisture; (8) respiration rates and raw dissolved oxygen values; (9) specific conductance; (10) pH; (11) temperature; (12) a summary containing median values of each data type for each treatment (wet and dry); (13) methods codes; (14) FTICR-MS methods; and (15) a subfolder of 9.4 Tesla FTICR-MS data. This folder contains three subfolders, one containing the sediment .xml data files, one containing the sediment CoreMS output files, the other containing instructions and scripts for processing the files in CoreMS (https://github.com/EMSL-Computing/CoreMS). All files are .csv, .pdf, .R, .ref, or .xml.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Aqueous Ni-rich-cathode dispersions processed with phosphoric acid for lithium-ion batteries with ultra-thick electrodes

Lithium-ion battery (LIB) production can benefit both economically and environmentally from aqueous processing. Although these electrodes have the potential to surpass electrodes conventionally processed with N -methyl-2-pyrrolidone (NMP) in terms of performance, significant issues still exist with respect to ultra-thick cathodes ($\gg$4 mAh/cm 2 areal capacities). A major concern for these types of electrodes with high-nickel active material stems from lithium leaching from active material, which drives the pH of the dispersion in excess of 12 and subsequently corrodes the current collector interface. As this corrosion reaction proceeds, hydrogen generation at the interface creates bubbles which cause severe cracking in the dried electrode surface. When areal loadings are increased, this effect becomes more pronounced and is detrimental to both mechanical and electrochemical properties of these electrodes. In this work, a technique for mitigating corrosion at the current collector by adjusting the pH of the dispersion with the addition of phosphoric acid is investigated. Phosphoric acid was added in 0.5 wt% increments between 0.0 and 1.5 wt%, and effects on rheology, adhesion, corrosion, and electrochemical performance were investigated. A technique is reported for producing aqueous processed cathodes with areal loadings of 6–8 mAh/cm 2 with reduced surface cracking and superior high-rate discharge capacity (i.e. high-power performance) for this class of cathode loadings.

25 ENERGY STORAGE↗

DOE OSTI2026

How Proton Incorporation Reshapes Lattice Dynamics In BaSnO 3 ‐Type Proton Conductors

Proton conduction in acceptor-doped perovskites is fundamentally a vibronic process: mobile H + and D + do not move independently, but dynamically co-vibrate with the surrounding oxygen–metal framework. Direct experimental evidence for this behavior is presented using in situ 119⁢ 𝑆⁢𝑛 nuclear resonance vibrational spectroscopy (NRVS) on hydrated, deuterated, and dry 𝐵⁢𝑎⁢𝑆⁢𝑛 1−𝑥⁢ 𝑌 𝑥 ⁢𝑂 3−𝛿 . Hydration induces systematic redistributions in the Sn-projected phonon density of states (PDOS), including an upshift of the first spectral moment by about 0.4 meV, indicating a stiffening of the extended Sn–O network. H/D isotopic substitution leaves the Sn-projected PDOS largely unchanged, with only subtle isotope-dependent spectral reweighting, demonstrating that protonic degrees of freedom are not localized oscillators but are embedded in collective lattice modes. These results are rationalized using a classical coupled proton–phonon oscillator model that links the observed PDOS variations to changes in effective force constants and vibrational mass terms. The model captures how H + and D + participate in cooperative lattice dynamics rather than forming isolated OH/OD entities. Overall, NRVS probes proton–lattice coupling in ceramic proton conductors and quantitatively describes how protonic defects modulate host lattice dynamics to enable phonon-assisted long-range proton transport.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Monsoon Depression Amplification by Horizontal Shear and Humidity Gradients: A Shallow Water Perspective

Transient, synoptic-scale vortices produce a large fraction of total rainfall in most monsoon regions and are often associated with extreme precipitation. However, the mechanism of their amplification remains a topic of active research. For monsoon depressions, which are the most prominent synoptic-scale vortex in the Asian–Australian monsoon, recent work has suggested that meridional gradients in zonal wind in the vortex environment may produce growth through barotropic instability, while meridional gradients in environmental humidity have also been proposed to cause amplification through coupling with precipitating convection. Here, a two-dimensional shallow water model on a sphere with parameterized precipitation is used to examine the relative role played by these two environmental gradients. By systematically varying the meridional moisture gradient and meridional wind shear for both weak, quasi-linear waves and finite-amplitude isolated vortices, we show that rotational winds in the initial vortex are amplified most strongly by meridional shear of the environmental zonal wind, while vortex precipitation rates are most sensitive to environmental moisture gradients. The growth rate in the presence of both gradients is less than the sum of growth rates in the presence of isolated gradients, as the phase relation between moisture and vorticity anomalies becomes distorted with increasing shear. In conclusion, these results suggest that background meridional gradients in both zonal wind and environmental humidity can contribute to the amplification of vortices to monsoon depression strength, but with some degree of decoupling of the dry rotational flow and the moist convection.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Interpreting pre-vegetation landscape dynamics: The Cambrian Lower Mount Simon Sandstone, Illinois, U.S.A.

ABSTRACT The Cambrian Mount Simon Sandstone has been the subject of extensive study and multiple industrial-scale carbon storage demonstrations at Decatur, Illinois, USA. The development of a reliable paleoenvironmental model is critical to successful large-scale carbon dioxide (CO2) storage, but is complicated by the need to interpret pre-vegetation sedimentation processes. The present study presents a paleoenvironmental model of the Lower Mount Simon Sandstone, based on analysis of primary sedimentary structures in two cores and four complete high-resolution resistivity logs (FMI). The Lower Mount Simon Sandstone represents a vertical “drying-up” sequence composed of three associated depositional units: a north–south oriented coastal system at the base, an eastward-directed fluvial unit in the middle, and a westward-directed eolian system at the top that recycled medium- and fine-grained sand in the basin. Quantitative analysis of fluvial cross-strata indicates that the perennial river system was shallow (c. 1 m deep) with relatively narrow channel belts (c. 1 km). Adjacent sandy eolian-floodplain deposits contain abundant thin, crinkly planar laminae that are enriched in fines and are interpreted as cementation surfaces, likely of biological origin. Deflation lags and wind-ripple strata are commonly interbedded with the crinkly strata, suggesting that the recurrence of erosion and deposition that controlled sedimentary preservation on the floodplain were dominated by eolian transport, re-wetting, and (bio-) cementation. Such a prominent role of exposure to the wind, basin-scale sediment recycling, and eolian removal of fine-grained sediment would have ceased to exist for most climates after the development of vegetation on land, yet, may well be key to understanding the environmental context for early life on Earth.

Geology↗

DOE OSTI2022

Demonstration of Novel Monitoring Techniques for a North Dakota Carbon Capture and Storage Project

Conference paper presented at 16th International Conference on Greenhouse Gas Control Technologies (GHGT-16), Lyon, France, October 23–27, 2022. We present an overview and initial results of the novel and sustainable monitoring techniques developed by the Energy & Environmental Research Center (EERC) and its commercial partners associated with the Red Trail Energy (RTE) carbon capture and storage (CCS) project. RTE is an investor-owned 64-million-gallon dry mill ethanol production plant in Richardton, North Dakota, USA. Currently in operation as of June 2022, the RTE facility will capture 180,000 tonnes of carbon dioxide (CO 2 ) annually (>99% CO 2 ) that is otherwise emitted during the ethanol production process and inject it into the Broom Creek Formation, a deep saline aquifer, for permanent on-site geologic storage.

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