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198 records · Page 11
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Atmospheric CO 2 estimates for the Miocene to Pleistocene based on foraminiferal $δ^{11}$B at Ocean Drilling Program Sites 806 and 807 in the Western Equatorial Pacific

Constraints on the evolution of atmospheric CO 2 levels throughout Earth's history are foundational to our understanding of past variations in climate. Despite considerable effort, records vary in their temporal and spatial coverage and estimates of past CO 2 levels do not always converge, and therefore new records and proxies are valuable. Here we reconstruct atmospheric CO 2 values across major climate transitions over the past 16 million years using the boron isotopic composition (δ 11 B) of planktic foraminifera from 89 samples obtained from two sites in the West Pacific Warm Pool, Ocean Drilling Program (ODP) Sites 806 and 807, measured using high-precision multi-collector inductively coupled plasma mass spectrometry. We compare our results to published data from ODP Site 872, also in the Western Equatorial Pacific, that goes back to 22 million years ago. These sites are in a region that today is near equilibrium with the atmosphere and are thought to have been in equilibrium with the atmosphere for the interval studied. We show that δ 11 B data from this region are consistent with other boron-based studies. The data show evidence for elevated pCO 2 during the Middle Miocene and Early to Middle Pliocene, and reductions in pCO 2 of ~200 ppm during the Middle Miocene Climate Transition, ~250 ppm during Pliocene Glacial Intensification and ~50 ppm during the Mid-Pleistocene Climate Transition. During the Mid-Pleistocene Transition there is a minimum pCO 2 at marine isotopic stage (MIS) 30. Our results are consistent with a coupling between pCO 2 , temperature and ice sheet expansion from the Miocene to the late Quaternary.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Reaching 1.5 and 2.0 °C global surface temperature targets using stratospheric aerosol geoengineering

A new set of stratospheric aerosol geoengineering (SAG) model experiments has been performed with Community Earth System Model version 2 (CESM2) with the Whole Atmosphere Community Climate Model (WACCM6) that are based on the Coupled Model Intercomparison Project phase 6 (CMIP6) overshoot scenario (SSP5-34-OS) as a baseline scenario to limit global warming to 1.5 or 2.0 °C above 1850–1900 conditions. The overshoot scenario allows us to applying a peak-shaving scenario that reduces the needed duration and amount of SAG application compared to a high forcing scenario. In addition, a feedback algorithm identifies the needed amount of sulfur dioxide injections in the stratosphere at four pre-defined latitudes, 30 °N, 15 °N, 15 °S, and 30 °S, to reach three surface temperature targets: global mean temperature, and interhemispheric and pole-to-Equator temperature gradients. These targets further help to reduce side effects, including overcooling in the tropics, warming of high latitudes, and large shifts in precipitation patterns. These experiments are therefore relevant for investigating the impacts on society and ecosystems. Comparisons to SAG simulations based on a high emission pathway baseline scenario (SSP5-85) are also performed to investigate the dependency of impacts using different injection amounts to offset surface warming by SAG. We find that changes from present-day conditions around 2020 in some variables depend strongly on the defined temperature target (1.5 °C vs. 2.0 °C). These include surface air temperature and related impacts, the Atlantic Meridional Overturning Circulation, which impacts ocean net primary productivity, and changes in ice sheet surface mass balance, which impacts sea level rise. Others, including global precipitation changes and the recovery of the Antarctic ozone hole, depend strongly on the amount of SAG application. Furthermore, land net primary productivity as well as ocean acidification depend mostly on the global atmospheric CO 2 concentration and therefore the baseline scenario. Multi-model comparisons of experiments that include strong mitigation and carbon dioxide removal with some SAG application are proposed to assess the robustness of impacts on societies and ecosystems.

42 ENGINEERING↗
DOE OSTI2020

Observations for Model Intercomparison Project (Obs4MIPs): status for CMIP6

The Observations for Model Intercomparison Project (Obs4MIPs) was initiated in 2010 to facilitate the use of observations in climate model evaluation and research, with a particular target being the Coupled Model Intercomparison Project (CMIP), a major initiative of the World Climate Research Programme (WCRP). To this end, Obs4MIPs (1) targets observed variables that can be compared to CMIP model variables; (2) utilizes dataset formatting specifications and metadata requirements closely aligned with CMIP model output; (3) provides brief technical documentation for each dataset, designed for nonexperts and tailored towards relevance for model evaluation, including information on uncertainty, dataset merits, and limitations; and (4) disseminates the data through the Earth System Grid Federation (ESGF) platforms, making the observations searchable and accessible via the same portals as the model output. Taken together, these characteristics of the organization and structure of obs4MIPs should entice a more diverse community of researchers to engage in the comparison of model output with observations and to contribute to a more comprehensive evaluation of the climate models. At present, the number of obs4MIPs datasets has grown to about 80; many are undergoing updates, with another 20 or so in preparation, and more than 100 are proposed and under consideration. A partial list of current global satellite-based datasets includes humidity and temperature profiles; a wide range of cloud and aerosol observations; ocean surface wind, temperature, height, and sea ice fraction; surface and top-of-atmosphere longwave and shortwave radiation; and ozone (O 3 ), methane (CH 4 ), and carbon dioxide (CO 2 ) products. A partial list of proposed products expected to be useful in analyzing CMIP6 results includes the following: alternative products for the above quantities, additional products for ocean surface flux and chlorophyll products, a number of vegetation products (e.g., FAPAR, LAI, burned area fraction), ice sheet mass and height, carbon monoxide (CO), and nitrogen dioxide (NO 2 ). While most existing obs4MIPs datasets consist of monthly-mean gridded data over the global domain, products with higher time resolution (e.g., daily) and/or regional products are now receiving more attention. Along with an increasing number of datasets, obs4MIPs has implemented a number of capability upgrades including (1) an updated obs4MIPs data specifications document that provides additional search facets and generally improves congruence with CMIP6 specifications for model datasets, (2) a set of six easily understood indicators that help guide users as to a dataset's maturity and suitability for application, and (3) an option to supply supplemental information about a dataset beyond what can be found in the standard metadata. With the maturation of the obs4MIPs framework, the dataset inclusion process, and the dataset formatting guidelines and resources, the scope of the observations being considered is expected to grow to include gridded in situ datasets as well as datasets with a regional focus, and the ultimate intent is to judiciously expand this scope to any observation dataset that has applicability for evaluation of the types of Earth system models used in CMIP.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

CMIP7 data request: land and land ice priorities and opportunities

The Land and Land Ice Theme in the Coupled Model Intercomparison Project Phase 7 (CMIP7) represents the current understanding of physical processes in land surface ecosystems, hydrology, cryosphere, and their physical interactions with other Earth system components. Simulations from Earth system models (ESMs) could provide crucial information for assessing planetary safety, such as critical tipping elements, and be used to inform climate risks for improving climate impact assessments and policy decisions. This paper presents a collaborative effort to identify scientific opportunities in the Land and Land Ice Theme of the CMIP7 Data Request. The proposed opportunities build upon advances in ESMs, including new freshwater system and land ice processes being included in CMIP7, as well as the scientific community's demand for high-frequency and sub-grid-scale land surface outputs. In total, 25 variable groups that contain 716 variables have been identified to be potentially available to the broad scientific audience for performing analysis in land–atmosphere coupling, hydrological processes and freshwater systems, glacier and ice sheet mass balance and their influence on the sea levels, land use, and plant phenology. Key reflections from this data request effort include advocacy for closer engagement between the user community and modeling groups, reduction in the technical barriers to tracking existing parameters and defining new variables, and more streamlined variable management. These will be essential to enhance the usability and reliability of CMIP7 outputs for climate and Earth system research and applications to a broad audience that relies on the CMIP7 endeavor.

Li, Yue [Univ. of California, Los Angeles, CA (Uni↗
DOE OSTI2025

Emulator-based Bayesian calibration of a subglacial drainage model

Subglacial drainage models, often motivated by the relationship between hydrology and ice flow, sensitively depend on numerous unconstrained parameters. We explore using borehole water-pressure time series to calibrate the uncertain parameters of a popular subglacial drainage model, taking a Bayesian perspective to quantify the uncertainty in parameter estimates and in the calibrated model predictions. To reduce the computation time associated with Markov Chain Monte Carlo sampling, we construct a fast Gaussian process emulator to stand in for the subglacial drainage model. We first carry out a calibration experiment using synthetic observations consisting of model simulations with hidden parameter values as a demonstration of the method. Using real borehole water pressures measured in western Greenland, we find meaningful constraints on four of the eight model parameters and a factor-of-three reduction in uncertainty of the calibrated model predictions. These experiments illustrate Gaussian process-based Bayesian inference as a useful tool for calibration and uncertainty quantification of complex glaciological models using field data. However, significant differences between the calibrated model and the borehole data suggest that structural limitations of the model, rather than poorly constrained parameters or computational cost, remain the most important constraint on subglacial drainage modelling.

58 GEOSCIENCES↗
DOE OSTI2020

Bathymetric Influences on Antarctic Ice-Shelf Melt Rates

Ocean bathymetry exerts a strong control on ice sheet-ocean interactions within Antarctic ice-shelf cavities, where it can limit the access of warm, dense water at depth to the underside of floating ice shelves. However, ocean bathymetry is challenging to measure within or close to ice-shelf cavities. It remains unclear how uncertainty in existing bathymetry datasets affect simulated sub-ice-shelf melt rates. In this work, we infer linear sensitivities of ice-shelf melt rates to bathymetric shape with grid-scale detail by means of the adjoint of an ocean general circulation model. Both idealized and realistic-geometry experiments of sub-ice-shelf cavities in West Antarctica reveal that bathymetry has a strong impact on melt in localized regions such as topographic obstacles to flow. Moreover, response of melt to bathymetric perturbation is found to be non-monotonic, with deepening leading to either increased or decreased melt depending on location. Our computational approach provides a comprehensive way of identifying regions, where refined knowledge of bathymetry is most impactful, and also where bathymetric errors have relatively little effect on modeled ice sheet-ocean interactions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

5.1.6 Demo #6: NanoStitch (NAWAStitch) Multifunctional Composites Trade Validation

The overall objective of the NanoStitch Multifunctional Composites Trade Validation Demonstration project was to determine the value proposition of adding NanoStitch to rapid-cure composite systems for structures used in the expanding sector of advanced air mobility (AAM) and specifically electric vertical take-off and landing (eVTOL) aircraft. The expected value proposition was stronger composite parts, with new multifunctional attributes, that are lower cost to fabricate and maintain. NanoStitch is a new composite innovation where a contiguous vertically aligned carbon nanotube (VACNT) forest is located between each ply of a laminate composite resulting in improved mechanical properties as well as other multifunctional properties such as enhanced thermal and electrical conductivity. NanoStitch was originally distributed by N12, later acquired by NAWA Technologies, now called NAWAStitch, and henceforth referred to in this document as NAWAStitch. Two significant evaluations were framed to help meet the overall objective. First, was Task 1 to evaluate the effects that adding NAWAStitch to a rapid cure material system would have on the mechanical and processing properties of the material. Second, was Task 2 to evaluate the workability of adding NAWAStitch to practical flight demonstration articles. From previous research, it was already known that the application of NAWAStitch to a composite structure can enhance the mechanical properties of that structure. However, this project will help the engineering community understand those benefits and the basic structural strength values to apply when incorporating NAWAStitch material into composite structure that utilizes a rapid-cure resin system, which is novel. Testing showed that by adding NAWAStitch to the prepreg, most material properties were improved because the VACNTs strengthened the resin to fiber interface, and the interface itself, between plies. For example compression strength improved by more than 20%, and erosion resistance by more than 50%. The UDRI team identified two flight demonstration articles through discussions with Aurora Flight Sciences (Aurora) and reviewing literature on air mobility and the eVTOL market. The demonstration articles were a thin skin honeycomb panel and a section from an eVTOL propeller blade. The manufacturing and testing trials of the demonstration articles were as follows: • NAWAStitch added no manufacturing complexity or detriment to the article physical qualities, while at the same time added multifunctional properties such as enhanced rain erosion and electrothermal de-icing besides enhanced mechanical properties • VACNTs did not increase or hurt the mechanical properties of the interface between honeycomb core materials and the thin skin face sheet • Demonstrated successful de-icing function in an eVTOL propeller meeting real-world specifications in uniformity and endurance • Multifunctional eVTOL propeller cost analysis showed a cost savings of at least 67 % for a single propeller blade with multifunctional de-icing capability and improved mechanical properties which equates to a potential savings of $10,116 per eVTOL aircraft with six three-bladed propellers Overall, the results of this project can provide additional tools for the composite industry to optimize energy efficiency through faster and stronger composite parts that are lower cost to fabricate and maintain. Additionally, the results of this effort can help US industry like NAWA America set the stage for rapid growth and establishment of a manufacturing facility in Ohio. The project has given NAWA America the basic understanding of how the addition of VACNTs to a composite structure can affect the mechanical properties and hence point them to potential commercial applications. The project has also provided Teijin Carbon US with another potential material application for their rapid cure materials that are manufactured at the Renegade facility in Miamisburg, OH.

36 MATERIALS SCIENCE↗
DOE OSTI2020

High-Volume Precipitation Spectrometer (HVPS) Instrument Handbook

The high-volume precipitation spectrometer (HVPS) is a U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility instrument for measuring hydrometeors larger than 150 μm. It is an open-path instrument located on the outside of the aircraft, typically below the wing. A laser sheet throws a shadowgraph image of the hydrometeor (cloud droplets or ice crystals) in the sample volume on a photodiode array. As the hydrometeor moves through the sample volume, this optical array records the moving shape and a two-dimensional picture can be recorded. At an air speed of 100 m/s, the sample volume is 310 l/s. The recorded images can be analyzed for size distributions, number concentrations, and further cloud properties detailed below. Hydrometeors in the range of 0.3-19.2 mm can be fully recorded at a 150 μm resolution; larger particles can only be sized along the direction of flight.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Structural Implications of Interfacial Hydrogen Bonding in Hydrated Wyoming-Montmorillonite Clay

Montmorillonite (MMT) clay - a layered porous nanomaterial used as seals in engineered waste containment barriers for spent nuclear fuel - adopts discrete hydration/swelling states depending upon surrounding water and ion activities and confining pressure. The structure of nanoconfined water and charge-balancing counterions in the clay mineral interlayers dictate the swelling and mechanical behavior of MMT, so a molecular model for this clay with high structural fidelity is required to accurately predict the reliability of long-term nuclear waste storage. Here, we present a molecular model for MMT that is based on high resolution transmission electron microscopy of Wyoming-MMT single crystals. Imaging data unambiguously show a cis-vacant arrangement of structural hydroxyl groups in the octahedral sheet, whereas existing molecular models assume a centrosymmetric trans-vacant configuration for MMT. Furthermore, using atomistic simulations, we find that the cis-vacant arrangement of structural hydroxyl groups significantly affects the structure of adsorbed water yielding a larger population of hydrogen bonds with bridging oxygens on the tetrahedral sheet and weak hydrogen bonding between the hydroxyl groups in the octahedral sheet and water in the clay mineral interlayers. As a result, water adsorbed in the interlayer is more "ice-like", with stronger ordering and lower density, although the diffusivity of the interlayer species is not significantly diminished. Our improved structural model for MMT provides insight into the energetics of water adsorption, which ultimately dictates its pore- to macro-scale swelling, transport, and fracture properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Why Firn Quakes

Snow dampens sounds, but anecdotal reports concisely describe audible propagating collapse events—firnquakes—in Antarctic and Arctic snowfields. We propose combining granular and continuum mechanics to form a testable theory for conditioning, triggering, and propagation of firnquakes consistent with scarce data. A central condition for collapse events is unconsolidated firn at depth. As firn grains compact, stresses are transmitted along force chains which carry the overburden and transition into a continuous medium by pressure sintering. This granular legacy creates solid-like supports of denser layers that keep the material below unconsolidated. Dynamic amplification triggers local brittle failure of the supports, which induces a cascade of collapse propagation. Using bulk density from ice cores as proxy for stiffness, we find the flexural wave speed by collapsing supports matches the recorded firnquake velocities on the order of 100 m/s. Our theory is to be tested in firn sheets and other compacting granular materials.

Voigtländer, A. [Lawrence Berkeley National Labora↗
DOE OSTI2024

Emergent disorder and mechanical memory in periodic metamaterials

Ordered mechanical systems typically have one or only a few stable rest configurations, and hence are not considered useful for encoding memory. Multistable and history-dependent responses usually emerge from quenched disorder, for example in amorphous solids or crumpled sheets. In contrast, due to geometric frustration, periodic magnetic systems can create their own disorder and espouse an extensive manifold of quasi-degenerate configurations. Inspired by the topological structure of frustrated artificial spin ices, we introduce an approach to design ordered, periodic mechanical metamaterials that exhibit an extensive set of spatially disordered states. While our design exploits the correspondence between frustration in magnetism and incompatibility in meta-mechanics, our mechanical systems encompass continuous degrees of freedom, and thus generalize their magnetic counterparts. We show how such systems exhibit non-Abelian and history-dependent responses, as their state can depend on the order in which external manipulations were applied. We demonstrate how this richness of the dynamics enables to recognize, from a static measurement of the final state, the sequence of operations that an extended system underwent. Thus, multistability and potential to perform computation emerge from geometric frustration in ordered mechanical lattices that create their own disorder.

36 MATERIALS SCIENCE↗
DOE OSTI2022

6.26 Low Cost Basalt Fiber for Automotive Applications

Vehicle lightweighting is an essential component to the automotive industry to improve fuel economy of internal combustion engine (ICE) vehicles to meet ever improving emission standards and to improve the range of electric vehicles (EV). Composite materials offer high specific modulus and specific strength, which makes them appealing for these light weighting efforts. Sheet molding compounds (SMC) are particularly interesting from an automotive perspective because of the relatively low cost and high volume of producing SMC parts. Traditionally, composite materials for automotive application are glass fiber reinforced because of the attractive price - performance ratio, but basalt fibers are a cost and recycling competitive reinforcement alternative in this market. The aim of this project was to examine the feasibility of utilizing basalt fiber for automotive applications. More specifically, an effort was made to examine different fiber sizings on basalt fiber combined with vinyl-ester (VE) resin, and their performance as part of an SMC process. In addition to offering vehicle lightweighting with fiber reinforced polymer composites, basalt fiber is a fully recyclable material and thus supports the IACMI technical goal of: Demonstrate that the technology is capable at a sufficient scale for >80% recyclability or reuse of fiber reinforced polymer composites in five years into useful components with projected cost and quality at commercial scale competitive with virgin materials on a pathway to 95% recyclability or reuse starting in ten years. Three different fiber sizings were applied to a continuous roving of basalt fiber and compared to a traditional Electrical/Chemical Resistance (E-CR) glass fiber that is typically used in these types of applications. Fiber tows were examined for Loss on Ignition percentage (LOI%), Tex, and tow strength. Some sizings clearly outperformed others, and the ability to process these fibers on a pilot scale SMC line was demonstrated. A test plan for the manufacturing and mechanical testing of SMC panels was developed. This work continues outside the time frame allocated for this project. When this work is completed, it will be added to this report and posted as Appendix C. Glass fiber reinforced SMC materials have already proven feasible as a light weighting method for traditionally steel parts like the Volkswagen (VW) Atlas lift-gate (Figure 1); this project team is seeking the feasibility of basalt fiber as a drop-in replacement for glass fiber reinforced SMC. Sizing development for basalt fibers has proven that the mechanical properties are better than E-glass and closer to S-glass, which makes it an interesting material for SMC applications. Better mechanical properties translate to less material needed to achieve load case requirement for target applications. The business case has already been demonstrated for 100,000 parts per year of glass fiber reinforced SMC Atlas lift-gates compared to traditional steel manufacturing processes. Reduced overhead and assembly costs are offset by glass fiber SMC higher cost per kg beyond 100,000 parts per year, which is still a relatively low volume for the automotive industry. For basalt fiber reinforced SMC to become feasible for automotive applications, the price-performance ratio has to be precisely determined. Based on the mechanical performance it is possible to establish a range of applications and technical solutions in which the potential of basalt SMC can be utilized, while the price of the material can be used to compile the business case for such applications. Based on these business cases and the sustainability indicators, glass fiber reinforcement (or other) materials can be directly substituted. Volkswagen’s commitment to reducing carbon emissions cannot be understated. Basalt fiber shows promise of reducing the carbon footprint in SMC materials, especially if sizing optimizations can be made with thermoplastic based SMC. To fully realize the value of basalt fiber reinforced materials, a lifecycle cost analysis should be performed on basalt’s production and recycling, and then compared against E-glass. From this assessment, a true judgement can be made on the commercialization potential of this material. Figure 1. Example of Fiber Reinforced Polymer Composite Liftgate As a conclusion, we can state that Mafic basalt fiber is not a direct replacement for E-glass or E-CR glass based on price, but should be considered a technical solution when E-glass does not provide adequate performance in a composite design and S-glass, aramid and carbon fibers are too costly. Mafic basalt fiber can be placed on the high-performance fiber spectrum next to S-glass for performance but at one third the price. It should be considered for more technically challenging structural designs wherein the performance can demonstrate 20-25% performance enhancement over E-glass to elicit more strength or a weight reduction. Both Michelman and Mafic produce thermoplastic sizings which, in combination with Nylon and polypropylene resin and fibers, can further advance high speed composite implementations while maintaining an eco-friendly manufacturing process.

36 MATERIALS SCIENCE↗
DOE OSTI2025

CO2 and CH4 leaf-level fluxes and soil porewater concentrations from common vegetation patches in Louisiana’s coastal wetlands

This dataset contains leaf-level flux and soil porewater concentration measurements of carbon dioxide (CO2) and methane (CH4 ) in plots in the footprint of Ameriflux sites US-LA2 and US-LA3. Leaf fluxes in US-LA2 were measured on patches dominated by Sagittaria lancifolia and co-dominated by Sagittaria lancifolia and Typha latifolia. In US-LA3, fluxes were measured from distinct Juncus roemerianus and Spartina alterniflora patches. The porewater concentrations were collected across a vertical profile (~50 cm depth) at centric locations within 25 m2 plots where we measured the leaf fluxes. US-LA3 included an additional set of measurements in open water spots. We aimed to evaluate differences in leaf fluxes and porewater pools of CO2 and CH4 of representative ecohydrological patches across a salinity gradient. We also used this dataset to help develop ELM-Wet, a more realistic representation of wetland carbon biogeochemical processes within the U.S. Department of Energy’s Energy Exascale Earth System Model (E3SM) Land Model version 1 (ELM v.1). The files can be opened with regular text editors or spreadsheet programs. Version 2.0 (8/26/2025): This is the latest version of this dataset. The update includes additional samples of soil porewater CH4/CO2 concentrations from June-2021 to November-2022, as well as minor adjustments made to V1 samples via changing Henry's solubility to account for porewater salinity. Additionally leaf-level measurments of spectral indices, PSRI, NDVI, and PRI have been added to complement Leaf-level flux measurements. All V1 data sets have been integrated into V2 sheets, ensuring data from the previous version is contained with the additional samples and consistent with V2 metadata.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Data associated with Quaternary Research manuscript Latest Pleistocene glacial chronology and paleoclimate reconstruction for the East River watershed, Colorado, USA

The data here are associated with Quaternary Research manuscript Latest Pleistocene glacial chronology and paleoclimate reconstruction for the East River watershed, Colorado, USA and include data associated with cosmogenic exposure and depth profile dating as well as glacier-climate numerical modeling. Reconstructing Pleistocene glaciation timing and extent is vital for understanding paleoclimate. While late Pleistocene glaciation has been studied extensively in western North American mountain ranges, the glacial history of the western Elk Range in Colorado remains understudied, particularly in the East River watershed, a site of intense scientific focus. Here we use cosmogenic nuclide exposure and depth–profile dating methods to determine the timing of glaciation in the East River watershed. We use glacier modeling to reconstruct paleoglacier extents and quantify past climate conditions. Our findings indicate that the East River glacier retreated from its maximum position approximately 17–18 ka, moving to recessional positions between 13–15 ka, before experiencing more substantial retreat to high-elevation cirques around 12.9 ka. Glacier modeling suggests that the maximum ice extents at 17–18 ka could have been sustained by temperature depressions of approximately −6.5°C compared to modern conditions, assuming consistent precipitation. Additionally, the ice position at 13–15 ka could have been supported by temperature depressions of around −4.0°C. These results offer insights into the deglaciation timeline in the East River watershed and broader western Elk Range as well as paleoclimate conditions during the late Pleistocene, which may aid future research on critical zone evolution in the East River watershed.The data files include: 1. Table 1 In situ-produced 10Be sample data (.pdf, .csv, .xlsx)2. Table 2 In situ-produced 10Be exposure age results (.pdf, .csv, .xlsx)3. S1_A CRONUS calculator input assuming no erosion (.csv)4. S1_B CRONUS calculator input assuming erosion (.csv)5. S1_C CRONUS calculator results and comparison (.csv)6. S2_A In situ-produced 10Be sample data for depth profile (.csv)7. S2_B In situ-produced 10Be depth profile model input (.csv)8. S2_C In situ-produced 10Be depth profile model results (.csv)9. S3 Monthly cloudiness, rH, and windspeed data used in glacier climate model (.csv)10. S4 Glacier climate model results (.csv)

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Laboratory-Scale Coal-Derived Graphene Process (Final Report)

The Energy & Environmental Research Center (EERC) conducted a laboratory-scale coal-derived graphene (CDG) project focused on developing a technological process for making graphene from four U.S. domestic coal or coal wastes, including lignite from North Dakota, subbituminous coal from Wyoming, bituminous coal from Utah, and anthracite from Pennsylvania. The project was divided into two performance or budget periods (BPs), with BP1 comprising the up-front laboratory experiments to make graphene materials from coal beginning on May 1, 2020, to April 30, 2022. BP2 was conducted from May 1, 2022, to April 30, 2023, and was focused on analyzing the CDG process economic feasibility and the technical gaps for technological scale-up and commercialization. During this project, a few different coal-derived high-value products have been demonstrated, including graphite, graphene oxide (GO), reduced graphene oxide (rGO), and graphene quantum dots (GQDs). A new graphite microstructure was discovered and named “croissant graphite” because of the exterior morphological and textural resemblance to croissant food items sold in commercial groceries stores. The new graphite structure and the associated preparation from coal or coal waste feedstocks has been the subject of a U.S. patent application. The systematic experimental processes involving coal cleaning, upgrading, and conversion to high-value carbon products culminated into a developed upgraded coal-to-products (UCP) technology that is being pursued for potential fast-track commercialization, if funding is available. It is envisioned that commercialization of the UCP technology would increase consumption of U.S. domestic coals or coal wastes to make environmentally sustainable high-value products for the electronics industry, high-energy-storage applications, and clean energy technologies such as electric vehicle (EV) lithium-ion batteries (LIBs), for which graphite has become a critical mineral commodity. Croissant graphite microstructures, when observed by field emission scanning electron microscopy (FESEM), display wavy surface morphology and often grow from a base that is made of graphitized particles with honeycomb-like layers, which are believed to be graphene layers. While more studies are needed to fully ascertain the mechanisms of the croissant graphite microstructure formation, it is postulated that their growth may begin from curling of the graphene sheets into ribbon-like structures, and continuous growth and densification of the ribbon-like structures forms croissant microstructures. Additional studies are ongoing to evaluate the electrochemical performance of croissant graphite for LIB applications and to determine the experimental conditions necessary to tune on/off croissant formation so that it can be either optimized or suppressed depending on performance evaluation results. In addition to the discovery of croissant graphite, the graphitization process from the four coal ranks in general was successful. X-ray diffraction (XRD) analysis showed that the degree of graphitization (DoG) ranged from 12% to 80% in an early sample set, and further optimization on lignite coal produces a DoG of about 92%, which was spectacular to see as lignite is the lowest-rank coal. Thus, it is expected that the graphitization performance for higher-rank coals will be similar or better when optimized as well. The coal-derived graphite was used to make GO and rGO. Analytical characterization, e.g., by methods such as Raman spectroscopy, XRD, Fourier transform infrared (FTIR) spectroscopy and FESEM, showed that the sequence of converting the coal to graphite, exfoliating it to GO, and then chemically reducing the GO to rGO was successful. Although coal naturally contains aromatic compounds and some relatively small-sized condensed aromatic units, it does not contain graphene sheets. In the UCP process, the aromatic domains in the coals, particularly low-rank coals, are concentrated and condensed further into graphene sheets, which are ordered into a 3D stack during graphitization. The synthesized graphite is then unpacked by methods such as exfoliation to various graphene products. GQDs were synthesized from all four coal types, and their optical properties were demonstrated to be tunable by the coal precursor preprocessing treatments. In all four coal types, enhanced optical properties were observed for the produced GDQs with incremental improvements made to the coal precursors. GQDs produced from raw coal samples displayed lower ultraviolet–visible (UV–Vis) spectroscopy absorbance intensity compared to those obtained from cleaned and upgraded coal residues. The photoluminescence (PL) intensities also varied with pretreatment conditions and with the concentration of GQDs in aqueous solutions. GQDs obtained from anthracite show longer emission wavelengths and can be excited by visible light as opposed to GQDs derived from the other coal ranks. UV fluorescence 3D maps and spectra revealed that the emission wavelength at which the GQDs solutions display the highest intensity was slightly redshifted based on the coal precursor pretreatments. In low-rank coal (lignite and subbituminous) samples, two clusters were observed in the maps for GQDs, which may suggest that there are potentially two types of fluorophores in solution or two main size populations. The ability to tune the properties of GQDs based on processing methods can be exploited to make GQDs for various optical display or optoelectronics applications. The results also highlight the importance of removing coal-borne impurities to improve the quality of the coal precursor for preparation of graphene products. Coal and/or coal wastes preprocessing methods were developed and applied to clean and upgrade the coal precursors prior to graphitization and subsequent conversion to graphene products. The preprocessing methods involve high specific-gravity separations, mineral acid cleaning (no hydrofluoric acid), and subsequent upgrading by reducing the coal-borne heteroatom (nitrogen, sulfur, and oxygen) content using proprietary chemical agents. Analytical characterization revealed that the preprocessing steps were successful, with ash reductions that range from 38% to 80% and residual ash content that was below the 5 wt% initial target. Based on proximate and ultimate analysis, the heteroatom reduction reactions produced upgraded coal residues with the oxygen content reduced by 8% to 24%, with additional reductions in the nitrogen and sulfur contents. An initial assessment of the waste streams from the UCP process shows very small to negligible environmental impact due to CO 2 , NO x , and SO x because most process steps are performed under inert atmosphere with argon. Consequently, reactive oxygen environments that tend to create these species are avoided. The inorganic and potentially hazardous species are released into aqueous waste streams that are easy to handle for proper disposal. The liquid waste streams were found to contain low-level concentrations of rare-earth elements (REEs), which could be concentrated and recovered as value-added by-products. Additionally, the volatile and gaseous fractions from carbonization and heat treatment contain useful organic compounds that can also be recovered as potential valuable by-products. Thus, the UCP technology is considered an environmentally sustainable and promising emerging technology for making high-value products from coal and coal wastes, with potential additional value-added by-products. Analysis of potential markets for the coal-derived carbon products shows a strong demand in both niche market sectors and across a wide variety of other industrial sectors. Graphite is currently considered a critical mineral commodity that has a large and growing demand in the LIB industry for EV applications. Based on data from Fortune Business Insights (2022) and Marketwatch (2023) reports, the average global graphite market is projected to reach about 33 billion by 2028, growing at a compound annual growth rate (CAGR) of about 7%, with much of this growth expected to be in the LIB industry. GO and rGO have strong market potentials in various application areas, such as coatings for anticorrosion, anti-icing, and antimicrobial protection, thermal barriers, wear resistance, sensors, additive manufacturing such as 3D inks, and others. GQDs are the emerging key player in the bioimaging, photovoltaics, and light-emitting diodes (LEDs) applications, with the potential to replace traditional semiconductor quantum dots (SQDs), which are based on metallic systems that are more toxic and more expensive. Biomedical applications of GQDs are becoming more attractive because of low to no toxicity and extremely low cost compared to SQDs. The major challenges for scale-up and commercialization of coal-derived carbon products such as graphene vary from the inherent attributes of graphene itself to reluctance to accept graphene in new manufacturing processes because of the uncertainty of the unknown. The 2D nature of graphene materials with a thickness of one atom presents significant challenges to proper handling/processing, and process scale-up becomes difficult because it requires high-end, expensive equipment, even for routine handling and analysis for quality assurance and control. Pristine graphene can also be extremely difficult to work into other matrices, thus hindering downstream processibility, especially at large scale. Currently, the cost of graphene and graphene products is still high and presents an economic risk that tends to slow down investment in scaling up emerging technologies. The lack of a standard for graphene materials for quality assurance and quality control poses a great challenge not only for the markets but also for commercialization efforts. A first-look economic feasibility analysis of the UCP technology provided valuable information that suggests the UCP process would be feasible, especially when it is scaled to a pilot scale and could be more competitive at the full scale. Graphitization was found to be the most energy-consuming and most capital-intensive step in the overall process. In small laboratory- and bench-scale experiments, labor is a significant contributor to the total process costs. Although these energy, capital, and labor constraints contribute to a higher selling price for the product, a preliminary economic model suggests that the process would be feasible at large scale when the process is fully integrated, optimized, and automated.

01 COAL, LIGNITE, AND PEAT↗