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At least 235 records · Page 13
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Changing chemistry of particulate manganese in the near- and far-field hydrothermal plumes from 15°S East Pacific Rise and its influence on metal scavenging

Dissolved Mn(II) in the hydrothermal plume is known to be microbially oxidized to form Mn(III/IV) oxides, and the Mn oxides scavenge other trace elements in seawater. In the GEOTRACES GP16 cruise, dissolved Mn (dMn) and particulate Mn (pMn) were found to be transported over 4000 km westwards from the Southern Eastern Pacific Rise. Previous studies in this plume showed different removal rates of dMn and pMn as well as pMn size distribution between the near-field (<80 km from the ridge axis) and far-field (>80 km) plumes. In order to understand Mn cycling in these plumes, spatial distribution, oxidation states, and mineral structures of Mn in small size fraction (SSF; 0.8–51 μm) and large size fraction (LSF; >51 μm) particles from the near-field and far-field plumes were examined using micro X-ray fluorescence spectrometry (μ-XRF), X-ray absorption near-edge structure spectroscopy (XANES), chemical species mapping, and extended X-ray absorption fine-structure spectroscopy (EXAFS). In the near-field plume, pMn in the SSF is dominated by oxidized Mn with Mn(III) fractions of ~30%. They are a mixture of δ-MnO 2 and triclinic birnessites that is known to be formed as a result of autocatalytic Mn(II) oxidation at the surface of freshly-formed δ-MnO2, suggesting that both microbial and autocatalytic Mn oxidation occur in the near-field plume. The LSF pMn in the near-field plume is also oxidized and often found in large aggregates several hundreds of μm in size. These aggregates settle out in the near-field and during transport, and are not found in the far-field plume. In the far-field plume where Mn oxides are not newly formed, pMn in the SSF is oxidized, but their Mn(III) fractions are smaller than in the near-field pMn. Unlike the SSF, the far-field plume LSF pMn is dominated by reduced Mn, implying very slow aggregation of pMn in the far-field plume. The different characteristics of pMn between the near-field and far-field plumes affect its scavenging of other trace elements. In the near-field plume, Co, Mo, 231 Pa are associated with pMn, but not in the far-field plume. 231 Pa is adsorbed to pFe rather than pMn in the far-field plume, and Pb is adsorbed to pFe in the entire plume. The result shows that freshly-formed Mn oxides in the near-field plume have higher scavenging capacity than the far-field plume pMn. Our findings suggest that the mineralogical age of Mn oxides may be an important parameter that controls the scavenging of many other trace elements and isotopes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Toward reducing uncertainty quantification costs in DEM models of particulate flow: Testing simple, sensitivity-based, forward uncertainty propagation techniques

The performance of two conceptually-simple uncertainty quantification techniques are tested against the rigorous nested-loop sampling technique of Roy and Oberkampf (Comput Methods Appl Mech Eng, 200: 2131–2144, 2011) (herein called full-sampling) using two very small-scale DEM-based models of particulate flow (one gas-solid flow and one granular flow). The first simplified forward uncertainty propagation technique, reduced-sampling, uses a sensitivity analysis to eliminate uncertain inputs that have little impact on the model output prior to nested-loop sampling. The second technique, boundary-sampling, uses a sensitivity analysis to inform the selection of two bounding cases for each key model output. In conclusion, the uncertainties in the model outputs obtained via the reduced- and boundary-sampling methods agree well with those from full-sampling for both the gas-solid and granular flow models while yielding computational savings of 65–75% (reduced sampling) and 94–97% (boundary sampling).

42 ENGINEERING↗
DOE OSTI2020

Particulate plutonium released from the Fukushima Daiichi meltdowns

Traces of Pu have been detected in material released from the Fukushima Daiichi Nuclear Power Plant (FDNPP) in March of 2011; however, to date the physical and chemical form of the Pu have remained unknown. Here we report the discovery of particulate Pu associated with cesium-rich microparticles (CsMPs) that formed in and were released from the reactors during the FDNPP meltdowns. The Cs-pollucite-based CsMP contained discrete U(IV)O 2 nanoparticles, <~10 nm, one of which is enriched in Pu adjacent to fragments of Zr-cladding. The isotope ratios, 235 U/ 238 U, 240 Pu/ 239 Pu, and 242 Pu/ 239 Pu, of the CsMPs were determined to be ~0.0193, ~0.347, and ~0.065, respectively, which are consistent with the calculated isotopic ratios of irradiated-fuel fragments. Thus, considering the regional distribution of CsMPs, the long-distance dispersion of Pu from FNDPP is attributed to the transport by CsMPs that have incorporated nanoscale fuel fragments prior to their dispersion up to 230 km away from the Fukushima Daiichi reactor site.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2025

Compressibility and permeability of particulated non-recyclable municipal solid waste

Biofuels from non-recyclable municipal solid waste (NMSW) stand at the forefront of energy sustainability. However, their widespread adoption is hampered by persistent material handling issues stemming from the variability in NMSW material properties. An enhanced understanding of particulated NMSW properties, particularly compressibility and permeability, is essential to address the feedstock handling challenges and optimize the handling equipment. This study measures the compressibility and gas permeability of five streams of NMSW materials (i.e., rigid plastics, cardboard, thin film, paper, and foam) and their mixtures under different stress conditions. The results highlight the significant variability in compressibility and gas permeability among different streams, as well as the impacts of particle sizes. A semi-empirical model capable of predicting the gas permeability of NMSW mixtures is established and validated. Here, the results also highlight that reduced NMSW particle size helps promote consistency in NMSW feedstock’s physical and mechanical properties, which is favored for handling equipment design in waste-to-energy recovery facilities.

09 BIOMASS FUELS↗
DOE OSTI2025

Ceramic High Efficiency Particulate Air (HEPA) Filter Research and Development at Lawrence Livermore National Laboratory

Ceramic high efficiency particulate air (HEPA) filter development program began at Lawrence Livermore National Laboratory (LLNL) over 20 years ago. Historical incidents motivated current safety systems at nuclear facilities. A ceramic filter that can survive a fire can provide robust, passive safety protection. Research has been conducted to improve the safety of nuclear facilities and to reduce operational and lifecycle costs, through ceramic filter technology that can survive fire conditions. Here, the research focused on applications in both new facilities as well as meeting operational requirements necessary to retrofit filters into existing DOE facilities. The research has developed multiple filter technologies spanning traditional HEPA filter materials to advanced manufacturing technologies (e.g., electrospinning, additive manufacturing, etc.). This communication will present highlights of selected development efforts for ceramic HEPA filter research, current state-of-the-art for ceramic filters, and future needs including technical, regulatory, and commercial efforts.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2022

Tight Coupling of Surface and In-Plant Biochemistry and Convection Governs Key Fine Particulate Components over the Amazon Rainforest

We report that throughout the troposphere over the Amazon rainforest, isoprene epoxydiol-secondary organic aerosols (IEPOX-SOA) are key components of submicrometer particle mass. IEPOX-SOA is thought to form by multiphase chemical pathways in the atmosphere, but using detailed model simulations, we show that these pathways are strongly inhibited by the solid particle phase state prevailing in the upper troposphere. We find that 2-methyltetrol gases formed by in-plant biochemical oxidation pathways, their partitioning to fine particles, and dissolution in cloud droplets can explain over 90% of IEPOX-SOA mass concentrations in the upper troposphere. In agreement with previous PM10 chiral measurements, our simulations indicate that plant biochemical processes are the dominant source of particulate 2-methyltetrols in the lower troposphere as well (>70%). Our results imply that in-plant biochemistry plays a central but previously unidentified role in aerosol processes and atmosphere-biosphere-climate interactions over the rainforest.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Topological Data Analysis for Particulate Gels

Soft gels, formed via the self-assembly of particulate materials, exhibit intricate multiscale structures that provide them with flexibility and resilience when subjected to external stresses. Here, this work combines particle simulations and topological data analysis (TDA) to characterize the complex multiscale structure of soft gels. Our TDA analysis focuses on the use of the Euler characteristic, which is an interpretable and computationally scalable topological descriptor that is combined with filtration operations to obtain information on the geometric (local) and topological (global) structure of soft gels. We reduce the topological information obtained with TDA using principal component analysis (PCA) and show that this provides an informative low-dimensional representation of the gel structure. We use the proposed computational framework to investigate the influence of gel preparation (e.g., quench rate, volume fraction) on soft gel structure and to explore dynamic deformations that emerge under oscillatory shear in various response regimes (linear, nonlinear, and flow). Our analysis provides evidence of the existence of hierarchical structures in soft gels, which are not easily identifiable otherwise. Moreover, our analysis reveals direct correlations between topological changes of the gel structure under deformation and mechanical phenomena distinctive of gel materials, such as stiffening and yielding. In summary, we show that TDA facilitates the mathematical representation, quantification, and analysis of soft gel structures, extending traditional network analysis methods to capture both local and global organization.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Wintertime particulate matter decrease buffered by unfavorable chemical processes despite emissions reductions in China

Extreme and persistent haze events frequently occur during wintertime China. While recent emissions reductions reduced annual mean fine particulate matter (PM2.5) concentrations over eastern China, their effectiveness on wintertime PM2.5 trend remains uncertain. We use observations and model simulations to quantify seasonal differences in PM2.5 trends and investigate the underlying chemical mechanisms driving such differences. We find a much slower decrease in observed wintertime PM2.5 (–3.2% yr-1) since 2014, in contrast to a drastic summertime decrease (–10.3% yr-1). Simulations show two previously underappreciated mechanisms buffering wintertime PM2.5 decrease, including an increase in oxidation capacity due to nitrogen oxides (NOx) reductions under wintertime volatile organic compound (VOC)- limited chemistry, and an enhanced conversion of nitric acid to nitrate by ammonia due to sulfur dioxide reductions. Our findings suggest that control policies targeting VOC and deep NOx reductions are needed to improve wintertime PM2.5 air quality over China.

Leung, Danny M.↗
DOE OSTI2020

Effects of Low-Carbon Energy Adoption on Airborne Particulate Matter Concentrations With Feedbacks to Future Climate Over California

California plans to reduce emissions of long-lived greenhouse gases (GHGs) through adoption of new energy systems that will also lower concentrations of short-lived absorbing soot contained in airborne particulate matter (PM). Here we examine the direct and indirect effects of reduced PM concentrations under a low-carbon energy (GHG-Step) scenario on radiative forcing in California. Simulations were carried out using the source-oriented WRF/Chem (SOWC) model with 12 km spatial resolution for the year 2054. Furthermore, the avoided aerosol emissions due to technology advances in the GHG-Step scenario reduce ground level PM concentrations by ~8.85% over land compared to the Business-as-Usual (BAU) scenario, but changes to meteorological parameters are more modest. Top-of-atmospheric forcing predicted by the SOWC model increased by 0.15 W m -2 , surface temperature warmed by 0.001 K, and planetary boundary layer height (PBLH) increased by 2.20 cm in the GHG-Step scenario compared to the BAU scenario. PM climate feedbacks are small because the significant changes in ground level PM concentrations associated with the GHG-Step scenario are limited to the first few hundred meters of the atmosphere, with little change for the majority of the vertical column above that level. As an order-of-magnitude comparison, the long-term effects of global reductions in GHG emissions (RCP8.5–RCP4.5) lowered average surface temperature over the California study domain by approximately 0.76 K. The effects of long-lived climate pollutants such as CO 2 are much stronger than the effects of short-lived climate pollutants such as PM soot over California in the year 2054.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

River Organic Carbon Fluxes Modulated by Hydrodynamic Sorting of Particulate Organic Matter

Rivers regulate the global carbon cycle by transferring particulate organic carbon (POC) from terrestrial landscapes to marine sedimentary basins, but the processes controlling the amount and composition of fluvially exported POC are poorly understood. We propose that hydrodynamic sorting processes modify POC fluxes during fluvial transit. We test this hypothesis by studying POC transported along a ~1,200 km reach of the Rio Bermejo, Argentina. Nanoscale secondary ion mass spectrometry revealed that POC was either fine, mineral-associated organic matter, or coarse discrete organic particles. Mineral-associated POC is more resistant to oxidation and has a lower particle settling velocity than discrete POC. Consequently, hydraulic sorting and downstream fining amplify the proportion of fine, mineral-associated POC from ~55% to ~78% over 1,220 km of downstream transit. This suggests that mineral-associated POC has a greater probability of export and preservation in marine basins than plant detritus, which may be oxidized to CO 2 during transit.

58 GEOSCIENCES↗
DOE OSTI2023

Composition and Flux of Dissolved and Particulate Carbon and Nitrogen in the Lower Tocantins River

The Tocantins River contributes ~5 % of the total flux of water to the Amazon River plume in the Atlantic Ocean. Here, we evaluate monthly variability in the composition and abundance of carbon, nitrogen, and suspended sediment in the lower reaches of the Tocantins River from 2014-2016. Dissolved organic carbon (DOC) concentrations generally increased during periods of high discharge and are ~1.5 times lower than average concentrations at the mouth of the Amazon River. Dissolved inorganic carbon (DIC) similarly increased during periods of high discharge. Total dissolved nitrogen (TDN) and individual nitrogen species followed a similar temporal pattern, increasing during high water. $\text{NO}^-_3$ predominated the dissolved inorganic nitrogen (DIN) pool, followed by $\text{NH}_4^+$, and $\text{NO}_2^-$ , characteristic of environments with a relatively low anthropogenic impact. Dissolved fractions represented 92 % of the total carbon exported and 78 % of the total nitrogen exported. The suspended particulate sediment flux was 2.72 x 10 6 t yr -1 , with fine suspended sediment (FSS) dominating (71.3 %). Concentrations of carbon relative to nitrogen indicate a primarily terrigenous source of organic matter and CO 2 derived from in situ respiration of this material during the rainy season and a primarily algal/bacterial source of organic matter during the dry season. Considering past estimates of dissolved carbon and nitrogen fluxes from the Amazon River to the Atlantic Ocean, the Tocantins River contributes 3 and 3.7 % to total fluxes to the Amazon River plume region, respectively. While this contribution is relatively small, it may be influenced by future changes to the basin’s land use and hydrology.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Heterogeneity in Permeability and Particulate Organic Carbon Content Controls the Redox Condition of Riverbed Sediments at Different Timescales

Abstract The hydrological and biogeochemical properties of the hyporheic zone in stream and riverine ecosystems have been extensively studied over the past two decades. Although it is widely acknowledged that sediment heterogeneity can influence biogeochemical reactions, little effort has been made to understand the role of heterogeneity on the spatiotemporal variability of riverbed redox conditions under changing flow dynamics at different timescales. Here we integrate a mechanistic model and field data to demonstrate that heterogeneity in permeability plays a vital role in modulating sediment redox conditions at both seasonal (annual) and event (daily‐to‐weekly) timescales, whereas heterogeneity in particulate organic carbon (POC) content only has a comparable influence on redox conditions at the seasonal timescale. These findings underscore the importance of accurately characterizing sediment heterogeneity, in terms of permeability and POC content, in quantifying biogeochemical dynamics in the riverbed and hyporheic zones of riverine ecosystems.

Geology↗
DOE OSTI2026

Global hotspots of particulate organic carbon losses under climate change

Soil organic carbon (SOC) comprises particulate (POC) and mineral-associated organic carbon (MAOC), which differ in formation, stabilization, and loss mechanisms. While the current global distribution of POC and MAOC is characterized, their vulnerability under future climate scenarios remains unclear. Using 3284 topsoil (0-30 cm) observations from six continents, we identify high-latitude soils as global hotspots of SOC vulnerability under shared socioeconomic pathway scenarios (SSP126, SSP245, and SSP585). Under a high-emission scenario (SSP585), high-latitude soils are projected to lose substantial POC by 2100, accounting for about 81 ± 10% of total SOC losses. These declines are driven by the high proportion of SOC stored as POC (f POC ) and its high temperature sensitivity. We show that f POC is a robust indicator of SOC vulnerability to climate change. Globally, the projected POC decline corresponds to a cumulative carbon dioxide (CO 2 ) release of 81.34 Pg CO 2 -equivalent by 2100, highlighting the importance of preserving POC to mitigate climate feedbacks.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Pore architecture and particulate organic matter in soils under monoculture switchgrass and restored prairie in contrasting topography

Bioenergy cropping systems can substantially contribute to climate change mitigation. However, limited information is available on how they affect soil characteristics, including pores and particulate organic matter (POM), both essential components of the soil C cycle. The objective of this study was to determine effects of bioenergy systems and field topography on soil pore characteristics, POM, and POM decomposition under new plant growth. We collected intact soil cores from two systems: monoculture switchgrass (Panicum virgatum L.) and native prairie, at two contrasting topographical positions (depressions and slopes), planting half of the cores with switchgrass. Pore and POM characteristics were obtained using X-ray computed micro-tomography (μCT) (18.2 µm resolution) before and after new switchgrass growth. Diverse prairie vegetation led to higher soil C than switchgrass, with concomitantly higher volumes of 30–90 μm radius pores and greater solid-pore interface. Yet, that effect was present only in the coarse-textured soils on slopes and coincided with higher root biomass of prairie vegetation. Surprisingly, new switchgrass growth did not intensify decomposition of POM, but even somewhat decreased it in monoculture switchgrass as compared to non-planted controls. Our results suggest that topography can play a substantial role in regulating factors driving C sequestration in bioenergy systems.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2020

A description of structured waves in shock compressed particulate composites

Dynamic compression of composite materials is of scientific interest because the mechanical mismatch between internal phases challenges continuum theories. Typical assumptions about steady wave propagation and quasi-instantaneous state changes require reexamination along with the need for time-dependent models. To that end, data and models are presented here for the shock compression of an idealized particulate composite. To serve as a generic representative of this material class, a polymer matrix was filled with tungsten particles, ranging from 1 to 50 vol. %. This creates a simple microstructure containing randomly scattered particles with an extreme impedance mismatch to the binding matrix. These materials were parallel plate impact loaded by Al flyers traveling at 1.8–5.0 km/s. Velocimetry provided records of the equilibrium state and the compression wave structure for each case with trends quantified by an empirical fit. The same quantities were also studied as a function of the wave's propagation distance. A homogenized viscoelastic model then made it possible to progress from cataloging trends to making predictions. Starting from a Mie–Gruneisen equation of state, additional time varying terms were added to capture the transient response. After calibration, accurate predictions of the steady wave structure were possible.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Investigations of room temperature multiferroic and magneto-electric properties of (1-Φ) PZTFT-Φ CZFMO particulate composites

Multiferroic composites consisting of a single-phase multiferroic [0.6(PbZr 0.53 Ti 0.47 O 3 )-0.4(PbFe 0.5 Ta 0.5 )O 3 ] as a matrix and a magnetostrictive phase (Co 0.6 Zn 0.4 Fe 1.7 Mn 0.3 O 4 ) dispersed in the matrix are fabricated via hybrid synthesis technique. The structure and surface morphology studies using x-ray diffraction and field emission scanning electron microscopy techniques indicate the formation of 3-0 type particulate composites. Coexistence of soft-magnetic behavior and ferroelectric characteristics are confirmed for composites from magnetization vs magnetic field (M–H) and polarization vs electric field (P–E) measurements, respectively. Magneto-dielectric (MD) measurement shows significant changes in the dielectric properties with the application of a magnetic field, indicating the existence of strong MD behavior. The biquadratic nature of magneto-electric (ME) coupling is described by the Landau free energy equation arising from the strain transfer at the interfaces between the constituent phases. The direct magneto-electric voltage coefficient measurement also confirms very strong coupling between ferroelectricity and magnetism and supports the strain-mediated magneto-electric effect in composites. The Φ = 0.3 composite exhibits the maximum ME coefficient of 20.72 mV/cm Oe with M S = 24.62 emu/g, H C = 59.66 Oe, and piezoelectric coefficient value d 33 = 19 pC/N. In conclusion, the strong magneto-electric effect along with low dielectric loss at room temperature in these composites suggests their suitability for multifunctional magneto-electric device applications such as magnetic sensors, etc.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Observations of Atmospheric Corrosion Testing on Heated Austenitic Stainless Steel Surfaces: Exploring the Role of Inert Dust Particulates and Seawater

Relevant atmospheric corrosion laboratory testing environments were developed to explore the influence of inert dust and seawater on the corrosion susceptibility of stainless steel in spent nuclear fuel dry storage conditions. Measurements from dust collected on in-service dry storage canisters were applied to develop exposure conditions. Three atmospheric exposure conditions, two static and one cyclic, were examined with three different surface coverages: co-deposited large dust and seawater, co-deposited small dust and seawater, and solely seawater. Stainless steel coupons representative of spent nuclear fuel dry storage canister material were subjected to the various corrosion environments, with the results from exposures up to 1 year presented here. Post exposure, corrosion damage was analyzed using optical microscopy, scanning electron microscopy, and energy dispersive X-ray spectroscopy. Initial observations are presented herein, and potential implications with respect to the influence of inert dust particles on corrosion susceptibility are summarized. In general, the co-deposition of dust and salt resulted in larger pits and exhibited mixed modes of corrosion that were not observed in the no-dust conditions (i.e., crevicing, filiform, and pits within pits). The presence of the inert dust may influence brine spreading and/or act as crevice formers, leading to enhanced corrosion. This study highlights the significance of incorporating dust particulate(s) beyond the deliquescent chemistries to fully evaluate atmospheric corrosion severity.

Sea salt↗