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NASA NTRS2022

Mapping Firn Saturation over Greenland using NASA’s Soil Moisture Active Passive Satellite

Mapping the spatial extent of recently identified englacial hydrological features (i.e., ice slabs and perennial firn aquifers) formed by meters-thick water-saturated firn layers over the percolation facies of the Greenland Ice Sheet using L-band microwave radiometry has recently been demonstrated. However, these initial maps are binary, and do not provide a parameter to estimate the spatial variability in the thickness and volumetric fraction of meltwater stored within the firn pore space. Here, we exploit enhanced-resolution vertical-polarization L-band brightness temperature (T^(B)_(V)) imagery (2015–2019) generated using observations collected over Greenland by NASA’s Soil Moisture Active Passive (SMAP) satellite and a simple two-layer L-band brightness temperature model. We map water-saturated firn layers via a “firn saturation” parameter, and interpret our results together with ice slab and perennial firn aquifer spatial extents, estimates of snow accumulation simulated via the Regional Atmospheric Climate Model (RACMOp2.3), and airborne radar surveys collected via NASA’s Operation IceBridge (OIB) campaigns. We find that variable firn saturation parameter values are mapped in lower snow accumulation ice slab areas in western, northern, and northeastern Greenland, where firn is colder and water-saturated firn layers seasonally refreeze as solid-ice. Higher firn saturation parameter values are mapped in higher snow accumulation perennial firn aquifer areas in southeastern, southern, and northwestern Greenland, where firn is near the melting point, and meters-thick water-saturated firn layers exist. Our results have implications for identifying expansive englacial reservoirs that store significant volumes of meltwater in locations that are vulnerable to meltwater-induced hydrofracturing and accelerated outlet glacier flow year-round.

Greenland ice sheet↗

NASA NTRSDate not supplied

Effect of Pressure on Trace Element Activity Coefficients in Metal-Silicate Systems

The partitioning of trace elements between metal and silicate melts serves as the foundation for understanding the differentiation of a planetary body into a metallic core and silicate mantle. Element activity influences metal-silicate partitioning behavior. Activity coefficients are directly dependent on composition and temperature, and can be indirectly dependent on oxygen fugacity and pressure. Distinguishing the effect of pressure from other variables on the activity coefficients and partitioning is important for understanding the chemical evolution of different planetary bodies during differentiation. In this study, we investigated the influence of pressure on the activity coefficients of Cu, Mo, Pd, Pt, As, Sb, and Bi in Fe-Si metallic liquids. All of these elements exhibit moderate to high activity coefficients in Fe-Si liquids at low pressure, which significantly controls their metal-silicate partitioning behavior. Identifying whether this strong dependence persists at higher pressures is critical to modeling and understanding the chemical consequences of core formation. New experiments at 10 GPa were used to derive activity coefficients for these metals which can be compared to activity coefficients determined at 1 GPa. Experiments were conducted at 10 GPa and 2373K using a 10/5 assembly in the 880-ton multi-anvil press at NASA Johnson Space Center. The standard 10/5 COMPRES assembly was slightly modified to accommodate a sample capsule machined from single-crystal MgO that minimizes melt percolation out of the sample volume during the experiment. Experiment starting materials were comprised of 70 wt.% Knippa basalt and 30 wt.% metal. The metal mixture (~85 wt.% Fe) was created by adding the elements of interest (Cu, Mo, Pd, Pt, As, Sb, Bi) to Fe metal powder. Varied amounts of Si metal (0-10 wt.% Si) were added to the metal-silicate mixtures to generate a systematic series of starting materials. For each element, an epsilon interaction parameter in Fe-Si liquid was derived from the results of our 0-10 wt.% Si metal series. To investigate whether pressure influences the trace element activity coefficients in the 1-10 GPa pressure range, we compared our results at 10 GPa to those at 1-4 GPa [1-3]. Our results can also be directly compared to interaction parameters for Au, P, V, Mn, Ga, Zn, Cd, Sn, W, Pb, and Nb previously determined at 10 GPa and 2373K following the same methods [4]. Combined, this suite of interaction parameters will directly inform metal-silicate partitioning between 1 and 10 GPa, and assess whether these values can be extrapolated to modeling differentiation processes at pressures >10 GPa.

Kelsey Prissel↗

NASA NTRSDate not supplied

Effect of Pressure and Oxidation State on Pnictogen Metal-Silicate Partitioning

The partitioning of trace elements between metal and silicate melts serves as the foundation for understanding the differentiation of a planetary body into a metallic core and silicate mantle. Element activity influences metal-silicate partitioning behavior. Activity coefficients are directly dependent on composition and temperature, and can be indirectly dependent on oxygen fugacity and pressure. Distinguishing the effect of pressure from other variables on the activity coefficients and partitioning is important for understanding the chemical evolution of different planetary bodies during differentiation. In this study, we investigated the influence of pressure on the activity coefficients of Cu, Mo, Pd, Pt, As, Sb, and Bi in Fe-Si metallic liquids. All of these elements exhibit moderate to high activity coefficients in Fe-Si liquids at low pressure, which significantly controls their metal-silicate partitioning behavior. Identifying whether this strong dependence persists at higher pressures is critical to modeling and understanding the chemical consequences of core formation. New experiments at 10 GPa were used to derive activity coefficients for these metals which can be compared to activity coefficients determined at 1 GPa. Experiments were conducted at 10 GPa and 2373K using a 10/5 assembly in the 880-ton multi anvil press at NASA Johnson Space Center. The standard 10/5 COMPRES assembly was slightly modified to accommodate a sample capsule machined from single-crystal MgO that minimizes melt percolation out of the sample volume during the experiment. Experiment starting materials were comprised of 70 wt.% Knippa basalt and 30 wt.% metal. The metal mixture (~85 wt.% Fe) was created by adding the elements of interest (Cu, Mo, Pd, Pt, As, Sb, Bi) to Fe metal powder. Varied amounts of Si metal (0-10 wt.% Si) were added to the metal-silicate mixtures to generate a systematic series of starting materials. For each element, an epsilon interaction parameter in Fe-Si liquid was derived from the results of our 0-10 wt.% Si metal series. To investigate whether pressure influences the trace element activity coefficients in the 1-10 GPa pressure range, we compared our results at 10 GPa to those at 1-4 GPa [1-3]. Our results can also be directly compared to interaction parameters for Au, P, V, Mn, Ga, Zn, Cd, Sn, W, Pb, and Nb previously determined at 10 GPa and 2373K following the same methods [4]. Combined, this suite of interaction parameters will directly inform metal- silicate partitioning between 1 and 10 GPa, and assess whether these values can be extrapolated to modeling differentiation processes at pressures >10 GPa. [1] Righter et al. (2018) GCA 232, 101-123 [2] Righter et al. (2019) MaPS 54, 1379-1394 [3] Steenstra et al. (2020) Icarus, 335, 113391 [4] Righter et al. (2020) Geochem. Persp. Let. 15, 44-49

Kelsey Prissel↗

NASA NTRSDate not supplied

Improved Treatment of Snow Over Ice Sheets in the NASA GISS Climate Model: Towards Ice Sheet–Climate Coupling

Representing the interactions between ice sheets and climate is essential for more accurate prediction of climate change and sea level rise. Ice sheets interact with the overlying atmosphere via the accumulation of snow and its compaction into firn, then ice, as well as the melting of surface snow and ice and the creation of runoff water. Getting an adequate representation of heat transfer, compaction, and melting processes is essential for an accurate representation of snow on land ice in global climate models. We are implementing an improved snow model on top of land ice as part of an effort to couple the NASA GISS climate model with the PISM ice sheet model. The new snow model includes additional layers and processes that are not currently incorporated (e.g., liquid water retention, percolation and refreezing, and snow densification), and mass and energy transfer methods that are consistent with both static ice sheets (with implicit iceberg fluxes) and interactive ice sheets (with explicit dynamics). We are tuning the densification scheme of this snow model with temperature and density data from common FirnCover and SumUp observations at locations in the accumulation zone of Greenland, and we compare the resulting density profiles to other SumUp density profiles in Greenland and Antarctica. We will assess the impact of this new snow model in climate model simulations with a static ice sheet compared with the previous (simpler) 2-layer snow model. Finally, we aim to use the non-coupled simulations as a baseline to assess the impact of dynamic coupling with an interactive ice sheet model.

snow↗

NASA NTRS2024

Launch Complex 39B, SWMU 009, 2023 Performance Monitoring and Air Sparge Expansion Construction Completion Report, Kennedy Space Center, Florida

The 2023 Performance Monitoring and Construction Completion Report (PM-CCR) presents the findings, observations, and results for Air Sparging (AS) operations and expansion activities, as well as sitewide groundwater monitoring for Launch Complex 39B (LC39B), Solid Waste Management Unit (SWMU) 009, at Kennedy Space Center (KSC), Florida. The reporting period for activities covered under this PM-CCR is from January 1, 2023, to December 31, 2023. At LC39B, AS operations began in 2017 in the area west of the launch pad, in the liquid oxygen (LOX) tank area located northwest of the launch pad, and in an area outside of the perimeter fence to protect nearby Outstanding Florida Waters (OFW). The LC39B AS system was installed with 279 AS wells to depths ranging from 23 to 60 feet below land surface (bls), including the sump, correlating to top of screen depths ranging from 20 to 57 feet bls. In December 2022, a total of 22 AS wells were abandoned to support launch pad crane operations, and in November 2023, the system was expanded with five additional AS wells installed to 13 or 17 feet bls near the LOX tank. The remedial objective of the LC39B AS Interim Measure (IM) is to actively decrease concentrations of contaminants of concern (COCs) in groundwater, specifically trichloroethene (TCE), cis-1,2-Dichloroethene (cDCE), and vinyl chloride (VC), to less than their respective Natural Attenuation Default Concentrations (NADCs), so LC39B can transition into a Long-Term Monitoring (LTM) program. This PM-CCR presents the following information for LC39B: • AS system operations and maintenance (O&M) (Year 7 of operation) from January 2023 to December 2023, to include AS trailer relocation in March 2023 and subsequent replacement and re-start in June 2023. • Construction completion details for AS system expansion, which included installation of five new AS wells and one new monitoring well in November 2023. As part of expansion activities, soil samples were also collected for petroleum analysis; no exceedances were identified, and no further investigation for petroleum is warranted. • Performance monitoring results for groundwater sampling events conducted in May/June 2023 (30 wells) and November 2023 (31 wells) in the AS IM area and in the Low Concentration Plume (LCP) areas located north and east of the launch pad for volatile organic compound (VOC) analysis. • Sampling results for one monitoring well, LOX-IW0012S, which is sampled for aluminum on an annual basis (May/June 2023). This well was resampled in November 2023 for both total and dissolved aluminum. Due to a communication error with the laboratory, the May/June 2023 sample was analyzed for total aluminum only. • Groundwater sampling results for per- and polyfluoroalkyl substances (PFAS) collected from seven monitoring wells during the May/June 2023 event to further investigate the Former Sewage Treatment Plant #6 and Percolation Pond area, west of the launch pad. O&M and performance monitoring results show that the AS system at LC39B is operating as designed and meeting performance criteria. Overall runtime was 45 percent (%) during the reporting period (January to December), but the operational runtime was 78% during the timeframe when the system could run (June to December). The most significant downtime contributor was post-launch crane operations following the Artemis launch on November 16, 2022, which lasted until June 2023. During that timeframe, the AS trailer at LC39B was relocated to another KSC remediation site (Wilson Corners) and was subsequently replaced with the AS trailer from the Paint & Oil Locker (POL) remediation site at KSC to resume AS system operations. Performance monitoring results in the AS IM and LCP areas continue to show reduction in COC concentrations over time when compared to baseline levels. In 2023, only one monitoring well (MW0048) detected a COC exceeding its NADC (VC at 740 micrograms per liter [µg/L]), which marks the baseline result for this new well installed during system expansion. Across the rest of the site, VC concentrations have declined or remained stable during the 2023 sampling events. Excluding MW0048, the highest VC result in 2023 was during the May/June sampling event with a concentration of 63 µg/L at MW0032, which is located near MW0048 and the AS expansion area by the LOX tank. TCE was detected in select monitoring wells in the IM area in 2023, but only two locations exceeded the State of Florida Groundwater Cleanup Target Level (GCTL): MW0032 (21 µg/L in May/June 2023 and 9.1 µg/L in November 2023) and MW0036 (5.0 µg/L in November 2023). MW0036 is also located near the LOX tank, on the north side, where the AS system is still operational (Zone Z4). cDCE and trans-1,2-dichloroethene concentrations were less than laboratory method detection limits or their respective GCTLs in all wells sampled in 2023. Near the OFW located northwest of the launch complex, all COC concentrations were less than laboratory method detection limits from monitoring wells (MW0039, MW0040, and LOXTA0002S) sampled in 2023. Aluminum results from LOX-IW0012S, which has been sampled routinely since 2006, detected a total aluminum concentration of 3,900 µg/L during the May/June 2023 sampling event. Results from the November 2023 event detected 5,700 µg/L for total aluminum and 5,500 µg/L for dissolved aluminum. These concentrations slightly decreased from the previous year but remain relatively consistent with historical detections. Aluminum will continue to be sampled on an annual basis at this well as results still exceed the GCTL of 200 µg/L and the Upper Limit of the KSC Background Concentration of 280 µg/L. PFAS results detected nine different PFAS compounds (out of 32 analyzed) from seven wells sampled. Two PFAS compounds, perfluorooctanesulfonic acid (PFOS) and perfluorooctanoic acid (PFOA), currently have FDEP Provisional GCTLs of 70 nanograms per liter (ng/L). All seven samples collected resulted in concentrations less than the FDEP Provisional GCTLs for both PFAS compounds; no exceedances were observed. PFOS and PFOA also have assigned United States Environmental Protection Agency (USEPA) Maximum Contaminant Levels (MCLs) of 4 nanograms per liter (ng/L). None of the PFOS results exceeded the USEPA MCLs. PFOA was detected in two samples above the USEPA MCL at concentrations of 5.8 ng/L (ECS-IW0009I) and 5.5 ng/L (ECS-IW0009S). Three other PFAS compounds, perfluorohexanesulfonic acid (PFHxS), perfluoro-n-nonanoic acid (PFNA), and hexafluoropropylene oxide dimer acid (GenX), currently have USEPA MCLs of 10 ng/L. PFHxS, PFNA, and GenX were not detected at concentrations greater than their respective USEPA MCLs in any of the seven wells. PFAS compounds without FDEP Provisional GCTLs or USEPA MCLs were screened against USEPA RSLs. No other detections exceeded their respective USEPA RSLs. Additional PFAS sampling will be conducted as part of a future PFAS Site Assessment. Based on O&M activities and performance monitoring, the following is recommended for LC39B: • Continue with Year 8 AS system operation within Zone Z4, which includes the AS expansion area. Zone Z3, which has been off since 2018, should remain off as no rebound has been observed. Zones Z1 and Z2, which were turned off at the end of 2022, will remain shut down as monitoring well results have consistently been below GCTLs or have low-level detections with stable or decreasing trends (Meeting Minute 2402-M10, Decision 2402-D30). • Continue with performance monitoring in 2024 with the same monitoring well network as 2023, except with the addition of MW0048 in both semi-annual events. Baseline concentrations for this well were collected during the November 2023 performance monitoring event. Semi-annual sampling should be planned for the May 2024 and November 2024 timeframes (Meeting Minute 2402-M10, Decision 2402-D31). • Continue sampling monitoring well, LOX-IW0012S, for aluminum (total and dissolved) on an annual basis in May 2024. It is also recommended to re-develop this well prior to the next sampling event (Meeting Minute 2402-M10, Decision 2402-D32). The above recommendations for LC39B were presented at the February 2024 KSCRT Meeting, with Team consensus reached on the path forward. The contents of this PM-CCR were also presented at this meeting.

Deborah M Wilson↗

NASA NTRS2026

Application of Energy-efficient Electromagnetic Melt-Processing for the Upcycling of Recycled Polyphenylene Sulfide into Multifunctional Segregated Nanocomposites

Polyphenylene sulfide (PPS) is widely used in structural and functional composites because of its thermal stability, chemical resistance, and mechanical strength. As circular manufacturing becomes increasingly important, extending the service life of recycled PPS (rPPS) is essential. However, conventional high-temperature reprocessing accelerates thermo-oxidative degradation, reducing recycled composite performance. This study proposes a rapid and potentially energy-saving upcycling strategy for rPPS using electromagnetic (EM) melt-processing to form segregated carbon nanotube (CNT) networks and produce EM-responsive nanocomposites. The aim was to determine whether CNT-assisted EM heating could reduce polymer degradation while improving multifunctional properties at ultralow filler loadings. rPPS micropellets were coated with CNTs by ball milling to create conductive shells, then compacted into green bodies (GBs) and selectively melted by rapid EM irradiation. Structural, electrical, mechanical, rheological, and electromagnetic interference (EMI) shielding properties were evaluated. Electrical percolation occurred at an ultralow CNT loading of 0.08 wt%, with conductivity reaching (1.24 ± 0.74) × 10 -5 S⋅m -1 at 0.1 wt%. At this concentration, tensile strength and modulus increased by 72% and 99%, respectively. At ~ 0.7 mm thickness, X-band EMI shielding effectiveness reached 6 dB for GBs and 3 dB after EM processing. This shows that EM melt-processing upcycles rPPS into high-performance multifunctional nanocomposites with minimum thermal degradation.

recycled↗

DOE OSTI2012

Random-Walk Monte Carlo Simulation of Intergranular Gas Bubble Nucleation in UO2 Fuel

Using a random-walk particle algorithm, we investigate the clustering of fission gas atoms on grain bound- aries in oxide fuels. The computational algorithm implemented in this work considers a planar surface representing a grain boundary on which particles appear at a rate dictated by the Booth flux, migrate two dimensionally according to their grain boundary diffusivity, and coalesce by random encounters. Specifically, the intergranular bubble nucleation density is the key variable we investigate using a parametric study in which the temperature, grain boundary gas diffusivity, and grain boundary segregation energy are varied. The results reveal that the grain boundary bubble nucleation density can vary widely due to these three parameters, which may be an important factor in the observed variability in intergranular bubble percolation among grain boundaries in oxide fuel during fission gas release.

36 MATERIALS SCIENCE↗

DOE OSTI2012

Advanced Remedial Methods for Metals and Radionuclides in Vadose Zone Environments

Functionally, the methods for addressing contamination must remove and/or reduce transport or toxicity of contaminants. This problem is particularly challenging in arid environments where the vadose zone can be up to hundreds of feet thick, rendering transitional excavation methods exceedingly costly and ineffective. Delivery of remedial amendments is one of the most challenging and critical aspects for all remedy-based approaches. The conventional approach for delivery is through injection of aqueous remedial solutions. However, heterogeneous vadose zone environments present hydrologic and geochemical challenges that limit the effectiveness. Because the flow of solution infiltration is dominantly controlled by gravity and suction, injected liquid preferentially percolates through highly permeable pathways, bypassing low-permeability zones which frequently contain the majority of the contamination. Moreover, the wetting front can readily mobilize and enhance contaminant transport to underlying aquifers prior to stabilization. Development of innovative, in-situ technologies may be the only way to meet remedial action objectives and long-term stewardship goals. Shear-thinning fluids (i.e., surfactants) can be used to lower the liquid surface tension and create stabile foams, which readily penetrate low permeability zones. Although surfactant foams have been utilized for subsurface mobilization efforts in the oil and gas industry, so far, the concept of using foams as a delivery mechanism for transporting reactive remedial amendments into deep vadose zone environments to stabilize metal and long-lived radionuclide contaminants has not been explored. Foam flow can be directed by pressure gradients rather than being dominated by gravity, and, foam delivery mechanisms limit the volume of water (< 20% vol.) required for remedy delivery and emplacement, thus mitigating contaminant mobilization. We will present the results of an integrated laboratory- / intermediate-scale investigation to simulate, develop, demonstrate, and monitor (using advanced geophysical techniques and natural marker monitoring) foam-based delivery of remedial amendments to stabilize metals and radionuclides in vadose zone environments.

Foam Delivery↗

DOE OSTI2014

SISGR: Atom chip microscopy: A novel probe for strongly correlated materials

Microscopy techniques co-opted from nonlinear optics and high energy physics have complemented solid-state probes in elucidating the order manifest in condensed matter materials. Up until now, however, no attempts have been made to use modern techniques of ultracold atomic physics to directly explore properties of strongly correlated or topologically protected materials. Our current program is focused on introducing a novel magnetic field microscopy technique into the toolbox of imaging probes. Our prior DOE ESPM program funded the development of a novel instrument using a dilute gas Bose-Einstein condensate (BEC) as a scanning probe capable of measuring tiny magnetic (and electric) DC and AC fields above materials. We successfully built the world's first “scanning cryogenic atom chip microscope”, and we now are in the process of characterizing its performance before using the instrument to take the first wide-area images of transport flow within unconventional superconductors, pnictides and oxide interfaces (LAO/STO), topological insulators, and colossal magnetoresistive manganites. We will do so at temperatures outside the capability of scanning SQUIDs, with ~10x better resolution and without 1/f-noise. A notable goal will be to measure the surface-to-bulk conductivity ratio in topological insulators in a relatively model-independent fashion. We have completed the construction of this magnetic microscope. The instrument uses atom chips—substrates supporting micron-sized current-carrying wires that create magnetic microtraps near surfaces for ultracold thermal gases and BECs—to enable single-shot and raster-scanned large-field-of-view detection of magnetic fields. The fields emanating from electronic transport may be detected at the 10 -7 flux quantum (Φ0) level and below; that is, few to sub-micron resolution of sub-nanotesla fields over single-shot, millimeter-long detection lengths. By harnessing the extreme sensitivity of atomic clocks and BECs to external perturbations, we are now in a position to use atom chips for imaging transport in new regimes. Scanning quantum gas atom chip microscopy introduces three very important features to the toolbox of high-resolution scanning microscopy of strongly correlated or topological materials: simultaneous detection of magnetic and electric fields (down to the sub-single electron charge level; no invasive large magnetic fields or gradients; simultaneous micro- and macroscopic spatial resolution; DC to MHz detection bandwidth; freedom from 1/ƒ flicker noise at low frequencies; and, perhaps most importantly, the complete decoupling of probe and sample temperatures. The atom chip microscope can operate at maximum sensitivity and resolution without regard to the substrate temperature. While the BEC is among the coldest objects realizable (100 nK temperatures are typical), the atom chip substrate can be positioned 1 μm away from the BEC and be as hot as 400 K or as cold as the cryostat can cool. This is because unlike superconducting probes, whose temperature is closely coupled to nearby materials, quantum gases are immune to radiative heating. The energy gap between a Rb atom’s ground state and first excited state far exceeds the typical energy of room-temperature blackbody radiation; such atoms are therefore transparent to radiation heating by materials at room temperature or below. We experimentally demonstrated a new atom chip trapping system that allows the placement and high-resolution imaging of ultracold atoms within microns from any ≤100 μm-thin, UHV-compatible material, while also allowing sample exchange with minimal experimental downtime. The sample is not connected to the atom chip, allowing rapid exchange without perturbing the atom chip or laser cooling apparatus. Exchange of the sample and retrapping of atoms has been performed within a week turnaround, limited only by chamber baking. Moreover, the decoupling of sample and atom chip provides the ability to independently tune the sample temperature and its position with respect to the trapped ultracold gas, which itself may remain in the focus of a high-resolution imaging system. We confine 100-nK BECs of 104 87Rb atoms near a gold-mirrored 100-μm-thick silicon substrate. The substrate can be cooled to 35 K without use of a heat shield, while the atom chip, 120-μm away, remains at room temperature. Atoms may be imaged with 1-μm resolution and retrapped every 16 s, allowing rapid data collection. Straightforward improvements will allow us to push sample temperatures close to 4 K, and improve imaging resolution from 1 μm down to a few-100 nm, thereby providing 10 -9 Φ0 detection sensitivity. We will test the utility of this technique by imaging the magnetic fields emanating from electronic transport and domain percolation in several interesting examples of strongly correlated or topologically protected materials. STM, transport, and x-ray scattering experiments have, among others, revealed the existence of a quantum liquid crystal state in iron (pnictide) and cuprate superconductors. This strongly correlated state of matter could also be detected by imaging the fluctuating transport (spatially and in time) of electrons as the phase/regime boundary is crossed between the pnictide non-Fermi liquid (cuprate strange metal) and the pnictide magnetic phase (cuprate pseudogap regime). Our ability to image wide-area inhomogeneous current flow from room-temperature to <10 K will allow us to study the developing domain structure and transport near twin boundary interfaces through the T N ≈50–150 K nematic transition recently identified in bulk transport experiments by Ian Fisher's group in underdoped Fe-arsinide superconductors. Again, this highlights a main feature of our cryogenic atom chip microscope: the ability to image transport regardless of the sample temperature since the BEC, at nK temperatures, is transparent to blackbody radiation, even when held a microns from the surface.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Rates and Mechanisms of Oil Shale Pyrolysis: A Chemical Structure Approach

Three pristine Utah Green River oil shale samples were obtained and used for analysis by the combined research groups at the University of Utah and Brigham Young University. Oil shale samples were first demineralized and the separated kerogen and extracted bitumen samples were then studied by a host of techniques including high resolution liquid-state carbon-13 NMR, solid-state magic angle sample spinning 13C NMR, GC/MS, FTIR, and pyrolysis. Bitumen was extracted from the shale using methanol/dichloromethane and analyzed using high resolution 13C NMR liquid state spectroscopy, showing carbon aromaticities of 7 to 11%. The three parent shales and the demineralized kerogens were each analyzed with solid-state 13C NMR spectroscopy. Carbon aromaticity of the kerogen was 23-24%, with 10-12 aromatic carbons per cluster. Crushed samples of Green River oil shale and its kerogen extract were pyrolyzed at heating rates from 1 to 10 K/min at pressures of 1 and 40 bar and temperatures up to 1000°C. The transient pyrolysis data were fit with a first-order model and a Distributed Activation Energy Model (DAEM). The demineralized kerogen was pyrolyzed at 10 K/min in nitrogen at atmospheric pressure at temperatures up to 525°C, and the pyrolysis products (light gas, tar, and char) were analyzed using 13C NMR, GC/MS, and FTIR. Details of the kerogen pyrolysis have been modeled by a modified version of the chemical percolation devolatilization (CPD) model that has been widely used to model coal combustion/pyrolysis. This refined CPD model has been successful in predicting the char, tar, and gas yields of the three shale samples during pyrolysis. This set of experiments and associated modeling represents the most sophisticated and complete analysis available for a given set of oil shale samples.

Fletcher, Thomas↗

DOE OSTI2017

Engineered glass seals for solid-oxide fuel cells

A seal for a solid oxide fuel cell includes a glass matrix having glass percolation therethrough and having a glass transition temperature below 650.degree. C. A deformable second phase material is dispersed in the glass matrix. The second phase material can be a compliant material. The second phase material can be a crushable material. A solid oxide fuel cell, a precursor for forming a seal for a solid oxide fuel cell, and a method of making a seal for a solid oxide fuel cell are also disclosed.

30 DIRECT ENERGY CONVERSION↗

DOE OSTI2016

SILICON CARBIDE GRAIN BOUNDARY DISTRIBUTIONS, IRRADIATION CONDITIONS, AND SILVER RETENTION IN IRRADIATED AGR-1 TRISO FUEL PARTICLES

Precession electron diffraction in the transmission electron microscope was used to map grain orientation and ultimately determine grain boundary misorientation angle distributions, relative fractions of grain boundary types (random high angle, low angle or coincident site lattice (CSL)-related boundaries) and the distributions of CSL-related grain boundaries in the SiC layer of irradiated TRISO-coated fuel particles. Two particles from the AGR-1 experiment exhibiting high Ag-110m retention (>80%) were compared to a particle exhibiting low Ag-110m retention (<19%). Irradiated particles with high Ag-110m retention exhibited a lower fraction of random, high angle grain boundaries compared to the low Ag-110m retention particle. An inverse relationship between the random, high angle grain boundary fraction and Ag-110m retention is found and is consistent with grain boundary percolation theory. Also, comparison of the grain boundary distributions with previously reported unirradiated grain boundary distributions, based on SEM-based EBSD for similarly fabricated particles, showed only small differences, i.e. a greater low angle grain boundary fraction in unirradiated SiC. It was, thus, concluded that SiC layers with grain boundary distributions susceptible to Ag-110m release were present prior to irradiation. Finally, irradiation parameters were found to have little effect on the association of fission product precipitates with specific grain boundary types.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2019

Electrothermal coating with nanostructures mixture and method for making the same

An electrothermal coating can include a nanostructure mixture randomly dispersed in a polymer matrix with more than one type of low-dimensional nanostructure. These types of low-dimensional nanostructures can include a combination of a nanospheroid plus one or both of a linear nanostructure and a planar nanostructure. Useful conductivity is achieved, while concentration of the mixed nanostructures is within the cured polymer composite coating being below the percolation limit of each individual carbon nanostructure type, alone, within an identical polymer matrix.

36 MATERIALS SCIENCE↗

DOE OSTI2019

High optical transparent two-dimensional electronic conducting system and process for generating same

Hybrid transparent conducting materials are disclosed with combine a polycrystalline film and conductive nanostructures, in which the polycrystalline film is “percolation doped” with the conductive nanostructures. The polycrystalline film preferably is a single atomic layer thickness of polycrystalline graphene, and conductive nanostructures preferably are silver nanowires.

Alam, Muhammad Ashraful↗

DOE OSTI2015

A Dual Stage Sodium Thermo-Electro-Chemical Converter

The need for reliable and distributable energy sources is evident given the current forecasting of the world’s energy demand [1]. One prominent obstacle is the lack of an efficient direct heat-to-electricity conversion technology. The sodium thermo-electro-chemical converter (Na-TECC) is a highly efficient thermally regenerative electrochemical system (TRES) that can fill this void. The advantage of the Na-TECC over other direct conversion technologies is that it is a closed device (unlike fuel cells) requiring nothing more than a heat input (similar to thermoelectrics). It also has a high power density (> 1 W/cm2) and specific power up to 0.5 kW/kg , with the potential to achieve > 45% heat to electricity conversion efficiencies [2]. Furthermore, the converter rejects heat at a temperature hot enough to make it amenable for cogeneration, potentially under air-cooled operation. This electrochemical technology uses a special ion-selective solid-electrolyte called beta-alumina (Na2O•11Al2O3), that is highly conductive to sodium cations. A more conducting variation of this compound is beta”-alumina (Na2O•MgO•5Al2O3), where the magnesium acts as a stabilizer [3]. In the device, liquid sodium enters an evaporator where it is heated isobarically and vaporizes. The vapor is then oxidized at the interface between the anode and the solid-electrolyte. The Na-TECC generates electric power by allowing the high pressure oxidized sodium vapor ions to expand isothermally through the solid-electrolyte from the anode to the cathode. The liberated electrons are simultaneously conducted through an external load and recombine with the cations at the cathode. The low pressure sodium vapor is subsequently condensed and a wick pumps the liquid into the high pressure plenum to complete the cycle. Previous Na-TECCs have achieved efficiencies of 18% due to practical losses, whereas the potential efficiencies are above 45% [4]. Thermodynamic limitations and design constraints have limited previous devices from attaining these record efficiencies. Specifically, the maximum potential voltage in these previous devices was substantially reduced by the kinetic limitations of the charge transfer in the cathode (referred to as the overpotential) and by Joule heating losses due to the solid-electrolyte resistance, electrode resistance, and current collector resistance. Moreover, previous devices experienced a steady loss in performance throughout their lifetime. The drop in performance has been attributed to the electrolyte undergoing thermal and chemical breakdown due to crack propagation, loss of sodium oxide, and the formation of molten dendrites that create electrical shorts [5]. Finally, previous designs have also had a substantial problem with proper thermal management, with some showing thermal losses as great as 50% of the heat input. To improve the efficiency, a dual stage conversion process is being explored. Rather than using one isothermal expansion step, the dual cycle will employ two separate electrolytes to allow two separate expansion steps: one at the high temperature, and another at an intermediate temperature. This new cycle is thermodynamically favorable as it allows for regeneration from the isobaric cooling of the first expansion step, and reheat to complete the expansion in the second step. This allows the engine to reach a lower condenser temperature than its single stage counterpart, thus increasing the overall efficiency. The temperature drop across each electrolyte in the dual stage device (e.g., ~ 400 K) is smaller than the temperature drop across a comparable single stage device (e.g., ~ 800 K). This is amenable for better thermal management and allows for less heat loss. This will also mitigate the thermal shock across the very thin (< 1 mm) solid electrolytes, reduce crack propagation and limit the percolation of the molten dendrites, and ultimately increase the lifetime of the device. As an additional benefit the dual stage can be designed using planer geometries, rather than tubular geometries used in previous single stage models, which can be manufactured less expensively. This modified geometry can be tailored to improve the thermal management by reducing the radiation losses, which has been the biggest source of thermal losses [2]. A dual stage concept for the Na-TECC has never been demonstrated in literature. In this presentation, the operation of a single stage device will be revisited and, by adopting concepts used for similar converters, the thermodynamic operation of the dual stage will be developed [6]. Using the dual stage approach, the efficiency and power equations have been redefined to include regeneration and reheat. Questions such as what current densities optimize the power output or which intermediate temperature maximizes the efficiency will also be answered. Initial calculations of the dual stage show that the thermal management is the most sensitive parameter. Although the ideal voltage produced by the dual stage can be higher, there are potential drawbacks. For example, by using a lower condenser temperature the dual stage device will have a higher open circuit voltage, but it will also have a larger overpotential due to the limited cathodic kinetics that occur at a lower temperature. In short, there are several trade-offs in this device that need to be balanced. It will be demonstrated that the dual stage device must have lower thermal losses than a single stage device if it is to have a higher efficiency.

14 SOLAR ENERGY↗

DOE OSTI2016

Thermodynamics of a Dual Stage Sodium Thermo-Electro-Chemical Converter

The need for reliable and distributable energy is evident, but one prominent obstacle is the lack of an efficient direct heat-to-electricity converter. The sodium thermo-electro-chemical converter (Na-TECC) is a highly efficient thermally regenerative electrochemical system (TRES) that can fill this void. This electrochemical technology uses an ion-selective solid-electrolyte called beta-alumina that is highly conductive to sodium cations. The Na-TECC generates electric power by allowing high pressure sodium cations to expand isothermally through the solid-electrolyte. Theoretically, a device interacting with thermal reservoirs at 1150 K and 550 K should operate above 45% efficiency, but actual devices have not surpassed efficiencies of 20%. The maximum potential voltage in these previous devices was substantially reduced by the kinetic limitations of the charge transfer in the cathode (referred to as the overpotential) and by Joule heating losses due to the solid-electrolyte resistance, electrode resistance, and current collector resistance. To overcome this discrepancy, a dual stage conversion process is being proposed. Rather than using one isothermal expansion step, the dual cycle will employ two separate electrolytes to allow two separate expansion steps: one at the high temperature, and another at an intermediate temperature. This new cycle is thermodynamically favorable as it allows for regeneration from the isobaric cooling of the first expansion step, and reheat to complete the expansion in the second step. This allows the engine to reach a lower condenser temperature than its single stage counterpart for a given heat input, resulting in an increased overall efficiency. The temperature drop across each electrolyte in the dual stage device (e.g., ~ 400 K) is smaller than the temperature drop across a comparable single stage device (e.g., ~ 800 K). This makes the device amenable to better thermal management and allows for less heat loss. Also, the intermediate stage will mitigate the thermal shock across the very thin (< 1 mm) solid electrolyte, reduce crack propagation, limit the percolation of the molten dendrites, and ultimately increase the lifetime of the device. A dual stage concept for the Na-TECC has never been demonstrated in literature, so it is necessary to properly re-define the thermodynamic parameters such as heat loss, maximum power, and optimal current density. Certain drawbacks from a dual stage concept will also be addressed, such as the need for larger electrochemical area and the increased pressure losses. It will be demonstrated that the dual stage device must have lower thermal losses than a single stage device if it is to have a higher efficiency. The improved operation of the Na-TECC can have a transformational effect on small combined heat and power (CHP) systems at the 1-5 kW range.

14 SOLAR ENERGY↗

DOE OSTI2017

Dual Stage Sodium Thermo-Electro-Chemical Converter (Na-TEC)

The need for reliable and distributable energy is evident, but one prominent obstacle is the lack of an efficient direct heat-to-electricity converter. The sodium thermo-electro-chemical converter (Na-TECC) is a highly efficient thermally regenerative electrochemical system (TRES) that can fill this void. This device uses an ion-selective solid-electrolyte called beta”-alumina that is highly conductive to sodium cations. The Na-TECC generates electric power by allowing high pressure sodium cations to expand isothermally through the solid-electrolyte. Theoretically, a device interacting with thermal reservoirs at 1150 K and 550 K should operate above 45% efficiency, but actual devices have not surpassed efficiencies of 20%. The maximum potential voltage in these previous devices was substantially reduced by the kinetic limitations of the charge transfer in the cathode, by pressure losses through the porous electrodes, and by Joule heating losses caused by the solid-electrolyte, electrode, and current collector resistances. To overcome these low efficiencies, a dual stage conversion process is being proposed. Rather than using one isothermal expansion step, the dual cycle will employ a second electrolyte to allow two separate expansion steps: one at the high temperature, and another at an intermediate temperature. This new cycle is thermodynamically favorable as it allows for regeneration from the isobaric cooling of the first expansion step, and reheat to complete the expansion in the second step. This allows the engine to reach a lower condenser temperature than its single stage counterpart for a given heat input, resulting in an increased overall efficiency. The temperature drop across each electrolyte in the dual stage device (e.g., ~ 400 K) is smaller than the temperature drop across a comparable single stage device (e.g., ~ 600 K). This makes the device amenable to better thermal management and allows for less heat loss. Also, the intermediate stage will mitigate the thermal shock across the very thin (< 1 mm) solid electrolyte, reduce crack propagation, limit the percolation of the molten dendrites, and ultimately increase the lifetime of the device. A dual stage concept for the Na-TECC has never been demonstrated in literature, so it is necessary to properly re-define the thermodynamic parameters such as heat loss, maximum power, and optimal current density. Certain drawbacks from a dual stage concept will also be addressed, such as the need for larger electrochemical area and the increased pressure losses. It will be demonstrated that the dual stage device must have lower thermal losses than a single stage device if it is to have a higher efficiency. The improved operation of the Na-TECC can have a transformational effect on small combined heat and power (CHP) systems at the 1-5 kW range.

14 SOLAR ENERGY↗

DOE OSTI2020

High optical transparent two-dimensional electronic conducting system and process for generating same

Alam, Muhammad Ashraful↗