A selective solubility-driven separation of used nuclear fuel
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Gibbs, Taryn (ORCID:0000000335293934)↗
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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
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The influence of the 6s 2 configuration of Bi 3+ on the structures of A′BiNb 2 O 7 (A′ = Rb, Na, Li) layered perovskite oxides
Solid state compounds which exhibit non-centrosymmetric crystal structures are of great interest due to the physical properties they can exhibit. Here, the ‘hybrid improper’ mechanism – in which two non-polar distortion modes couple to, and stabilize, a further polar distortion mode, yielding an acentric crystal structure – offers opportunities to prepare a range of novel non-centrosymmetric solids, but examples of compounds exhibiting acentric crystal structures stabilized by this mechanism are still relatively rare. Here we describe a series of bismuth-containing layered perovskite oxide phases, RbBiNb 2 O 7 , LiBiNb 2 O 7 and NaBiNb 2 O 7 , which have structural frameworks compatible with hybrid-improper ferroelectricity, but also contain Bi 3+ cations which are often observed to stabilize acentric crystal structures due to their 6s 2 electronic configurations. Neutron powder diffraction analysis reveals that RbBiNb 2 O 7 and LiBiNb 2 O 7 adopt polar crystal structures (space groups I2cm and B2cm respectively), compatible with stabilization by a trilinear coupling of non-polar and polar modes. The Bi 3+ cations present are observed to enhance the magnitude of the polar distortions of these phases, but are not the primary driver for the acentric structure, as evidenced by the observation that replacing the Bi 3+ cations with Nd 3+ cations does not change the structural symmetry of the compounds. In contrast the non-centrosymmetric, but non-polar structure of NaBiNb 2 O 7 (space group P2 1 2 1 2 1 ) differs significantly from the centrosymmetric structure of NaNdNb 2 O 7 , which is attributed to a second-order Jahn-Teller distortion associated with the presence of the Bi3+ cations.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Elimination of the bias-stress effect in ligand-free quantum dot field-effect transistors
Field-effect transistors (FETs) made from colloidal quantum dot (QD) solids commonly suffer from current–voltage hysteresis caused by the bias-stress effect (BSE), which complicates fundamental studies of charge transport in QD solids and the use of QD FETs in electronics. Here, we show that the BSE can be eliminated in n-channel PbSe QD FETs by first removing the QD ligands with a dose of H 2 S gas and then infilling the QD films with alumina by atomic layer deposition (ALD). The H 2 S-treated, alumina-infilled FETs have stable, hysteresis-free device characteristics (total short-term stability), indefinite air stability (total long-term stability), and a high electron mobility of up to 14 cm 2 V −1 s −1 , making them attractive for QD circuitry and optoelectronic devices. The BSE-free devices are utilized to conclusively establish the dependence of the electron mobility on temperature and QD diameter. We demonstrate that the BSE in these devices is caused by both electron trapping at the QD surface and proton drift within the film. The H 2 S/alumina chemistry produces ligand-free PbSe/PbS/Al 2 O 3 interfaces that lack the traps that cause the electronic part of the BSE, while full alumina infilling stops the proton motion responsible for the ionic part of the BSE. In conclusion, our matrix engineering approach should aid efforts to eliminate the BSE, boost carrier mobilities, and improve charge transport in other types of nanocrystal solids.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Large ecosystem-scale effects of restoration fail to mitigate impacts of land-use legacies in longleaf pine savannas
Ecological restoration is a global priority, with potential to reverse biodiversity declines and promote ecosystem functioning. Yet, successful restoration is challenged by lingering legacies of past land-use activities, which are pervasive on lands available for restoration. Although legacies can persist for centuries following cessation of human land uses such as agriculture, we currently lack understanding of how land-use legacies affect entire ecosystems, how they influence restoration outcomes, or whether restoration can mitigate legacy effects. Using a large-scale experiment, we evaluated how restoration by tree thinning and land-use legacies from prior cultivation and subsequent conversion to pine plantations affect fire-suppressed longleaf pine savannas. In this work, we evaluated 45 ecological properties across four categories: 1) abiotic attributes, 2) organism abundances, 3) species diversity, and 4) species interactions. The effects of restoration and land-use legacies were pervasive, shaping all categories of properties, with restoration effects roughly twice the magnitude of legacy effects. Restoration effects were of comparable magnitude in savannas with and without a history of intensive human land use; however, restoration did not mitigate numerous legacy effects present prior to restoration. As a result, savannas with a history of intensive human land use supported altered properties, especially related to soils, even after restoration. The signature of past human land-use activities can be remarkably persistent in the face of intensive restoration, influencing the outcome of restoration across diverse ecological properties. Understanding and mitigating land-use legacies will maximize the potential to restore degraded ecosystems.
60 APPLIED LIFE SCIENCES↗
Environmental outcomes of the US Renewable Fuel Standard
Biofuels are included in many proposed strategies to reduce anthropogenic greenhouse gas emissions and limit the magnitude of global warming. The US Renewable Fuel Standard is the world’s largest existing biofuel program, yet despite its prominence, there has been limited empirical assessment of the program’s environmental outcomes. Even without considering likely international land use effects, we find that the production of corn-based ethanol in the United States has failed to meet the policy’s own greenhouse gas emissions targets and negatively affected water quality, the area of land used for conservation, and other ecosystem processes. Our findings suggest that profound advances in technology and policy are still needed to achieve the intended environmental benefits of biofuel production and use.
54 ENVIRONMENTAL SCIENCES↗
Peripheral positions encode transport specificity in the small multidrug resistance exporters
In secondary active transporters, a relatively limited set of protein folds have evolved diverse solute transport functions. Because of the conformational changes inherent to transport, altering substrate specificity typically involves remodeling the entire structural landscape, limiting our understanding of how novel substrate specificities evolve. In the current work, we examine a structurally minimalist family of model transport proteins, the small multidrug resistance (SMR) transporters, to understand the molecular basis for the emergence of a novel substrate specificity. We engineer a selective SMR protein to promiscuously export quaternary ammonium antiseptics, similar to the activity of a clade of multidrug exporters in this family. Using combinatorial mutagenesis and deep sequencing, we identify the necessary and sufficient molecular determinants of this engineered activity. Using X-ray crystallography, solid-supported membrane electrophysiology, binding assays, and a proteoliposome-based quaternary ammonium antiseptic transport assay that we developed, we dissect the mechanistic contributions of these residues to substrate polyspecificity. We find that substrate preference changes not through modification of the residues that directly interact with the substrate but through mutations peripheral to the binding pocket. Our work provides molecular insight into substrate promiscuity among the SMRs and can be applied to understand multidrug export and the evolution of novel transport functions more generally.
Science & Technology - Other Topics↗
Process for the Recovery of Actinide and Lanthanide Oxides via Thermal Decomposition and Calcination of Loaded Diglycolamide Resin
Diglycolamide (DGA) resin, a product produced by Eichrom Technologies, Inc. employs TODGA (N,N,N',N'-tetraoctyldiglycolamide) as the active extractant, which will be used by Savannah River National Laboratory to extract trivalent actinides and lanthanides from dissolved irradiated Mark-18A targets. The final form of the extracted material will be an oxide suitable for shipment. A two-step process was developed and validated for the direct recovery of actinides and lanthanides loaded on I-grade DGA resin as nitrates by thermally drying and decomposing resin loaded with Nd(III), a surrogate for trivalent actinides and lanthanides, under inert conditions followed by calcining the resultant residue in air to provide an oxide product. Further, a stepwise heating profile up to 385°C under argon gas flow resulted in 85% to 89% mass loss during the resin drying and decomposition step, and calcination of the resultant Nd-loaded resin residue provided an overall material mass loss of ≥ 98%. Recoveries from resin saturated with Nd(III) from 7 M and 0.35 M nitric acid subjected to this process were 30.7 mg and 27.6 mg Nd/g dry resin, respectively, representing an average of 96.1% of Nd retained in the resin bed.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Mechanical rolling and annealing of wire-arc additively manufactured stainless steel plates
Thin walls of 304L stainless steel were fabricated by wire-arc additive manufacturing (WAAM) followed by post build thermomechanical processing to modify the as built microstructure and properties. The walls were made using a high-deposition-rate robotically controlled gas-metal arc welding system and were characterized using optical microscopy and tensile tested for mechanical properties. Post processing consisted of mechanical rolling the walls to 25% and 40% strains, followed by annealing at 1050°C to demonstrate a wide range of properties. Results show that WAAM can be used to build custom sized semi-finished parts or blanks that can later be thermomechanically processed to increase strength and ductility through recrystallization of the as built microstructure, and/or processed into desired shapes with improved mechanical properties.
304L stainless steel↗
Astigmatic electron beam propagation
An astigmatic electron beam with an ellipticity ratio of approximately 2:1 was examined using the Enhanced Modified Faraday Cup (EMFC) diagnostic to measure its properties and show how the power density distribution varies near the beam waist. Results show that the beam has two power density peaks, one on either side of the beam crossover point, resulting from different focal distances of the major and minor axes of the elliptical beam shape. Quantification of the beam properties was used to establish a depth-of-field where the beam diameter and peak power densities are relatively constant. For the 1 kW beam studied here, the depth-of-field measured approximately ±5 mm from the beam crossover point, illustrating how electron beam diagnostics can be used to identify process control limits for repeatable and reliable welds under non-ideal electron beam power density distribution conditions.
36 MATERIALS SCIENCE↗
Modeling optical systematics for the Taurus CMB experiment
We simulate a variety of optical systematics for Taurus, a balloon-borne cosmic microwave background (CMB) polarisation experiment, to assess their impact on large-scale E-mode polarisation measurements and constraints of the optical depth to reionisation τ. We model a one-month flight of Taurus from Wanaka, New Zealand aboard a super-pressure balloon (SPB). We simulate night-time scans of both the CMB and dust foregrounds in the 150 GHz band, one of Taurus's four observing bands. We consider a variety of possible systematics that may affect Taurus's observations, including non-gaussian beams, pointing reconstruction error, and half-wave plate (HWP) non-idealities. For each of these, we evaluate the residual power in the difference between maps simulated with and without the systematic, and compare this to the expected signal level corresponding to Taurus's science goals. Our results indicate that most of the HWP-related systematics can be mitigated to be smaller than sample variance by calibrating with Planck's TT spectrum and using an achromatic HWP model, with a preference for five layers of sapphire to ensure good systematic control. However, additional beam characterization will be required to mitigate far-sidelobe pickup from dust on larger scales.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
Comment on ‘Carbon Intensity of corn ethanol in the United States: state of the science’
Abstract In their recent contribution, Scully et al (2021 Environ. Res. Lett. 16 043001) review and revise past life cycle assessments of corn-grain ethanol’s carbon (C) intensity to suggest that a current ‘central best estimate’ is considerably less than all prior estimates. Their conclusion emerges from selection and recombination of sector-specific greenhouse gas emission predictions from disparate studies in a way that disproportionately favors small values and optimistic assumptions without rigorous justification nor empirical support. Their revisions most profoundly reduce predicted land use change (LUC) emissions, for which they propose a central estimate that is roughly half the smallest comparable value they review (figure 1). This LUC estimate represents the midpoint of (a) values retained after filtering the predictions of past studies based on a set of unfounded criteria; and (b) a new estimate they generate for domestic (i.e. U.S.) LUC emissions. The filter the authors apply endorses a singular means of LUC assessment which they assert as the ‘best practice’ despite a recent unacknowledged review (Malins et al 2020 J. Clean. Prod. 258 120716) that shows this method almost certainly underestimates LUC. Moreover, their domestic C intensity estimate surprisingly suggests that cropland expansion newly sequesters soil C, counter to ecological theory and empirical evidence. These issues, among others, prove to grossly underestimate the C intensity of corn-grain ethanol and mischaracterize the state of our science at the risk of perversely affecting policy outcomes.
Spawn-Lee, Seth A. (ORCID:0000000188215345)↗
Variability in terrestrial characteristics and erosion rates on the Alaskan Beaufort Sea coast
Abstract Arctic coastal environments are eroding and rapidly changing. A lack of pan-Arctic observations limits our ability to understand controls on coastal erosion rates across the entire Arctic region. Here, we capitalize on an abundance of geospatial and remotely sensed data, in addition to model output, from the North Slope of Alaska to identify relationships between historical erosion rates and landscape characteristics to guide future modeling and observational efforts across the Arctic. Using existing datasets from the Alaska Beaufort Sea coast and a hierarchical clustering algorithm, we developed a set of 16 coastal typologies that captures the defining characteristics of environments susceptible to coastal erosion. Relationships between landscape characteristics and historical erosion rates show that no single variable alone is a good predictor of erosion rates. Variability in erosion rate decreases with increasing coastal elevation, but erosion rate magnitudes are highest for intermediate elevations. Areas along the Alaskan Beaufort Sea coast (ABSC) protected by barrier islands showed a three times lower erosion rate on average, suggesting that barrier islands are critical to maintaining mainland shore position. Finally, typologies with the highest erosion rates are not broadly representative of the ABSC and are generally associated with low elevation, north- to northeast-facing shorelines, a peaty pebbly silty lithology, and glaciomarine deposits with high ice content. All else being equal, warmer permafrost is also associated with higher erosion rates, suggesting that warming permafrost temperatures may contribute to higher future erosion rates on permafrost coasts. The suite of typologies can be used to guide future modeling and observational efforts by quantifying the distribution of coastlines with specific landscape characteristics and erosion rates.
54 ENVIRONMENTAL SCIENCES↗
A comparative analysis of US state-level policies and programs to advance energy justice
Abstract The US energy system is undergoing massive changes that have environmental, technological, and societal implications. Decisions and actions taken now will dramatically alter the trajectory of our future energy system. Though new technologies can lessen the dangers of anthropogenic climate change, an effective and sustainable transition requires addressing social justice issues as a priority. To this end, many states have implemented policies and programs that address energy justice. A formal survey of state-level energy justice policies and programs is needed to better understand the methods used to assist communities targeted and the impacts of these efforts. Such an analysis should include an analysis of the metrics used to judge the effectiveness of the enacted policies and programs. In this paper, we analyze the energy justice policies and programs of seven different US states. From this analysis, we identify three important aspects of state energy policies. First, most policies and programs do not articulate their goals, nor cite metrics to judge their successes. This lack of transparency and accountability is a major roadblock to truly just solutions. Second, states focus on a very narrow range of solutions for energy justice issues. The most prevalent being utility bill assistance, which does not address the systemic and enduring challenges faced by many low-income or historically marginalized communities. Lastly, comprehensive energy policy does not acknowledge and address housing, employment, education, and healthcare inequities that exacerbate energy system inequities. The work presented in this paper sheds light on the progress of state-level energy justice policies and programs across the United States, and we argue more work needs to be done to understand best practices in energy justice policymaking.
29 ENERGY PLANNING, POLICY, AND ECONOMY↗
Sawfly Genomes Reveal Evolutionary Acquisitions That Fostered the Mega-Radiation of Parasitoid and Eusocial Hymenoptera
The tremendous diversity of Hymenoptera is commonly attributed to the evolution of parasitoidism in the last common ancestor of parasitoid sawflies (Orussidae) and wasp-waisted Hymenoptera (Apocrita). However, Apocrita and Orussidae differ dramatically in their species richness, indicating that the diversification of Apocrita was promoted by additional traits. These traits have remained elusive due to a paucity of sawfly genome sequences, in particular those of parasitoid sawflies. Here, we present comparative analyses of draft genomes of the primarily phytophagous sawfly Athalia rosae and the parasitoid sawfly Orussus abietinus. Our analyses revealed that the ancestral hymenopteran genome exhibited traits that were previously considered unique to eusocial Apocrita (e.g., low transposable element content and activity) and a wider gene repertoire than previously thought (e.g., genes for CO 2 detection). Moreover, we discovered that Apocrita evolved a significantly larger array of odorant receptors than sawflies, which could be relevant to the remarkable diversification of Apocrita by enabling efficient detection and reliable identification of hosts.
59 BASIC BIOLOGICAL SCIENCES↗
The lowdown on breakdown: Open questions in plant proteolysis
Abstract Proteolysis, including post-translational proteolytic processing as well as protein degradation and amino acid recycling, is an essential component of the growth and development of living organisms. In this article, experts in plant proteolysis pose and discuss compelling open questions in their areas of research. Topics covered include the role of proteolysis in the cell cycle, DNA damage response, mitochondrial function, the generation of N-terminal signals (degrons) that mark many proteins for degradation (N-terminal acetylation, the Arg/N-degron pathway, and the chloroplast N-degron pathway), developmental and metabolic signaling (photomorphogenesis, abscisic acid and strigolactone signaling, sugar metabolism, and postharvest regulation), plant responses to environmental signals (endoplasmic-reticulum-associated degradation, chloroplast-associated degradation, drought tolerance, and the growth-defense trade-off), and the functional diversification of peptidases. We hope these thought-provoking discussions help to stimulate further research.
Eckardt, Nancy A. (ORCID:0000000316581412)↗
Anthropogenic uranium signatures in turtles, tortoises, and sea turtles from nuclear sites
Chelonians (turtles, tortoises, and sea turtles) grow scute keratin in sequential layers over time. Once formed, scute keratin acts as an inert reservoir of environmental information. For chelonians inhabiting areas with legacy or modern nuclear activities, their scute has the potential to act as a time-stamped record of radionuclide contamination in the environment. Here, we measure bulk (i.e., homogenized scute) and sequential samples of chelonian scute from the Republic of the Marshall Islands and throughout the United States of America, including at the Barry M. Goldwater Air Force Range, southwestern Utah, the Savannah River Site, and the Oak Ridge Reservation. We identify legacy uranium ( 235 U and 236 U) contamination in bulk and sequential chelonian scute that matches known nuclear histories at these locations during the 20th century. Our results confirm that chelonians bioaccumulate uranium radionuclides and do so sequentially over time. This technique provides both a time series approach for reconstructing nuclear histories from significant past and present contexts throughout the world and the ability to use chelonians for long-term environmental monitoring programs (e.g., sea turtles at Enewetok and Bikini Atolls in the Republic of the Marshall Islands and in Japan near the Fukushima Daiichi reactors).
63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗
Beam-based rf station fault identification at the SLAC Linac Coherent Light Source
Not Available
43 PARTICLE ACCELERATORS↗
Metastable ordered states induced by low-temperature annealing of δ − Ag 2 / 3 V 2 O 5
Not provided.
Materials Science↗