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DOE OSTI2022

Sex comparisons in physiological and cognitive performance during hypoxic challenge

Within the tactical aviation community, human performance research lags in considering potential psychophysiological differences between male and female aviators due to little inclusion of females during the design and development of aircraft systems. A poor understanding of how male and female aviators differ with respect to human performance results in unknown potential sex differences on aeromedically relevant environmental stressors, perchance leading to suboptimal performance, safety, and health guidelines. For example, previous hypoxia studies have excluded female participants or lacked a sizeable sample to examine sex comparisons. As such, progress toward sensor development and improving hypoxia familiarization training are stunted due to limited knowledge of how individual differences, including sex, may or may not underlie hypoxia symptoms and performance impairment. Investigating sex differences bridges the gap between aerospace medicine and operational health, and addressing hypoxia is one of many facets yet to be studied. In the current study, we retrospectively examined N = 6 hypoxia studies with male-female participant samples (total, N = 189; male, n = 118; female, n = 71). We explored sex as a predictor of physiological response, sensory deficits, the severity of cognitive performance declines, and symptom manifestation via linear and binary logistic regression models. We found that the female sex predicted lower peripheral oxygen saturation and the likelihood of headache reporting in response to hypoxic challenge, yet explained little variance when combined with age and body mass index. The sensory and cognitive performance models did not converge, suggesting high intra-individual variability. Together, sex, age, and body mass index were not the most robust predictors in responses to hypoxic challenge; we cannot infer this for sensory deficits and cognitive performance within an experimentally induced hypoxic environment. The findings have implications for improving hypoxia familiarization training, monitoring sensor development, and emergency response and recovery protocols in case of a hypoxia occurrence suitable for all aircrew. We recommend continuing to elucidate the impact of sex and intrapersonal differences in hypoxia and other aeromedically relevant stressors in tactical aviation.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2022

A Framework for Effective Science Communication and Outreach Strategies and Dissemination of Research Findings for Marine Energy Projects

Marine energy is an emerging renewable energy industry with the potential to produce 2300 terawatt-hours per year from resources within the United States. As development and testing of marine energy devices advance, regulatory and permitting decision-makers are concerned about the uncertainty surrounding the potential environmental effects resulting from the introduction of these novel devices in coastal and riverine environments. The Triton Initiative researches and provides recommendations for environmental monitoring technologies and methods to inform industry stakeholders with the data necessary to permit the testing of marine energy systems. Effective dissemination of the research findings is essential for improving the accessibility of data to stakeholders who may use the results to inform policy decisions, yet few frameworks for conducting science communications for marine energy projects exist. In this paper, we present tools, channels, and tactics for developing a science communication framework for marine energy projects, or similar areas of study, using the Triton Initiative’s pilot science communication program as a case study. By leveraging existing bodies of work in disciplines such as communications theory, marketing, public relations, and social science, the presented framework includes audience identification and analysis; channel development, including a website, blog, newsletter, social media, and webinars and presentations; and metrics for determining success. Outcomes from one year of Triton’s case study are presented, including the most effective tactics and lessons learned.

communication framework↗

DOE OSTI2023

Toughening Brittle Bio‐P3HB with Synthetic P3HB of Engineered Stereomicrostructures

Abstract Poly(3‐hydroxybutyrate) (P3HB), a biologically produced, biodegradable natural polyester, exhibits excellent thermal and barrier properties but suffers from mechanical brittleness, largely limiting its applications. Here we report a mono‐material product design strategy to toughen stereoperfect, brittle bio or synthetic P3HB by blending it with stereomicrostructurally engineered P3HB. Through tacticity ([ mm ] from 0 to 100 %) and molecular weight ( M n to 788 kDa) tuning, high‐performance synthetic P3HB materials with tensile strength to ≈30 MPa, fracture strain to ≈800 %, and toughness to 126 MJ m −3 (>110× tougher than bio‐P3HB) have been produced. Physical blending of the brittle P3HB with such P3HB in 10 to 90 wt % dramatically enhances its ductility from ≈5 % to 95–450 % and optical clarity from 19 % to 85 % visible light transmittance while maintaining desirably high elastic modulus (>1 GPa), tensile strength (>35 MPa), and melting temperature (160–170 °C). This P3HB‐toughening‐P3HB methodology departs from the traditional approach of incorporating chemically distinct components to toughen P3HB, which hinders chemical or mechanical recycling, highlighting the potential of the mono‐material product design solely based on biodegradable P3HB to deliver P3HB materials with diverse performance properties.

Zhang, Zhen↗

DOE OSTI2023

Toughening Brittle Bio‐P3HB with Synthetic P3HB of Engineered Stereomicrostructures

Chemistry↗

DOE OSTI2021

Plasticity of Behavioral and Growth Responses to Two Feeding Regimes and Implications for the Domestication of Steelhead Trout

Abstract The effects of domestication selection on fitness are of serious concern in hatchery-reared anadromous salmonids, which often experience selection for rapid growth and associated deviations from natural agonistic and feeding behaviors. The high rations that are used to raise age-1 smolts and the reduced rations that are used to produce age-2 smolts potentially result in very different behavioral tactics and social dynamics of competition in hatchery tanks. Consequently, steelhead Oncorhynchus mykiss hatchery programs with recovery or conservation goals may need to change their aquaculture practices to minimize domestication selection. This study investigated how the feeding rate (proportion of presented food items that were successfully captured) and relative competitive ability (ability to monopolize food items in small groups) of age-1 and age-2 steelhead corresponded to feeding location (surface or bottom) and growth rate in hatchery rearing tanks. We raised steelhead from a common broodstock to smolt at age 1 or age 2 by manipulating their rations (age-1 fish received the high ration, age-2 the low ration). The fish in the age-1 treatment had a lower feeding rate than did those in the age-2 treatment. Feeding rate was positively correlated with both body size and with growth rate in the rearing tanks at both rations. The age-2 steelhead were more likely to be detected at a single feeding location than were the age-1 fish, which were more frequently detected at both locations. The more competitive age-1 fish were more frequently detected at both feeding locations, and the less competitive fish were detected at only one location. Relative competitive ability was not associated with feeding location in the age-2 treatment, nor was it associated with growth rate in either treatment. Age-2 steelhead that were detected only at the bottom or at both feeding locations had higher growth rates than those that were detected only at the surface, suggesting greater scramble competition near the point of food delivery under the restricted ration. Feeding location was not associated with growth rate in the age-1 treatment. The results indicate that ration directly affects feeding rate and that ration and relative competitive ability interact to influence feeding rate. Because feeding rate was positively associated with growth rate at both ration levels in the hatchery tanks, behaviors that are associated with feeding motivation may be an important trait under selection in salmonid hatcheries.

Tatara, Christopher P.↗

DOE OSTI2022

Universally Accessible Structural Data on Macromolecular Conformation, Assembly, and Dynamics by Small Angle X-Ray Scattering for DNA Repair Insights.

Structures provide a critical breakthrough step for biological analyses, and small angle X-ray scattering (SAXS) is a powerful structural technique to study dynamic DNA repair proteins. As toxic and mutagenic repair intermediates need to be prevented from inadvertently harming the cell, DNA repair proteins often chaperone these intermediates through dynamic conformations, coordinated assemblies, and allosteric regulation. By measuring structural conformations in solution for both proteins, DNA, RNA, and their complexes, SAXS provides insight into initial DNA damage recognition, mechanisms for validation of their substrate, and pathway regulation. Here, we describe exemplary SAXS analyses of a DNA damage response protein spanning from what can be derived directly from the data to obtaining super resolution through the use of SAXS selection of atomic models. We outline strategies and tactics for practical SAXS data collection and analysis. Making these structural experiments in reach of any basic and clinical researchers who have protein, SAXS data can readily be collected at government-funded synchrotrons, typically at no cost for academic researchers. In addition to discussing how SAXS complements and enhances cryo-electron microscopy, X-ray crystallography, NMR, and computational modeling, we furthermore discuss taking advantage of recent advances in protein structure prediction in combination with SAXS analysis.

Chinnam, Naga Babu↗

DOE OSTI2020

Hypergraph Analytics of Domain Name System Relationships

We report on the use of novel mathematical methods in hypergraph analytice over a large quantity of DNS data. Hypergraphs generalize graphs, as used in network science, to better model complex multiway relations in cyber data. Specifically, casting DNS data from Georgia Tech's ActiveDNS repository as hypergraphs allows us to fully represent the interactions between {\em collections} of domains and IP addresses. To facilitate large-scale analytics, we fielded an analytical pipeline of two capabilities. HyperNetX (HNX) is a Python package for the exploration and visualization of hypergraphs, acting as a frontend. For the backend, the Chapel HyperGraph Library (CHGL) is a library for high performance hypergraph analytics written in the exascale programming language Chapel. CHGL was used to process gigascale DNS data, performing compute-intensive calculations for data reduction and segmentation. Identified portions are then sent to HNX for both exploratory analysis and knowledge discovery targeting known tactics, techniques, and procedures.

Joslyn, Cliff A.↗

DOE OSTI2022

Application of thermal energy storage with electrified heating and cooling in a cold climate

Ground source heat pumps (GSHPs) have been shown to be an effective means of decarbonizing building heating and cooling, but the operation of these systems at scale presents challenges to sites and the grid due to increases in peak demand. Here, in this study, we investigate how the use of Thermal Energy Storage (TES), in the form of stratified water storage, could reduce the peak daily demand associated with GSHP systems and thus improve their cost effectiveness. This system was compared to a Combined Heat and Power (CHP) plant, to investigate the potential cost and emissions impacts of electrification on large energy users transitioning from high efficiency fossil fuel equipment. This study builds on previous research by using a significant campus area, and investigating the various impacts of an electrified system versus a state of the art fossil fuel system. An established method of TRNSYS modeling is used for the heat pumps and borehole heat exchangers (BHEs), along with the TES. The GSHP system with TES is modeled to follow industry standards and sized to provide an optimal balance of capital and operating costs. Costs were investigated for a unique large energy user rate structure, as well as for a more common generalized rate structure. The results show that the addition of TES to the GSHP system could reduce operating costs by 4.5%, but still incurs a 5.64% cost increase from the baseline CHP system. It is also shown, however, that a tactical integration of heat pumps into the CHP system is the most cost effective solution, only increasing the operating costs by 4.71%. Likewise, the impacts of different rate structures are highlighted, with the TES only resulting in 0.75% cost savings under the generalized utility rate. Furthermore, it is shown that thermal storage has great potential for demand reduction, with the addition of storage incurring a decrease of 7–22% in annual peak demand kW, dependent on the rate structure.

25 ENERGY STORAGE↗

DOE OSTI2020

Enhancing perovskite electrocatalysis through synergistic functionalization of B-site cation for efficient water splitting

The family of perovskite oxides is a promising class of catalysts for diverse energy conversion processes including water splitting. In this work, a facile two-step manipulation (in-situ exsolution and post-sulfurization) strategy was proposed and applied to LaCo 0.2 Fe 0.8 O 3 (LCF) perovskite parent, through which, the electronic state, spatial immersion and intrinsic activity of B-site cobalt (Co) were stepwise tuned at nanoscale proximity accordingly (i.e., lattice Co ions segregated Co 0 → embedded CoS 2 ). Impressively, the as-prepared catalyst (S-LCF) obtains an emergent oxygen deficient microstructure seamlessly pinned with uniformly distributed CoS 2 nanoparticles (NPs), which demonstrates enhanced performance toward both oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), and shows good stability in overall water splitting. The density functional theory (DFT) calculations illustrate the optimized metal-oxygen covalency and hydrogen adsorption Gibbs free energy (Δ G H *) on S-LCF, which further buttresses the prominence of our B-site cation engineering tactics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

An integrated approach to optimizing concentration shock wave electrodialysis using 2D multicell simulation and response surface models

Shock wave electrodialysis (SWED) is a highly promising technique for energy-efficient ion separation in the context of a circular economy. This paper presents a approach way of modeling and improving SWED using a two-dimensional multicell model combined with the COMSOL program and response surface methodology. The model integrates the Nernst-Planck equation, Darcy's law, and first-order electroosmosis to examine the local concentration, flux of ionic species, distribution of current, and velocity of flow in SWED cells under various operating conditions. We first illustrate the clear depiction of concentration, velocity, and electric potential distribution through contours which aids in identifying optimal operating conditions and designing scalable SWED systems. The results emphasize the significance of surface charge density and voltage in influencing the features of shock waves for obtaining effective ion separation while optimizing energy consumption and improving current efficiency by controlling the retention time of feed flow. Here, this study defines two crucial characteristics of shock waves, namely the length of the flat depletion zone of a fully developed shock wave (shock wave height) and the distance of shock wave propagation (shock wave length). These properties significantly impact separation performance, as determined by the simulation results. Additionally, the response surface methodology is incorporated with the COMSOL models to develop predictive models and graph responses, enabling a more comprehensive understanding of the interactions between parameters and performance indicators, such as removal ratio, energy consumption, and water recovery. Finally, this work suggests design tactics for expanding SWED processes and outlines potential areas for further research. This research provides valuable insights into the prospective applications, design optimization, and scalability of SWED in the field of electrokinetic separation technologies for green chemistry and a circular economy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Dynamic modeling studies of basin-scale pressure interference and CO 2 plume evolution in multi-well geologic CO 2 storage

This research employs numerical modeling to analyze how CO 2 plumes and pressure fronts evolve when CO 2 is injected into a single storage formation from multiple projects located in proximity. Here, this analysis also evaluates the extent to which injection well spacing alleviates pressure buildup in the absence of active pressure management tactics. The simulation approach was based on a single, homogenous saline aquifer in which CO 2 injection occurs under a one-injector baseline case and several multi-well cases where well spacing varies. Analysis results show that the extent of pressure buildup is in the range of tens or a few hundreds of kilometers and contingent upon the defining pressure buildup demarcating the front edge. For the geological setting evaluated in this paper, our analysis suggests that without active basin pressure management strategies, commercial-scale projects would likely need to be sited far apart to avoid pressure interference from one another. Analysis results show the radius of CO 2 plume varies approximately from 2 to 3 km from injection wells (each injecting 1 Mt/year for 30 years) depending on cases and modeling parameters assumed. Given the pressure interference, this paper thus draws attention to the importance of greater coordination among storage operators and regulatory stakeholders. Because this analysis assumes a very specific geologic setting, this exploratory analysis bears further investigations across other geologic scenarios.

42 ENGINEERING↗

DOE OSTI2022

Synthetic biodegradable polyhydroxyalkanoates (PHAs): Recent advances and future challenges

This article reviews the advances made over the past five decades of research in developing effective chemocatalytic pathways to synthesize polyhydroxyalkanoates (PHAs), a prominent class of biodegradable polyesters found in nature and considered as sustainable alternatives to petroleum-based non-degradable plastics. Focused in this review are recent efforts that seek to address the key challenges facing the biosynthetic routes by taking advantage of precision in synthesis, expedient tunability in polymer stereomicrostructures and structures of monomers and molecular catalysts, as well as scalability and speed in polymer production that chemical catalysis can offer. This article is organized by poly(3-hydroxybutyrate) (P3HB) stereomicrostructures (tacticities), from isotactic to syndiotactic to atactic P3HB materials, followed by other PHA homopolymers and copolymers. Under each type of stereochemically defined PHAs, monomers, catalysts, and polymerizations employed for the synthesis, as well as mechanistic aspects when possible, are described. Next, recent advances in expanding the PHA scope and developing functionalized, uncommon or unnatural PHAs, inaccessible by biological methods, especially block and stereoblock or stereosequenced PHAs, are highlighted in their synthetic methods and advanced materials properties. As a result, four key remaining challenges, and thus corresponding future directions directed at addressing those challenges, are discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Update 1.1 to “pysimm: A python package for simulation of molecular systems”, (PII: S2352711016300395)

This update of the pysimm application programming interface, pysimm 1.1, provides both infrastructural as well as functional updates. Moreover, improvements to the random walk application that allow it to construct polymers with controlled tacticity are highlighted. Additions to the forcefield module include an update to enable working with the family of CHARMM forcefields and automated typing with the CHARMM generalized forcefield (CGenFF). Finally, new detailed examples demonstrating new features are also provided.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Desorption of Phosphate from Iron-Bearing Soil Minerals by a Plant Secondary Metabolite

In soils, phosphorus readily adsorbs to the surfaces of ubiquitous iron (oxyhydr)oxide minerals, rendering it less accessible to plants and microorganisms. Plants have a number of strategies to access iron, among them the secretion of redox-active metabolites from their roots. Although these strategies likely increase the bioavailability of surface-adsorbed phosphorus through reductive dissolution, their effect on phosphorus cycling has not yet been investigated. We tested the ability of fraxetin, a coumarin-type redox-active metabolite produced by the model plant Arabidopsis thaliana and other dicotyledon plant species, to reductively solubilize phosphate from the surface of ferrihydrite. Our findings show that, at low and neutral pH, fraxetin increased aqueous phosphate concentrations under both oxic and anoxic conditions; at high pH, it was only effective in anoxic experiments. Additionally, a combination of liquid chromatography–mass spectrometry and spectroscopic methods demonstrated substantial fraxetin adsorption to the mineral surface but showed that iron reduction did not alter the mineral structure or change the nature of the chemical environment of the phosphorus atom over short time scales. These results provide evidence that the secretion of redox-active metabolites from roots is likely to be an effective phosphorus acquisition tactic in iron-rich soils.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Harnessing Intermolecular Interactions to Promote Long-Lived Photoinduced Charge Separation from Copper Phenanthroline Chromophores

In this study, facilitating photoinduced electron transfer (PET) while minimizing rapid charge-recombination processes to produce a long-lived charge-separated (CS) state represents a primary challenge associated with achieving efficient solar fuel production. Natural photosynthetic systems employ intermolecular interactions to arrange the electron-transfer relay in reaction centers and promote a directional flow of electrons. This work explores a similar tactic through the synthesis and ground- and excited-state characterization of two Cu(I)bis(phenanthroline) chromophores with homoleptic and heteroleptic coordination geometries and which are functionalized with negatively charged sulfonate groups. The addition of sulfonate groups enables solubility in pure water, and it also induces assembly with the dicationic electron acceptor methyl viologen (MV 2+ ) via bimolecular, dynamic electrostatic interactions. The effect of the sulfonate groups on the ground- and excited-state properties was evaluated by comparison with the unsulfonated analogues in 1:1 acetonitrile/water. The excited-state lifetimes for all sulfonated complexes are similar to what we expect from previous literature, with the exception of the sulfonated heteroleptic complex whose metal-to-ligand charge-transfer (MLCT) lifetime in water has two components that are fit to 10 and 77 ns. For the sulfonated complexes, we detected reduced MV +$\bullet$ in both solvent environments following MLCT excitation, but control measurements in 1:1 acetonitrile/water with the unsulfonated analogues showed no PET to MV 2+ , indicating that electrostatically driven supramolecular assemblies of the sulfonated complexes with MV 2+ facilitate the observed PET. Additionally, the strength of the intermolecular interactions driving the formation of these assemblies changes drastically with the solvent environment. In 1:1 acetonitrile/water, PET occurred from both sulfonated complexes with quantum yields (Φ ET ) of 2-3% but increased to a remarkable 98% for the sulfonated heteroleptic complex with a 3 μs CS-state lifetime in water.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Sequence-Structure–Property Relationships in Short-Chain Polyesters: How Primary Structure Governs Macroscopic Performance

While polymer properties are fundamentally linked to their nanostructure, the influence of monomer sequence remains less understood than stereochemical factors like tacticity. This study examines how sequence distribution affects the thermal behavior and morphology of homo- and copolyesters, specifically comparing polymers derived from constitutionally identical monomers but with varying degrees of sequence regularity depending on monomer structure or polymerization selectivity. Our findings show that increasing sequence defects progressively diminish thermal stability, crystallinity, melting temperatures, and morphological order. As new materials become more compositionally complex, this work underscores the importance of sequence control in the design of advanced polymers for emerging applications.

Bocharova, Vera [Oak Ridge National Laboratory (OR↗

DOE OSTI2021

Nanolatticed Architecture Mitigates Damage in Shark Egg Cases

Structural versatility and multifunctionality of biological materials have resulted in countless bioinspired strategies seeking to emulate the properties of nature. The nanostructured egg case of swell sharks is one of the toughest permeable membranes known and, thus, presents itself as a model system for materials where the conflicting properties, strength and porosity, are desirable. The egg case possesses an intricately ordered structure that is designed to protect delicate embryos from the external environment while enabling respiratory and metabolic exchange, achieving a tactical balance between conflicting properties. Herein, structural analyses revealed an enabling nanolattice architecture that constitutes a Bouligand-like nanoribbon hierarchical assembly. Three distinct hierarchical architectural adaptations enhance egg case survival: Bouligand-like organization for in-plane isotropic reinforcement, noncylindrical nanoribbons maximizing interfacial stress distribution, and highly ordered nanolattices enabling permeability and lattice-governed toughening mechanisms. Furthermore, these discoveries provide fundamental insights for the improvement of multifunctional membranes, fiber-reinforced soft composites, and mechanical metamaterials.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2021

Drawing on Membrane Photocatalysis for Fouling Mitigation

Photocatalysis is an effective and environmentally friendly approach for degrading organic pollutants, particularly in scenarios where sunlight can be utilized as the energy source. Opportunities are emerging to apply materials and methods from photocatalytic pollutant degradation to address the challenge of fouling. Membrane fouling, attributed to organic foulants, is a prevalent problem for all membrane-based technologies and represents a major deleterious impact on membrane performance. Integration of tactics developed in photocatalysis more broadly to membranes reveals new strategies for membrane fouling control-an approach taken by an increasing number of researchers. Furthermore, this review summarizes key developments in photocatalytic materials and methods in water treatment and presents recent progress in the development of processes for photocatalytic alleviation of membrane fouling, including photocatalyst design and modification strategies aimed at enhancing photocatalytic efficiency, as well as different configurations of photocatalysis-membrane systems (PMS). Perspectives on future research and development opportunities for photocatalytic membrane fouling control are also provided.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗