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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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At least 361 records · Page 20
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Microbial sensor variation across biogeochemical conditions in the terrestrial deep subsurface

ABSTRACT Microbes can be found in abundance many kilometers underground. While microbial metabolic capabilities have been examined across different geochemical settings, it remains unclear how changes in subsurface niches affect microbial needs to sense and respond to their environment. To address this question, we examined how microbial extracellular sensor systems vary with environmental conditions across metagenomes at different Deep Mine Microbial Observatory (DeMMO) subsurface sites. Because two-component systems (TCSs) directly sense extracellular conditions and convert this information into intracellular biochemical responses, we expected that this sensor family would vary across isolated oligotrophic subterranean environments that differ in abiotic and biotic conditions. TCSs were found at all six subsurface sites, the service water control, and the surface site, with an average of 0.88 sensor histidine kinases (HKs) per 100 genes across all sites. Abundance was greater in subsurface fracture fluids compared with surface-derived fluids, and candidate phyla radiation (CPR) bacteria presented the lowest HK frequencies. Measures of microbial diversity, such as the Shannon diversity index, revealed that HK abundance is inversely correlated with microbial diversity ( r 2 = 0.81). Among the geochemical parameters measured, HK frequency correlated most strongly with variance in dissolved organic carbon ( r 2 = 0.82). Taken together, these results implicate the abiotic and biotic properties of an ecological niche as drivers of sensor needs, and they suggest that microbes in environments with large fluctuations in organic nutrients (e.g., lacustrine, terrestrial, and coastal ecosystems) may require greater TCS diversity than ecosystems with low nutrients (e.g., open ocean). IMPORTANCE The ability to detect extracellular environmental conditions is a fundamental property of all life forms. Because microbial two-component sensor systems convert information about extracellular conditions into biochemical information that controls their behaviors, we evaluated how two-component sensor systems evolved within the deep Earth across multiple sites where abiotic and biotic properties vary. We show that these sensor systems remain abundant in microbial consortia at all subterranean sampling sites and observe correlations between sensor system abundances and abiotic (dissolved organic carbon variation) and biotic (consortia diversity) properties. These results suggest that multiple environmental properties may drive sensor protein evolution and highlight the need for further studies of metagenomic and geochemical data in parallel to understand the drivers of microbial sensor evolution.

response regulator↗
DOE OSTI2026

Fundamental chemical physics revealed by scattering reactive open-shell atoms from surfaces

The dynamics of reactive atoms at surfaces are centrally important to areas such as heterogeneous catalysis, corrosion, materials degradation in extreme environments, and plasma etching. Remarkably detailed understanding of dynamical processes at surfaces has been extracted from scattering molecules and inert atoms under well-defined conditions. However, traditional techniques for generating beams of reactive atoms often result in impure mixtures, broad energy distributions, and poorly defined contributions of metastable electronically excited atoms. In this perspective article, we review the state-of-the-art in reactive atom surface scattering with a focus on experiments performed under controlled conditions on well-defined surfaces. We highlight a new technique for controlled state-to-state scattering of polyelectronic atoms from surfaces, based on vacuum ultraviolet photolysis and state-selective ion imaging. The new capabilities provide an avenue for research into the underexplored area of excited state and spin selective chemical dynamics at surfaces.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

3D modeling of deep borehole electromagnetic measurements with energized casing source for fracture mapping at the Utah Frontier Observatory for Research in Geothermal Energy

Here, we present a 3D numerical modelling analysis evaluating the deployment of a borehole electromagnetic measurement tool to detect and image a stimulated zone at the Utah Frontier Observatory for Research in Geothermal Energy geothermal site. As the depth to the geothermal reservoir is several kilometres and the size of the stimulated zone is limited to several 100 m, surface-based controlled-source electromagnetic measurements lack the sensitivity for detecting changes in electrical resistivity caused by the stimulation. To overcome the limitation, the study evaluates the feasibility of using a three-component borehole magnetic receiver system at the Frontier Observatory for Research in Geothermal Energy site. To provide sufficient currents inside and around the enhanced geothermal reservoir, we use an injection well as an energized casing source. To efficiently simulate energizing the injection well in a realistic 3D resistivity model, we introduce a novel modelling workflow that leverages the strengths of both 3D cylindrical-mesh-based electromagnetic modelling code and 3D tetrahedral-mesh-based electromagnetic modelling code. The former is particularly well-suited for modelling hollow cylindrical objects like casings, whereas the latter excels at representing more complex 3D geological structures. In this workflow, our initial step involves computing current densities along a vertical steel-cased well using a 3D cylindrical electromagnetic modelling code. Subsequently, we distribute a series of equivalent current sources along the well's trajectory within a complex 3D resistivity model. We then discretize this model using a tetrahedral mesh and simulate the borehole electromagnetic responses excited by the casing source using a 3D finite-element electromagnetic code. This multi-step approach enables us to simulate 3D casing source electromagnetic responses within a complex 3D resistivity model, without the need for explicit discretization of the well using an excessive number of fine cells. We discuss the applicability and limitations of this proposed workflow within an electromagnetic modelling scenario where an energized well is deviated, such as at the Frontier Observatory for Research in Geothermal Energy site. Using the workflow, we demonstrate that the combined use of the energized casing source and the borehole electromagnetic receiver system offer measurable magnetic field amplitudes and sensitivity to the deep localized stimulated zone. The measurements can also distinguish between parallel-fracture anisotropic reservoirs and isotropic cases, providing valuable insights into the fracture system of the stimulated zone. Besides the magnetic field measurements, vertical electric field measurements in the open well sections are also highly sensitive to the stimulated zone and can be used as additional data for detecting and imaging the target. We can also acquire additional multiple-source data by grounding the surface electrode at various locations and repeating borehole electromagnetic measurements. This approach can increase the number of monitoring data by several factors, providing a more comprehensive dataset for analysing the deep-localized stimulated zone. The numerical analysis indicates that it is feasible to use the combination of the energized casing and downhole electromagnetic measurements in monitoring localized stimulated zone at large depths.

58 GEOSCIENCES↗
DOE OSTI2021

Ten Years of Progress in the Synthesis and Development of MXenes

Since their discovery in 2011, the number of 2D transition metal carbides and nitrides (MXenes) has steadily increased. Currently more than 40 MXene compositions exist. The ultimate number is far greater and in time they may develop into the largest family of 2D materials known. MXenes’ unique properties, such as their metal-like electrical conductivity reaching ≈20 000 S cm –1 , render them quite useful in a large number of applications, including energy storage, optoelectronic, biomedical, communications, and environmental. The number of MXene papers and patents published has been growing quickly. The first MXene generation is synthesized using selective etching of metal layers from the MAX phases, layered transition metal carbides and carbonitrides using hydrofluoric acid. Since then, multiple synthesis approaches have been developed, including selective etching in a mixture of fluoride salts and various acids, non-aqueous etchants, halogens, and molten salts, allowing for the synthesis of new MXenes with better control over their surface chemistries. In this paper, a brief historical overview of the first 10 years of MXene research and a perspective on their synthesis and future development are provided. The fact that their production is readily scalable in aqueous environments, with high yields bodes well for their commercialization.

2D materials↗
DOE OSTI2020

Anion Reactivity in Cation‐Disordered Rocksalt Cathode Materials: The Influence of Fluorine Substitution

Abstract The demand for high energy‐density, mass‐producible cathode materials has spurred the exploration of new material structures and compositions. Lithium‐excess, cation‐disordered rocksalt (DRX) materials are a new class of transition metal oxides that display high capacity and environmental friendly composition. These materials achieve their high capacities partially through oxygen redox, which leads to oxygen loss and detrimental reactivity with the electrolyte. It has previously been shown that oxygen loss can be suppressed by partial substitution of the lattice oxygen for fluorine, but the explicit mechanism behind this effect remains unknown. In this work, differential electrochemical mass spectrometry (DEMS) and titration mass spectrometry are used to quantify the primary electrochemical reactions occurring during the first cycle in DRX materials. Comparing a DRX oxide and a DRX oxyfluoride, it is shown that fluorination limits oxygen redox and suppresses oxygen loss. Additionally, DEMS is coupled with fluoride‐scavenging to demonstrate that small amounts of fluorine dissolve from DRX oxyfluorides during the first cycle. Finally, these techniques are extended over the first several cycles, demonstrating that CO 2 evolution persists and fluoride dissolution continues to a diminishing extent during the first few cycles. These findings motivate surface modifications to control interfacial reactivity and improve long‐term cycling.

Crafton, Matthew J.↗
DOE OSTI2022

Tailoring solid-electrolyte interphase and solvation structure for subzero temperature, fast-charging, and long-cycle-life sodium-ion batteries

The sluggish Na + reaction kinetics with carbon materials limits the fast-charging capability, Coulombic efficiency, and cycle life of sodium-ion batteries, especially at low temperatures. Herein, free-standing carbon nanofiber films, with controllable crystallinity and surface chemistry, are used as a platform to investigate the correlation between Na + reaction kinetics, storage mechanism, and electrolyte environment. The ion solvation effect and solid-electrolyte interphase (SEI) properties determine the kinetics and storage mechanism. A strong Na + -solvent interaction, such as Na + -diglyme, tends to form a "pseudo-SEI" layer dominated by anion decomposition, enabling fast Na + -solvent co-intercalation kinetics. Tuning the SEI chemistries by pre-cycling in the weakly solvated electrolyte (e.g., ester electrolyte), the intercalation capacity rapidly disappears due to the high energy barrier for Na + transport. Finally, such mechanistic insights allow us to develop the optimal combination of electrode materials and electrolyte chemistry to achieve high initial Coulombic efficiency, ultra-long cycle life under fast charging, and excellent low-temperature performance.

25 ENERGY STORAGE↗
DOE OSTI2022

Reticulated porous lanthanum strontium manganite structures for solar thermochemical hydrogen production

Porous ceramic foams are utilized in various fields and applications due to their advantageous properties such as high porosity, high specific surface area, and controlled permeability. Non-stoichiometric oxide foams are of particular interest for the solar thermochemical production of hydrogen in directly irradiated solar receivers due to their enhanced heat transfer capabilities and structural integrity. Here we report the fabrication of lanthanum strontium manganite replica foams and their solar thermochemical water splitting performance. Highly porous (>80%) foams were produced with controlled structure and tested in a high temperature water splitting furnace to demonstrate stability and overall performance. The temperature profile of the burnout and sintering of the foam structure were altered based on simultaneous differential scanning calorimetry and thermal gravimetry analysis. Two-step sintering was used both to retain micron-sized pores (D50 = 0.4 μm) on the foam's struts and to limit grain growth to a grain size of ~1 μm. The structural characteristics were confirmed by porosimetry and scanning electron microscopy. The foams were repeatedly cycled, producing approximately 200 μmol/g of H 2 per cycle. Water splitting performance was tested for 50 cycles and approximately 35 h at 1400 °C. No statistical difference in the effective hydrogen production per cycle was observed, which is promising for long-term redox cycle stability.

08 HYDROGEN↗
DOE OSTI2020

ECCI analysis of shear accommodations at grain boundaries in commercially pure alpha titanium

This study uses a novel approach that couples electron channeling contrast imaging (ECCI) with controlled removal of surface material to investigate the slip system/grain boundary interactions by assessing the geometry of slip planes and grain boundaries as a function of depth. The comparison of spacing, relative distributions, and correlations of slip bands across grain boundaries reveals surface biasing on the slip band behavior in the grain boundary region. Furthermore, using analysis of the compatibility factor m’, the Schmid factor of each slip system, and the angles θ between slip planes, a more comprehensive understanding of the details of the mechanisms of strain transfer and heterogeneous deformation is developed. In general, the misalignment of primary slip systems on the grain boundary planes necessitates the activation of secondary accommodating slip systems close to the grain boundary area that are better aligned (higher m’ and lower θ) with respect to the incoming slip system across the grain boundary. Such systems have the same Burgers vector as the primary slip systems within the respective grains, but are typically on low mobility slip planes.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2020

Ion redistributions at interfaces facilitate nucleation and growth of branched Ag 3 PO 4 polypods

Branched structures are of spectacular interest due to their improved light-harvesting, direct carrier transportation pathway, high surface area, and controllable electronic structures. Understanding their growth mechanisms and controlling factors enables the design of materials with improved functions. Interfaces of liquid-solid and air-liquid are known to change the chemical and physical properties of the liquid solution. However, their role in crystal growth, especially of branched structures, is seldom investigated. In this work we synthesized branched silver phosphate polypods in a thin layer of aqueous solution at room temperature taking advantage of the unique properties near the interfaces. The branched crystals nucleate and grow with a liquid thickness of 810 µm or below requiring the presence of both the gas-liquid and liquid-solid interfaces. The hydrophilicity of the solid substrate also facilitates nucleation and growth. Our results indicate that the synergism of long-range electric fields (ion distributions) at the interfaces promotes not only the nucleation and growth of silver phosphate but also the formation of branched structures. This work can be a reference for facilitating crystal nucleation and growth and controlling structures with specific morphologies, such as branched ones, by understanding and mimicking the properties at the interfaces.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Wavefront preserving X-ray optics for Synchrotron and Free Electron Laser photon beam transport systems

We report in the last two decades, after the first light from the new Free Electron Lasers, either in the UV (FLASH and FERMI@Elettra) or X-ray (LCLS and SACLA), more and more new diffraction limited sources have been either constructed or planned. Third generation storage rings are upgraded to provide a more collimated, brighter, and coherent light for the next generation experimental techniques. X-ray optics are the bridge between the light sources and the experimental stations. They are the key to the success of advanced experiments but also the potential bottleneck preventing the exploitation of the full characteristics of the source. The beam degradation originated by any mirror defect (either from mirror polishing or from contamination) is amplified with a coherent source. Delivering diffraction-limited spots, including the option for variable spot sizes in and out of focus, requires the control of the surface of the optics at the 1 nm rms level, if not better. At LCLS, only very recently an almost perfectly uniform beam out of focus has been obtained in the hard X-rays. It has been obtained after two 1-m long mirrors with 0.5 nm rms shape precision (after installation). Those mirrors were not readily available just a decade ago. But, thanks to the pioneering work performed at the Osaka University, those optics are now commercially available with arbitrary tangential profiles. This new generation of mirrors permits achieving unprecedented results. However, they do not remove all road blocks to a perfect photon transport system. Instead, they highlighted the critical importance of mirror mounting, handling of the thermal deformation, and the need of advanced diagnostics to properly exploit all the new potentiality of these optics. Besides the need of “perfect” mirrors, other aspects of the beamline design and elements may impact the quality of the beam in the experimental station, from the lack of blaze gratings to the need of advanced simulation tools, just to cite two. In this article, after a brief historical excursus, we will present the current state of the art of mirrors, gratings, crystals, lenses, diagnostics, and simulation tools. The main problems yet to solve and a look ahead at what would be achievable in the next decade will give the reader an idea on the search for an almost ideal photon transport system and how the path toward experiments, not conceivable today, will unfold.

47 OTHER INSTRUMENTATION↗
DOE OSTI2025

Facet-Dependent Adsorption of Pb(II) on Hematite (001), (116), and (104) Surfaces

Hematite’s common (001) and (012) facets are frequently used in model studies of lead (Pb) adsorption behavior, but there is a lack of research on the high-energy facets, e.g. (104), present in nature. Also, few studies have attempted to connect the molecular details of facet-specific Pb adsorption to macroscopic uptake behavior. Here, to address these knowledge gaps, we investigated Pb(II) adsorption behaviors on facet-engineered hematite nanoparticles dominated by (001), (104), and (116). Adsorption experiments revealed significant variations in Pb(II) uptake among the three samples, with (001) demonstrating the highest capacity and (116) showing the best adsorption efficiency when normalized to specific surface area. Adsorption kinetics followed the pseudo-second-order model, indicating the adsorption process is governed mostly by chemisorption. Adsorption isotherms were well fitted by the Langmuir model, indicating uptake proceeds until roughly monolayer adsorption. Detailed characterization revealed Pb(II) was adsorbed as single atoms with complex inner-sphere binding modes that varied across different facets, indicating adsorption is both structurally and energetically facet-dependent. Co-adsorption experiments further demonstrated Cu 2+ , Zn 2+ , and humic acid significantly promoted Pb(II) adsorption. This study advances the understanding of hematite surface reactivity in controlling macroscopic wet adsorption behaviors, providing valuable insights into the environmental fate of Pb(II).

Contaminant removal↗
DOE OSTI2022

Electrochemical Hydrogenation of CO on Cu(100): Insights from Accurate Multiconfigurational Wavefunction Methods

Copper (Cu) remains the most efficacious electrocatalyst for electrochemical CO 2 reduction (CO 2 R). Its activity and selectivity are highly facet-dependent. We recently examined the commonly proposed rate-limiting CO hydrogenation step on Cu(111) via embedded correlated wavefunction (ECW) theory and demonstrated that only this higher-level theory yields predictions consistent with potential-dependent experimental kinetics. Here, to understand the differing activities of Cu(111) and Cu(100) in catalyzing CO 2 R, we explore CO hydrogenation on Cu(100) using ECW theory. We predict that the preferred pathway involves the reduction of adsorbed CO (*CO) to *COH via proton-coupled electron transfer (PCET) at working potentials, although *CHO also may form with a kinetically accessible but higher barrier. In contrast, our earlier work on Cu(111) concluded that *COH and *CHO formation via PCET are equally feasible. Furthermore, this work illustrates one possible origin of the facet dependence of CO 2 R mechanisms and products on Cu electrodes and sheds light on how the selectivity of CO 2 R electrocatalysts can be controlled by the surface morphology.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2020

Dialing in Catalytic Sites on Metal Organic Framework Nodes: MIL-53(Al) and MIL-68(Al) Probed with Methanol Dehydration Catalysis

Many metal organic frameworks (MOFs) incorporate metal oxide clusters as nodes. Node sites where linkers are missing can be catalytic sites. We now show how to dial in the number and occupancy of such sites in MIL-53 and MIL-68, which incorporate aluminum-oxide-like nodes. Here, the methods involve modulators used in synthesis and postsynthesis reactions to control the modulator-derived groups on these sites. We illustrate the methods using formic acid as a modulator, giving formate ligands on the sites, and these can be removed to leave μ 2 -OH groups and open Lewis acid sites. Methanol dehydration was used as a catalytic reaction to probe these sites, with infrared spectra giving evidence of methoxide ligands as reaction intermediates. Control of node surface chemistry opens the door for placement of a variety of ligands on a wide range of metal oxide cluster nodes for dialing in reactivity and catalytic properties of a potentially immense class of structurally well-defined materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Tailoring the Near-Surface Environment of Rh Single-Atom Catalysts for Selective CO 2 Hydrogenation

For this study, we used a combination of experimental spectroscopies, density functional theory calculations, and CO 2 hydrogenation studies to investigate the effects of modifying single-atom Rh 1 /TiO 2 catalysts with functionalized phosphonic acid monolayers. We found that the deposition of specific amine-functionalized ligands resulted in an ~8× increase in site-specific CO 2 reduction turnover frequency at 150 °C and a ~2× increase at 250 °C. On-stream stability also improved following ligand deposition. The effect of the modifier on reactivity was highly sensitive to the proximity of the amine functional group to the surface, which was controlled by adjusting the length of the phosphonic acid tail. Furthermore, deposition of alkyl phosphonic acids without an amine functional group resulted in blocked CO 2 adsorption and a near-complete loss of catalytic activity. Infrared spectroscopy studies suggested that the amine group provided binding sites for CO 2 that enabled hydrogenation when the amine was positioned near a Rh1 site. Phosphonic acid-modified catalysts also exhibited high selectivity to CO over the series product methane; the selectivity effect was traced to modification of the Rh1 sites to favor CO desorption. Phosphonic acid deposition resulted in 80–90% loss of accessible Rh1 sites, likely due to blocking by tail groups. However, even with the loss of sites, under low-temperature reaction conditions, the rates of CO 2 hydrogenation were improved with the coatings, indicating that the remaining sites are highly efficient. Organic functionalization of the supports for atomically dispersed catalysts offers the opportunity to precisely control the positioning of functional groups in the vicinity of a well-defined active site, potentially enabling an additional level of control over active site design.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Impacts of Pore Network-Scale Wettability Heterogeneity on Immiscible Fluid Displacement: A Micromodel Study

The mixed-wet nature of reservoir formations imposes a wide range of rock wettability from strong resident-fluid wetting to strong invading-fluid wetting. The characteristics of two-phase flow in porous media composed of mixed-wetting surfaces remain poorly understood. In this study, we investigated the displacement of resident ethylene glycol (EG) by hexane in two mixed-wet micromodels of identical 2.5-D geometry heterogeneity, with uniformly or heterogeneously distributed patches strongly wetting to hexane. These patches are mixed among pores with unaltered EG-wetting surfaces. Along with control tests in the originally EG-wet micromodel, here we show the classic fingering and transitions in flow regimes at $logCa$ (capillary number) from -7.2 to -3.9. Moreover, pore-scale distributions of wettability and their spatial correlation influence displacement efficiency. In the two mixed-wet micromodels, we found (a) an increase of steady-state hexane saturation at the end of experiments by up to 0.12 in the capillary fingering regime and a decrease of at most by 0.06 in the viscous fingering regime, compared to the EG-wet micromodel, and (b) dispersed and fragmented hexane distribution after displacement. Brine drainage during supercritical CO 2 (scCO 2 ) injections in these micromodels occurs with lower wettability contrasts, and under similar viscosity ratios and interfacial tensions resulted in higher displacement efficiency relative to displacement of EG by hexane. While mixed-wettability can enhance displacement efficiency compared to uniform wettability, the dynamics of immiscible fluids in strong mixed-wet reservoirs are expected to be less pronounced in contributing to the efficiency of geological CO 2 sequestration, oil recovery, and remediation of hydrocarbon-contaminated aquifers.

2.5-D micromodel↗
DOE OSTI2024

Local and General Patterns of Terrestrial Water‐Carbon Coupling

Abstract Terrestrial carbon uptake and water availability have coupled feedbacks; specifically water uptake for plant growth and soil drying via transpiration. While we might expect this coupling over time at arid sites, climatic water availability also widely covaries geographically with biomass variables that control photosynthetic rates. Using eddy covariance data globally, we find convex, positively‐covarying relations between carbon uptake and a turbulent flux metric controlled by land surface moisture (r = 0.73 monthly across sites) at the site level. We estimate a general, empirical relationship based on site‐wise water‐carbon dynamics. Most sites, and the general relationship, show strong power‐law dependence, implicating the role of sub‐seasonal land‐cover dynamics. We also find that long‐term mean carbon/water states follow a similar convex relationship to the site‐specific temporal dynamics. We discuss opportunities and caveats for space‐for‐time frameworks of carbon/water feedback processes globally.

Geology↗
DOE OSTI2023

Synthesis of core/shell nanocrystals with ordered intermetallic single-atom alloy layers for nitrate electroreduction to ammonia

Structurally ordered intermetallic nanocrystals (NCs) and single-atom catalysts (SACs) are two emerging catalytic motifs for sustainable chemical production and energy conversion. However, both have synthetic limitations which can lead to the aggregation of NCs or metal atoms. Single-atom alloys (SAAs), which contain isolated metal atoms in a host metal, can overcome the aggregation concern because of the thermodynamic stabilization of single atoms on host metal surfaces. We report a direct solution-phase synthesis of Cu/CuAu core/shell NCs with tunable SAA layers. This synthesis can be extended to other Cu/CuM (M = Pt, Pd) systems, in which M atoms are isolated in the copper host. Using this method, the density of SAAs on a copper surface can be controlled, resulting in both low and high densities of single atoms. Alloying gold into the copper matrix introduced ligand effects that optimized the chemisorption of *NO 3 and *N. As a result, the densely packed Cu/CuAu material demonstrated a high selectivity toward NH 3 from the electrocatalytic nitrate reduction reaction with an 85.5% Faradaic efficiency while maintaining a high yield rate of 8.47 mol h -1 g -1 . This work advances the design of atomically precise catalytic sites by creating core/shell NCs with SAA atomic layers, opening an avenue for broad catalytic applications.

36 MATERIALS SCIENCE↗