Search NASA⌕ Search

SEARCH · Search NASA

Results for “Facets”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 559 records · Page 31
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Alternating Conditional Expectations: Introducing a Non‐Parametric Statistical Method to Interpret Long‐Term Greenhouse Gas Flux Measurements Over Semi‐Arid and Wetland Ecosystems

Abstract We explore the potential of using a non‐parametric statistical method called Alternating Conditional Expectations, ACE, to quantify functional relationships in biogeosciences. Here, ACE is used to quantify the non‐linear and multi‐faceted responses of greenhouse gas fluxes to a set of biophysical forcings, when the shapes of those response surfaces are unknown. We evaluated the statistical method over two contrasting ecosystems and two contrasting time steps. One case involved quantifying the biophysical controls of water vapor and carbon dioxide (CO 2 ) fluxes over a semi‐arid oak savanna using daily integrated fluxes. The other case evaluated the responses of CO 2 and methane (CH 4 ) flux measurements to a set of biophysical forcings at a restored tidal wetland using thirty‐minute averages. The statistical model, based on 4 independent variables, explained up over 90% of the variation in daily integrated flux densities of water vapor and net carbon dioxide exchange at the savanna site. This fit was defined by distinct non‐linear responses to such drivers as gross primary production, photosynthetically active radiation, air temperature, vapor pressure deficit and soil moisture. At the tidal wetland site, we evaluated net carbon dioxide and methane fluxes with short‐term measurements to capture the influence of rising and falling tides and seasonality in biological activity. The statistical model defined the shape of the forcing of fluxes due to the roles of carbon exudates, water table depth, oxygen level in the water column, temperature and vegetation status. The statistical fits of the greenhouse gas fluxes were less precise than the savanna case. The fetch varies on a run‐to‐run basis as it is comprised of a heterogeneous mosaic of open water and vegetation. Furthermore, it is difficult to monitor the environmental conditions of the archaea and bacteria in the sediments that produce methane and carbon dioxide.

Environmental Sciences & Ecology↗
DOE OSTI2026

Importance of Spatially Continuous Urban Surface Properties in Urban‐Resolving Earth System Modeling

Accurate representation of urban properties and processes at higher resolutions in global modeling systems is essential for advancing our ability to capture the complexities of urban systems and informing effective resilience strategies. However, the prescription of coarse global-scale urban properties in most state-of-the-art Earth system models (ESMs) is limiting their potential for capturing urban signals as they advance toward kilometer-scale simulation capabilities. To bridge this gap in inadequate urban property representation and to advance urban-resolving Earth system modeling, this work integrates the newly-developed global 1 km-resolution facet-level urban surface property data set, U-Surf, into the land component of Community Earth System Model (CESM)—Community Terrestrial System Model (CTSM). The land-only CTSM simulations are validated against satellite measurements, ground-based urban weather stations, flux tower observations, and reanalysis data. Results demonstrate that the enhanced urban properties allow improved simulations of urban meteorology and surface energy fluxes compared to the default coarse-resolution categorical urban canopy parameters. Spatial scaling analysis reveals regime-dependent information loss during resolution aggregation, as well as substantial scale-dependent variations in urban surface energy flux representation. Furthermore, these findings have critical implications for coupled Earth system modeling when including the effect of land-atmosphere interaction. This work establishes a foundation for future urban-resolving kilometer-scale ESM development, which will enable systematic intra- and inter-city comparisons that inform urban adaptation strategies across diverse global urban environments.

Cheng, Yifan [University of Illinois Urbana-Champa↗
DOE OSTI2020

Bismuthene for highly efficient carbon dioxide electroreduction reaction

Bismuth (Bi) has been known as a highly efficient electrocatalyst for CO 2 reduction reaction. Stable free-standing two-dimensional Bi monolayer (Bismuthene) structures have been predicted theoretically, but never realized experimentally. Here, we show the first simple large-scale synthesis of free-standing Bismuthene, to our knowledge, and demonstrate its high electrocatalytic efficiency for formate (HCOO - ) formation from CO 2 reduction reaction. The catalytic performance is evident by the high Faradaic efficiency (99% at -580 mV vs. Reversible Hydrogen Electrode (RHE)), small onset overpotential (<90 mV) and high durability (no performance decay after 75 h and annealing at 400 °C). Density functional theory calculations show the structure-sensitivity of the CO2 reduction reaction over Bismuthene and thicker nanosheets, suggesting that selective formation of HCOO - indeed can proceed easily on Bismuthene (111) facet due to the unique compressive strain. This work paves the way for the extensive experimental investigation of Bismuthene in many different fields.

Science & Technology - Other Topics↗
DOE OSTI2020

Microbial diversity drives carbon use efficiency in a model soil

Abstract Empirical evidence for the response of soil carbon cycling to the combined effects of warming, drought and diversity loss is scarce. Microbial carbon use efficiency (CUE) plays a central role in regulating the flow of carbon through soil, yet how biotic and abiotic factors interact to drive it remains unclear. Here, we combine distinct community inocula (a biotic factor) with different temperature and moisture conditions (abiotic factors) to manipulate microbial diversity and community structure within a model soil. While community composition and diversity are the strongest predictors of CUE, abiotic factors modulated the relationship between diversity and CUE, with CUE being positively correlated with bacterial diversity only under high moisture. Altogether these results indicate that the diversity × ecosystem-function relationship can be impaired under non-favorable conditions in soils, and that to understand changes in soil C cycling we need to account for the multiple facets of global changes.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Three-dimensional strain dynamics govern the hysteresis in heterogeneous catalysis

Understanding catalysts strain dynamic behaviours is crucial for the development of cost-effective, efficient, stable and long-lasting catalysts. Here, we reveal in situ three-dimensional strain evolution of single gold nanocrystals during a catalytic CO oxidation reaction under operando conditions with coherent X-ray diffractive imaging. We report direct observation of anisotropic strain dynamics at the nanoscale, where identically crystallographically-oriented facets are qualitatively differently affected by strain leading to preferential active sites formation. Interestingly, the single nanoparticle elastic energy landscape, which we map with attojoule precision, depends on heating versus cooling cycles. The hysteresis observed at the single particle level is following the normal/inverse hysteresis loops of the catalytic performances. This approach opens a powerful avenue for studying, at the single particle level, catalytic nanomaterials and deactivation processes under operando conditions that will enable profound insights into nanoscale catalytic mechanisms.

36 MATERIALS SCIENCE↗
DOE OSTI2021

On the crystallography and reversibility of lithium electrodeposits at ultrahigh capacity

Abstract Lithium metal is a promising anode for energy-dense batteries but is hindered by poor reversibility caused by continuous chemical and electrochemical degradation. Here we find that by increasing the Li plating capacity to high values ( e.g ., 10–50 mAh cm −2 ), Li deposits undergo a morphological transition to produce dense structures, composed of large grains with dominantly (110) Li crystallographic facets. The resultant Li metal electrodes manifest fast kinetics for lithium stripping/plating processes with higher exchange current density, but simultaneously exhibit elevated electrochemical stability towards the electrolyte. Detailed analysis of these findings reveal that parasitic electrochemical reactions are the major reason for poor Li reversibility, and that the degradation rate from parasitic electroreduction of electrolyte components is about an order of magnitude faster than from chemical reactions. The high-capacity Li electrodes provide a straightforward strategy for interrogating the solid electrolyte interphase (SEI) on Li —with unprecedented, high signal to noise. We find that an inorganic rich SEI is formed and is primarily concentrated around the edges of lithium particles. Our findings provide straightforward, but powerful approaches for enhancing the reversibility of Li and for fundamental studies of the interphases formed in liquid and solid-state electrolytes using readily accessible analytical tools.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

Adsorbate chemical environment-based machine learning framework for heterogeneous catalysis

Abstract Heterogeneous catalytic reactions are influenced by a subtle interplay of atomic-scale factors, ranging from the catalysts’ local morphology to the presence of high adsorbate coverages. Describing such phenomena via computational models requires generation and analysis of a large space of atomic configurations. To address this challenge, we present Adsorbate Chemical Environment-based Graph Convolution Neural Network (ACE-GCN), a screening workflow that accounts for atomistic configurations comprising diverse adsorbates, binding locations, coordination environments, and substrate morphologies. Using this workflow, we develop catalyst surface models for two illustrative systems: (i) NO adsorbed on a Pt 3 Sn(111) alloy surface, of interest for nitrate electroreduction processes, where high adsorbate coverages combined with low symmetry of the alloy substrate produce a large configurational space, and (ii) OH* adsorbed on a stepped Pt(221) facet, of relevance to the Oxygen Reduction Reaction, where configurational complexity results from the presence of irregular crystal surfaces, high adsorbate coverages, and directionally-dependent adsorbate-adsorbate interactions. In both cases, the ACE-GCN model, trained on a fraction (~10%) of the total DFT-relaxed configurations, successfully describes trends in the relative stabilities of unrelaxed atomic configurations sampled from a large configurational space. This approach is expected to accelerate development of rigorous descriptions of catalyst surfaces under in-situ conditions.

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

Epitaxial growth of highly symmetrical branched noble metal-semiconductor heterostructures with efficient plasmon-induced hot-electron transfer

Epitaxial growth is one of the most commonly used strategies to precisely tailor heterostructures with well-defined compositions, morphologies, crystal phases, and interfaces for various applications. However, as epitaxial growth requires a small interfacial lattice mismatch between the components, it remains a challenge for the epitaxial synthesis of heterostructures constructed by materials with large lattice mismatch and/or different chemical bonding, especially the noble metal-semiconductor heterostructures. Here, we develop a noble metal-seeded epitaxial growth strategy to prepare highly symmetrical noble metal-semiconductor branched heterostructures with desired spatial configurations, i.e., twenty CdS (or CdSe) nanorods epitaxially grown on twenty exposed (111) facets of Ag icosahedral nanocrystal, albeit a large lattice mismatch (more than 40%). Importantly, a high quantum yield (QY) of plasmon-induced hot-electron transferred from Ag to CdS was observed in epitaxial Ag-CdS icosapods (18.1%). This work demonstrates that epitaxial growth can be achieved in heterostructures composed of materials with large lattice mismatches. The constructed epitaxial noble metal-semiconductor interfaces could be an ideal platform for investigating the role of interfaces in various physicochemical processes.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Revealing CO 2 dissociation pathways at vicinal copper (997) interfaces

Size- and shape-tailored copper (Cu) nanocrystals can offer vicinal planes for facile carbon dioxide (CO 2 ) activation. Despite extensive reactivity benchmarks, a correlation between CO 2 conversion and morphology structure has not yet been established at vicinal Cu interfaces. Herein, ambient pressure scanning tunneling microscopy reveals step-broken Cu nanocluster evolutions on the Cu(997) surface under 1 mbar CO 2 (g). The CO 2 dissociation reaction produces carbon monoxide (CO) adsorbate and atomic oxygen (O) at Cu step-edges, inducing complicated restructuring of the Cu atoms to compensate for increased surface chemical potential energy at ambient pressure. The CO molecules bound at under-coordinated Cu atoms contribute to the reversible Cu clustering with the pressure gap effect, whereas the dissociated oxygen leads to irreversible Cu faceting geometries. Synchrotron-based ambient pressure X-ray photoelectron spectroscopy identifies the chemical binding energy changes in CO-Cu complexes, which proves the characterized real-space evidence for the step-broken Cu nanoclusters under CO(g) environments. Our in situ surface observations provide a more realistic insight into Cu nanocatalyst designs for efficient CO 2 conversion to renewable energy sources during C 1 chemical reactions.

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

Revealing the aging process of solid electrolyte interphase on SiOx anode

Abstract As one of the most promising alternatives to graphite negative electrodes, silicon oxide (SiO x ) has been hindered by its fast capacity fading. Solid electrolyte interphase (SEI) aging on silicon SiO x has been recognized as the most critical yet least understood facet. Herein, leveraging 3D focused ion beam-scanning electron microscopy (FIB-SEM) tomographic imaging, we reveal an exceptionally characteristic SEI microstructure with an incompact inner region and a dense outer region, which overturns the prevailing belief that SEIs are homogeneous structure and reveals the SEI evolution process. Through combining nanoprobe and electron energy loss spectroscopy (EELS), it is also discovered that the electronic conductivity of thick SEI relies on the percolation network within composed of conductive agents (e.g., carbon black particles), which are embedded into the SEI upon its growth. Therefore, the free growth of SEI will gradually attenuate this electron percolation network, thereby causing capacity decay of SiO x . Based on these findings, a proof-of-concept strategy is adopted to mechanically restrict the SEI growth via applying a confining layer on top of the electrode. Through shedding light on the fundamental understanding of SEI aging for SiO x anodes, this work could potentially inspire viable improving strategies in the future.

25 ENERGY STORAGE↗
DOE OSTI2024

Low-index mesoscopic surface reconstructions of Au surfaces using Bayesian force fields

Metal surfaces have long been known to reconstruct, significantly influencing their structural and catalytic properties. Many key mechanistic aspects of these subtle transformations remain poorly understood due to limitations of previous simulation approaches. Using active learning of Bayesian machine-learned force fields trained from ab initio calculations, we enable large-scale molecular dynamics simulations to describe the thermodynamics and time evolution of the low-index mesoscopic surface reconstructions of Au (e.g., the Au(111)-‘Herringbone,’ Au(110)-(1 × 2)-‘Missing-Row,’ and Au(100)-‘Quasi-Hexagonal’ reconstructions). This capability yields direct atomistic understanding of the dynamic emergence of these surface states from their initial facets, providing previously inaccessible information such as nucleation kinetics and a complete mechanistic interpretation of reconstruction under the effects of strain and local deviations from the original stoichiometry. We successfully reproduce previous experimental observations of reconstructions on pristine surfaces and provide quantitative predictions of the emergence of spinodal decomposition and localized reconstruction in response to strain at non-ideal stoichiometries. A unified mechanistic explanation is presented of the kinetic and thermodynamic factors driving surface reconstruction. Furthermore, we study surface reconstructions on Au nanoparticles, where characteristic (111) and (100) reconstructions spontaneously appear on a variety of high-symmetry particle morphologies.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Enhanced quantum state transfer by circumventing quantum chaotic behavior

The ability to realize high-fidelity quantum communication is one of the many facets required to build generic quantum computing devices. In addition to quantum processing, sensing, and storage, transferring the resulting quantum states demands a careful design that finds no parallel in classical communication. Existing experimental demonstrations of quantum information transfer in solid-state quantum systems are largely confined to small chains with few qubits, often relying upon non-generic schemes. Here, by using a superconducting quantum circuit featuring thirty-six tunable qubits, accompanied by general optimization procedures deeply rooted in overcoming quantum chaotic behavior, we demonstrate a scalable protocol for transferring few-particle quantum states in a two-dimensional quantum network. These include single-qubit excitation, two-qubit entangled states, and two excitations for which many-body effects are present. Our approach, combined with the quantum circuit’s versatility, paves the way to short-distance quantum communication for connecting distributed quantum processors or registers, even if hampered by inherent imperfections in actual quantum devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Spin-glass state in nickelate superconductors

Magneto-optical measurements in La 0.8 Sr 0.2 NiO 2 and Nd 0.825 Sr 0.175 NiO 2 reveal an intriguing new facet of infinite-layer nickelate superconductors: the onset of spin-glass behavior at a temperature far exceeding the superconducting critical temperature T c . This discovery sharply contrasts with copper oxide superconductors, where magnetism and superconductivity remain largely exclusive. Moreover, the magnitude and onset temperature of the polar Kerr effect in Nd 0.825 Sr 0.175 NiO 2 fabricated on SrTiO 3 and (LaAlO 3 ) 0.3 (Sr 2 TaAlO 6 ) 0.7 substrates differ dramatically, while T c does not.

FOS: Physical sciences↗
DOE OSTI2022

Micrometre-scale single-crystalline borophene on a square-lattice Cu(100) surface

Borophene, a crystalline monolayer boron sheet, is a new two-dimensional (2D) quantum material, predicted to feature tunable structure, intriguing physics and to find applications in flexible electronics, energy storage and catalysis. Nanoscale borophene flakes have been synthesized on noble-metal surfaces, but for device fabrication, one needs large single-crystal domains. In this work, we report the synthesis of borophene on a square lattice Cu(100) surface and show that incommensurate coordinations could reduce the borophene-substrate interactions and alter the borophene structures in interesting ways. Micrometer-scale single-crystal domains can form as isolated faceted islands or merge together to achieve full monolayer coverage. We have discovered a new crystal structure of borophene, with ten boron atoms and two hexagonal vacancies in the unit cell. First-principle calculations indicate that charge transfer rather than covalent bonding binds 2D boron to the copper surface, and confirm its integrity and uniformity The electronic band structure features multiple anisotropic tilted Dirac cones, heralding emergent quantum fermions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Rational design of high-performance low-loading oxygen reduction catalysts for alkaline fuel cells

The lack of mechanistic understanding and catalyst design principles for alkaline electrolytes, especially for the sluggish oxygen reduction reaction, has impeded the advancement of alkaline fuel cells. Here, in this study, we propose a modified volcano plot and apply this rationale to strategically design Pt nanosheets with PdH x nanosheets substrates. This catalyst exhibited high stability with a specific activity of 1.71 mA cm −2 at 0.95 V versus the reversible hydrogen electrode, surpassing the benchmark of Pt/C by 49-fold. Spectroscopic, electrochemical and electron microscopic characterizations revealed that such performance enhancement originated from tensile-strained Pt{111} facets, improving oxidative stability and suppressing carbon corrosion. In fuel cell testing, the catalyst enabled a peak power density of 1.67 W cm −2 with a loading of 10 µg PGM Cathode cm −2 . Further optimization delivered a peak power density of 21.7 W mg −1 PGM Cathode+Anode with a total specific catalyst cost US$\$$1.27 kW −1 , surpassing the US Department of Energy’s Pt group metal loading and cost targets. This study provides valuable insights into catalyst design for the alkaline oxygen reduction reaction.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Directional ballistic transport in the two-dimensional metal PdCoO2

Abstract In an idealized infinite crystal, the material properties are constrained by the symmetries of the unit cell. The point-group symmetry is broken by the sample shape of any finite crystal, but this is commonly unobservable in macroscopic metals. To sense the shape-induced symmetry lowering in such metals, long-lived bulk states originating from an anisotropic Fermi surface are needed. Here we show how a strongly facetted Fermi surface and the long quasiparticle mean free path present in microstructures of PdCoO 2 yield an in-plane resistivity anisotropy that is forbidden by symmetry on an infinite hexagonal lattice. We fabricate bar-shaped transport devices narrower than the mean free path from single crystals using focused ion beam milling, such that the ballistic charge carriers at low temperatures frequently collide with both of the side walls that define the channel. Two symmetry-forbidden transport signatures appear: the in-plane resistivity anisotropy exceeds a factor of 2, and a transverse voltage appears in zero magnetic field. Using ballistic Monte Carlo simulations and a numerical solution of the Boltzmann equation, we identify the orientation of the narrow channel as the source of symmetry breaking.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Correlative operando microscopy of oxygen evolution electrocatalysts

Transition metal (oxy)hydroxides are promising electrocatalysts for the oxygen evolution reaction.1–3 The properties of these materials evolve dynamically and heterogeneously4 with applied voltage through ion insertion redox reactions, converting inactive materials at open-circuit into active electrocatalysts during operation.5 Thus, the catalytic state is inherently far-from-equilibrium, complicating its direct observation. Here, we establish the link between the oxygen evolution activity and the local operational chemical, physical, and electronic nanoscale structure of single-crystalline β-Co(OH)2 platelet particles through a suite of newly developed correlative operando scanning probe and X-ray microscopy techniques. At pre-catalytic voltages, the particles swell to form an α-CoO2H1.5·0.5H2O-like structure with associated Co2.5+ oxidation state produced through hydroxide intercalation. With increasing voltage to drive oxygen evolution, interlayer water and protons de-intercalate to form contracted β-CoOOH particles with Co3+ species. While these transformations manifest heterogeneously through the bulk of the particles, the electrochemical current is primarily restricted to the particle edge facets. The observed Tafel behavior is correlated to the local concentration of Co3+ at these reactive edge sites, demonstrating the link between bulk ion-insertion and surface catalytic activity.

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

Shape memory in self-adapting colloidal crystals

We report reconfigurable, mechanically responsive crystalline materials are central components in many sensing, soft robotic, and energy conversion and storage devices1,2,3,4. Crystalline materials can readily deform under various stimuli and the extent of recoverable deformation is highly dependent upon bond type1,2,5,6,7,8,9,10. Indeed, for structures held together via simple electrostatic interactions, minimal deformations are tolerated. By contrast, structures held together by molecular bonds can, in principle, sustain much larger deformations and more easily recover their original configurations. In this report we study the deformation properties of well-faceted colloidal crystals engineered with DNA. These crystals are large in size (greater than 100 µm) and have a body-centred cubic (bcc) structure with a high viscoelastic volume fraction (of more than 97%). Therefore, they can be compressed into irregular shapes with wrinkles and creases, and, notably, these deformed crystals, upon rehydration, assume their initial well-formed crystalline morphology and internal nanoscale order within seconds. For most crystals, such compression and deformation would lead to permanent, irreversible damage. The substantial structural changes to the colloidal crystals are accompanied by notable and reversible optical property changes. For example, whereas the original and structurally recovered crystals exhibit near-perfect (over 98%) broadband absorption in the ultraviolet–visible region, the deformed crystals exhibit significantly increased reflection (up to 50% of incident light at certain wavelengths), mainly because of increases in their refractive index and inhomogeneity.

36 MATERIALS SCIENCE↗