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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 1,261 records · Page 70
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Electrochemical CO Reduction: A Property of the Electrochemical Interface

Electrochemical CO reduction holds the promise to be a cornerstone for sustainable production of fuels and chemicals. However, the underlying understanding of the carbon–carbon coupling toward multiple-carbon products is not complete. Here we present thermodynamically realistic structures of the electrochemical interfaces, determined by explicit ab initio simulations. We investigate how key CO reduction reaction intermediates are stabilized in different electrolytes and at different pH values. We find that the catalytic trends previously observed experimentally can be explained by the interplay between the metal surface and the electrolyte. For the Cu(100) facet with a phosphate buffer electrolyte, the energy efficiency is found to be limited by blocking of a phosphate anion, while in alkali hydroxide solutions (MOH, M = Na, K, Cs), OH* intermediates may be present, and at high overpotential the H* coverage limits the reaction. Furthermore the results provide insight into the electrochemical interface structure, revealing the limitations for multiple-carbon products, and offer a direct comparison to experiments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Nanorg Microbial Factories: Light-Driven Renewable Biochemical Synthesis Using Quantum Dot-Bacteria Nanobiohybrids

Living cells do not interface naturally with nanoscale materials, although such artificial organisms can have unprecedented multifunctional properties, like wireless activation of enzyme function using electromagnetic stimuli. Realizing such interfacing in a nanobiohybrid organism (or nanorg) requires (1) chemical coupling via affinity binding and self-assembly, (2) the energetic coupling between optoelectronic states of artificial materials with the cellular process, and (3) the design of appropriate interfaces ensuring biocompatibility. Here we show that seven different core-shell quantum dots (QDs), with excitations ranging from ultraviolet to near-infrared energies, couple with targeted enzyme sites in bacteria. When illuminated by light, these QDs drive the renewable production of different biofuels and chemicals using carbon-dioxide (CO2), water, and nitrogen (from air) as substrates. These QDs use their zinc-rich shell facets for affinity attachment to the proteins. Cysteine zwitterion ligands enable uptake through the cell, facilitating cell survival. Together, these nanorgs catalyze light-induced air-water-CO2 reduction with a high turnover number (TON) of ~106-108 (mols of product per mol of cells) to biofuels like isopropanol (IPA), 2,3-butanediol (BDO), C11-C15 methyl ketones (MKs), and hydrogen (H2); and chemicals such as formic acid (FA), ammonia (NH3), ethylene (C2H4), and degradable bioplastics polyhydroxybutyrate (PHB). Therefore, these resting cells function as nanomicrobial factories powered by light.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Revealing the Effects of the Non-solvent on the Ligand Shell of Nanoparticles and Their Crystallization

When nanoparticles (NPs) are assembled from solution, a common assembly method of choice is either solution destabilization or solvent evaporation technique. The destabilization of the NP solution by non-solvents results in the formation of faceted supercrystals (SCs) while periodic film-like assemblies are typically formed by solvent evaporation. In this article, we reveal the effect of non-solvents in washing, dispersing, and crystallizing NPs. Small angle neutron scattering (SANS) is employed for monitoring the ligand shell of NPs in solutions upon introduction of various non-solvents. The SC crystallization process is traced in situ with small-angle X-ray scattering (SAXS), and the structures of the resulting single-crystalline SCs are examined in detail by mapping the reciprocal space using SAXS and wide-angle X-ray scattering. Our study suggests that the relative miscibility of the non-solvent with solvents and ligands 4111 determines the solvation and thickness of the ligand shell and thereby the resulting structure of SCs. In the early stage of crystallization, truncated octahedral PbS NPs form SCs with face-centered cubic (fcc) symmetry. In the later stage, the fcc symmetry is preserved in the SC formed by larger (5.60 nm) NPs, but the SC assembled from smaller (4.14 nm) NPs undergoes a phase transition into body-centered cubic (bcc) lattice via Bain transformation, becoming a polycrystalline SC containing three structurally correlated bcc domains and one untransformed fcc domain. Our study provides the detailed understanding of the non-solvent effect that impacts beyond the formation of SCs, enabling the judicious selection of solvent/non-solvent mixtures for NP purification.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Origin of High Activity and Durability of Twisty Nanowire Alloy Catalysts under Oxygen Reduction and Fuel Cell Operating Conditions

The ability to control the surface composition and morphology of alloy catalysts is critical for achieving high activity and durability of catalysts for oxygen reduction reaction (ORR) and fuel cells. Here, this report describes an efficient surfactant-free synthesis route for producing a twisty nanowire (TNW) shaped platinum–iron (PtFe) alloy catalyst (denoted as PtFe TNWs) with controllable bimetallic compositions. PtFe TNWs with an optimal initial composition of ~24% Pt are shown to exhibit the highest mass activity (3.4 A/mg Pt , ~20 times higher than that of commercial Pt catalyst) and the highest durability (<2% loss of activity after 40000 cycles and <30% loss after 120000 cycles) among all PtFe-based nanocatalysts under ORR or fuel cell operating conditions reported so far. Using ex situ and in situ synchrotron X-ray diffraction coupled with atomic pair distribution function (PDF) analysis and 3D modeling, the PtFe TNWs are shown to exhibit mixed face-centered cubic (fcc)-body-centered cubic (bcc) alloy structure and a significant lattice strain. A striking finding is that the activity strongly depends on the composition of the as-synthesized catalysts and this dependence remains unchanged despite the evolution of the composition of the different catalysts and their lattice constants under ORR or fuel cell operating conditions. Notably, dealloying under fuel cell operating condition starts at phase-segregated domain sites leading to a final fcc alloy structure with subtle differences in surface morphology. Due to a subsequent realloying and the morphology of TNWs, the surface lattice strain observed with the as-synthesized catalysts is largely preserved. This strain and the particular facets exhibited by the TNWs are believed to be responsible for the observed activity and durability enhancements. These findings provide new insights into the correlation between the structure, activity, and durability of nanoalloy catalysts and are expected to energize the ongoing effort to develop highly active and durable low-Pt-content nanowire catalysts by controlling their alloy structure and morphology.

25 ENERGY STORAGE↗
DOE OSTI2022

Liquid-Phase Effects on Adsorption Processes in Heterogeneous Catalysis

Aqueous solvation free energies of adsorption have recently been measured for phenol adsorption on Pt(111). Endergonic solvent effects of ~1 eV suggest solvents dramatically influence a metal catalyst’s activity with significant implications for the catalyst design. However, measurements are indirect and involve adsorption isotherm models, which potentially reduces the reliability of the extracted energy values. Computational, implicit solvation models predict exergonic solvation effects for phenol adsorption, failing to agree with measurements even qualitatively. In this study, an explicit, hybrid quantum mechanical/molecular mechanical approach for computing solvation free energies of adsorption is developed, solvation free energies of phenol adsorption are computed, and experimental data for solvation free energies of phenol adsorption are reanalyzed using multiple adsorption isotherm models. Explicit solvation calculations predict an endergonic solvation free energy for phenol adsorption that agrees well with measurements to within the experimental and force field uncertainties. Computed adsorption free energies of solvation of carbon monoxide, ethylene glycol, benzene, and phenol over the (111) facet of Pt and Cu suggest that liquid water destabilizes all adsorbed species, with the largest impact on the largest adsorbates.

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

Adsorbate-Induced Adatom Formation on Lithium, Iron, Cobalt, Ruthenium, and Rhenium Surfaces

Recent experimental and theoretical studies have demonstrated the reaction-driven metal–metal bond breaking in metal catalytic surfaces even under relatively mild conditions. Here, we construct a density functional theory (DFT) database for the adsorbate-induced adatom formation energy on the close-packed facets of three hexagonal close-packed metals (Co, Ru, and Re) and two body-centered cubic metals (Li and Fe), where the source of the ejected metal atom is either a step edge or a close-packed surface. For Co and Ru, we also considered their metastable face-centered cubic structures. We studied 18 different adsorbates relevant to catalytic processes and predicted noticeably easier adatom formation on Li and Fe compared to the other three metals. The NH 3 - and CO-induced adatom formation on Fe(110) is possible at room temperature, a result relevant to NH 3 synthesis and Fischer-Tropsch synthesis, respectively. There also exist other systems with favorable adsorbate effects for adatom formation relevant to catalytic processes at elevated temperatures (500–700 K). Our results offer insight into the reaction-driven formation of metal clusters, which could play the role of active sites in reactions catalyzed by Li, Fe, Co, Ru, and Re catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

First-Principles Mechanistic Analysis of Dimethyl Ether Electro-Oxidation on Monometallic Single-Crystal Surfaces

Dimethyl ether is an attractive alternative to petroleum fuels due to its physical properties, comparable energy density to methanol and ethanol, and minimal deleterious environmental/toxicological effects. For direct fuel cells, it has a number of advantages over other prominent fuels, including easier storage with respect to hydrogen, lower toxicity and crossover when compared to methanol, and more facile complete oxidation as compared to ethanol (which includes a relatively difficult to break C–C bond). However, the dimethyl ether electro-oxidation reaction is poorly understood, hindering the development of improved electrocatalysts. Using periodic, self-consistent (PW91-GGA) density functional theory calculations, we evaluate the thermochemistry of dimethyl ether (DME) electro-oxidation, at the elementary step level, on 12 model, closed-packed facets of pure transition metals: Au, Ag, Cu, Pt, Pd, Ni, Ir, Rh, Co, Os, Ru, and Re. From the calculated thermochemistry, we determine the most probable reaction paths on each of these surfaces, focusing on Pt as a model system. Our results predict two key electro-oxidation peaks. At lower potentials, there is a peak corresponding to partial oxidation of DME to CO (and other surface poisoning species) or complete oxidation to CO 2 via formic acid as a key intermediate. A second, higher-potential peak is due to complete oxidation of adsorbed CO (and other surface poisoning species) to CO 2 . Assuming the catalysts remain in their metallic state during the DME electro-oxidation process, our results suggest that the onset potential of the surfaces increases in the order Cu < Ni < Os < Rh < Ir < Co < Ru < Pt < Ag < Pd < Re < Au. Using our results, we construct a theoretical phase diagram showing predicted catalyst activity based on two key reactivity descriptors, the free energies of adsorbed CO and OH. Here, we compare all results to methanol electro-oxidation to understand key mechanistic differences and their impacts on optimal catalyst design for direct DME fuel cells.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

An Atomic-Scale View of the Nucleation and Growth of Graphene Islands on Pt Surfaces

In this work, we study the nucleation and growth of epitaxial graphene on Pt(111) surfaces at the atomic level using scanning tunneling microscopy (STM). Graphene nucleation occurs both near Pt step edges and on Pt terraces, producing hexagonally shaped islands with atomically sharp zigzag edges. Graphene interacts strongly with Pt substrate during growth, by etching and replacement of Pt atoms from step edges, which results in faceting of the Pt steps. The favorable lattice orientations of graphene islands are found to be parallel to those of the Pt substrate, but other orientations are still possible. Grain boundaries are formed when two graphene islands merge with different lattice orientations. Improved growth conditions such as smaller nucleation density and higher growth rate can produce high quality graphene film with larger grain sizes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Evolution Of Lattice Structure And Chemical Composition Of The Surface Reconstruction Layer In Li1.2Ni0.2Mn0.6O2 Cathode Material For Lithium Ion Batteries

Voltage and capacity fading of layer structured lithium and manganese rich (LMR) transition metal oxide is directly related to the structural and composition evolution of the material during the cycling of the battery. However, understanding such evolution at atomic level remains elusive. Based on atomic level structural imaging, elemental mapping of the pristine and cycled samples and density functional theory calculations, it is found that accompanying the hoping of Li ions is the simultaneous migration of Ni ions towards the surface from the bulk lattice, leading to the gradual depletion of Ni in the bulk lattice and thickening of a Ni enriched surface reconstruction layer (SRL). Furthermore, Ni and Mn also exhibit concentration partitions within the thin layer of SRL in the cycled samples where Ni is almost depleted at the very surface of the SRL, indicating the preferential dissolution of Ni ions in the electrolyte. Accompanying the elemental composition evolution, significant structural evolution is also observed and identified as a sequential phase transition of C2/m →I41→Spinel. For the first time, it is found that the surface facet terminated with pure cation is more stable than that with a mixture of cation and anion. These findings firmly established how the elemental species in the lattice of LMR cathode transfer from the bulk lattice to surface layer and further into the electrolyte, clarifying the long standing confusion and debate on the structure and chemistry of the surface layer and their correlation with the voltage fading and capacity decaying of LMR cathode. Therefore, this work provides critical insights for designing of cathode materials with both high capacity and voltage stability during cycling.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2015

Atomic Layer-by-Layer Deposition of Platinum on Palladium Octahedra for Enhanced Catalysts toward the Oxygen Reduction Reaction

We systematically evaluated two different approaches to the syntheses of Pd@PtnL (n = 2–5) core–shell octahedra. We initially prepared the core–shell octahedra using a polyol-based route by titrating a Pt(IV) precursor into the growth solution containing Pd octahedral seeds at 200 °C through the use of a syringe pump. The number of Pt atomic layers could be precisely controlled from two to five by increasing the volume of the precursor solution while fixing the amount of seeds. We then demonstrated the synthesis of Pd@Pt nL octahedra using a water-based route at 95 °C through the one-shot injection of a Pt(II) precursor. Due to the large difference in reaction temperature, the Pd@Pt nL octahedra obtained via the water-based route showed sharper corners than their counterparts obtained through the polyol-based route. When compared to a commercial Pt/C catalyst based upon 3.2 nm Pt particles, the Pd@Pt nL octahedra prepared using both methods showed similar remarkable enhancement in terms of activity (both specific and mass) and durability toward the oxygen reduction reaction. These calculations based upon periodic, self-consistent density functional theory suggested that the enhancement in specific activity for the Pd@Pt nL octahedra could be attributed to the destabilization of OH on their Pt nL */Pd(111) surface relative to the {111} and {100} facets exposed on the surface of Pt/C. Finally. the destabilization of OH facilitates its hydrogenation, which was found to be the rate-limiting step of the oxygen reduction reaction on all these surfaces.

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

Finite Element Modeling of Diffusion in Fractured Porous Media by Using Hierarchical Material Properties

Abstract Fractured porous media challenge modeling approaches due to high computational costs and excessive mesh refinement imposed by the extreme scale variability of fractures and the heterogeneity of the surrounding porous rock. To overcome such difficulties, we utilize the hierarchical finite element method ( Hi ‐FEM) that has been developed previously to simulate the electrical potential distribution in complex geologic environments. The method employs the hierarchical basis functions in classical finite element analysis to enable representation of material properties on each dimensional component of a given 3D unstructured finite element, thereby inherently allowing for interactions at the boundary between fracture and a host rock. In this study, we extend its application to transient fluid flow and heat conduction in the Laplace domain. Time‐domain flow solutions are obtained by numerical inverse Laplace transform. We evaluate the accuracy of the method using different flow models and demonstrate its robustness for large‐scale, rock mass models featuring complex fracture networks. Moreover, for the computation of nodal Darcian velocity fields in fractured porous media where the fractures are represented as 2D features, a new approach that employs the Yeh's Galerkin model for both volume and facet elements is proposed. Results show that Hi ‐FEM can produce accurate flow solutions for fractured porous media without any need of coupling or transfer mechanism while still being computationally economical and numerically robust, even for large‐scale simulations.

Beskardes, G. D.↗
DOE OSTI2022

Modeling the Economic and Environmental Impacts of Land Scarcity Under Deep Uncertainty

Abstract Land scarcity is increasing over time, driven by complex multisector dynamics. The impacts of land scarcity on the economy and environment are multi‐faceted and regional, so any action to convert land will contain inherent tradeoffs. These impacts are complicated by the deeply uncertain evolution of the various sectors influencing land scarcity. A need therefore exists to provide multi‐metric and multi‐sector assessments that are robust to myriad uncertainties. Land conservation effectively limits the supply of productive land, while biofuel consumption increases the demand and competition for that land, and how these dynamics individually and jointly propagate to economic and environmental impacts is an important open question. To address this, we adopt the Global Change Analysis Model (GCAM) that has representations of various important systems including the climate, macroeconomic, energy, agriculture and land, and water resources systems. Various scenarios of increased land demand (from biofuels) and decreased land supply (from conservation) under various socioeconomic scenarios drawn from the SSPs were simulated using GCAM. We find that while biofuel consumption and land conservation reduce carbon emissions, this comes at the cost of higher food prices, reduced crop production, and increased water withdrawals. Additionally, some regions experience these tradeoffs more severely than others and are more heavily impacted from the same biofuel mandate or by an additional percent of protected land. These and other findings highlight the importance of multisector modeling frameworks that capture many cross‐sector linkages, and acknowledge the important uncertainties confronting the human‐Earth system when making any analysis of land scarcity impacts.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Evaluating the Water Cycle Over CONUS at the Watershed Scale for the Energy Exascale Earth System Model Version 1 (E3SMv1) Across Resolutions

Abstract The water cycle is an important component of the earth system and it plays a key role in many facets of society, including energy production, agriculture, and human health and safety. In this study, the Energy Exascale Earth System Model version 1 (E3SMv1) is run with low‐resolution (roughly 110 km) and high‐resolution (roughly 25 km) configurations—as established by the High Resolution Model Intercomparison Project protocol—to evaluate the atmospheric and terrestrial water budgets over the conterminous United States (CONUS) at the large watershed scale. The warm season water cycle slows down in the HR experiment relative to the LR, with decreasing fluxes of precipitation, evapotranspiration, atmospheric moisture convergence, and runoff. The reductions in these terms exacerbate biases for some watersheds, while reducing them in others. For example, precipitation biases are exacerbated at HR over the Eastern and Central CONUS watersheds, while precipitation biases are reduced at HR over the Western CONUS watersheds. The most pronounced changes with resolution to the water cycle come from reductions in precipitation and evapotranspiration. The reduction in evapotranspiration reduces the biases across nearly all of the CONUS. Additional exploratory metrics show improvements to water cycle extremes (both in precipitation and streamflow), fractional contributions of different storm types to total precipitation, and mountain snowpack.

54 ENVIRONMENTAL SCIENCES↗
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 OSTI2017

Phase transformation mechanism in lithium manganese nickel oxide revealed by single-crystal hard X-ray microscopy

Understanding the reaction pathway and kinetics of solid-state phase transformation is critical in designing advanced electrode materials with better performance and stability. Despite the first-order phase transition with a large lattice mismatch between the involved phases, spinel LiMn 1.5 Ni 0.5 O 4 is capable of fast rate even at large particle size, presenting an enigma yet to be understood. The present study uses advanced two-dimensional and three-dimensional nano-tomography on a series of well-formed LixMn 1.5 Ni 0.5 O 4 (0 ≤ x ≤ 1) crystals to visualize the mesoscale phase distribution, as a function of Li content at the sub-particle level. Inhomogeneity along with the coexistence of Li-rich and Li-poor phases are broadly observed on partially delithiated crystals, providing direct evidence for a concurrent nucleation and growth process instead of a shrinking-core or a particle-by-particle process. As a result, superior kinetics of (100) facets at the vertices of truncated octahedral particles promote preferential delithiation, whereas the observation of strain-induced cracking suggests mechanical degradation in the material.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Superlattices assembled through shape-induced directional binding

Organization of spherical particles into lattices is typically driven by packing considerations. Although the addition of directional binding can significantly broaden structural diversity, nanoscale implementation remains challenging. Here we investigate the assembly of clusters and lattices in which anisotropic polyhedral blocks coordinate isotropic spherical nanoparticles via shape-induced directional interactions facilitated by DNA recognition. We show that these polyhedral blocks—cubes and octahedrons—when mixed with spheres, promote the assembly of clusters with architecture determined by polyhedron symmetry. Moreover, three-dimensional binary superlattices are formed when DNA shells accommodate the shape disparity between nanoparticle interfaces. The crystallographic symmetry of assembled lattices is determined by the spatial symmetry of the block’s facets, while structural order depends on DNA-tuned interactions and particle size ratio. Lastly, the presented lattice assembly strategy, exploiting shape for defining the global structure and DNA-mediation locally, opens novel possibilities for by-design fabrication of binary lattices.

59 BASIC BIOLOGICAL SCIENCES↗