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At least 163 records · Page 9

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DOE OSTI2026

Tandem bulk oxygen diffusion and surface reactions in reducible metal oxides control redox cycle dynamics

The interplay between bulk oxygen diffusion and surface reactions in reducible metal oxides is key in heterogeneous catalysts, but direct measurements of oxygen mobility, transient kinetics, and in situ spectroscopies have been lacking. Here, we reveal complex dynamic behavior of ceria-zirconia by H 2 using transient kinetics via mass spectrometry and in situ Raman and near-ambient pressure x-ray photoelectron spectroscopies. Molecular dynamics simulations with a machine learning potential delineate competitive oxygen diffusion mechanisms, with an optimal mobility at intermediate reductions. We expose a compensation between vacancy availability and lattice distortion at intermediate to high reductions and Frenkel defects at low reductions, underscoring a potential deficiency of 16 O/ 18 O exchange experiments in deducing oxygen mobility. Vacancies in proximity require electron localization on Ce atoms further away. The continuous replenishment of surface oxygen results in a varying reduction rate, with H 2 dissociation being the rate-limiting step. Multiscale transient simulations, consistent with experiments, indicate catalysts of potentially spatially varying oxidation states. The approach is broadly applicable to reducible oxide materials.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Mechanistic Insights into the Interplay between Ion Intercalation and Water Electrolysis in Aqueous Batteries

Improving electrolyte stability to suppress water electrolysis represents a basic principle for designing aqueous batteries. Herein, we investigate counterintuitive roles that water electrolysis plays in regulating intercalation chemistry. Using the Na x Fe[Fe(CN) 6 ]∥NaTi 2 (PO 4 ) 3 (x < 1) aqueous battery as a platform, we report that high-voltage overcharging can serve as an electrochemical activation approach to achieving concurrent Na-ion intercalation and an electrolytic oxygen evolution reaction. When the cell capacity is intrinsically limited by deficient cyclable Na ions, the electrolytic water oxidation on the cathode allows for extra Na-ion intercalation from the electrolyte to the NaTi 2 (PO 4 ) 3 anode, leading to a major increase in cyclable Na ions and specific capacity. Furthermore, the parasitic oxygen generation and potential transition-metal dissolution, as proved by our synchrotron and imaging tools, can be significantly mitigated with a simple reassembling approach, which enables stable electrochemical performance and sheds light on manipulating ion intercalation and water electrolysis for battery fast charging and recycling.

25 ENERGY STORAGE↗

DOE OSTI2021

Robust passivation of CdSeTe based solar cells using reactively sputtered magnesium zinc oxide

Magnesium zinc oxide (MZO, Mg x Zn 1-x O) is a leading emitter for CdTe-based solar cells due to its transparency and the ability to tune its conduction band offset with the absorber. Devices employing alloyed cadmium selenide telluride (CST, CdSe y Te 1-y ) absorbers achieved high efficiency (>19%) using MZO deposited by reactive sputtering over a broad composition range (3.68–3.92 eV, x: 0.20–0.35). Minimal differences in implied and measured open circuit voltage indicate that the contacts are well passivated and highly selective across the spectrum of MZO employed. Device performance insensitivity to MZO composition, which is not observed in CdTe devices, is attributed to the formation of an oxygenated interface layer. Se volatility creates a group VI deficiency at the interface that drives O migration from the MZO into the absorber. This introduces conductivity in the emitter not present in its as-deposited state, contributing to the exceptional performance observed. It is shown that the quality of device passivation depends on the oxidation state of the as-deposited MZO such that intelligent control and management of the reactive sputtering process is required.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Photoprotection during iron deficiency is mediated by the bHLH transcription factors PYE and ILR3

Iron deficiency has many adverse effects on photosynthesis, which is not surprising given that 90% of foliar iron is found in the chloroplast. Although many iron-sparing mechanisms have been documented, a mechanistic understanding of how chloroplasts adapt to iron deficiency was lacking. Here, we show that the bHLH transcription factors ILR3 and PYE are required for photoprotection during iron deficiency. Changes in chloroplast morphology under the control of these transcription factors prevents the production of harmful reactive oxygen species and allows for repair of photosystem II. Understanding how plants adapt the photosynthetic machinery during iron deficiency may allow us to optimize plant growth in soils where iron is not bioavailable.

59 BASIC BIOLOGICAL SCIENCES↗

NASA NTRS1978

Detached auroral arcs in the trough region

In a previous paper, Moshupi et al. (1977) have reported on the occurrence of rare auroral 'patches' equatorward of the normally well-defined boundary of diffuse aurora. Some less spectacular but more common arclike features were observed in the same 'trough' region (between the plasmapause and the auroral oval) during the period 1972-1975. These 'detached' arcs show some similarities to stable auroral red arcs in terms of their location and occurrence, but are completely different spectroscopically in that the stable auroral red arcs produce almost pure atomic oxygen red line emissions, whereas the detached arcs are deficient in red line emission - a feature implying totally different production mechanisms. The characteristics of the detached lines are described, including their unusual local time/longitude dependence.

Anger, C. D.↗

DOE OSTI2024

Co-hydrotreatment of Bio-oil and Waste Cooking Oil to Produce Transportation Fuels

This paper reports the co-hydrotreatment of the heavy bio-oil fraction with waste cooking oil (WCO) using NiMo/γ-Al 2 O 3 catalyst, followed by the distillation of resulting deoxygenated oil and the characterization of resulting fuel cuts. The heavy BTG bio-oil fraction was obtained by removing the very reactive light-oxygenated compounds via rotary evaporation, subsequently mixed with 1-butanol. The resulting oil was blended with WCO and subjected to a two-step co-hydrotreatment process. The first step, called “stabilization,” is aimed at saturating highly reactive hydrogen-deficient compounds. The second step, called “deoxygenation,” aimed to remove bio-oil oxygen, primarily as H 2 O. This study examined the impact of varying bio-oil concentrations (0, 10, 20, 30, 40 wt.% of WCO) on the upgraded oil's yield, composition, and fuel properties. The resulting hydrotreated oil was distilled into gasoline-range, kerosene-range, and diesel-range hydrocarbons at <150 °C, 150 to 250 °C, and 250 to 350 °C, respectively. The yield of the hydrotreated oil indicates that as the bio-oil concentration increases, the amounts of coke (0.7 to 2.4 %) and water (2 to 10 wt. %) increase while the organic layer yields decrease (80 to 63 %). The coke yield was comparable to the coke yield obtained when co-processing the pyrolytic lignin fraction. This suggests that coke is formed from both the sugar oligomers and the lignin-derived oligomers. The UV-fluorescence analysis on the hydrotreated oil shows that more polycondensed and conjugated ring compounds formed as the bio-oil concentration is increased. These compounds are precursors of coke. FTIR results showed that most raw materials were converted to biofuels after the hydrotreatment. To achieve less than 1 wt. % of coke yield, blends with up to 20 wt. % pyrolysis oil should be used. An increase in bio-oil concentration leads to a slight increase in gasoline yield and a decrease in kerosene and diesel yields. The identified carbon species found in the fuel cuts include n-paraffin, iso-paraffin, cycloparaffin, and aromatics. Further, the jet fuel cut (kerosene) was characterized by density, surface tension, and viscosity. Our product conforms to the standard specifications for sustainable aviation fuels (Jet A-1). Further research is suggested to fine-tune the operating parameters for achieving reduced coke yield and enhanced kerosene yield.

09 BIOMASS FUELS↗

NASA NTRS1995

SPE (trademark) Oxygen Generator Assembly (OGA). (Refurbishment of the technology demonstrator LFSPE oxygen generation subsystem)

The SPE Oxygen Generator Assembly (OGA) has been modified to correct operational deficiencies present in the original system, and to effect changes to the system hardware and software such that its operating conditions are consistent with the latest configuration requirements for the International Space Station Alpha (ISSA). The effectiveness of these changes has recently been verified through a comprehensive test program which saw the SPE OGA operate for over 740 hours at various test conditions, including over 690 hours, or approximately 460 cycles, simulating the orbit of the space station. This report documents the changes made to the SPE OGA, presents and discusses the test results from the acceptance test program, and provides recommendations for additional development activities pertinent to evolution of the SPE OGA to a flight configuration. Copies of the test data from the acceptance test program are provided with this report on 3.5 inch diskettes in self-extracting archive files.

Roy, Robert J.↗

DOE OSTI2021

Precipitation of dopants on acceptor-doped LaMnO3±δ revealed by defect chemistry from first principles

Perovskite oxides degrade at elevated temperatures while precipitating dopant-rich particles on the surface. A knowledge-based improvement of surface stability requires a fundamental and quantitative understanding of the dopant precipitation mechanism on these materials. We propose that dopant precipitation is a consequence of the variation of dopant solubility between calcination and operating conditions in solid oxide fuel cells (SOFCs) and electrolyzer cells (SOECs). To study dopant precipitation, we use 20% (D = Ca, Sr, Ba)-doped LaMnO3+δ (LDM20) as a model system. We employ a defect model taking input from density functional theory calculations. The defect model considers the equilibration of LDM20 with a reservoir consisting of dopant oxide (DO), peroxide (DO2), and O2 in the gas phase. The equilibrated non-stoichiometry of the A-site and B-site as a function of temperature, T, and oxygen partial pressure, p(O2), reveals three regimes for LDM20: A-site deficient (oxidizing conditions), A-site rich (atmospheric conditions), and near-stoichiometric (reducing conditions). Assuming an initial A/B non-stoichiometry, we compute the dopant precipitation boundaries in a p–T phase diagram. Our model predicts precipitation both under reducing (DO) and under highly oxidizing conditions (DO2). We found precipitation under anodic, SOEC conditions to be promoted by large dopant size, while under cathodic, SOFC conditions precipitation is promoted by initial A-site excess. The main driving forces for precipitation are oxygen uptake by the condensed phase under oxidizing conditions and oxygen release assisted by B-site vacancies under reducing conditions. Possible strategies for mitigating dopant precipitation under in electrolytic and fuel cell conditions are discussed.

Hess, Franziska (ORCID:000000024460643X)↗

NASA NTRS2016

The Far-Ultraviolet Spectra of Two Hot PG1159 Stars

PG 1159 stars are hot, hydrogen-deficient (pre-) white dwarfs with atmospheres mainly composed of helium, carbon, and oxygen. The unusual surface chemistry is the result of a late helium-shell flash. Observed element abundances enable us to test stellar evolution models quantitatively with respect to their nucleosynthesis products formed near the helium-burning shell of the progenitor asymptotic giant branch stars. Because of the high effective temperatures (T(sub eff)), abundance determinations require ultraviolet spectroscopy and non-local thermodynamic equilibrium model atmosphere analyses. Up to now, we have presented results for the prototype of this spectral class and two cooler members (T(sub eff) in the range 85,000-140,000 K). Here we report on the results for two even hotter stars (PG 1520+525 and PG 1144+005, both with T(sub eff) = 150,000 K) which are the only two objects in this temperature-gravity region for which useful far-ultraviolet spectra are available, and revisit the prototype star. Previous results on the abundances of some species are confirmed, while results on others (Si, P, S) are revised. In particular, a solar abundance of sulphur is measured in contrast to earlier claims of a strong S deficiency that contradicted stellar evolution models. For the first time, we assess the abundances of Na, Al, andCl with newly constructed non-LTE model atoms. Besides the main constituents (He, C, O), we determine the abundances (or upper limits) of N, F, Ne, Na, Al, Si, P, S, Cl, Ar, and Fe. Generally, good agreement with stellar models is found.

Werner, K.↗

DOE OSTI2023

Long‐Range Confinement‐Driven Enrichment of Surface Oxygen‐Relevant Species Promotes C−C Electrocoupling in CO 2 Reduction

Abstract CO 2 reduction is a highly attractive route to transform CO 2 into useful feedstocks, of which C 2 products are more desired than C 1 , yet face high kinetic barriers of C−C electrocoupling. Here, the engineering of pore‐enabled local confinement reaction environments is reported for tuning the enrichment of surface‐adsorbed oxygen‐relevant species and the establishment of their pronounced benefits in promoting C−C coupling over oxide‐derived Cu‐based catalysts. A new approach of utilizing the microphase separation of a block copolymer is developed to fabricate bicontinuous mesoporous CuO nanofibers (CuO‐BPNF). The enhanced confinement from long‐range mesochannels enables the adsorption of OH ad /O ad on the Cu surface at a wide negative potential range of −0.7 – −1.3 V in CO 2 reduction, which cannot be achieved over conventional deficient and short‐range pores. Constant‐potential DFT calculations reveal that the surface‐bound oxygen species weakens *CO affinity with the Cu (111) surface and lowers the kinetic barriers for both *CO−CO dimerization and *CO hydrogenation to enable *CO−CHO coupling. Accordingly, a CO 2 ‐to‐C 2 Faradaic efficiency of 74.7% over CuO‐BPNF is shown, significantly larger than counterparts with conventional pores. This work offers a general design principle of confinement engineering to manage the adsorption of reactive species for steering reaction pathways in interfacial catalysis.

Chemistry↗

DOE OSTI2022

Quantifying the effect of CO 2 gasification on pulverized coal char oxy-fuel combustion

Previous research has provided strong evidence that CO 2 and H 2 O gasification reactions can provide non-negligible contributions to the consumption rates of pulverized coal (pc) char during combustion, particularly in oxy-fuel environments. Fully quantifying the contribution of these gasification reactions has proven to be difficult, due to the dearth of knowledge of gasification rates at the elevated particle temperatures associated with typical pc char combustion processes, as well as the complex interaction of oxidation and gasification reactions. Gasification reactions tend to become more important at higher char particle temperatures (because of their high activation energy) and they tend to reduce pc oxidation due to their endothermicity (i.e. cooling effect). The work reported here attempts to quantify the influence of the gasification reaction of CO 2 in a rigorous manner by combining experimental measurements of the particle temperatures and consumption rates of size-classified pc char particles in tailored oxy-fuel environments with simulations from a detailed reacting porous particle model. The results demonstrate that a specific gasification reaction rate relative to the oxidation rate (within an accuracy of approximately +/- 20% of the pre-exponential value), is consistent with the experimentally measured char particle temperatures and burnout rates in oxy-fuel combustion environments. Conversely, the results also show, in agreement with past calculations, that it is extremely difficult to construct a set of kinetics that does not substantially overpredict particle temperature increase in strongly oxygen-enriched N2 environments. This latter result is believed to result from deficiencies in standard oxidation mechanisms that fail to account for falloff in char oxidation rates at high temperatures.

42 ENGINEERING↗

DOE OSTI2020

Thermal evolution of ferroelectric behavior in epitaxial Hf 0.5 Zr 0.5 O 2

In this paper, we report a cryogenic-temperature study on the evolution of the ferroelectric properties of epitaxial Hf 0.5 Zr 0.5 O 2 thin films on silicon. Wake-up, endurance, and fatigue of these films are found to be intricately correlated, strongly hysteretic, and dependent on available thermal energy. Field-dependent measurements reveal a decrease in polarization with temperature, which has been determined not to be an intrinsic change of the material property, rather a demonstration of the increase in the coercive bias of the material. Our findings suggest that a deficiency in thermal energy suppresses the mobility of defects presumed to be oxygen vacancies during wake-up and trapped injected charge during fatigue, which is responsible for polarization evolution during cycling. This permits accelerated wake-up and fatigue effects at high temperatures where thermal energy is abundant but delays these effects at cryogenic temperatures.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Strontium-84 Enrichments in Presolar Grains Provide First Evidence of p -process Nucleosynthesis in Core-collapse Supernovae

This study reports detection of rare p-process isotopes within presolar grains. Presolar grains are relic dust grains from dying stars. These microscopic dust particles are found in primitive solar system materials. Their distinct isotopic compositions record the nucleosynthetic processes in their parent stars and the Galactic chemical environment in which these stars formed. We studied presolar graphite grains of high-density type from the Murchison meteorite and found five grains with subgrains that show enrichments in 84 Sr compared to the solar abundance. 84 Sr is the neutron-deficient isotope of strontium that can be produced in the deep oxygen-rich interior of high-mass stars that end their lives as core-collapse supernovae. The observed 84 Sr excesses cannot be produced in low-mass asymptotic giant branch stars, the source of most high-density presolar graphites found in meteorites. High-density graphites with embedded 84 Sr excesses are, instead, compatible with a core-collapse supernovae origin. The graphite subgrains condensed from carbon-rich materials in the outer layers of core-collapse supernovae, where 84 Sr was destroyed by neutron captures during hydrostatic evolution of the stars and their final explosion. Based on current theoretical stellar models, a few percent of contribution from the inner regions of core-collapse supernovae, which are enriched in p-process nuclides, to the outer carbon-rich regions is the most likely explanation for the observed enrichment of 84 Sr in the subgrains of the high-density graphites. In this study, we present the first observational evidence that core-collapse supernovae produce and eject isotopes made by the p-process.

Astronomy and AstroPhysics↗

NASA NTRS2024

Simplified Structure Models for Premixed n-Alkane Cool Flames

The chemical kinetics of cool flames in mixtures of normal alkanes, oxygen, and nitrogen recently have been reduced to obtain simplified asymptotic flame-structure models that can be used to compare theoretical predictions with experimental measurements. A key step that affects flame structures strongly, namely the abstraction of a hydrogen atom from the alkyl radical by an oxygen molecule, had not been taken into account in those models. This deficiency has now been remedied for diffusion flames. The present contribution reports the corresponding remedy for premixed-flame analyses. In the new model, non-zero chemical reaction rates are restricted to narrow regions in the vicinity of the maximum temperature, whereas previously they extended throughout the preheat zone. Comparisons of the new predictions with experimental burning-velocity measurements seem favorable.

premixed cool flames↗

DOE OSTI2021

Stabilizing Anionic Redox Chemistry in a Mn-Based Layered Oxide Cathode Constructed by Li-Deficient Pristine State

Li-rich cathode materials are of significant interest for coupling anionic redox with cationic redox chemistry to achieve high-energy-density batteries. However, lattice oxygen loss and derived structure distortion would induce serious capacity loss and voltage decay, further hindering its practical application. Herein, a novel Li-rich cathode material, O3-type Li 0.6 [Li 0.2 Mn 0.8 ]O 2 , is developed with the pristine state displaying both a Li excess in the transition metal layer and a deficiency in the alkali metal layer. Benefiting from stable structure evolution and Li migration processes, not only can high reversible capacity (≈329 mAh g -1 ) be harvested but also irreversible/reversible anionic/cationic redox reactions are comprehensively assigned via the combination of in/ex situ spectroscopies. Furthermore, irreversible lattice oxygen loss and structure distortion are effectively restrained, resulting in long-term cycle stability (capacity drop of 0.045% per cycle, 500 cycles). Altogether, tuning the Li state in the alkali metal layer presents a promising way for modification of high-capacity Li-rich cathode candidates.

anionic redox reactions↗

DOE OSTI2022

Floating Island International PHASE I FINAL TECHNICAL REPORT (Advancing the Development of Floating Solar-Powered Nanobubble Aeration Systems for Use with Floating Treatment Wetlands in Natural and Man-Made Waterbodies)

More and more freshwater lakes are suffering from algae blooms, which deprive water of oxygen and lead to widespread loss of aquatic life and production of dangerous toxins. When oxygen is lacking, methane is generated in the sediments as algae is decomposed; it has been calculated that more than half of global methane emissions come from nutrient-impaired freshwater systems (Beaulieu, 2021). Nutrients, mainly from agricultural run-off, feed algae blooms and are exacerbated by warming related to climate change. Artificial aeration is frequently used to restore oxygen to a waterbody. But diffuser aeration is inefficient and expensive, needs on-site grid power, and is failing to keep pace with the demands of water as it gets warmer with climate change. In the last five years, nanobubble aeration has been introduced into freshwater applications and shows promise for rapidly increasing dissolved oxygen effectively throughout the water column. Nanobubbles deliver oxygen in bubbles that have no buoyancy, so they stay in water longer and release their oxygen more fully, compared to large bubbles that rise and burst at the surface. The prospect of this new technology answering the deficiencies of diffuser aeration drove us to initiate the current project. During our Phase I period, we have successfully tested a nanobubble aeration system that can super-saturate oxygen levels. It is operated on solar power, and both the nanobubbler and solar array are mounted on a proprietary floating island platform, that also performs biological nutrient recycling. A rudimentary system was assembled and tested on a 6.5-acre research lake at our headquarters in Montana, where it was subjected to a summer drought that reduced water levels significantly, periods of severe cold in winter, and spring conditions that included heavy rainfall and violent thunderstorms. Our twice-weekly sampling throughout the project showed that dissolved oxygen levels rose rapidly and were maintained throughout winter and spring, well into June. The nanobubbler was able to run on solar power for long periods. Methane levels were tested periodically and found to decrease as oxygen increased. The nanobubbles appeared to have no adverse impact on fish or other aquatic life exposed to them. The stability of the installation survived the weather conditions. The many problems we encountered taught us what we need to improve in the next iteration. Towards the end of our Phase I, we were awarded a supplementary state grant that enabled us to acquire a new nanobubble system for testing that runs on DC, is extremely efficient and has few moving parts. We plan to team this with low-profile solar panels, lithium batteries and a controller that provides real-time data. The ultimate goal of this project is to commercialize an affordable and scalable lake management system that will oxygenate water from the surface down to the sludge. It will enliven fisheries, prevent toxic algae blooms and – most importantly for the fate of our planet - inhibit the production and release of methane from the sediments. We anticipate that as carbon credits expand to include methane, the cost of remediating waterbodies that produce methane will be offset. We firmly believe that this is a practical technology that works and will make a big difference when fully implemented.

14 SOLAR ENERGY↗

NASA NTRS1983

Role of metabolic rate and DNA-repair in Drosophila aging Implications for the mitochondrial mutation theory of aging

The notion that injury to mitochondrial DNA is a cause of intrinsic aging was tested by correlating the different respiration rates of several wild strains of Drosophila melanogaster with the life-spans. Respiration rate and aging in a mutant of D. melanogaster deficient in postreplication repair were also investigated. In agreement with the rate of living theory, there was an inverse relation between oxygen consumption and median life-span in flies having normal DNA repair. The mutant showed an abnormally low life-span as compared to the controls and also exhibited significant deficiency in mating fitness and a depressed metabolic rate. Therefore, the short life-span of the mutant may be due to the congenital condition rather than to accelerated aging.

Miquel, J.↗

DOE OSTI2020

LixNiO/Ni Heterostructure with Strong Basic Lattice Oxygen Enables Electrocatalytic Hydrogen Evolution with Pt-like Activity

The low-cost hydrogen production from water electrolysis is crucial for practical deployment of sustainable hydrogen economy, but is often constrained by the lack of active and robust electrocatalysts from Earth-abundant materials. We describe here an unconventional heterostructure composed of strongly coupled Ni-deficient LixNiO nanoclusters and polycrystalline Ni nanocrystals, and its exceptional activities toward hydrogen evolution reaction (HER) in aqueous electrolytes. The presence of unique lattice oxygen species with strong Brønsted basicity is a significant feature, which spontaneously split water molecules and effectively accelerate the sluggish Volmer H-OH dissociation step in neutral and alkaline HER. In combination with the unpreceded level of intimate LixNiO and Ni interfacial junctions that produces abundant “hotspots” for promoted hydride coupling, the catalyst exhibited kinetic activities almost identical as Pt/C and decent long term stability in universal pH.

Lu, Ke↗