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At least 865 records · Page 48
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Regulating the Electron Distribution of Metal-Oxygen for Enhanced Oxygen Stability in Li-rich Layered Cathodes

Li-rich Mn-based layered oxides (LLO) hold great promise as cathode materials for lithium-ion batteries (LIBs) due to their unique oxygen redox (OR) chemistry, which enables additional capacity. However, the LLOs face challenges related to the instability of their OR process due to the weak transition metal (TM)-oxygen bond, leading to oxygen loss and irreversible phase transition that results in severe capacity and voltage decay. Herein, a synergistic electronic regulation strategy of surface and interior structures to enhance oxygen stability is proposed. In the interior of the materials, the local electrons around TM and O atoms may be delocalized by surrounding Mo atoms, facilitating the formation of stronger TM—O bonds at high voltages. Besides, on the surface, the highly reactive O atoms with lone pairs of electrons are passivated by additional TM atoms, which provides a more stable TM—O framework. Hence, this strategy stabilizes the oxygen and hinders TM migration, which enhances the reversibility in structural evolution, leading to increased capacity and voltage retention. This work presents an efficient approach to enhance the performance of LLOs through surface-to-interior electronic structure modulation, while also contributing to a deeper understanding of their redox reaction.

25 ENERGY STORAGE↗
DOE OSTI2021

Layered Transition Metal Oxides as Ca Intercalation Cathodes: A Systematic First-Principles Evaluation

Finding high-voltage Ca cathode materials is a critical step to unleashing the full potential of high-energy-density Ca-ion batteries. Therefore, first-principles calculations are used to demonstrate that P-type layered calcium transition metal (TM) oxide materials (CaTM 2 O 4 ) with a range of TM substitutions (TM = Ti, V, Cr, Mn, Fe, Co, and Ni) have excellent battery-related properties including thermodynamic stability, average voltage, energy density, synthesizability, ionic mobility, and electronic structure. However, the thermodynamic stability of the charged phase and TM redox activity are shown to be sensitive to TM selection, with CaCo 2 O 4 having the best balance of all considered properties. The utility of combining multiple TMs to expand the chemical search space for TM substitutions is demonstrated by mixing Co and Ni in layered CaTM 2 O 4 .

25 ENERGY STORAGE↗
DOE OSTI2020

Role of Redox-Inactive Transition-Metals in the Behavior of Cation-Disordered Rocksalt Cathodes

Owing to the capacity boost from oxygen redox activities, Li-rich cation-disordered rocksalts (LRCDRS) represent a new class of promising high-energy Li-ion battery cathode materials. Redox-inactive transition-metal (TM) cations, typically d 0 TM, are essential in the formation of rocksalt phases, however, their role in electrochemical performance and cathode stability is largely unknown. In the present study, the effect of two d 0 TM (Nb 5+ and Ti 4+ ) is systematically compared on the redox chemistry of Mn-based model LRCDRS cathodes, namely Li 1.3 Nb 0.3 Mn 0.4 O 2 (LNMO), Li 1.25 Nb 0.15 Ti 0.2 Mn 0.4 O 2 (LNTMO), and Li 1.2 Ti 0.4 Mn 0.4 O 2 (LTMO). Although electrochemically inactive, d 0 TM serves as a modulator for oxygen redox, with Nb 5+ significantly enhancing initial charge storage contribution from oxygen redox. Further studies using differential electrochemical mass spectroscopy and resonant inelastic X-ray scattering reveal that Ti 4+ is better in stabilizing the oxidized oxygen anions (O n- , 0 < n < 2), leading to a more reversible O redox process with less oxygen gas release. As a result, much improved chemical, structural and cycling stabilities are achieved on LTMO. Detailed evaluation on the effect of d 0 TM on degradation mechanism further suggests that proper design of redox-inactive TM cations provides an important avenue to balanced capacity and stability in this newer class of cathode materials.

25 ENERGY STORAGE↗
DOE OSTI2020

Prussian blue analogues as platform materials for understanding and developing oxygen evolution reaction electrocatalysts

Transition metal based materials containing Fe have drawn great attention as oxygen evolution reaction (OER) catalysts. The nature of the electrocatalytic active species remains under debate due to the ambiguous physicochemical properties of the catalyst materials, such as the oxidation states and crystal structures. Here, in order to address this issue, transition metal Prussian blue analogues (TM-PBA, Na(TM)(Fe)(CN) 6 , TM = V, Fe, Co, and Ni) with an isomorphous structure are investigated for OER catalysis. Our combined experimental measurements and density functional theory (DFT) calculations reveal that TM-PBAs exhibit volcano-like OER activity with Ni-PBA located near the top of the volcano. Such a volcano-like activity profile can be attributed to the distinctive binding energy difference between *O and *OH on different TM-PBAs surfaces. This research demonstrates that TM-PBAs can be used as platform materials for understanding structure-property-activity relationships in OER catalysts.

25 ENERGY STORAGE↗
DOE OSTI2021

Unraveling transition-metal-mediated stability of spinel oxide via in situ neutron scattering

The energy materials performance is intrinsically determined by structures from the average lattice structure to the atom arrangement, valence, and distribution of the containing transition metal (TM) elements. Understanding the mechanism of the structure transition and atom rearrangement via synthesis or processing is key to expediting the exploration of excellent energy materials. In this work, in situ neutron scattering is employed to reveal the real-time structure evolution, including the TM-O bonds, lattice, TM valence and the migration of the high-voltage spinel cathode LiNi 0.5 Mn 1.5 O 4 . The transition-metal-mediated spinel destabilization under the annealing at the oxygen-deficient atmosphere is pinpointed. Additionally, the formation of Mn 3+ is correlated to the TM migration activation, TM disordered rearrangement in the spinel, and the transition to a layered-rocksalt phase. The further TM interdiffusion and Mn 2+ reduction are also revealed with multi-stage thermodynamics and kinetics. The mechanisms of phase transition and atom migrations as functions of temperature, time and atmosphere present important guidance on the synthesis in various-valence element containing oxides.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Effect of anisotropic thermal transport on tearing mode stability in negative versus positive triangularity plasmas

The combined effects of anisotropic thermal transport and the plasma shaping, including negative triangularity, on the n = 1 (n is the toroidal mode number) tearing mode (TM) stability are numerically investigated utilizing the MARS-F code [Liu et al., Phys. Plasmas 7, 3681–3690 (2000)]. While varying the plasma boundary triangularity, the TM stability is found to be dictated by the competing effects of the Shafranov shift induced stabilization and the bad-curvature induced destabilization. The negative triangularity shape increases the Shafranov shift (stabilizing) in the plasma core but also enlarges bad-curvature regions (destabilizing) near the plasma edge, with the net effect being largely destabilizing for the TM as compared to the positive triangularity counter-part. Large negative triangularity however can also lead to more stabilization for the plasma core-localized TM. Anisotropic thermal transport reduces the stabilizing effect on the TM associated with the favorable averaged curvature, resulting in more unstable core-localized TMs in both negative and positive triangularity plasmas. But the opposite effect can also take place for the edge-localized TM in finite-pressure plasmas with negative triangularity.

Physics↗
DOE OSTI2024

Effects of irradiation damage on the hardness and elastic properties of quaternary and high entropy transition metal diborides

Multi-principal component transition metal (TM) diborides represent a class of high-entropy ceramics (HECs) that have received considerable interest in recent years owing to their promising properties for extreme environment applications that include thermal/ environmental barriers, hypersonic vehicles, turbine engines, and next-generation nuclear reactors. While the addition of chemical disorder through the random distribution of TM elements on the cation sublattice has offered opportunities to tailor elastic stiffness and hardness, the effects of irradiation-induced structural damage on the physical properties of these complex materials have remained largely unexplored. To this end, changes in the hardness and elastic moduli of a high-entropy TM diboride (Hf 0.2 Nb 0.2 Ta 0.2 Ti 0.2 Zr 0.2 )B 2 and three of its quaternary subsets following irradiation with 10 MeV gold (Au) ions to fluences of up to 6 × 10 15 Au cm -2 are investigated at the micrometer and sub-micrometer length-scales via the dispersion of laser-generated surface acoustic waves (SAW) and nanoindentation, respectively. The nanoindentation measurements show that the TM diborides exhibit an initial increase in hardness following irradiation with energetic Au ions, with a subsequent decrease in hardness following further irradiation. One quaternary composition, (Hf 1/3 Ta 1/3 Ti 1/3 )B 2 , exhibits a notable exception to the trend and continues to exhibit an increase in hardness with ion irradiation fluence. Although differences in the absolute values of the effective elastic moduli obtained from the measured SAW dispersion and nanoindentation are observed (and attributed to microstructural variations at the measurement length-scale), both techniques yield similar trends in the form of an initial reduction and subsequent saturation in the elastic modulus with increasing ion irradiation fluence. The quaternary TM diboride (Hf 1/3 Ta 1/3 Ti 1/3 )B 2 again exhibits a departure from this trend. The high-entropy TM diboride (Hf 0.2 Nb 0.2 Ta 0.2 Ti 0.2 Zr 0.2 )B 2 exhibits the greatest recovery in hardness and modulus when irradiated to high ion fluences following initial changes at low fluence, indicating superior resistance to radiation-induced damage over its quaternary counterparts. Opportunities for designing HECs with superior hardness and modulus for enhanced radiation resistance (compared to their single constituent counterparts) by tailoring chemical disorder and bond character in the lattice are discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Transition metal elements as donor dopants in CdO

CdO has been shown to achieve a high electron concentration N (> 10 21 cm -3 ) and at the same time a high mobility μ (> 100cm 2 /V s) when doped with conventional shallow dopants (In or Ga), and consequently making it a transparent conducting oxide with very low resistivity ρ <10 -4 $\Omega$ cm. In this work, the properties of CdO thin films doped with a series of transition metal elements (CdO:TM) with partially filled 3d and 4d shells, including Sc, Ti, V, Cr, Fe, Y, Mo, and W, were investigated. We find that doping with these TM elements can effectively increase the N in CdO to a maximum N (N max ) of ~(7-12)×10 20 cm -3 with a dopant concentration x max of 4-7 %. However, unlike CdO:In, the μ of CdO:TM films drops rapidly from > 100 to < 10cm 2 /Vs as the dopant concentration x increases, so that they can only achieve a minimum ρ of ~ (1-2) × 10 -4 $\Omega$ cm, ~ a factor of 2-3 higher than that in CdO:In. As a result, free-carrier absorption and plasma reflection effects limit their optical transparency to <1200 nm. For most 3d TM dopants, a qualitatively higher d-donor level E d,donor gives rise to higher E F,max or a higher N max . Although at low x, the optical band gap E opt of CdO:TM follows the calculated values due to free-carrier effects, as x increases, E opt values are significantly higher than the calculated values. This is believed to be an effect of the anticrossing interaction of the localized d-levels and the extended CdO conduction-band (CB) states, giving rise to a lower occupied E - and an upper unoccupied E + subband. In conclusion, the restructured CBs have much flatter dispersion, which also results in a much higher effective mass $m^{\star}_{e}$, hence it can also explain the much lower μ of CdO:TM films with high N.

36 MATERIALS SCIENCE↗
DOE OSTI2022

In vivo stabilization of a less toxic asparaginase variant leads to a durable antitumor response in acute leukemia

Asparagine is a non-essential amino acid since it can either be taken up via the diet or synthesized by asparagine synthetase. Acute lymphoblastic leukemia (ALL) cells do not express asparagine synthetase or express it only minimally, which makes them completely dependent on extracellular asparagine for their growth and survival. This dependency makes ALL cells vulnerable to treatment with L-asparaginase, an enzyme that hydrolyzes asparagine. To date, all clinically approved L-asparaginases have significant L-glutaminase co-activity, associated with non-immune related toxic side effects observed during therapy. Therefore, reduction of L-glutaminase co-activity with concomitant maintenance of its anticancer L-asparaginase effect may effectively improve the tolerability of this unique drug. Previously, we designed a new alternative variant of Erwinia chrysanthemi (ErA; Erwinaze) with decreased L-glutaminase co-activity, while maintaining its L-asparaginase activity, by the introduction of three key mutations around the active site (ErA-TM). However, Erwinaze and our ErA-TM variant have very short half-lives in vivo. Here, we show that the fusion of ErA-TM with an albumin binding domain (ABD)-tag significantly increases its in vivo persistence. In addition, we evaluated the in vivo therapeutic efficacy of ABD-ErA-TM in a B-ALL xenograft model of SUP-B15. Our results show a comparable long-lasting durable antileukemic effect between the standard-of-care pegylated-asparaginase and ABD-ErA-TM L-asparaginase, but with fewer co-glutaminase-related acute side effects. Since the toxic side effects of current L-asparaginases often result in treatment discontinuation in ALL patients, this novel ErA-TM variant with ultra-low L-glutaminase co-activity and long in vivo persistence may have great clinical potential.

60 APPLIED LIFE SCIENCES↗
NASA NTRS1983

LANDSAT 4 investigations of thematic mapper and multispectral scanner applications

The utility of TM data natural resource assessment was evaluated with emphasis on manual interpretation and digital classification. The improved spatial resolution of TM data, as compared with MSS data, aided in the location of roads, small stock ponds, and many other land features, permitting positive identification of landmarks. With the TM, there was more efficient manual interpretation of land use, better identification of resource types, and improved assessment of the ecological status of natural vegetation. Band 5 and band 7 aided in defining water resources, wetland vegetation resources, and other terrain features. Results from TM and TM simulator data suggest that the coefficient of variation for major land cover types is less for TM data than for equivalent MSS data. Although the amount of information in bands 5 and 7 is small, it is unique since the same information cannot be derived from the MSS four-band spectral region.

Lauer, D. T.↗
NASA NTRS1983

The use of thematic mapper data for land cover discrimination: Preliminary results from the UK SATMaP programme

The principal objectives of the UK SATMaP program are to determine thematic mapper (TM) performance with particular reference to spatial resolution properties and geometric characteristics of the data. So far, analysis is restricted to images from the U.S. and concentrates on spectra and radiometric properties. The results indicate that the data are inherently three dimensional compared with the two dimensional character of MSS data. Preliminary classification results indicate the importance of the near infrared band (TM 4), at least one middle infrared band (TM 5 or TM 6) and at least one of the visible bands (preferably either TM 3 or TM 1). The thermal infrared also appears to have discriminatory ability despite its coarser spatial resolution. For band 4 the forward and reverse scans show somewhat different spectral responses in one scene but this effect is absent in the other analyzed. From examination of the histograms it would appear that the full 8-bit quantization is not being effectively utilized for all the bands.

Jackson, M. J.↗
NASA NTRS1984

Evaluation of corn/soybeans separability using Thematic Mapper and Thematic Mapper Simulator data

Multitemporal Thematic Mapper, Thematic Mapper Simulator, and detailed ground truth data were collected for a 9- by 11-km sample segment in Webster County, IA, in the summer of 1982. Three dates were acquired each with Thematic Mapper Simulator (June 7, June 23, and July 31) and Thematic Mapper (August 2, September 3, and October 21). The Thematic Mapper Simulator data were converted to equivalent TM count values using TM and TMS calibration data and model based estimates of atmospheric effects. The July 31, TMS image was compared to the August 2, TM image to verify the conversion process. A quantitative measure of proportion estimation variance (Fisher information) was used to evaluate the corn/soybeans separability for each TM band as a function of time during the growing season. The additional bands in the middle infrared allowed corn and soybeans to be separated much earlier than was possible with the visible and near-infrared bands alone. Using the TM and TMS data, temporal profiles of the TM principal components were developed. The greenness and brightness exhibited behavior similar to MSS greenness and brightness for corn and soybeans.

Pitts, D. E.↗
NASA NTRS1984

Landsat-4 thematic mapper and thematic mapper simulator data for a porphyry copper deposit

Aircraft thematic mapper (TM) data were analyzed to evaluate the potential utility of the Landsat-4 thematic mapper for geologic mapping and detection of hydrothermal alteration zones in the Silver Bell porphyry copper deposit in southern Arizona. The data allow a comparison between aircraft TV simulator data and the Landsat-4 TM satellite data which possess similar spectral bands. A color rationcomposite of 30-m pixels was resampled, in order to clearly define a number of hydroxyl bearing minerals, (kaolinite, sericite, white mica), pyrite and iron oxide/hydroxide minerals. The iron oxide minerals have diagnostic absorption bands in the 0.45 and 0.85 micron regions of the spectrum, and the hydrous minerals are characterized by an absorption in the 2.2 micron region. The position of the spectral bands allow the TM to identify regions of hydrothermal alteration without resorting to a data processing algorithm. The comparison of the aircraft and Landsat-4 TM data showed considerable agreement, and confirmed the utility of TM data for identifying hydrothermal alteration zones. Samples of some color TM images are provided.

Abrams, M. J.↗
NASA NTRS1984

A prospectus for Thematic Mapper research in the Earth sciences

Earth science applications of Thematic Mapper (TM) imagery are discussed. Prospective research themes are defined in a general sense in relation to the technical measurement capabilities of the TM and the various types of Earth information that can potentially be derived from multispectral TM imagery. An overview of the system developed to acquire and reduce TM data is presented. The technical capabilities of this system are presented in detail. The orbital performance of the TM sensor is described, based upon the analysis of LANDSAT 4 and 5 TM data collected to date.

Source record↗
NASA NTRS1985

An Initial Analysis of LANDSAT-4 Thematic Mapper Data for the Discrimination of Agricultural, Forested Wetlands, and Urban Land Cover

The capabilities of TM data for discriminating land covers within three particular cultural and ecological realms was assessed. The agricultural investigation in Poinsett County, Arkansas illustrates that TM data can successfully be used to discriminate a variety of crop cover types within the study area. The single-date TM classification produced results that were significantly better than those developed from multitemporal MSS data. For the Reelfoot Lake area of Tennessee TM data, processed using unsupervised signature development techniques, produced a detailed classification of forested wetlands with excellent accuracy. Even in a small city of approximately 15,000 people (Union City, Tennessee). TM data can successfully be used to spectrally distinguish specific urban classes. Furthermore, the principal components analysis evaluation of the data shows that through photointerpretation, it is possible to distinguish individual buildings and roof responses with the TM.

Quattrochi, D. A.↗
NASA NTRS1985

The Use of Thematic Mapper Data for Land Cover Discrimination: Preliminary Results from the UK Satmap Programme

The principal objectives of the UK SATMaP program are to determine thematic mapper (TM) performance with particular reference to spatial resolution properties and geometric characteristics of the data. So far, analysis is restricted to images from the U.S. and concentrates on spectra and radiometric properties. The results indicate that the data are inherently three dimensional compared with the two dimensional character of MSS data. Preliminary classification results indicate the importance of the near infrared band (TM 4), at least one middle infrared band (TM 5 or TM 6) and at least one of the visible bands (preferably either TM 3 or TM 1). The thermal infrared also appears to have discriminatory ability despite its coarser spatial resolution. For band 4 the forward and reverse scans show somewhat different spectral responses in one scene but this effect is absent in the other analyzed. From examination of the histograms it would appear that the full 8 bit quantization is not being effectively utilized for all the bands.

Jackson, M. J.↗
NASA NTRS1983

Geometric correction process for the Landsat-4 Thematic Mapper

The processing approaches which form the basis of the Landsat-4 Thematic Mapper (TM) geometric correction system are summarized. The correction is accomplished in two phases. In the first phase, correction data are generated. The spacecraft position, TM frame attitude, TM scanning mirror position, and detector sampling are found as a function of time through a combination of flight segment measurements, ground segment modeling, and control point information. The data, along with the earth position and geoid model, are used to determine the earth location for each TM image sample. Then, using map projections, correction data can be generated which define the location of each TM image sample on the output coordinate system. In the second phase, the correction data are used to resample TM detector samples onto the output coordinate system.

Beyer, E. P.↗
NASA NTRS1984

Evaluation of atmospheric particulate concentrations derived from analysis of ratio Thematic Mapper data

An approach for atmospheric particulate concentration evaluation above urban areas using ratio Thematic Mapper (TM) data is discussed. October 25, 1982 TM data over Chicago, IL are analyzed using TM band ratios of 1/2, 1/3, 1/4, 1/5, and 1/6 and particulate concentration estimates derived from TM ratios are tested over low reflective turbid water sites and highly reflective concrete highways. From analysis of the data it is evident that for water, the pattern of increasing particulate concentration is associated with decreasing ratio values in all band combinations used. Over concrete features, the TM band 1/4 ratio values follow the predicted pattern, while the TM band 1/6 has ratios which are reversed from anticipated values.

Carnahan, W. H.↗