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At least 1,567 records · Page 87
All sourcesNASA NTRSDOE OSTI
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 OSTI2021

Reply to: Insufficient evidence for ageing in protein dynamics

Reference 1 states that we claimed that internal motions in single protein molecules exhibit ageing over 13 decades of time. In contrast, our primary conclusion, as expressed in the title, was that over these timescales the dynamics of single protein molecules is non-equilibrium and self-similar. Notwithstanding, we demonstrate in this reply that protein dynamics does indeed exhibit ageing according to the criteria of ref. 1.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2017

Aging and rejuvenation of active matter under topological constraints

The coupling of active, self-motile particles to topological constraints can give rise to novel nonequilibrium dynamical patterns that lack any passive counterpart. Here we study the behavior of self-propelled rods confined to a compact spherical manifold by means of Brownian dynamics simulations. We establish the state diagram and find that short active rods at sufficiently high density exhibit a glass transition toward a disordered state characterized by persistent self-spinning motion. By periodically melting and revitrifying the spherical spinning glass, we observe clear signatures of time-dependent aging and rejuvenation physics. We quantify the crucial role of activity in these nonequilibrium processes, and rationalize the aging dynamics in terms of an absorbing-state transition toward a more stable active glassy state. In conclusion, our results demonstrate both how concepts of passive glass phenomenology can carry over into the realm of active matter, and how topology can enrich the collective spatiotemporal dynamics in inherently non-equilibrium systems.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Stratification of fluoride uptake among enamel crystals with age elucidated by atom probe tomography

Dental enamel is subjected to a lifetime of de- and re-mineralization cycles in the oral environment, the cumulative effects of which cause embrittlement with age. However, the understanding of atomic scale mechanisms of dental enamel aging is still at its infancy, particularly regarding where compositional differences occur in the hydroxyapatite nanocrystals and what underlying mechanisms might be responsible. Here, we use atom probe tomography to compare enamel from a young (22 years old) and a senior (56 years old) adult donor tooth. Findings reveal that the concentration of fluorine is elevated in the shells of senior nanocrystals relative to young, with less significant differences between the cores or intergranular phases. It is proposed that the embrittlement of enamel is driven, at least in part, by the infusion of fluorine into the nanocrystals and that the principal mechanism is de- and re-mineralization cycles that preferentially erode and rebuild the nanocrystals shells.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Effects of catholyte aging on high-nickel NMC cathodes in sulfide all-solid-state batteries

Sulfide solid-state electrolytes (SSEs) in all-solid-state batteries (SSBs) are recognized for their high ionic conductivity and inherent safety. The LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cathode offers a high thermodynamic potential of approximately 3.8 V vs. Li/Li + and a theoretical specific capacity of 200 mA h g −1 . However, the practical utilization of NMC811 in sulfide SSBs faces significant interfacial challenges. The oxidation instability of sulfide solid electrolytes against NMC811 and the formation of the cathode electrolyte interphase (CEI) during cycling lead to degradation and reduced cell performance. Volumetric changes in NMC during lithiation and de-lithiation can also cause detachment from sulfide electrolytes or internal particle cracking. Despite extensive galvanostatic cycling studies to address the issues, the calendar life of sulfide SSBs remains poorly understood. Here, we systematically studied the effects of four different catholytes on the calendar aging of LiNbO 3 (LNO)-coated NMC811, including Li 6 PS 5 Cl (LPSCl), Li 3 InCl 6 –Li 6 PS 5 Cl (LIC–LPSCl), Li 3 YCl 6 –Li 6 PS 5 Cl (LYC–LPSCl), and Li 10 GeP 2 S 12 (LGPS). Our results indicate that LPSCl provides optimal capacity retention when stored at high state-of-charge (SOC) at room temperature, but the LIC–LPSCl cathode shows significant capacity degradation and chemical incompatibility. We also established an effective electrochemical calendar aging testing protocol to simulate daily usage, enabling quick inference of the calendar life of SSBs. In conclusion, this new testing approach accelerates materials selection strategies for high-nickel NMC composite cathodes in sulfide SSBs.

25 ENERGY STORAGE↗
DOE OSTI2021

The dependence of the gradients of oxygen and nitrogen-to-oxygen on stellar age in MaNGA galaxies

For this work, we derived the oxygen abundance (O/H), the nitrogen-to-oxygen (N/O) abundance ratio, and their corresponding radial gradients for a sample of 1431 galaxies from the MaNGA DR15 survey using two different realisations of the strong line method: empirical R calibration and the Bayesian model-based HII-CHI-MISTRY (HCM) code. We find that both abundance calculation methods reveal a correlation between the O/H gradient and the stellar mass of a galaxy. This relation is non-linear, with the steepest average gradients in the intermediate mass range and flatter average gradients for high- and low-mass galaxies. The relation between the N/O gradient and the stellar mass is, on average, non-linear with the steepest gradients in the intermediate mass range (log(M/M ⊙ )~10), flatter gradients for high-mass galaxies, and the flattest gradients for low-mass galaxies. However, the general trend of steepening N/O gradients for higher masses, as reported in previous studies, remains evident. We find a dependence between the O/H and N/O gradients and the galaxy mean stellar age traced by the D(4000) index. For galaxies of lower masses, both gradients are, generally, steeper for intermediate values of D(4000) and flatter for low and high values of D(4000). Only the most massive galaxies do not show this correlation. We interpret this behaviour as an evolution of the metallicity gradients with the age of stellar population. Though the galaxies with a positive slope of the D(4000) radial gradient tend to have flatter O/H and N/O gradients, as compared to those with a negative D(4000) gradient.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2024

Strategies for Developing High-Volume Fly Ash Concrete with High Early-Age Strength for Precast Applications

Partial replacement of portland cement with supplementary cementitious materials (SCMs), such as fly ash, is an effective strategy for improving durability and reducing the CO 2 footprint of concrete. However, using high-volume fly ash (HVFA) binders in precast and prestressed concrete is currently limited; largely due to reduced early-age strength development that impedes rapid production and prestressing of precast concrete. To investigate and address this challenge, HVFA mortars with a minimum of 40% fly ash by mass of cementitious materials were developed and tested in this study. Two fresh fly ashes (an ASTM C618 Class F and a Class C) and a landfilled fly ash (Class F) were included. Various strategies for improving the early strength were evaluated, including gypsum optimization, chemical accelerators, steam curing, use of CSA cements, and adding other reactive SCMs like silica fume, calcined clay, and slag cement. Steam curing and the use of CSA cement at high dosages (40% of total binder) were found to be the most successful strategies across all three fly ashes. Additionally, significant improvements were observed with gypsum optimization (for Class C fly ash) and the use of accelerators (for Class F fly ashes), and these strategies are likely to be more feasible considering later-age strength and economic viability. Interestingly, HVFA mixtures made with the landfilled fly ash used in this study were able to achieve high early strengths with water-to-cementitious materials ratio adjustment alone. As a result, these HVFA mixtures were also found to be less responsive to accelerators when compared to the fresh Class F fly ash, highlighting an important distinction between the materials despite the similarity in chemical composition.

42 ENGINEERING↗
DOE OSTI2014

Molecular ageing: Free radical initiated epimerization of thymopentin – A case study

The epimerization of amino acid residues increases with age in living organisms. In the present study, the structural consequences and thermodynamic functions of the epimerization of thymopentin (TP-5), the active site of the thymic hormone thymopoietin, were studied using molecular dynamics and density functional theory methods. The results show that free radical-initiated D-amino acid formation is energetically favoured (−130 kJmol{sup −1}) for each residue and induces significant changes to the peptide structure. In comparison to the wild-type (each residue in the L-configuration), the radius of gyration of the D-Asp{sup 3} epimer of the peptide decreased by 0.5 Å, and disrupted the intramolecular hydrogen bonding of the native peptide. Beyond establishing important structural, energetic and thermodynamic benchmarks and reference data for the structure of TP-5, these results disseminate the understanding of molecular ageing, the epimerization of amino acid residues.

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

Ageing effect in spray pyrolysed B:SnO{sub 2} thin films for LPG sensing

For LPG sensing, boron doped (0.2 to 0.8 wt. %) polycrystalline tin oxide thin films are deposited by spray pyrolysis in the temperature range 325 - 430 °C. Sensor response of 56 % is achieved for 1000 ppm of LPG, at an operating temperature of 350 °C. The effects of ageing under ambient conditions on the sensor response are investigated for a storage period of six years. Ageing increases the film resistance but the gas response is lowered. XRD, SEM, FESEM, FTIR and XPS are utilized for structural, morphological and compositional charaterisations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Intercalation of p-methycinnamic acid anion into Zn-Al layered double hydroxide to improve UV aging resistance of asphalt

A UV absorber, p-methycinnamic acid (PMCA), was intercalated into Zn-Al layered double hydroxide (LDH) by calcination recovery. Fourier transform infrared spectroscopy showed that the PMCA anions completely replaced the CO{sub 3}{sup 2−} anions in the interlayer galleries of Zn-Al-LDH containing PMCA anions (Zn-Al-PMCA-LDH). X-ray diffraction and transmission electron microscopy showed that the interlayer distance increased from 0.78 nm to 1.82 nm after the substitution of PMCA anions for CO{sub 3}{sup 2−} anions. The similar diffraction angles of the CO{sub 3}{sup 2−} anion-containing Zn-Al-LDH (Zn-Al-CO{sub 3}{sup 2−}-LDH) and the Zn-Al-CO{sub 3}{sup 2−}-LDH/styrene–butadiene–styrene (SBS) modified asphalt implied that the asphalt molecules do not enter into the LDH interlayer galleries to form separated-phase structures. The different diffraction angles of Zn-Al-PMCA-LDH and Zn-Al-PMCA-LDH/SBS modified asphalt indicated that the asphalt molecules penetrated into the LDH interlayer galleries to form an expanded-phase structure. UV-Vis absorbance analyses showed that Zn-Al-PMCA-LDH was better able to block UV light due to the synergistic effects of PMCA and Zn-Al-LDH. Conventional physical tests and atomic force microscopy images of the SBS modified asphalt, Zn-Al-CO{sub 3}{sup 2−}-LDH/SBS modified asphalt and Zn-Al-PMCA-LDH/SBS modified asphalt before and after UV aging indicated that Zn-Al-PMCA-LDH improved the UV aging resistance of SBS modified asphalts.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Modelling safety of multistate systems with ageing components

An innovative approach to safety analysis of multistate ageing systems is presented. Basic notions of the ageing multistate systems safety analysis are introduced. The system components and the system multistate safety functions are defined. The mean values and variances of the multistate systems lifetimes in the safety state subsets and the mean values of their lifetimes in the particular safety states are defined. The multi-state system risk function and the moment of exceeding by the system the critical safety state are introduced. Applications of the proposed multistate system safety models to the evaluation and prediction of the safty characteristics of the consecutive “m out of n: F” is presented as well.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2018

AGES: Automated Gas Environment System for in situ neutron powder diffraction

High fluxes available at modern neutron and synchrotron sources have opened up a wide variety of in situ and operando studies of real processes using scattering techniques. This has allowed the user community to follow chemistry in the beam, which often requires high temperatures, gas flow, etc. In this paper, we describe an integrated gas handling system for the general-purpose powder diffraction beamline Powgen at the Spallation Neutron Source. The Automated Gas Environment System (AGES) allows control of both gas flow and temperature (room temperature to 850 °C), while measuring the partial pressure of oxygen and following the effluent gas by mass spectrometry, concurrent with neutron powder diffraction, in order to follow the structural evolution of materials under these conditions. The versatility of AGES is illustrated by two examples of experiments conducted with the system. In solid oxide fuel cell electrode materials, oxygen transport pathways in double perovskites PrBaCo 2 O 5+δ and NdBaCo 2 O 5+δ were elucidated by neutron diffraction measurements under atmosphere with oxygen partial pressures (pO 2 ) of 10 –1 to 10 –4 (achieved using mixtures of nitrogen and oxygen) and temperatures from 575 to 850 °C. In another example, the potential oxygen storage material La 1–x Sr x FeO 3 was measured under alternating flows of 15% CH 4 in N 2 and air (20% O 2 in N 2 ) at temperatures from 135 to 835 °C. As a result, from the oxygen stoichiometry, the optimal composition for oxygen storage was determined.

47 OTHER INSTRUMENTATION↗
DOE OSTI2019

Inter-digital capacitive sensor for evaluating cable jacket and insulation aging

An inter-digital capacitive (TDC) sensor has previously been used to measure dielectric properties of cable insulation polymer material when placed in direct contact with the insulation. Often cable insulation is covered by a polymer jacket. The dielectric properties of many cable jacket and insulation polymers are known to change due to thermal and radiation exposure-related damage. These dielectric properties frequently track with other measures of cable aging, such as tensile elongation-at-break and indenter modulus that have been broadly established as cable insulation polymer assessment methods. The external jacket of a cable is likely to have a different permittivity from the underlying insulation, and frequently the jacket material exhibits more severe damage than the insulation material due to environmental exposure. Because the jacket serves primarily to guard the cable during installation, as long as the underlying insulation condition is acceptable, the jacket condition is relatively unimportant in service. As part of a continuing program to develop and evaluate nondestructive examination methods that may be applied to cable condition assessment, a set of tools has been developed including (1) a parallel-plate sensor to directly measure the permittivity spectrum of flat sheet material and (2) an TDC and fixture to measure the effect of cable polymer dielectric property change on the sensor response. The TDC consists of two fork-like electrodes facing each other with the fork tines interspersed and separated by a small gap. The electrodes are printed on one side of a flexible substrate that can be conformed to the surface of a cylindrical cable, with tines parallel to the cable axis. The electrodes are connected to a broad-frequency-spectral impedance meter that senses the capacitance between the narrowly gapped electrode tines. This capacitance is known to vary as a function of the permittivity of any material in close proximity to the electrodes. By finite element modeling (FEM) and experimentation, this study investigates the effect of tine spacing and other design parameters associated with the TDC on the voltage (potential) distribution and electric field depth of penetration. The TDC measurement of an unshielded ethylene-propylene rubber (EPR)-insulated cable is shown to track with the degree of aging and quantities obtained by established methods. For jacketed cable systems, the TDC response is dominated by the jacket but, by analyzing measurements from TDC sensors with different depths-of-field penetration into the cable under test, the influence of the chlorinated polyethylene (CPE) cable jacket material degradation can be separated from an assessment of the cable insulation thereby enabling assessment of the insulation beneath/through the jacket.

Cable NDE, Interdigital Capacitance, Cable test↗
DOE OSTI2024

Analysis of differential scanning calorimetry data for aged plutonium

Differential scanning calorimetry data for samples of a 52 year old plutonium alloy with 3.3 at. % Ga that were heated beyond the melting point is analyzed using transition state theory to find activation energies for the δ to ε and ε to liquid phase transitions. A Bayesian statistical method involving a Gaussian process model is used to find mean values and confidence intervals for the activation energies. The activation energy for the δ to ε phase transition increases by 3.3 ± 3.8% per decade, relative to the case when all age related plutonium lattice point defects have been removed through annealing. The corresponding increase in activation energy for the ε to liquid transition is shown to be 7.1 ± 1.8% per decade. It is postulated that the change in activation energy with age for both phase transitions is caused, in part, by the accumulation of the same type of lattice point defects associated with the observed increase in elastic bulk modulus over time.

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

Steeper declines in forest photosynthesis than respiration explain age-driven decreases in forest growth

Significance Advancing our understanding of how and why forests dynamically change in their productivity is important to predict the future change. The traditional view of forest dynamics originated by Kira, Shidei, and Odum suggests a decline in net primary productivity [or gross primary productivity (GPP) − autotrophic respiration (R a )] in aging forests due to stabilized GPP and continuously increased R a . We found that, in contrast to the traditional view, both GPP and R a decline in aging forests while GPP decreases more rapidly than R a does, and thus generalize the alternative hypothesis initiated by Ryan and colleagues with a large dataset. We presented a new quantitative model to describe forest dynamics that can be incorporated into ecosystem models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Aging heat treatment design for Haynes 282 made by wire-feed additive manufacturing using high-throughput experiments and interpretable machine learning

Wire-feed additive manufacturing (WFAM) produces superalloys with complex thermal cycles and unique microstructures, often requiring optimized heat treatments. To address this challenge, we present a hybrid approach that combines high-throughput experiments, precipitation simulation, and machine learning to design effective aging conditions for the WFAM Haynes 282 superalloy. Our results demonstrate that the γ’ radius is the critical microstructural feature for strengthening Haynes 282 during post-heat treatment compared with the matrix composition and γ’ volume fraction. New aging conditions at 770°C for 50 hours and 730°C for 200 hours were discovered based on the machine learning model and were applied to enhance yield strength, bringing it on par with the wrought counterpart. This approach has significant implications for future AM alloy production, enabling more efficient and effective heat treatment design to achieve desired properties.

CALPHAD↗
DOE OSTI2011

THE DYNAMICAL DISTANCE, RR LYRAE ABSOLUTE MAGNITUDE, AND AGE OF THE GLOBULAR CLUSTER NGC 6266

The internal proper motion dispersion of NGC 6266 was measured using Hubble Space Telescope Wide Field Planetary Camera 2 images with an epoch difference of eight years. The dispersion was found to be 0.041 {+-} 0.001 arcsec century{sup -1}. This value was then equated to the cluster's radial velocity dispersion of 13.7 {+-} 1.1 km s{sup -1} to yield a distance to NGC 6266 of 7054 {+-} 583 pc. Based on this distance we find that the NGC 6266 RR Lyrae stars have M{sub V} = 0.51 {+-} 0.18 mag. This magnitude is in good agreement with that predicted by the M{sub V} versus [Fe/H] relation found by Benedict et al. Using an average [Fe/H] of -1.25 for NGC 6266, their relation predicts M{sub V} = 0.49 {+-} 0.06. Based on the RR Lyrae M{sub V} versus age relation determined by Chaboyer et al., we estimate that NGC 6266 has an age of 11.4 {+-} 2.2 Gyr.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2011

NONTHERMAL EMISSION FROM MIDDLE-AGED SUPERNOVA REMNANTS INTERACTING WITH MOLECULAR CLOUDS

Supernova remnants (SNRs) interacting with dense molecular clouds (MCs) are proven to be bright {gamma}-ray emitters by recent observations in the GeV-TeV band. We theoretically investigate the multiband radiative properties of the four middle-aged SNRs IC443, W51C, W28, and W44 with a time-dependent injection model. In the model, part of the SNR shell transports into a dense MC, with the other part of the shell evolving in a relatively tenuous interstellar medium. We find a broken power law with a break energy of {approx}3-40 GeV that must be imposed to reproduce the observed multiwavelength spectra for the four remnants. The results indicate that the observed {gamma}-ray spectra can be reproduced as a p-p interaction of the high-energy protons injected by the shell interacting with the MC with the dense matter, whereas the radio emission is produced via synchrotron radiation of the injected electrons from the other part of the shell for the four middle-aged SNRs.

79 ASTRONOMY AND ASTROPHYSICS↗