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DOE OSTI2024

Advancing the Performance of Lithium-Rich Oxides in Concert with Inherent Complexities: Domain-Selective Substitutions

Historically, modifications to Li- and Mn-rich (LMR) cathodes have been studied in relation to their efficacy in solving challenges such as oxygen loss and voltage fade, which are inherent to the activation process of these electrodes. However, even in the presence of these phenomena, well-optimized LMR cathodes show considerable promise as earth-abundant options, particularly if other barriers to implementation can be overcome or mitigated. As the complex mechanisms of LMR electrodes are known to stem from the local, chemical inhomogeneities that define the nanocomposite domain nature of these oxides, strategies aimed at manipulating the performance of activated electrodes, irrespective of voltage fade, through domain-selective modifications, could prove instructive. In this work, we use a novel synthesis process aimed at influencing the site occupancy of substituted Sn 4+ , as an example 4+ cation, into a Co-free Li 1.13 Mn 0.57(1–x) Sn 0.57x Ni 0.3 O 2 LMR oxide. We show that Sn 4+ can be selectively substituted into Li-rich environments. The consequences are revealed to be both chemical and morphological, and the domain-selective doping strategy provides a knob for directed control of the low state-of-charge impedance behavior. In conclusion, these results reveal new clues and insights with respect to further advancing the practical relevance of LMR cathode particles and electrodes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

LiNi0.8Mn0.1Co0.1O2 Thin Films Prepared by Polymer-Assisted Deposition for the Study of Cathode-Electrolyte Interphases in Lithium-Ion Batteries

High-nickel layered oxide cathodes such as LiNi0.8Mn0.1Co0.1O2 (NMC811) are critical for next-generation lithium-ion batteries (LIBs) due to their superior energy density and reduced reliance on cobalt. However, many Ni-rich cathodes suffer from rapid capacity fade and structural instability originating from complex interfacial reactions at the cathode-electrolyte interface. Traditional composite electrodes exhibit degradation mechanisms that are challenging to quantitatively understand due to additives, including binders and carbon black. In this study, we demonstrate a new synthesis approach for binder- and additive-free NMC811 thin films using polymer-assisted deposition (PAD). PAD-NMC811 are model thin-film cathodes for investigating interfacial phenomena that can be obscured in composite cathodes. Structural and chemical characterization by X-ray diffraction, soft X-ray absorption spectroscopy, and atomic force microscopy show that PAD-NMC811 films possess high phase purity, crystallinity, chemical homogeneity, and morphological uniformity. Electrochemical analyses using cyclic voltammetry and galvanostatic cycling revealed electrochemical behavior consistent with that of composite electrodes, along with a moderate capacity fade indicative of cathode-electrolyte interphase (CEI) formation. Our findings illustrate the effectiveness of PAD synthesis of thin films tailored for detailed mechanistic studies, which offer critical insights into CEI evolution and cathode degradation pathways.

25 ENERGY STORAGE↗

DOE OSTI2026

Prelithiated SiO x /Graphite-NMC811 Cells: Capacity Loss, Impedance Rise and Hidden Degradation Pathways Revealed Using Three-Electrode Diagnostics

Electrodes containing SiO x /graphite (Gr) materials are attractive as anodes for high-energy lithium-ion batteries. However, their mechanical deformation, electrochemical response, and impedance evolution during long-term cycling are strongly coupled, complicating accurate diagnosis of performance fade mechanisms. In this work, the behavior of electrochemically prelithiated SiO x /Gr anodes paired with NMC811 cathodes is systematically investigated using techniques that include in-situ dilatometry, three-electrode electrochemistry, and multiscale post-cycling microscopy. The SiO x /Gr electrode exhibits a maximum expansion of 49% upon lithiation to 10 mV vs Li + /Li, with 84% of the expansion and 91% of the capacity being reversible. In full cells, relatively stable cycling with only 12% capacity fade over 500 cycles is observed. Three-electrode experiments reveal cell-level impedance growth, which is dominated by the NMC811 cathode: the SiO x /Gr anode exhibits minimal net impedance rise and an initial impedance decrease at low potentials. Despite this apparent electrochemical stability, cross-sectional SEM, PFIB tomography, and cryo-STEM reveal irreversible anode thickening caused by the accumulation of an inorganic-rich solid electrolyte interphase (SEI) permeating the anode bulk. Electrode potential-shift analysis further demonstrates that Li + ions released from lithium reservoirs in the prelithiated anode mask true lithium inventory loss during aging. These results demonstrate that low-expansion SiO x /Gr anodes can simultaneously exhibit favorable cycling and impedance metrics while undergoing substantial, hidden degradation, underscoring the importance of electrode-resolved diagnostics for evaluating prelithiated silicon-based anodes.

25 ENERGY STORAGE↗

DOE OSTI2025

A Quasi-Ordered Mn-Rich Cathode with Highly Reversible Oxygen Anion Redox Chemistry

Anionic oxygen redox chemistry in Li-rich Mn-based layer oxide cathodes represents a transformative approach for boosting the energy density of next-generation lithium-ion batteries. However, conventional oxygen redox reactions often induce oxygen dimerization at high voltages, leading to irreversible lattice oxygen loss and a rapid voltage fade. Herein, we achieve highly reversible oxygen redox chemistry through a new quasi-ordered structural design that incorporates both intra- and interlayer cation disorder configurations. This unique structure significantly enhances lattice oxygen stability, effectively stabilizes oxidized oxygen, and inhibits the formation of peroxo- or superoxol-like species, thereby enabling anionic redox reactions to proceed reversibly even at deep delithiation states. The quasi-ordered design mitigates irreversible phase transitions and preserves the structural integrity throughout extended cycling. Consequently, the proposed cathode demonstrates exceptional cyclability with negligible capacity and voltage fade, retaining 99% capacity and 98% average voltage after long-term cycling. Finally this work provides fresh insights into addressing issues related to lattice oxygen instabilities and reforming strategies for developing long-life, high-energy-density anionic redox cathode materials for advanced batteries.

chemical structure↗

DOE OSTI2024

Ultrastable cathodes enabled by compositional and structural dual-gradient design

Cathodes for next-generation batteries are pressed for higher voltage operation (≥4.5 V) to achieve high capacity with long cyclability and thermal tolerance. Current cathodes fail to meet these requirements owing to structural and electrochemical strains at high voltages, leading to fast capacity fading. Here, in this work, we present a cathode with a coherent architecture ranging from ordered to disordered frameworks with concentration gradient and controllable Ni oxidation activities, which can overcome voltage ceilings imposed by existing cathodes. This design enables simultaneous high-capacity and high-voltage operation at 4.5 V without capacity fading, and up to 4.7 V with negligible capacity decay. Multiscale diffraction and imaging techniques reveal the disordered surface is electrochemically and structurally indestructible, preventing surface parasitic reactions and phase transitions. Structural coherence from ordering to disordering limits lattice parameter changes, mitigating lattice strain and enhancing morphological integrity. The dual-gradient design also notably improves thermal stability, driving the advancement of high-performance cathode materials.

36 MATERIALS SCIENCE↗

NASA NTRS1971

Investigation of line-of-sight propagation in dense atmosphere, phase 3, part 1

The investigation of microwave absorption in the 1 to 10 GHz frequency band by the Jovian atmosphere has continued, and an estimate of the strength of signal fading at these frequencies due to layers of turbulence in Jupiter's atmosphere is given. The microwave absorption due to gaseous ammonia is estimated both in terms of a power loss in dB/km, and in total power loss in dB for slant-path communication with a probe at altitudes down to pressures of several tens of atmospheres. The graphs indicate a frequency-squared scaling of the absorption, and appreciable losses at altitudes where the pressure is several atmospheres. An estimate of turbulence strength is given. This may turn out to be quite crude considering the absence of any relevant data. A planetary scaling law which appears to hold reasonably well for Earth to Venus, is extrapolated to Jupiter. No reasonable modifications of the estimate can alter the conclusion that direct-path fading is negligible for pressure regimes up to 20 atm.

Dewolf, D. A.↗

NASA NTRS1970

Simulation of the TDRS multipath environment

Design principles and implementation methods are discussed for simulating the propagation path between a tracking and data relay satellite and a mission spacecraft. The emphasis is on multipath and Doppler simulation but additive disturbances are also considered. The recommended form of the simulator is fed separately with the unmodulated carrier, the unmodulated subcarriers (or spread-spectrum components) and the data signals. The perturbations are also introduced separately; then successive modulation operations are performed. The simulator is segmented into elements that perform the various functions of direct and specular multipath, diffuse fading, Doppler shift and delay spread. Delay spreads are realized by discrete delays operating on baseband signals. Doppler simulation and ionospheric or diffuse multipath fading are applied to individual paths before or after modulation of the carrier by delayed baseband signals. Block diagrams are presented on how the different elements are combined to create a complete channel simulator.

Baghdady, E. J.↗

NASA NTRS1973

Low data rate digital space communications

The low available transmitter power and the large frequency uncertainty constrain the data rate to be low. An all-digital communication receiver is proposed, and its feasibility is established. Although coherent systems should be used whenever practical, the noncoherent MFSK system is more suitable for very low data rates. The effect of Rician fading on the performance of MFSK receiver is studied. Fading characteristics of the Venus channel are examined based on the exponential model and available experimental data on the Venus atmosphere. Because of the requirement of high communication efficiency, three codes are evaluated and compared. The rapidly varying phase error at low data rate has great effects on the tracking loop behaviors which are examined by extensive computer study of the phase plane trajectories.

Chen, C. H.↗

NASA NTRS1974

Channel simulation for optical communication systems

A technique is reported for simulating the signal fading that will be experienced by typical optical communication systems. The desired irradiance or amplitude fading statistics can be simulated by incorporating a linearized optical modulator subsystem between the transmitter and receiver. This technique has been implemented in the design and construction of a laboratory channel simulator. The design of the processing electronics is discussed along with the results of tests performed for each mode of operation.

Tycz, M.↗

NASA NTRS1974

Convolutional code performance in planetary entry channels

The planetary entry channel is modeled for communication purposes representing turbulent atmospheric scattering effects. The performance of short and long constraint length convolutional codes is investigated in conjunction with coherent BPSK modulation and Viterbi maximum likelihood decoding. Algorithms for sequential decoding are studied in terms of computation and/or storage requirements as a function of the fading channel parameters. The performance of the coded coherent BPSK system is compared with the coded incoherent MFSK system. Results indicate that: some degree of interleaving is required to combat time correlated fading of channel; only modest amounts of interleaving are required to approach performance of memoryless channel; additional propagational results are required on the phase perturbation process; and the incoherent MFSK system is superior when phase tracking errors are considered.

Modestino, J. W.↗

NASA NTRS1974

Burst-error characteristics of the equatorial transionospheric channel

Analyses of AGC analog data from the Small Astronomy Satellite (SAS) at VHF (136 MHz) have shown amplitude fluctuations in the signals received at several equatorial tracking sites operated by NASA. Errors in data are shown to increase markedly for nighttime satellite passes around the periods of the two equinoxes as compared to the errors observed during other periods. Qualitative and quantitative correlations are established between the ionospheric scintillation phenomenon and the occurrence of errors. Strong time and geographic cause-and-effect relationships are established by determining the statistical correlation between scintillation indices and bit error rates. Detailed analyses of the AGC fading statistics and the fine grain error statistics, such as the block-error distribution and the bit-error autocorrelation function, establish the strong correlation between deep fades and their effects on the burst error structure associated with the transionospheric channel and the communication receiver being employed.

Blank, H. A.↗

NASA NTRS1975

Phase and amplitude scintillations at 9.6 GHz on an elevated path

Deep fading, e.g., greater than 40 dB, was observed at 9.6 GHz on a 150 km path with terminals at 3025 and 3300 m elevations and with no significant illumination of the earth's surface. Fades at two antennas separated horizontally by 100 m were largely uncorrelated. Phase variability was also measured and is presented in terms of spectra and coherency between antennas with 10 m and 100 m horizontal spacing.

Thompson, M. C.↗

NASA NTRS1977

Prediction of attenuation of the 28 GHz COMSTAR beacon signal using radar and measured rain drop spectra

Disdrometer measurements and radar reflectivity measurements were injected into a computer program to estimate the path attenuation of the signal. Predicted attenuations when compared with the directly measured ones showed generally good correlation on a case by case basis and very good agreement statistically. The utility of using radar in conjunction with disdrometer measurements for predicting fade events and long term fade distributions associated with earth-satellite telecommunications is demonstrated.

Goldhirsh, J.↗

NASA NTRS1977

ATS-6 ascending - Near horizon measurements over water at 30 GHz

The return of the ATS-6 satellite to a western longitude during the fall of 1976 presented a unique opportunity to perform low-angle-of-elevation measurements at 30 GHz. For this purpose a receiver using a 1.5 m antenna was set up at Port Aransas, Texas, resulting in a propagation path entirely over water. The 30 GHz beacon was monitored daily for at least one hour from 8 September to 21 September 1976. During the time the elevation angle changed from 1.5 to 17.3 deg, the mean attenuation decreased from 20 to 2 dB and the standard deviation from over 6 dB to less than .2 dB. The deep fades at angles below 4 deg show significantly sharper nulls than peaks on a log scale. Spectra of the log amplitude fluctuations vary as the (-8/3) power of the spectral frequency in the limit. A flattening is noticeable at the low frequencies. A precipitation even at 8.5 deg elevation produced a 16 dB fade and significantly increased the variance.

Vogel, W. J.↗

NASA NTRS1979

Determination of the time delay in the case of two-path propagation on the basis of the attenuation characteristics for two adjacent frequencies

Pronounced fading occurring in the line of sight radio links at frequencies below 10 GHz can be traced to the effects of multipath propagation. Modulation disturbances depend on travel time differences between the direct wave and the wave which is reflected at atmospheric layers. A method described for the determination of the time delay is based on an indirect approach which utilizes the difference in fading at various frequencies. The method was employed in measurements involving a distance of 181 km. The results obtained in the measurement are discussed.

Gilroi, H. G.↗

NASA NTRS1977

ATS-6 ascending: Near horizon measurements over water at 30 GHz

The return of the ATS 6 satellite to a western longitude during the fall of 1976 presented a unique opportunity to perform low angle of elevation measurements at 30 GHz. For this purpose a receiver using a 1.5 m antenna was set up at Port Aransas, Texas, resulting in a propagation path entirely over water. The 30 GHz beacon was monitored daily for at least one hour from 8 September 1976 to 21 September 1976. During the time the elevation angle changed from 1.5 deg to 17.3 deg, the mean attenuation decreased from 20 dB to 2 dB and the standard deviation from over 6 dB to less than .2 dB. The deep fades at angles below 4 deg show significantly sharper nulls than peaks on a log scale. Spectra of the log amplitude fluctuations vary as the (-8/3) power of the spectral frequency in the limit. A flattening is noticeable at the low frequencies. A precipitation event at 8.5 deg elevation produced a 16 dB fade and significantly increased the variance.

Vogel, W. J.↗

NASA NTRS1980

Radar estimation of slant path rain attenuation at frequencies above 10 GHz and comparisons with measured multi-season results

Techniques and results pertaining to estimating Earth satellite path rain attenuation events and statistics using radar at nonattenuating wavelengths are presented. The radar formulation and beam scanning methods are described and the procedure for relating the radar measured Rayleigh reflectivity to the high frequency Mie attenuation coefficient are given. Examples of radar derived single terminal statistics and estimation criteria as they relate to path angle and frequency are reviewed. Radar derived space diversity statistics and their dependence on terminal spacing and frequency are described. Site diversity performance curves obtained by radar and radiometry are compared with each other demonstrating the utility of radar methods. Results of a multi-year experiment to test, refine, and establish accuracies of radar methods for arriving at estimates of rain attenuation along an Earth-satellite path are discussed. Comparisons of measured and radar estimated fade events are presented and found to be good. Comparisons of cumulative fade distributions show agreement to be excellent giving an rms deviation of 1 dB.

Goldhirsh, J.↗

NASA NTRS1981

A model for simulation and processing of radar images

A model for recording, processing, presentation, and analysis of radar images in digital form is presented. The observed image is represented as having two random components, one which models the variation due to the coherent addition of electromagnetic energy scattered from different objects in the illuminated areas. This component is referred to as fading. The other component is a representation of the terrain variation which can be described as the actual signal which the radar is attempting to measure. The combination of these two components provides a description of radar images as being the output of a linear space-variant filter operating on the product of the fading and terrain random processes. In addition, the model is applied to a digital image processing problem using the design and implementation of enhancement scene. Finally, parallel approaches are being employed as possible means of solving other processing problems such as SAR image map-matching, data compression, and pattern recognition.

Stiles, J. A.↗