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DOE OSTI2024

Mechanochemically Robust LiCoO 2 with Ultrahigh Capacity and Prolonged Cyclability

Pushing intercalation-type cathode materials to their theoretical capacity often suffers from fragile Li-deficient frameworks and severe lattice strain, leading to mechanical failure issues within the crystal structure and fast capacity fading. This is particularly pronounced in layered oxide cathodes because the intrinsic nature of their structures is susceptible to structural degradation with excessive Li extraction, which remains unsolved yet despite attempts involving elemental doping and surface coating strategies. Herein, a mechanochemical strengthening strategy is developed through a gradient disordering structure to address these challenges and push the LiCoO 2 (LCO) layered cathode approaching the capacity limit (256 mAh g -1 , up to 93% of Li utilization). This innovative approach also demonstrates exceptional cyclability and rate capability, as validated in practical Ah-level pouch full cells, surpassing the current performance benchmarks. Comprehensive characterizations with multiscale X-ray, electron diffraction, and imaging techniques unveil that the gradient disordering structure notably diminishes the anisotropic lattice strain and exhibits high fatigue resistance, even under extreme delithiation states and harsh operating voltages. Consequently, this designed LCO cathode impedes the growth and propagation of particle cracks, and mitigates irreversible phase transitions. In conclusion, this work sheds light on promising directions toward next-generation high-energy-density battery materials through structural chemistry design.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Two-Dimensional Electronic Spectroscopy of the Far-Red-Light Photosystem II Reaction Center

Understanding the role of specific pigments in primary energy conversion in the photosystem II (PSII) reaction center has been impeded by the spectral overlap of its constituent pigments. When grown in far-red light, some cyanobacteria incorporate chlorophyll-f and chlorophyll-d into PSII, relieving the spectral congestion. Here we employ two-dimensional electronic spectroscopy to study PSII at 77 K from Synechococcus sp. PCC 7335 cells that were grown in far-red light (FRL-PSII). We observe the formation of a radical pair within ~3 ps that we assign to Chl D1 •– P D1 •+ . While Pheo D1 is thought to act as the primary electron acceptor in PSII from cells grown in visible light, we see no evidence of its involvement, which we attribute to its reduction by dithionite treatment in our samples. Our work demonstrates that primary charge separation occurs between Chl D1 and P D1 in FRL-PSII, suggesting that P D1 /P D2 may play an underappreciated role in PSII’s charge separation mechanism.

14 SOLAR ENERGY↗

DOE OSTI2023

Reinforcement Learning Approach to Cybersecurity in Space (RELACSS)

Securing satellite groundstations against cyber-attacks is vital to national security missions. However, these cyber threats are constantly evolving. As vulnerabilities are discovered and patched, new vulnerabilities are discovered and exploited. In order to automate the process of discovering existing vulnerabilities and the means to exploit them, a reinforcement learning framework is presented in this report. We demonstrate that this framework can learn to successfully navigate an unknown network and detect nodes of interest despite the presence of a moving target defense. The agent then exfiltrates a file of interest from the node as quickly as possible. This framework also incorporates a defensive software agent that learns to impede the attacking agents progress. This setup allows for the agents to work against each other and improve their abilities. We anticipate that this capability will help uncover unforeseen vulnerabilities and the means to mitigate them. The modular nature of the framework enables users to swap out learning algorithms and modify the reward functions in order to adapt the learning tasks to various use cases and environments. Several algorithms, viz., tabular Q learning, deep Q networks, proximal policy optimization, advantage actor-critic, generative adversarial imitation learning, are explored for the agents and the results highlighted. The agent learns to solve the tasks in a light-weight abstract environment. Once the agent learns to perform sufficiently well, it can be deployed in a minimega virtual machine environment (or a real network) with wrappers that map abstract actions to software commands. The agent also uses a local representation of the actions called a ‘slot-mechanism’. This allows the agent to learn in a certain network and generalize it to different networks. The defensive agent learns to predict the actions taken by an offensive agent and uses that information to anticipate the threat. This information can then either be used to raise an alarm or to take actions to thwart the attack. We believe that with the appropriate reward design, a representative environment, and action set, this framework can be generalized to tackle other cybersecurity tasks. By sufficiently training these agents, we can anticipate vulnerabilities leading to robust future designs. We can also deploy automated defensive agents that can help secure satellite groundstation and their vital national security missions.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

DOE OSTI2022

Carbon-Binder Weight Loading Optimization for Improved Lithium-Ion Battery Rate Capability

Battery performance is strongly correlated with electrode microstructure and weight loading of the electrode components. Among them are the carbon-black and binder additives that enhance effective conductivity and provide mechanical integrity. However, these both reduce effective ionic transport in the electrolyte phase and reduce energy density. Therefore, an optimal additive loading is required to maximize performance, especially for fast charging where ionic transport is essential. Such optimization analysis is however challenging due to the nanoscale imaging limitations that prevent characterizing this additive phase and thus quantifying its impact on performance. Herein, an additive-phase generation algorithm has been developed to remedy this limitation and identify percolation threshold used to define a minimal additive loading. Improved ionic transport coefficients from reducing additive loading has been then quantified through homogenization calculation, macroscale model fitting, and experimental symmetric cell measurement, with good agreement between the methods. Rate capability test demonstrates capacity improvement at fast charge at the beginning of life, from 37% to 55%, respectively for high and low additive loading during 6C CC charging, in agreement with macroscale model, and attributed to a combination of lower cathode impedance, reduced electrode tortuosity and cathode thickness.

25 ENERGY STORAGE↗

DOE OSTI2024

Carbon-Binder Optimization for Lithium-Ion Battery Extreme Fast Charge

carbon-binder additives↗

NASA NTRS2011

Lunar Ion Transport Near Magnetic Anomalies: Possible Implications for Swirl Formation

The bright swirling features on the lunar surface in areas around the Moon but most prominently at Reiner Gamma, have intrigued scientists for many years. After Apollo and later Lunar Prospector (LP} mapped the Lunar magnetic fields from orbit, it was observed that these features are generally associated with crustal magnetic anomalies. This led researchers to propose a number of explanations for the swirls that invoke these fields. Prominent among these include magnetic shielding in the form of a mini-magnetosphere which impedes space weathering by the solar wind, magnetically controlled dust transport, and cometary or asteroidal impacts that would result in shock magnetization with concomitant formation ofthe swirls. In this presentation, we will consider another possibility, that the ambient magnetic and electric fields can transport and channel secondary ions produced by micrometeorite or solar wind ion impacts. In this scenario, ions that are created in these impacts are under the influence of these fields and can drift for significant distances before encountering the magnetic anomalies when their trajectories are disrupted and concentrated onto nearby areas. These ions may then be responsible for chemical alteration of the surface leading either to a brightening effect or a disruption of space weathering processes. To test this hypothesis we have run ion trajectory simulations that show ions from regions about the magnetic anomalies can be channeled into very small areas near the anomalies and although questions remain as to nature of the mechanisms that could lead to brightening of the surface it appears that the channeling effect is consistent with the existence of the swirls.

Keller, J. W.↗

DOE OSTI2021

Lettuce ( Lactuca sativa ) productivity influenced by microbial inocula under nitrogen-limited conditions in aquaponics

The demand for food will outpace productivity of conventional agriculture due to projected growth of the human population, concomitant with shrinkage of arable land, increasing scarcity of freshwater, and a rapidly changing climate. While aquaponics has potential to sustainably supplement food production with minimal environmental impact, there is a need to better characterize the complex interplay between the various components (fish, plant, microbiome) of these systems to optimize scale up and productivity. Here, we investigated how the commonly-implemented practice of continued microbial community transfer from pre-existing systems might promote or impede productivity of aquaponics. Specifically, we monitored plant growth phenotypes, water chemistry, and microbiome composition of rhizospheres, biofilters, and fish feces over 61-days of lettuce (Lactuca sativa var. crispa) growth in nitrogen-limited aquaponic systems inoculated with bacteria that were either commercially sourced or originating from a pre-existing aquaponic system. Lettuce above- and below-ground growth were significantly reduced across replicates treated with a pre-existing aquaponic system inoculum when compared to replicates treated with a commercial inoculum. Reduced productivity was associated with enrichment in specific bacterial genera in plant roots, including Pseudomonas, following inoculum transfer from pre-existing systems. Increased productivity was associated with enrichment of nitrogen-fixing Rahnella in roots of plants treated with the commercial inoculum. Thus, we show that inoculation from a pre-existing system, rather than from a commercial inoculum, is associated with lower yields. Further work will be necessary to test the putative mechanisms involved.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2006

Assessment of Bulk Absorber Properties for Multi-Layer Perforates in Porous Honeycomb Liners

CONTINUING progress in materials technology provides potential for improved acoustic liners for attenuating broadband fan noise emissions from aircraft engine nacelles. Conventional liners (local-reacting perforate-over-honeycomb structures) provide significant narrow-band attenuation, but limited attenuation over wide bandwidths. Two approaches for increasing attenuation bandwidth are to (1) replace the honeycomb structure with bulk material, or (2) cascade multiple layers of perforate/honeycomb structures. Usage of the first approach is limited because of mechanical and maintenance reasons, while multi-layer liners are limited to about three layers because of their additional mechanical complexity, depth and weight. The current research concerns a novel approach reported by the University of Cincinnati, in which a single-layer conventional liner is converted into an extended-reaction, broadband absorber by making the honeycomb core structure porous. This modified single-layer liner requires no increase in depth and weight, and minimal increase in mechanical complexity. Langley has initiated research to identify potential benefits of liner structures with porous cell walls. This research has two complementary goals: (1) develop and validate experimental techniques for treating multi-layer perforates (representative of the internal cells of a liner with porous cell walls) as 1-D bulk materials, and (2) develop analytical approaches to validate this bulk material assumption. If successful, the resultant model can then be used to design optimized porous honeycomb liners. The feasibility of treating an N-layer perforate system (N porous plates separated by uniform air gaps) as a one-dimensional bulk absorber is assessed using the Two-Thickness Method (TTM), which is commonly used to educe bulk material intrinsic acoustic parameters. Tests are conducted with discrete tone and random noise sources, over an SPL range sufficient to determine the nonlinearity of the test specimens, for test specimens consisting of 5, 10 and 15% porous plates. Measured impedances for two liner thicknesses (e.g., 12 and 24 layers) are used as input to the TTM to determine the characteristic impedance and propagation constant that characterize these liners as bulk absorbers. These parameters are then used to calculate the predicted impedance of liners with different thicknesses (e.g., 36 layers), and a comparison of predicted and measured impedances for these other thicknesses is used to determine the efficacy of this approach. Finally, an independent method is used to educe the propagation constant for a single representative sample, and excellent comparison between the results for this method and those for the TTM provides increased confidence in the results achieved with the TTM. In general, the results demonstrate these multi-layer perforates can be acceptably treated as bulk absorbers.

Jones, Michael G.↗

DOE OSTI2024

Dynamic Structural Change of Plant Epidermal Cell Walls under Strain

Abstract The molecular foundations of epidermal cell wall mechanics are critical for understanding structure–function relationships of primary cell walls in plants and facilitating the design of bioinspired materials. To uncover the molecular mechanisms regulating the high extensibility and strength of the cell wall, the onion epidermal wall is stretched uniaxially to various strains and cell wall structures from mesoscale to atomic scale are characterized. Upon longitudinal stretching to high strain, epidermal walls contract in the transverse direction, resulting in a reduced area. Atomic force microscopy shows that cellulose microfibrils exhibit orientation‐dependent rearrangements at high strains: longitudinal microfibrils are straightened out and become highly ordered, while transverse microfibrils curve and kink. Small‐angle X‐ray scattering detects a 7.4 nm spacing aligned along the stretch direction at high strain, which is attributed to distances between individual cellulose microfibrils. Furthermore, wide‐angle X‐ray scattering reveals a widening of (004) lattice spacing and contraction of (200) lattice spacing in longitudinally aligned cellulose microfibrils at high strain, which implies longitudinal stretching of the cellulose crystal. These findings provide molecular insights into the ability of the wall to bear additional load after yielding: the aggregation of longitudinal microfibrils impedes sliding and enables further stretching of the cellulose to bear increased loads.

59 BASIC BIOLOGICAL SCIENCES↗

NASA NTRS2007

Reliability Effects of Surge Current Testing of Solid Tantalum Capacitors

Solid tantalum capacitors are widely used in space applications to filter low-frequency ripple currents in power supply circuits and stabilize DC voltages in the system. Tantalum capacitors manufactured per military specifications (MIL-PRF-55365) are established reliability components and have less than 0.001% of failures per 1000 hours (the failure rate is less than 10 FIT) for grades D or S, thus positioning these parts among electronic components with the highest reliability characteristics. Still, failures of tantalum capacitors do happen and when it occurs it might have catastrophic consequences for the system. This is due to a short-circuit failure mode, which might be damaging to a power supply, and also to the capability of tantalum capacitors with manganese cathodes to self-ignite when a failure occurs in low-impedance applications. During such a failure, a substantial amount of energy is released by exothermic reaction of the tantalum pellet with oxygen generated by the overheated manganese oxide cathode, resulting not only in destruction of the part, but also in damage of the board and surrounding components. A specific feature of tantalum capacitors, compared to ceramic parts, is a relatively large value of capacitance, which in contemporary low-size chip capacitors reaches dozens and hundreds of microfarads. This might result in so-called surge current or turn-on failures in the parts when the board is first powered up. Such a failure, which is considered as the most prevalent type of failures in tantalum capacitors [I], is due to fast changes of the voltage in the circuit, dV/dt, producing high surge current spikes, I(sub sp) = Cx(dV/dt), when current in the circuit is unrestricted. These spikes can reach hundreds of amperes and cause catastrophic failures in the system. The mechanism of surge current failures has not been understood completely yet, and different hypotheses were discussed in relevant literature. These include a sustained scintillation breakdown model [1-3]; electrical oscillations in circuits with a relatively high inductance [4-6]; local overheating of the cathode [5,7, 8]; mechanical damage to tantalum pentoxide dielectric caused by the impact of MnO2 crystals [2,9, 10]; or stress-induced-generation of electron traps caused by electromagnetic forces developed during current spikes [11]. A commonly accepted explanation of the surge current failures is that at unlimited current supply during surge current conditions, the self-healing mechanism in tantalum capacitors does not work, and what would be a minor scintillation spike if the current were limited, becomes a catastrophic failure of the part [l, 12]. However, our data show that the scintillation breakdown voltages are significantly greater that the surge current breakdown voltages, so it is still not clear why the part, which has no scintillations, would fail at the same voltage during surge current testing (SCT).

Teverovsky, Alexander↗

DOE OSTI2022

Investigation of SiO x anode fading mechanism with limited capacity cycling

Silicon suboxide (SiO x ) is one of the promising anode materials for the next-generation lithium-ion batteries. However, SiO x has a severe capacity fading problem during cycling. It is thus desired to investigate the detailed fading mechanisms of SiO x anode materials. In this study, limited capacity cycling was employed to examine the electrochemical behaviors of the SiO x anode, and the lithiation/delithiation cycling was limited within a range of 10% theoretical capacity. This strategy minimizes the volume variation of SiO x materials upon charging/discharging, which helps to reveal their decay factors other than volume fluctuation. It is demonstrated that the instability of the SiO x surface during cycling was likely a parallel factor of active material fading, which seems to cause unfavored electrode interface rearrangements with lowered electric conductivity.

electric vehicles↗

DOE OSTI2026

Electro-chemo-mechanically Driven Ni Exsolution from (Pr,Ce,Ni)O 2−δ : Controlled Nucleation Density and Enhanced Electrode Kinetics

In situ exsolution of metal nanoparticles is a promising strategy to prepare electrocatalysts with enhanced activity and resistance to agglomeration for efficient chemical transformations and energy conversion. Achieving a high nucleation density of nanoparticles under mild conditions and understanding how to tailor the process is important for performance of these electrodes in electrochemical cells. In this work, we demonstrate facile exsolution of Ni nanoparticles using fluorite-structured (Pr,Ce)O 2−δ as the support oxide, driven by electrochemical potential and aided by the metastability of Ni in the solid solution (elastic driving force). We prepare single-phase oriented thin films of (Pr,Ce,Ni)O 2−δ (NPCO) on (Zr,Y)O 2−δ (YSZ) substrates by pulsed laser deposition. With the aid of a high-throughput electrochemical cell that provides a lateral gradient in Nernst voltage, we apply in situ near-ambient pressure synchrotron X-ray photoelectron spectroscopy and ex situ atomic force microscopy to investigate the impact of electrochemical potential on Ni nucleation density. We find that metallic Ni can be successfully exsolved at 550 °C upon cathodic biasing in 20 mTorr O 2 , and its nucleation density increases with increasing electrochemical driving force/decreasing oxygen chemical potential. We further evaluate the electrochemical performance under highly reducing (fuel electrode) conditions by electrochemical impedance spectroscopy. With the exsolved Ni nanoparticles, the surface exchange coefficient of the NPCO is found to be ∼4× higher than for PCO without exsolution. This work confirms mixed conducting fluorites as beneficial host lattices for facile transition-metal exsolution and suggests the possibility for constructing an all ceria-based electrochemical cell with PCO serving as both the cathode and the anode.

36 MATERIALS SCIENCE↗

NASA NTRSDate not supplied

Investigating Material Behavior in Atmospheric Entry Conditions: Arc-Jet Testing Insights from Meteorite Ablation to High-Temperature Coatings.

Arc-jet testing is an indispensable tool in elucidating the complex interactions materials undergo when subjected to the extreme thermal and mechanical stresses of atmospheric entry. By replicating these harsh conditions, arc-jets enable researchers to explore critical phenomena such as ablation, melting, and spallation, generating invaluable data that informs the development of sophisticated, physics-based models. These models are pivotal not only in predicting material performance for spacecraft re-entry systems but also in assessing the threat posed by celestial bodies as they encounter Earth’s atmosphere. One of the leading facilities for such investigations is the Hypersonic Materials Environmental Test System (HyMETS) at NASA’s Langley Research Center. A pioneering test campaign conducted at HyMETS focused on unraveling the ablation mechanisms of an ordinary chondrite meteorite (Tamdakht H5) and a terrestrial analog (basalt). These studies unveiled distinct material behaviors: Tamdakht demonstrated a remarkably stable melt flow, with mass loss primarily driven by the volatilization of elements such as iron and sodium, whereas basalt exhibited more aggressive surface degradation due to the rapid decomposition of hydrated minerals, culminating in significant spallation and surface material ejection. Beyond meteorite analysis, HyMETS has also been integral in the exploration of advanced Thermal Protection Systems (TPS) such as Phenolic Impregnated Carbon Ablator (PICA), a material with extensive flight heritage in missions like Stardust, Mars Science Laboratory, Mars 2020, and Osiris-REx. PICA, when coated with NuSil CV-1144-0—a polysiloxane resin designed to prevent particle shedding—undergoes a remarkable transformation upon heating. The resin pyrolyzes to form a thin, oxidation-resistant silicon oxycarbide layer that profoundly influences the material’s thermal response through a sophisticated four-stage process. Initially, the silicon oxycarbide acts as a formidable barrier, impeding reactive interactions with the PICA char and effectively suppressing surface temperature rise and material recession. However, as the heating persists, the protective layer decomposes via carbothermal reduction, exposing the underlying char, which in turn leads to a dramatic spike in surface temperature and accelerated material erosion. In the final stage, equilibrium is reached, with recession rates aligning with those of the virgin material. This intricate understanding of PICA-NuSil behavior under extreme conditions offers valuable insights, enhancing material response models and advancing the development of next-generation TPS for space exploration.

Chemistry↗

DOE OSTI2020

Bi-cross validation of spectral clustering hyperparameters

One challenge impeding the analysis of terabyte scale X-ray scattering data from the Linac Coherent Light Source (LCLS) is determining the number of clusters required for the execution of traditional clustering algorithms. Here, we demonstrate that the previous work using bi-cross validation to determine the number of singular vectors directly maps to the spectral clustering problem of estimating both the number of clusters and hyperparameter values. Here by applying this method to LCLS X-ray scattering data enables the identification of dropped shots without manually setting boundaries on detector fluence and provides a path toward identifying rare and anomalous events.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2020

An Overview of R and D on Retrievability and Retrieval Technology in Germany - 20462

Retrievability is a term that is included in most radioactive waste management programs around the world. Although national definitions vary, the overall understanding of retrievability concerns the ability to recover waste packages from the repository mine after their emplacement. Different countries may implement retrievability in very different ways, ranging from a built-in reversibility into the emplacement process to the stipulation that retrievability may in no way impede passive safety in the post-closure phase. Germany takes a middle course such that retrievability in a HLW repository (repository for high level radioactive waste) may have no significant detrimental effect on passive safety. In Germany, the current siting process considers rock salt, clay rock, and crystalline rock as potential host rocks. Therefore, Research and Development (R and D) has been investigating repository concepts and retrievability in all host rocks. After introduction of retrievability in 2010, existing repository concepts were modified to facilitate retrieval. The changes made comprised, for example, equipping boreholes with steel liners, developing new technologies, and modifying existing emplacement devices. Apart from retrieval of HLW, retrieval of other wastes from underground repositories that were designed and operated without retrievability in mind, poses major technical and scientific challenges. Currently, studies are under way to investigate the feasibility and costs of partial retrieval of waste from an underground repository for hazardous and highly toxic waste in France, Stocamine. With regard to retrieval, the rock-mechanical conditions are deteriorating rapidly, so time is of the essence. In the Asse II mine in Germany, about 126,500 waste casks with low and intermediate level waste await retrieval. The repository mine suffers from difficult rock-mechanical conditions and inflow of brine, locally into emplacement areas. The Federal Company for Radioactive Waste Disposal (BGE) is legally required to retrieve all wastes from the Asse. Due to the specific challenges, R and D is needed to develop technical solutions for the safe retrieval from each of the emplacement chambers. R and D on retrievability and retrieval technology does not only address challenges in radioactive or toxic waste retrieval but may also help to germinate innovation to better master complex underground situations in general, e.g. in deep mining, tunneling, or repository construction. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NASA NTRSDate not supplied

A Flat-Panel 8x8 Sequentially Rotated Wideband Microstrip Patch Phased Array Antenna for K/Ka-band 6U CubeSat Communications Applications

Flat-panel electronically-scanned phased arrays have recently become a mainstream technology in the areas of radar and satellite applications, particularly due to their low profile and not having to steer the beams mechanically, both of which helps in realizing a lightweight phased array solution that also occupies a smaller volume. Typically for satellite applications, circularly polarized element radiators are often employed in order to deal with the signal fading problem. In this project, the main objective was to design a flat-panel phased array solution for 6U CubeSat communication applications. As for the required specifications, the array should have two operating bands: 22.55–23.55 GHz and 25.5–27.5 GHz, which span part of the K and Ka bands. For both these bands, the panel should be able to radiate dual circular polarization, in both transmit and receive modes, and with a stable gain performance. Since the individual bands are very closely spaced, it was realized that a single wideband design would be a better solution than a closely spaced dual-band design. Thus, a stacked microstrip patch configuration was selected for the element radiator design, which is known to be wideband. Now, it is rather difficult to realize both wide impedance and axial ratio bandwidths simultaneously, and at high frequencies, without complicating the element stacked patch design.. As a result, a sequential rotation technique wasemployed to significantly improves the axial ratio bandwidth and circular polarization purity of an array, all the while improving the pattern symmetry (P. S. Hall, “Application of Sequential Feeding to Wide Bandwidth, Circularly Polarised Microstrip Patch Arrays,” IEE Proc. H (Microw., Antennas Propag.), vol. 136, no. 5, pp. 390–398, Oct. 1989). The designed element radiator is a circularly-polarized probe-fed stacked patch antenna, which has a 10-dB matching bandwidth of 22.3– 30 GHz, with only a 5.14% axial ratio bandwidth around the center frequency of the required band, i.e., ~25 GHz. However, the resulting array demonstrates a very low axial ratio (≪ 3 dB) over the entire bandwidth, due to the application of the sequential rotation technique. The 8×8 array was able to scan up to ±51° and ±40° at frequencies 23.05 GHz and 26.5 GHz (center frequencies of the lower and upper bands), respectively, while maintaining a ≤ 3 dB axial ratio and a ≤ 3 dB gain drop from the corresponding peak broadside value at both the principle and the diagonal radiation planes. The designed layout for the 8×8 phased array prototype is shown in Fig. 1, which is currently undergoing fabrication and RF assembly. The antenna will be tested in the far-field anechoic chambers of the Antenna and Microwave Laboratory (AML) at San Diego State University and at NASA Glenn Research Center (GRC).

5G↗

DOE OSTI2025

Synthetic Accessibility and Sodium Ion Conductivity of the Na8–x A x P2O9 (NAP) High-Temperature Sodium Superionic Conductor Framework

Advancement of solid-state electrolytes (SSEs) for all solid-state batteries typically focuses on modification of a known structural framework to improve conductivity, e.g., cation substitution for an immobile ion or varying the concentration of the mobile ions. Novel frameworks can be disruptive by enabling fast ion conduction aided by different structure and diffusion mechanisms, thereby unlocking optimal conductors with different properties. Herein, we perform a high-throughput survey of a structural framework for sodium ion conduction, Na8–x A x P2O9 (NAP), to understand the family’s thermodynamic stability, synthesizability, and ionic conduction. We show that the parent phase Na4TiP2O9 (NTP) undergoes a structural distortion (with accompanying conductivity transition) due to unstable phonons arising from pseudo-Jahn–Teller mode in the 1D titanium chains. Screening compounds in which Ti is substituted by other metals computationally reveal a number of candidates that are predicted to be low in formation energy and have high predicted ionic conductivities. High-throughput experimental and subsequent methodology optimization trials deliver one new compound, Na4SnP2O9 (NSP). X-ray diffraction (XRD), microscopy, and spectroscopy characterization indicate that the room-temperature structure of NSP is similar to the high-temperature, orthorhombic NTP phase but with some small unresolved structural differences. These uncharacterized structural details are speculated to limit the ion conductivity. Temperature-dependent XRD and electrochemical impedance spectroscopy indicate multiple coupled conductivity–structure transitions at a high temperature. We demonstrate the challenges with synthesis development and a priori identification of promising SSE phases as a major bottleneck in new (energy) materials development.

Chemical reactions↗

DOE OSTI2021

Assessment of Electrode Contamination Mitigation at 0.5 MA Scale

The Z Machine at Sandia National Laboratories uses current pulses with peaks up to 27 MA to drive target implosions and generate high energy density conditions of interest for stockpile stewardship programs pertinent to the NNSA program portfolio . Physical processes in the region near the Z Machine target create electrode plasmas which seed parasitic current loss that reduce the performance and output of a Z experiment. Electrode surface contaminants (hydrogen, water, hydrocarbons) are thought to be the primary constituent of electrode plasmas which contribute to loss mechanisms. The Sandia team explore d in situ heating and plasma discharge techniques by integrating requisite infrastructure into Sandia's Mykonos LTD accelerator, addressing potential impacts to accelerator operation, and reporting on the impact of these techniques on electrode plasma formation and shot performance. The in situ discharge cleaning utilizes the electrodes of the accelerator to excite an argon-oxygen plasma to sputter and chemically react contaminants from electrode surfaces. Insulating breaks are required to isolate the plasma in electrode regions where loss processes are most likely to occur. The shots on Mykonos validate that these breaks do not perturb experiment performance, reducing the uncertainty on the largest unknown about the in situ cleaning system. Preliminary observations with electrical and optical diagnostics suggest that electrode plasma formation is delayed, and overall inventory has been substantively reduced. In situ heating embeds cartridge heaters into accelerator electrodes and employs a thermal bakeout to rapidly desorb contaminants from electrode surfaces. For the first time, additively manufactured (AM) electrode assemblies were used on a low impedance accelerator to integrate cooling channels and manage thermal gradients. Challenges with poor supplier fabrication to specifications, load alignment, thermal expansion and hardware movement and warpage appears to have introduced large variability in observed loss, though, preventing strong assertions of loss reduction via in situ heating. At this time, an in situ discharge cleaning process offers the lowest risk path to reduce electrode contaminant inventories on Z, though we recommend continuing to develop both approaches. Additional engineering and testing are required to improve the implementation of both systems. .

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗