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All sources NASA NTRS DOE OSTI

NASA NTRS2016

Post-Test Inspection of NASA's Evolutionary Xenon Thruster Long-Duration Test Hardware: Discharge and Neutralizer Cathodes

The NEXT Long-Duration Test is part of a comprehensive thruster service life assessment intended to demonstrate overall throughput capability, validate service life models, quantify wear rates as a function of time and operating condition, and identify any unknown life-limiting mechanisms. The test was voluntarily terminated in February 2014 after demonstrating 51,184 hours of high-voltage operation, 918 kg of propellant throughput, and 35.5 MN-s of total impulse. The post-test inspection of the thruster hardware began shortly afterwards with a combination of non-destructive and destructive analysis techniques, and is presently nearing completion. This paper presents relevant results of the post-test inspection for both discharge and neutralizer cathodes. Discharge keeper erosion was found to be significantly reduced from what was observed in the NEXT 2 kh wear test and NSTAR Extended Life Test, providing adequate protection of vital cathode components throughout the test with ample lifetime remaining. The area of the discharge cathode orifice plate that was exposed by the keeper orifice exhibited net erosion, leading to cathode plate material building up in the cathode-keeper gap and causing a thermally-induced electrical short observed during the test. Significant erosion of the neutralizer cathode orifice was also found and is believed to be the root cause of an observed loss in flow margin. Deposition within the neutralizer keeper orifice as well as on the downstream surface was thicker than expected, potentially resulting in a facility-induced impact on the measured flow margin from plume mode. Neutralizer keeper wall erosion on the beam side was found to be significantly lower compared to the NEXT 2 kh wear test, likely due to the reduction in beam extraction diameter of the ion optics that resulted in decreased ion impingement. Results from the post-test inspection have led to some minor thruster design improvements.

Electric Propulsion↗

NASA NTRS2015

The Importance of the Cathode Plume and Its Interactions with the Ion Beam in Numerical Simulations of Hall Thrusters

Hall2De is a first-principles, 2-D axisymmetric code that solves the equations of motion for ions, electrons, and neutrals on a magnetic-field-aligned grid. The computational domain downstream of the acceleration channel exit plane is large enough to include self-consistently the cathode boundary. In this paper, we present results from numerical simulations of the H6 laboratory thruster with an internally mounted cathode, with the aim of highlighting the importance of properly accounting for the interactions between the ion beam and cathode plume. The anomalous transport of electrons across magnetic field lines in Hall2De is modelled using an anomalous collision frequency, νanom, yielding νanom approximately equal to omega ce (i.e., the electron cyclotron frequency) in the plume. We first show that restricting the anomalous collision frequency to only regions where the current density of ions is large does not alter the plasma discharge in the Hall thruster as long as the interaction between the ion beam and the cathode plume is captured properly in the computational domain. This implies that the boundary conditions must be placed sufficiently far as to not interfere with the electron transport in this region. These simulation results suggest that electron transport across magnetic field lines occurs largely inside the beam and may be driven by the interactions between beam ions and electrons. A second finding that puts in relevance the importance of including the cathode plume in numerical simulations is on the significance of accounting for the ion acoustic turbulence (IAT), now known to occur in the vicinity of the cathode exit. We have included in the Hall2De simulations a model of the IAT-driven anomalous collision frequency based on Sagdeev's model for saturation of the ion-acoustic instability. This implementation has allowed us to achieve excellent agreement with experimental measurements in the near plume obtained during the operation of the H6 thruster at nominal conditions (300V, 20A) and chamber background pressure of approximately 1.5 x 10(exp -5) Torr. In addition, the numerical results obtained with the latter approach exhibit less sensitivity to background pressure than previous attempts at explaining the features of the plasma properties in the near plume.

Lopez Ortega, Alejandro↗

NASA NTRS2018

Design and Development of Advanced Air-Cathodes for Li-Air Battery

NASA's future missions demand high energy density batteries. Current state-of-the-art lithium-ion batteries (LIBs) reach the specific energy capacity limits (<250 Wh/kg), thus new electrochemical storage technologies are needed to meet NASA's future mission requirement of >400 Wh/kg. Battery chemistries with higher theoretical energy densities in particular, Li-metal based battery chemistries such as Li-air, are being actively pursued, but there remains a number of issues to be solved. Development of advanced and optimized air cathodes will be crucial for improving capacity retention and cycle life of Li-air battery. The microstructure of carbon substrates and the catalytic oxygen reduction of the air-cathode play critical roles in the electrochemical performance in Li-air batteries. With the development and proper design of air cathodes, the energy efficiency and energy density can be enhanced significantly. In this presentation, the results of advanced permeable air cathodes design with different substrates such as 2D carbon paper or carbon cloth, vs 3D graphene or metal foam, different high surface area carbon materials and incorporation with catalysts on oxygen reduction reactions, different porosity controlling of air cathode as well the additives in electrolyte will be presented. The cycling and rate capability performance of these air-cathodes in the Li-air cells will be discussed as well.

Wu, James J.↗

NASA NTRS2016

Laser-Induced Fluorescence Measurements of Energetic Ions in a 100-A LaB6 Hollow Cathode

Increasingly long-duration space missions require a better understanding of the failure mechanisms of hollow cathodes to enable prediction of lifetime. Energetic ions have been measured in the plume of hollow cathodes but the energies are higher than can be explained classically. One of the mechanisms that appears to be contributing to the ion heating is ion acoustic turbulence (IAT), which has been investigated with plasma probes recently at JPL. In this work the ion velocity distribution has been measured using laser-induced fluorescence (LIF) at several high-current operating conditions on the centerline of a 100 A class hollow cathode at JPL. A retarding potential analyzer was (RPA) was used to measure the ion energy profile in the far plume and a Langmuir probe was used to measure electron temperature and plasma potential fluctuations. RPA energies are shown to correlate with the values measured by LIF. The ion temperature is shown to increase with distance downstream of the cathode. A parametric study of the ion heating as a function of discharge current and cathode flow rate was performed. It was found that for increasing current the ion temperature evolution did not vary even though the wave IAT wave energy increased. The effect of flow rate was more pronounced, with higher values reducing both ion temperature and wave energy linearly. These results indicate that IAT is at least partially responsible for energetic ion production in the hollow cathode plume.

Dodson, Christopher A.↗

NASA NTRS2019

Characterization of a Fixed-Volume Release System for Initiating an Arc Discharge in a Heaterless Hollow Cathode

Heaterless hollow cathodes may provide improved reliability, simplicity, and portability when compared with traditional heater-equipped hollow cathodes, traits which are well suited for low-power Hall-effect thrusters that are currently being developed for small satellite propulsion. Despite the advantages, there are concerns that the ignition process in heaterless hollow cathodes may impose an excessive burden on the propellant feed and/or electrical systems of a small satellite. To address this concern, a fixed-volume release flow protocol, which can be used to temporarily increase the propellant mass flow rate, was developed, modeled, and experimentally evaluated. The new protocol allowed for a heaterless hollow cathode to be ignited reliably with a moderate bias voltage and a minimal electrical power requirement. Specifically, a xenon fed heaterless hollow cathode was ignited with a 375 V bias using 17.3 mg of propellant. Repeating the tests with krypton showed that ignition could be achieved in the same heaterless hollow cathode assembly with a 300 V bias using 13.1 mg of propellant. We judge that a fixed-volume release system could be implemented in a satellite feed system while introducing minimal additional complexity.

Heaterless↗

NASA NTRS2019

Characterization of a Fixed-Volume Release System for Initiating an Arc Discharge in a Heaterless Hollow Cathode

Heaterless↗

NASA NTRS2017

Work function reduction in lanthanum hexaboride hollow cathodes operated in gas discharges

Thermal characterization of lanthanum hexaboride (LaB6) hollow cathodes has revealed lower than expected electron emitter temperatures when the cathode reaches steady state. This phenomenon is observed at discharge currents ranging from 5 to 35 A and xenon mass ow rates of 5 to 25 sccm in cathodes with three di erent ori ce diameters. Thus, the accepted value of the work function for polycrystalline LaB6, 2.66 eV, does not describe well the emission characteristics of LaB6 hollow cathodes operating with internal gas discharges at steady state. The measured temperatures and a model of the hollow cathode emitter and xenon discharge were used to estimate the value of the work function in these experiments, yielding a value ranging from 2.1 - 2.44 eV. Measurements of the work function as a function of depth on a hollow cathode emitter using X-ray photoelectron spectroscopy and ion beam milling indicate that the work function in a thin layer near the emitting surface is lower than in the bulk material. We postulate that a lanthanum-rich emitting surface with a lower work function develops as a result of lanthanum recycling in the internal plasma.

Lopez Ortega, Alejandro↗

NASA NTRS2021

Post-test Inspection of NASA’s Evolutionary Xenon Thruster Long-Duration Test Hardware: Discharge and Neutralizer Cathodes

The NEXT Long-Duration Test is part of a comprehensive thruster service life assessment intended to demonstrate overall throughput capability, validate service life models, quantify wear rates as a function of time and operating condition, and identify any unknown life-limiting mechanisms. The test was voluntarily terminated in February 2014 after demonstrating 51,184 h of high-voltage operation, 918 kg of propellant throughput, and 35.5 MN-s of total impulse. The post-test inspection of the thruster hardware began shortly afterwards with a combination of non-destructive and destructive analysis techniques, and is presently nearing completion. This paper presents relevant results of the post-test inspection for both discharge and neutralizer cathodes. Discharge keeper erosion was found to be significantly reduced from what was observed in the NEXT 2 kh wear test and NSTAR Extended Life Test, providing adequate protection of vital cathode components throughout the test with ample lifetime remaining. The area of the discharge cathode orifice plate that was exposed by the keeper orifice exhibited net erosion, leading to cathode plate material building up in the cathode-keeper gap and causing a thermally-induced electrical short observed during the test. Significant erosion of the neutralizer cathode orifice was also found and is believed to be the root cause of an observed loss in flow margin. Deposition within the neutralizer keeper orifice as well as on the downstream surface was thicker than expected, potentially resulting in a facility-induced impact on the measured flow margin from plume mode. Neutralizer keeper wall erosion on the beam side was found to be significantly lower compared to the NEXT 2 kh wear test, likely due to the reduction in beam extraction diameter of the ion optics that resulted in decreased ion impingement. Results from the post-test inspection have led to some minor thruster design improvements.

Ion engine↗

DOE OSTI2014

Beam Dynamics Simulations of Optically-Enhanced Field Emission from Structured Cathodes

Structured cathodes - cathodes with a segmented emission surface - are finding an increasing number of applications and can be combined with a variety of emission mechanisms, including photoemission and field emission. These cathodes have been used to enhance the quantum efficiency of metallic cathodes when operated as plasmonic cathodes, have produced high-current electron bunches though field emission from multiple tips, and can be used to form beams with transverse segmentations necessary for improving the performance of accelerator-based light sources. In this report we present recent progress towards the development of finite-difference time-domain particle-in-cell simulations using the emission process in structured cathodes based on the WARP framework. The simulations give further insight on the localized source of the emitted electrons which could be used for additional high-fidelity start-to-end simulations of electron accelerators that employ this type of electron source.

43 PARTICLE ACCELERATORS↗

DOE OSTI2017

Reflective article having a sacrificial cathodic layer

The present invention relates to reflective articles, such as solar mirrors, that include a sacrificial cathodic layer. The reflective article, more particularly includes a substrate, such as glass, having a multi-layered coating thereon that includes a lead-free sacrificial cathodic layer. The sacrificial cathodic layer includes at least one transition metal, such as a particulate transition metal, which can be in the form of flakes (e.g., zinc flakes). The sacrificial cathodic layer can include an inorganic matrix formed from one or more organo-titanates. Alternatively, the sacrificial cathodic layer can include an organic polymer matrix (e.g., a crosslinked organic polymer matrix formed from an organic polymer and an aminoplast crosslinking agent). The reflective article also includes an outer organic polymer coating, that can be electrodeposited over the sacrificial cathodic layer.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Direct regeneration of lithium ion cathodes by ionothermal relithiation

A method for relithiating cathode material from spent lithium-based batteries, the method comprising: (i) mixing delithiated cathode material and a lithium salt with an ionic liquid in which the lithium salt is at least partially soluble to form an initial mixture; (ii) heating the initial mixture to a temperature of 100° C. to 300° C. to result in relithiation of the delithiated cathode material; and (iii) separating the ionic liquid from the relithiated cathode material; wherein, in embodiments, the cathode material is a lithium metal oxide, wherein the metal is selected from the group consisting of Ni, Co, Fe, Mn, Al, Zr, Ti, Nb, and combinations thereof, or wherein the cathode material has the formula LiNi x Mn y Co z O 2 , wherein x>0, y>0, z>0, and x+y+z=1; wherein, in some embodiments, the ionic liquid has a nitrogen-containing cationic portion, such as an imidazolium ionic liquid.

Luo, Huimin↗

DOE OSTI2019

Ethylene Carbonate–Free Electrolytes for High–Nickel Layered Oxide Cathodes in Lithium–Ion Batteries

Layered lithium nickel oxide (LiNiO 2 ) can provide very high energy density among intercalation cathode materials for lithium-ion batteries, but suffers from poor cycle life and thermal-abuse tolerance with large lithium utilization. In addition to stabilization of the active cathode material, a concurrent development of electrolyte systems of better compatibility is critical to overcome these limitations for practical applications. Here, with nonaqueous electrolytes based on exclusively aprotic acyclic carbonates free of ethylene carbonate (EC), superior electrochemical and thermal characteristics are obtained with an ultrahigh-nickel cathode (LiNi 0.94 Co 0.06 O 2 ), capable of reaching a 235 mA h g –1 specific capacity. Pouch-type graphite | LiNi 0.94 Co 0.06 O 2 cells in EC-free electrolytes withstand several hundred charge–discharge cycles with minor degradation at both ambient and elevated temperatures. In thermal-abuse tests, the cathode at full charge, while reacting aggressively with EC-based electrolytes below 200 °C, shows suppressed self-heating without EC. Through 3D chemical and structural analyses, the intriguing impact of EC is visualized in aggravating unwanted surface parasitic reactions and irreversible bulk structural degradation of the cathode at high voltages. Finally, these results provide important insights in designing high-energy electrodes for long-lasting and reliable lithium-ion batteries.

25 ENERGY STORAGE↗

DOE OSTI2023

A High Energy–Density, Cobalt–Free, Low–Nickel LiNi 0.7 Mn 0.25 Al 0.05 O 2 Cathode with a High–Voltage Electrolyte for Lithium–Metal Batteries

Cobalt-free cathode materials have garnered increased attention for applications in next-generation batteries for electric vehicles, as cobalt is considered to have at a high supply chain risk. Here, the use of a localized saturated electrolyte (LSE) to enable stable cycling of a cobalt-free, low-nickel layered-oxide cathode LiNi 0.7 Mn 0.25 Al 0.05 O 2 (NMA-70) to higher voltages (4.6 V) in a lithium-metal battery is demonstrated. Compared to the baseline LP57 electrolyte, the LSE extends the cycle life from ≈100 cycles to ≈400 cycles before reaching 80% capacity retention. Visual indicators of cell degradation, such as product deposition, are observed on electrodes cycled in LP57. It is shown that cycling NMA-70 in LSE reduces the overall active material loss and overpotential growth during extended cycling. This is attributed to the formation of a beneficial fluorinated interphase layer, a lower degree of rock-salt phase formation, and a reduction in the gas evolution from the cathode surface. The decrease in gas evolution from the cathode cycled in LSE reflects a lower degree of electrolyte reactivity and an overall improvement in the safety characteristics of the cell. Furthermore, this study highlights the importance of a stable electrolyte to enable the high-voltage cycling of alternative, lower nickel, and cobalt-free cathodes.

25 ENERGY STORAGE↗

DOE OSTI2025

Cathode Upcycling for Direct Recycling of Lithium‐Ion Batteries Using a Precipitation Approach

With the increased production of electric vehicles to reduce carbon emissions, the lithium-ion battery market to supply those vehicles has grown dramatically. To enhance battery sustainability and circularity, direct recycling methods aim to recover intact cathode materials. However, end-of-life cathode materials are typically 15–20 years old and often have lower energy density compared to current cathode materials. To address this challenge, a rapid precipitation process is developed to boost energy density by converting low Ni-compositions, LiNi 0.33 Co 0.33 Mn 0.33 O 2 (NMC111), into higher Ni-compositions (NMC622). This process forms a Ni-rich coating on cathode particles that diffuses into the core upon high-temperature relithiation, increasing compositional homogeneity. The upcycling process leverages existing infrastructure, offering low capital cost and minimal additional chemical input. Through ex situ tomographic transmission X-ray microscopy (TXM), 3D Ni:Co elemental mixing is quantified, confirming that elemental content evens at the secondary particle level with a mean NMC622 composition upon relithiation. However, elemental gradients remain in the single crystalline primary particles. Ex situ high-resolution and in situ wide-angle X-ray diffraction reveals concurrent structural changes during the relithiation process. These findings provide key insights into the structural and chemical mechanisms of elemental diffusion to obtain further improvements of increased capacity and retention through compositional conversion of cathode materials.

Cathode Upcycling↗

DOE OSTI2015

Electrochemical characterization of B-site cation-excess Pr 2 Ni 0.75 Cu 0.25 Ga 0.05 O 4+δ cathode for IT-SOFCs

In this paper, the B-site cation-excess K 2 NiF 4 -type structure oxide, Pr 2 Ni 0.75 Cu 0.25 Ga 0.05 O 4+δ (PNCG) is investigated as a cathode for intermediate-temperature solid oxide fuel cells (IT-SOFCs). XRD result shows that PNCG cathode is chemically compatible with the electrolyte Gd 0.1 Ce 0.9 O 2-δ (GDC) at 900 °C for 5 h. The PNCG material exhibits a semiconductor to metal transition around 425 °C. The thermal expansion coefficient (TEC) of the PNCG sample is 12.72×10 -6 K -1 between 30 and 850 °C in air. The polarization resistance (R p ) of PNCG cathode on GDC electrolyte is 0.105, 0.197 and 0.300 Ω cm 2 at 800, 750, 700 °C, respectively. A maximum power density of 371 mW cm -2 is obtained at 800 °C for single-cell with 300 μm thick GDC electrolyte and PNCG cathode. Finally, the results of this study demonstrate that PNCG can be a promising cathode material for IT-SOFCs.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Cracking vs. surface reactivity in high-nickel cathodes for lithium-ion batteries

High-nickel layered oxide cathodes LiNi x Mn y Co z O 2 (NMC) experience microcracks during cycling. This can expose fresh cathode surfaces for parasitic reactions and isolate active cathode material from the conductive electrode matrix, resulting in impedance increase and capacity fade. The commonly held belief attributes microcracks to anisotropic lattice volume changes of primary particles during cycling. Nevertheless, recent reports suggest that certain electrolytes might reduce microcracks in NMC cathodes during deep cycling. This raises a crucial question on the origin of microcracks: do microcracks exacerbate surface stability, or does poor surface stability contribute to microcrack formation? This perspective aims to provide context and expound this “chicken or egg” dilemma. We contend that the consequence of surface reactivity on the cycle life of high-Ni cathodes is more pronounced than that of particle cracking. Here, we hypothesize that particle cracking is more of a symptom of severe surface reactivity rather than a cause of capacity fade.

25 ENERGY STORAGE↗

DOE OSTI2020

Revealing the Structural Evolution and Phase Transformation of O3-Type NaNi 1/3 Fe 1/3 Mn 1/3 O 2 Cathode Material on Sintering and Cycling Processes

O-type layered oxide cathode materials can be easily synthesized for a full sodium stoichiometry with high specific capacity, but they all suffer from a capacity fade on cycling. The sintering process control and optimization are critical to ensure a high quality and consistency of the prepared cathode materials with stable structure. Herein, in situ high-energy X-ray diffraction (HEXRD) was first employed to investigate the phase evolution of the oxides during the sintering process of O3-type NaNi 1/3 Fe 1/3 Mn 1/3 O 2 . The in situ HEXRD and both operando Bragg coherent diffraction (BCXD) and coherent multicrystal diffraction (CMCD) were utilized to investigate the phase transformation of the cathode materials during the sodiation/desodiation process. A composite structure comprised of O-type and P-type oxides was formed after the initial electrochemical activation of the cathode material, resulting in good structural and electrochemical stability. This finding implies that strain engineering can be a new design philosophy for the development of next generation high-performance sodium ion cathodes.

25 ENERGY STORAGE↗

DOE OSTI2020

Structural Degradation of High Voltage Lithium Nickel Manganese Cobalt Oxide (NMC) Cathodes in Solid-State Batteries and Implications for Next Generation Energy Storage

In this study, we report the stability of the layered high voltage cathode NMC622 with respect to a standard liquid electrolyte and in an all solid-state configuration. NMC622 cathodes with a (104) orientation were found to suffer from degradation at high voltage (4.5 V vs Li/Li + ) due to electrolyte-promoted degradation of the layered structure in a carbonate electrolyte. The lithium phosphorus oxynitride (LiPON) electrolyte was able to suppress the extent of this decomposition in solid-state cells but not totally prevent it from occurring. In the solid-state cells the capacity decreased from 203 to 93 mAh/g in the first cycle and from 93 to 79 mAh/g over the subsequent 99 cycles, whereas, after 20 cycles, the liquid cell charge capacity was dominated by the irreversible electrolyte degradation. Furthermore, the interfacial resistances of the solid-state cells were stable with cycling, suggesting minimal degradation of the NMC622/LiPON interface and incumbent losses due to structural evolution associated with cathode orientation. This data indicates that accessing stable high voltage capacity in NMCs will not be enabled by simply stabilizing the cathode–electrolyte interface. Optimizing cathode crystallographic orientation may be the key to accessing this high voltage regime.

25 ENERGY STORAGE↗