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NASA NTRS2018

Investigations of Spot-to-plume Mode Transition in a Hollow Cathode Discharge Using 2-D Axisymmetric Plasma Simulations

After decades of laboratory investigations that provided invaluable measurements and insight, the physics behind the transition from spot to plume modes in hollow cathodes remains one of the longest standing theoretical problems in electric propulsion. This has prohibited the development of ab initio models that allow for the prediction of the transition across different cathodes and operating conditions. Since the beginning of its development over a decade ago, simulations with the 2-D axisymmetric Orificed Cathode (OrCa2D) code have helped elucidate a wide range of processes in hollow cathode discharges. However, the code has never been used to investigate the onset of plume mode. We present results from the first OrCa2D simulations of a 25-A LaB6 cathode for a range of flow rates (5-20 sccm) in which transition from spot to plume modes is known to occur. The cathode in this study was one of the two technologies considered for the 12.5 kW Hall Effect Rocket with Magnetic Shielding (HERMeS) and operates nominally at 21 A and 14.8 sccm. The simulations capture the characteristic rise of the peak-to-peak amplitude in the keeper voltage oscillations and underscore the significance of the plume neutral gas in the transition. The plasma inside the cathode is found to be relatively quiescent throughout the transition, in agreement with previous experimental observations. The computed keeper voltage fluctuations at low flow rates (<8 sccm) are found to be driven by oscillations of the same frequency in the plasma plume with the following main characteristics: (1) they are of low frequency (<10 kHz), and associated with small longitudinal motion in the direction of the applied magnetic field, (2) they occur in a region of the plume where the neutral gas provided by the cathode has been fully depleted, and (3) they have a (small) wave velocity of about 100 m/s, which is at least ~10 smaller than the drift, thermal and acoustic speeds of the ions. At 8 sccm, when the transition to the large-amplitude oscillations begins, the ionization frequency in the neutral-depleted plume region ranges ~2-100 kHz. The frequency of the oscillations in the plasma (and keeper voltage) is found to be equal to the ionization frequency (~5 kHz) at the center of this region. The findings suggest that the transition to plume mode is driven by ionization processes in the near-plume of the cathode, in line with previous conjectures that were based solely on laboratory observations.

Polk, James E.↗

DOE OSTI2025

Promising performance of sulfide catholytes compared to halide alternatives in NMC811 cathodes for sheet-type sulfide solid-state batteries

Sulfide-based solid-state batteries (SSBs) show promise in achieving energy densities over 350 Wh/kg, yet challenges persist with their incorporation of high-voltage, nickel-rich layered oxide cathodes, such as LiNi₀.₈Mn₀.₁Co₀.₁O₂ (NMC811), due to the poor oxidation stability of sulfide solid-state electrolytes (SSEs) like Li₆PS₅Cl (LPSCl). Although halide SSEs such as Li₃InCl₆ (LIC) and Li₃YCl₆ (LYC) have previously shown promise in stabilizing high-voltage NMC cathodes, our research reveals that sulfide SSE catholytes, particularly when combined with surface-coated NMC cathodes, deliver superior performance. Here, this investigation assesses the cycling stability of various catholytes—LPSCl, LIC, Li₁₀GeP₂S₁₂ (LGPS), combined LIC-LPSCl, and LYC-LPSCl—in SSBs with LiNbO₃-coated NMC811 cathodes against sheet-type LPSCl separators. Findings indicate that while LGPS-based cathodes maintain higher capacity retention, they yield lower deliverable capacity, and LIC cathodes experience significant electrochemical degradation. Importantly, our results underscore that sulfide SSE catholytes, in conjunction with LiNbO₃-coated cathodes, optimize the cathode-electrolyte interphase (CEI), enhancing both kinetics and mass transport. These insights provide a strategic direction for optimizing catholyte composition in the development of sheet-type sulfide-based SSBs.

Catholyte↗

DOE OSTI2024

Cost‐Effective Layered Oxide – Olivine Blend Cathodes for High‐Rate Pulse Power Lithium‐Ion Batteries

Abstract Sustainability and supply‐chain concerns require lithium‐ion batteries (LIBs) free from critical minerals, such as nickel and cobalt. While recent advances provide encouraging signs that cobalt can be removed, the question remains how much Ni can be removed from Co‐free layered oxide cathodes before sacrificing critical performance metrics. This study highlights the effect of reducing Ni by benchmarking several Co‐free cathodes with decreasing Ni content. Keeping the energy density the same by increasing the charge voltage, cathodes below 80% Ni content exhibit worsened capacity fade due to increasing oxygen release and electrolyte decomposition. Charge transfer and diffusion kinetics are also hindered with increasing Mn content and exacerbated by resistive surface phases formed at high voltages, rendering lower‐Ni, Co‐free cathodes less competitive than high‐Ni cathodes for high energy and power applications. It is demonstrated blending layered oxide with olivine as an effective alternative to deliver energy density and cycling stability comparable to lower‐Ni cathodes with moderate charging voltages. Blending with 30 wt% olivine LiMn 0.5 Fe 0.5 PO 4 (LMFP) virtually eliminates the diffusion limitation of layered oxides at low state‐of‐charge, with enhanced pulse power characteristics rivaling the high‐Ni counterparts. Cathode blending can further reduce the overall Ni content and cost without the performance limitations of lower‐Ni, Co‐free cathodes.

Lee, Steven↗

DOE OSTI2025

Operando neutron imaging-guided gradient design of Li-ion solid conductor for high-mass-loading cathodes

High-mass-loading cathodes are crucial for achieving high energy density in all-solid-state batteries from the lab scale to industry. However, as mass-loading increases, electrochemical performance is significantly compromised due to sluggish kinetics. In this work, operando neutron imaging is deployed on a high-mass-loading NMC 811 cathode of 33 mg/cm 2 (5.0 mAh/cm 2 ) and directly visualizes the lithiation prioritization of the cathode active material (CAM) from the solid electrolyte membrane side to the current collector side. In addition to the tortuosity, another key limitation on ion transfer in the cathode arises from the mismatch between the uniform distribution of the solid electrolyte (catholyte) in the conventional composite cathode and the non-uniform Li + flux generated by the faradaic reaction of CAMs. Therefore, we engineer a gradient in the catholyte concentration to match the Li + flux distribution as a means of eliminating the ion transfer obstacle. This approach demonstrates enhanced rate performance, even with high-mass-loading cathodes. A LiCoO 2 composite cathode with 100 mg/cm 2 high-mass-loading exhibits an areal capacity of 10.4 mAh/cm 2 at a current density of 2.25 mA/cm 2 . This work provides insight into the ion-transport limitation in thick cathodes and demonstrates an effective gradient design to overcome the kinetic barrier and achieve high battery performance.

Batteries↗

NASA NTRS1989

Characterization of hollow cathode, ring cusp discharge chambers

An experimental study into the effects of changes in such physical design parameters as hollow cathode position, anode position and ring cusp magnetic field configuration and strength on discharge chamber performance, is described. The results are presented in terms of comparative plasma ion energy cost, extracted ion fraction and ion beam profile data. Such comparisons are used to demonstrate specific means by which changes in these design parameters induce changes in performance, i.e., through changes in the loss rates of primary electrons to the anode, of ions to discharge chamber walls or of ions to cathode and anode surfaces. Results show: (1) the rate of primary electron loss to the anode decreases as the anode is moved downstream of the ring cusp toward the screen grid, (2) the loss rate of ions to hollow cathode surfaces are excessive if the cathode is located upstream of a point of peak magnetic flux density on the discharge chamber centerline, and (3) the fraction of the ions produced that are lost to discharge chamber walls and ring magnet surfaces is reduced by positioning the magnet rings so the plasma density is uniform over the grid surface and so there are no steep magnetic flux density gradients near the walls through which ions can be lost by Bohm diffusion. The uniformity of the plasma density at the grids can also be improved by moving the point of primary electron injection into the discharge chamber off of the chamber centerline. Other results show the discharge chamber losses decrease when a filament cathode is substituted for a hollow cathode to the extent of the hollow cathode operating power. When plasma ion energy cost is determined in such a way that the cost of operating the hollow cathode is subtracted out, the performance using either electron source is similar.

Vaughn, Jason A.↗

NASA NTRS1990

Hollow cathode operation at high discharge currents

It was shown that ion thruster hollow cathode operation at high discharge current levels can induce reduced thruster lifetimes by causing cathode insert overheating and/or erosion of surfaces located downstream of the cathode. The erosion problem has been particularly baffling because the mechanism by which it occurs has not been understood. The experimental investigation described reveals the energies of the ions produced close to the cathode orifice can be several times the anode-to-cathode potential difference generally considered available to accelerate them. These energies (of order 50 eV) are sufficient to cause the observed erosion rates. The effects of discharge current (to 60 A), magnetic field configuration and the cathode flowrate, orifice diameter and insert design on the energies and current densities of these jet ions are examined. A model describing the mechanism by which the high energy ions could be produced when the anode-cathode potential difference is insufficient is proposed. The effects of discharge current on cathode temperature and internal pressure are also examined experimentally and described phenomenologically.

Friedly, Verlin Joe↗

NASA NTRS1994

Continuing life test of a xenon hollow cathode for a space plasma contactor

Implementation of a hollow cathode plasma contactor for charge control on the Space Station has required validation of long-life hollow cathodes. A test series of hollow cathodes and hollow cathode plasma contactors was initiated as part of the plasma contactor development program. An on-going wear-test of a hollow cathode has demonstrated cathode operation in excess of 10,000 hours with small changes in operating parameters. The discharge has experienced 10 shutdowns during the test, all of which were due to test facility failures or expellant replenishment. In all cases, the cathode was re-ignited at approximately 42 volts and resumed typical operation. This test represents the longest demonstrated stable operation of a high current (greater than 1 A) xenon hollow cathode reported to date.

Sarver-Verhey, Timothy R.↗

NASA NTRS1994

Extended test of a xenon hollow cathode for a space plasma contactor

Implementation of a hollow cathode plasma contactor for charge control on the Space Station has required validation of long-life hollow cathodes. A test series of hollow cathodes and hollow cathode plasma contactors was initiated as part of the plasma contactor development program. An on-going wear-test of a hollow cathode has demonstrated cathode operation in excess of 4700 hours with small changes in operating parameters. The discharge experienced 4 shutdowns during the test, all of which were due to test facility failures or expellant replenishment. In all cases, the cathode was reignited at approximately 42 volts and resumed typical operation. This test represents the longest demonstrated stable operation of a high current (greater than 1A) xenon hollow cathode reported to date.

Sarver-Verhey, Timothy R.↗

NASA NTRS1991

Multi-cathode unbalanced magnetron sputtering systems

Ion bombardment of a growing film during deposition is necessary in many instances to ensure a fully dense coating, particularly for hard coatings. Until the recent advent of unbalanced magnetron (UBM) cathodes, reactive sputtering had not been able to achieve the same degree of ion bombardment as other physical vapor deposition processes. The amount of ion bombardment of the substrate depends on the plasma density at the substrate, and in a UBM system the amount of bombardment will depend on the degree of unbalance of the cathode. In multi-cathode systems, the magnetic fields between the cathodes must be linked to confine the fast electrons that collide with the gas atoms. Any break in this linkage results in electrons being lost and a low plasma density. Modeling of the magnetic fields in a UBM cathode using a finite element analysis program has provided great insight into the interaction between the magnetic fields in multi-cathode systems. Large multi-cathode systems will require very strong magnets or many cathodes in order to maintain the magnetic field strength needed to achieve a high plasma density. Electromagnets offer the possibility of independent control of the plasma density. Such a system would be a large-scale version of an ion beam enhanced deposition (IBED) system, but, for the UBM system where the plasma would completely surround the substrate, the acronym IBED might now stand for Ion Blanket Enhanced Deposition.

Sproul, William D.↗

NASA NTRS1998

Destructive Evaluation of a Xenon Hollow Cathode after a 28,000 Hour Life Test

International Space Station (ISS) plasma contactor system requires a hollow cathode assembly (HCA) with a lifetime of at least 18,000 hours. In order to demonstrate the lifetime capability of the HCA, a series of hollow cathode wear tests was performed which included a life test operated at the maximum current of the HCA. This test sought to verify hollow cathode lifetime capability and contamination control protocols. This hollow cathode accumulated 27,800 hours of operation before it failed during a restart attempt. The cathode was subsequently destructively analyzed in order to determine the failure mechanism. Microscopic examination of the cathode interior determined that relatively small changes in the cathode physical geometry had occurred and barium tungstates, which are known to limit the emission process, had formed over a majority of the electron emitter surface. Because the final state of the insert was consistent with expected impregnate chemistry, the hollow cathode was believed to have reached the end of its usable life under the test conditions.

Sarver-Verhey, Timothy R.↗

NASA NTRS2001

Preliminary Results of Field Emission Cathode Tests

Preliminary screening tests of field emission cathodes such as chemical vapor deposited (CVD) diamond, textured pyrolytic graphite, and textured copper were conducted at background pressures typical of electric thruster test facilities to assess cathode performance and stability. Very low power electric thrusters which provide tens to hundreds micronewtons of thrust may need field emission neutralizers that have a capability of tens to hundreds of microamperes. From current voltage characteristics, it was found that the CVD diamond and textured metals cathodes clearly satisfied the Fowler-Nordheim emission relation. The CVD diamond and a textured copper cathode had average current densities of 270 and 380 mA/sq cm, respectively, at the beginning-of-life. After a few hours of operation the cathode emission currents degraded by 40 to 75% at background pressures in the 10(exp -5) Pa to 10(exp -4) Pa range. The textured pyrolytic graphite had a modest current density at beginning-of-life of 84 mA/sq cm, but this cathode was the most stable of all. Extended testing of the most promising cathodes is warranted to determine if current degradation is a burn-in effect or whether it is a long-term degradation process. Preliminary experiments with ferroelectric emission cathodes, which are ceramics with spontaneous electric polarization, were conducted. Peak current densities of 30 to 120 mA/sq cm were obtained for pulse durations of about 500 ns in the 10(exp -4) Pa pressure range.

Sovey, James S.↗

NASA NTRS1998

Methods and apparatus for using gas and liquid phase cathodic depolarizers

The invention provides methods for using gas and liquid phase cathodic depolarizers in an electrochemical cell having a cation exchange membrane in intimate contact with the anode and cathode. The electrochemical conversion of cathodic depolarizers at the cathode lowers the cell potential necessary to achieve a desired electrochemical conversion, such as ozone evolution, at the anode. When gaseous cathodic depolarizers, such as oxygen, are used, a gas diffusion cathode having the cation exchange membrane bonded thereto is preferred. When liquid phase cathodic depolarizers are used, the cathode may be a flow-by electrode, flow-through electrode, packed-bed electrode or a fluidized-bed electrode in intimate contact with the cation exchange membrane.

Murphy, Oliver J.↗

NASA NTRS2005

Improved Cathode Structure for a Direct Methanol Fuel Cell

An improved cathode structure on a membrane/electrode assembly has been developed for a direct methanol fuel cell, in a continuing effort to realize practical power systems containing such fuel cells. This cathode structure is intended particularly to afford better cell performance at a low airflow rate. A membrane/electrode assembly of the type for which the improved cathode structure was developed (see Figure 1) is fabricated in a process that includes brush painting and spray coating of catalyst layers onto a polymer-electrolyte membrane and onto gas-diffusion backings that also act as current collectors. The aforementioned layers are then dried and hot-pressed together. When completed, the membrane/electrode assembly contains (1) an anode containing a fine metal black of Pt/Ru alloy, (2) a membrane made of Nafion 117 or equivalent (a perfluorosulfonic acid-based hydrophilic, proton-conducting ion-exchange polymer), (3) a cathode structure (in the present case, the improved cathode structure described below), and (4) the electrically conductive gas-diffusion backing layers, which are made of Toray 060(TradeMark)(or equivalent) carbon paper containing between 5 and 6 weight percent of poly(tetrafluoroethylene). The need for an improved cathode structure arises for the following reasons: In the design and operation of a fuel-cell power system, the airflow rate is a critical parameter that determines the overall efficiency, cell voltage, and power density. It is desirable to operate at a low airflow rate in order to obtain thermal and water balance and to minimize the size and mass of the system. The performances of membrane/electrode assemblies of prior design are limited at low airflow rates. Methanol crossover increases the required airflow rate. Hence, one way to reduce the required airflow rate is to reduce the effect of methanol crossover. Improvement of the cathode structure - in particular, addition of hydrophobic particles to the cathode - has been demonstrated to mitigate the effects of crossover and decrease the airflow required.

Valdez, Thomas↗

NASA NTRS2012

Compact High Current Rare-Earth Emitter Hollow Cathode for Hall Effect Thrusters

An apparatus and method for achieving an efficient central cathode in a Hall effect thruster is disclosed. A hollow insert disposed inside the end of a hollow conductive cathode comprises a rare-earth element and energized to emit electrons from an inner surface. The cathode employs an end opening having an area at least as large as the internal cross sectional area of the rare earth insert to enhance throughput from the cathode end. In addition, the cathode employs a high aspect ratio geometry based on the cathode length to width which mitigates heat transfer from the end. A gas flow through the cathode and insert may be impinged by the emitted electrons to yield a plasma. One or more optional auxiliary gas feeds may also be employed between the cathode and keeper wall and external to the keeper near the outlet.

Hofer, Richard R.↗

NASA NTRS2011

Co-Flow Hollow Cathode Technology

Hall thrusters utilize identical hollow cathode technology as ion thrusters, yet must operate at much higher mass flow rates in order to efficiently couple to the bulk plasma discharge. Higher flow rates are necessary in order to provide enough neutral collisions to transport electrons across magnetic fields so that they can reach the discharge. This higher flow rate, however, has potential life-limiting implications for the operation of the cathode. A solution to the problem involves splitting the mass flow into the hollow cathode into two streams, the internal and external flows. The internal flow is fixed and set such that the neutral pressure in the cathode allows for a high utilization of the emitter surface area. The external flow is variable depending on the flow rate through the anode of the Hall thruster, but also has a minimum in order to suppress high-energy ion generation. In the co-flow hollow cathode, the cathode assembly is mounted on thruster centerline, inside the inner magnetic core of the thruster. An annular gas plenum is placed at the base of the cathode and propellant is fed throughout to produce an azimuthally symmetric flow of gas that evenly expands around the cathode keeper. This configuration maximizes propellant utilization and is not subject to erosion processes. External gas feeds have been considered in the past for ion thruster applications, but usually in the context of eliminating high energy ion production. This approach is adapted specifically for the Hall thruster and exploits the geometry of a Hall thruster to feed and focus the external flow without introducing significant new complexity to the thruster design.

Hofer, Richard R.↗

NASA NTRSDate not supplied

Cathode Modeling of Solid-State Batteries

The search for safe, reliable, and compact high-capacity energy storage devices has led to increased interest in all-solid-state battery research. The use of solid electrolytes provides enhanced safety and durability due to their reduced flammability and increased mechanical strength compared to organic liquid electrolytes. Still, the use of solid electrolytes remains challenging. Computational modeling plays a substantial role in addressing these challenges. A particle dynamics electromechanical model for simulating electrochemical processes in a solid-state battery cathode will be presented. The model presents cathode microstructure at the particle level as a mixture of ionically conductive solid electrolyte particles, electrically conductive carbon additives, and cathodic reactant particles. After densification, the particle connectivity is analyzed to reconstruct the complex electric network connecting reactant particles with an anodic and cathodic current collectors through the electrolyte and carbon particles. The Kirchhoff’s matrix equation describing this electric network, is solved to obtain values of various critical parameters, such as the overall conductivity of the cathode for lithium ions and electrons, cathodic reactant material utilization, and the distribution of the electric current and voltages within the cathode. In addition, by representing the reactant particles as electrolyte or galvanic microcells governed by the Butler-Volmer electrochemical equation, the overall performance of battery cells during charge or discharge processes, respectively, can be predicted for a given cathodic powder composition. The presented model, executed on a high-performance computing architecture, essentially provides a valuable guidance in designing and developing future solid-state batteries.

solid-state battery↗

DOE OSTI2024

Enhanced Electrochemical Performance of Disordered Rocksalt Cathodes in a Localized High‐Concentration Electrolyte

Abstract Lithium (Li)‐rich transition metal oxide cathodes with a cation disordered rock salt structure (DRX) are increasingly gaining popularity for advanced Li batteries as they offer high capacity and cost benefits over the commonly used layered Li transition metal oxide cathodes. However, the performance of DRX cathodes and their applications are limited by severe side reactions between the cathode and the state‐of‐the‐art carbonate‐based electrolytes at high voltage of 4.8 V, transition metal dissolution, and structural instability of the cathode particles. In this work, an advanced localized high‐concentration electrolyte (LHCE) is developed to form a stable cathode‐electrolyte interphase and mitigate structural instability of the Li 1.13 Mn 0.66 Ti 0.21 O 2 (LMTO) DRX during electrochemical cycling. Li||LMTO half cells with the LHCE demonstrate increased capacity, cycling stability, and superior rate capability compared with cells containing a conventional carbonate electrolyte. For instance, the Li||LMTO cells cycled in LHCE show a higher initial capacity of 205.2 mAh g −1 and a better capacity retention of 72.5% after 200 cycles at a current density of 20 mA g −1 than those with the conventional electrolyte (initial capacity of 187.7 mAh g −1 and capacity retention of 19.9%). This work paves the way to the development of practical DRX cathode‐based high‐energy Li batteries.

25 ENERGY STORAGE↗

NASA NTRS1996

Operation of a Solid-Rod Cathode in a Low-Pressure Discharge

Cathode erosion is one of the life-limiting mechanisms in several classes of electric thrusters. Since cathode erosion depends strongly on the cathode temperature, a quantitative understanding of the effects of cathode operation in the cathode temperature is required. A pure tungsten cathode was sucessfully operated in an argon discharge at pressures of 1.5 and 3.0 kPa and current levels of 600, 1000 and 1400 A.

cathode erosion cathode temperature cathode operat↗