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At least 505 records · Page 28
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Fe-single atom catalysts facilitate fast electron transfer with MoS 2 /SnS 2 cathodes in lithium–sulfur batteries

Lithium–sulfur batteries (LSBs) emerge as promising next-generation energy storage systems offering cost-effectiveness, environmental friendliness, and high theoretical energy density. The practical implementation of LSBs faces significant hindrances due to the shuttle effect and sluggish redox reactions. To address these challenges, single-atom catalyst (SAC) based combination materials from d-block elements can offer increased active catalytic sites, rapid charge transfer, accelerated electron migration, and fast sulfur redox conversion kinetics of lithium polysulfides (LiPSs). In this study, we fabricated three different LSB cathodes: pure S, S@MoS 2 /SnS 2 , and S@Fe–MoS 2 /SnS 2 . These cathodes were then used to explore the cycle life, capacity, rate capability, and redox kinetic reactions of LiPSs while assessing the influence of Fe-SACs on their performance. As a result, LSBs with S@Fe–MoS 2 /SnS 2 cathodes demonstrate an extended cycle life of 1000 cycles at a C-rate of 0.2C, maintaining a capacity close to 500 mA h g −1 , the highest initial discharge capacity of 1622 mA h g −1 and 1066 mA h g −1 at 0.05C and 0.2C, and excellent rate capabilities of 708 mA h g −1 and 558 mA h g −1 at 1C and 2C, respectively. The synergistic effect of the Fe-SAC-based combination cathode (S@Fe–MoS 2 /SnS 2 ) creates plentiful adsorptive and highly active catalytic sites, resulting in substantially enhanced capacity for adsorbing soluble long-chain LiPSs. This facilitates ultra-fast redox kinetics, surpassing the performance of the S@MoS 2 /SnS 2 and pure S cathodes. In the ex situ analysis, results from powder X-ray diffraction (XRD) to observe the new phase, soft X-ray absorption spectroscopy (XAS) to investigate the electronic structure, and hard X-ray photoelectron microscopy (HAXPES) with different energies (900 eV, 2000 eV, and 6000 eV) to track the chemical-state evolution of Fe-SACs in MoS 2 /SnS 2 cathodes displayed notable electrochemical reversibility involving S 8 ⇄ LiPSs ⇄ Li 2 S conversion even after 1000 cycles. Additionally, in situ, operando Raman analysis can unveil a novel catalytic mechanism of Fe-SACs in MoS 2 /SnS 2 “facilitating rapid electron transfer” during the discharge and charge processes of LSBs involving the conversion of S 8 ⇄ long-chain LiPSs ⇄ Li 2 S 2 /Li 2 S. This study elucidates the working mechanism of Fe-SAC cathodes, offering insights into overcoming the shuttle effect and facilitating sulfur redox kinetics to advance commercial LSBs.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Deciphering the Conflict Between Ion and Electron Percolating Networks in Solid-State Battery Cathodes

High-energy- and power-density solid state batteries require an optimal cathode composition and microstructural arrangement of cathode active material, solid-state electrolyte, conductive carbon, and binder to simultaneously support lithium-ion transport, electron conduction, and storage capacity. The ion and electron conducting phases in solid-state cathodes counteract each other's percolating networks as their mass ratios increase or decrease relative to each other. Here, we investigate targeted mass ratio variations of argyrodite solid electrolyte and two different types of conductive carbon (particles and fibers) in composite LiNi0.8Mn0.1Co0.1O2 (NMC811) solid-state cathodes to ascertain the ionic-electronic tradeoffs in cathode performance. Through ionic and electronic conductivity measurements on composite cathodes, as well as rate-testing and cycling performance in full cells, it is shown that the conductive carbon fibers form a percolative electronic network within the composite at a lower mass ratio (3-5 wt%) than particulate carbon (>5 wt%). The threshold to achieve electronic percolation coincides with higher accessible capacity in the cathode as the active material particles become electronically connected. However, carbon loadings beyond this percolation threshold lead to increased ion transport resistance, arising from disruptions to ionic conduction pathways and degraded contact at the interface between the electrolyte and active materials. Imaging, spectroscopy, and physics-based models quantitatively describe the relationship between carbon and electrolyte compositions and the cell's capacity and rate performance through percolation theory. This work demonstrates the importance of quantitatively understanding percolating networks in solid-state cells and that strategic engineering of conductive carbon morphologies can further increase the energy- and power-density of solid-state cells.

25 ENERGY STORAGE↗
DOE OSTI2019

Topological cathodes: Controlling the space charge limit of electron emission using metamaterials

The space charge limit (SCL) of emission from photocathodes sets an upper limit on the performance of both high- and low-field electron guns. Generally, one is forced to strike a compromise between the space charge limit and the cathode’s intrinsic emittance [I. Bazarov et al., Phys. Rev. Lett. 102, 104801 (2009)]. However, it is possible to nearly eliminate the SCL due to the image charge by engineering the topography of the cathode’s surface. A cathode with a surface plasma frequency below the frequency spectrum of the accelerating electrons will greatly reduce the polarization of the cathode and its image-charge field, thereby mitigating the cathode’s space charge limit for photoelectric, thermionic, and field emission. In the work presented here, a theory for the image-charge field of a disk of charge being accelerated from the cathode surface is developed which includes the frequency-dependent effects of the cathode’s dielectric function. This theory verifies the concept of SCL mitigation with a wire array metamaterial to design a metacathode with greatly reduced image-charge fields. The details of the holistic metacathode design spanning 6 orders of magnitude in scale are described.

47 OTHER INSTRUMENTATION↗
DOE OSTI2019

Methane-Linked Mechanisms of Electron Uptake from Cathodes by Methanosarcina barkeri

Methanosarcinales , a lineage of cytochrome-containing methanogens, have recently been proposed to participate in direct extracellular electron transfer interactions within syntrophic communities. To shed light on this phenomenon, we applied electrochemical techniques to measure electron uptake from cathodes by Methanosarcina barkeri , which is an important model organism that is genetically tractable and utilizes a wide range of substrates for methanogenesis. Here, we confirm the ability of M. barkeri to perform electron uptake from cathodes and show that this cathodic current is linked to quantitative increases in methane production. The underlying mechanisms we identified include, but are not limited to, a recently proposed association between cathodes and methanogen-derived extracellular enzymes (e.g., hydrogenases) that can facilitate current generation through the formation of reduced and diffusible methanogenic substrates (e.g., hydrogen). However, after minimizing the contributions of such extracellular enzymes and using a mutant lacking hydrogenases, we observe a lower-potential hydrogen-independent pathway that facilitates cathodic activity coupled to methane production in M. barkeri . Our electrochemical measurements of wild-type and mutant strains point to a novel and hydrogenase-free mode of electron uptake with a potential near -484 mV versus standard hydrogen electrode (SHE) (over 100 mV more reduced than the observed hydrogenase midpoint potential under these conditions). These results suggest that M. barkeri can perform multiple modes (hydrogenase-mediated and free extracellular enzyme-independent modes) of electrode interactions on cathodes, including a mechanism pointing to a direct interaction, which has significant applied and ecological implications. IMPORTANCE Methanogenic archaea are of fundamental applied and environmental relevance. This is largely due to their activities in a wide range of anaerobic environments, generating gaseous reduced carbon that can be utilized as a fuel source. While the bioenergetics of a wide variety of methanogens have been well studied with respect to soluble substrates, a mechanistic understanding of their interaction with solid-phase redox-active compounds is limited. This work provides insight into solid-phase redox interactions in Methanosarcina spp. using electrochemical methods. We highlight a previously undescribed mode of electron uptake from cathodes that is potentially informative of direct interspecies electron transfer interactions in the Methanosarcinales .

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

Phase Stability of Garnet Solid-Electrolyte Interfacing with Various Cathodes in All Solid-State Batteries

Garnet-structured Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 (LLZTO) is one of the most promising electrolyte materials for solid-state Li batteries (SS-LiB). The design and fabrication of a good cathode/electrolyte interface is an important criterion for the SS-LiB. In this work, we performed a systematic study on the impact of cathode crystal structure and chemical compositions on their chemical stabilities against the LLZTO at elevated temperatures, which are required for their adhesion during cell fabrication processes. X-ray Diffraction (XRD) and Rietveld refinement analyses revealed the chemical stabilities of various cathode materials in contact with the LLZTO. While layered LiCoO 2 cathode showed good stability in contact with LLZTO to 900 °C, LiNiO 2 or Ni-rich LiNi x Mn y Co 1–x–y O 2 (NMC) cathodes suffered from the formation of La 4 NiLiO 8 due to La-diffusion from LLZTO. Furthermore, Mn-rich LiMn 2 O 4 spinel and layered LiNi 1/3 Mn 1/3 Co 1/3 O 2 cathodes suffered from the formation of La 2 Zr 2 O 7 due to Li-diffusion and production of Li 2 MnO 3 . As a result, LiNi 0.6 Mn 0.2 Co 0.2 O 2 , having an ideal balance of Ni/Mn/Co composition, or Li 2 MnO 3 containing cathodes such as Li 1.2 Ni 0.15 Mn 0.55 Co 0.1 O 2 were found to have excellent phase stability as the cathodes for LLZTO-based SS-LiBs.

25 ENERGY STORAGE↗
DOE OSTI2024

The Dominant Effect of Electrolyte Concentration on Rechargeability of γ -MnO 2 Cathodes in Alkaline Batteries

Achieving high cycle life rechargeableγ-MnO 2 cathodes in alkaline batteries face many challenges. Chief among these is the inability of theγ-MnO 2 polymorph to retain its structural integrity when cycled to high utilization of its theoretical capacity ∼300 mAh g −1 . In this paper, we investigate the root cause of failure of MnO 2 cathodes under deep cycling in the one-electron discharge range and establish a strong link between capacity fade and the amount of birnessite formed. We uncover the underlying cause of failure by cycling industrial scaleγ-MnO 2 cathodes at various levels of theoretical capacity utilization (100%, 50%, and 30%) and in different KOH concentrations (37, 25, and 10 wt%). To determine materials evolution the cycled cathodes were dissected, characterized and analyzed using SEM, XRD, FIB/SEM, EIS, and XPS. Based on our findings, we propose that one major cause of failure of MnO 2 cathodes stems from the solubility of Mn +3 formed during discharge which effectively results in destruction of theγ-MnO 2 phase and amorphization of the cathode. The results show that the bulk of theγ-MnO 2 phase is preserved only in ∼10 wt% KOH, which indicates the attractive range of KOH concentration for cycling of rechargeableγ-MnO 2 cathodes.

Electrochemistry↗
DOE OSTI2025

On Rate-Limiting Mechanisms in NMC Cathodes: The Interplay of Low and High Current Constraints

In this study, we investigate the rate performance limits in LiNi 0.6 Mn 0.2 Co 0.2 O 2 cathodes for lithium-ion batteries, focusing on how cathode thickness, porosity, and threshold voltage impact discharge capacity. By conducting galvanostatic discharge experiments across a wide range of current densities using cathodes of varying thicknesses and porosities, we identify two distinct rate-limiting mechanisms: ionic liquid-diffusion and Ohmic/charge-transfer limitations. Our findings show that thick, dense cathodes are primarily limited by lithium diffusion in the electrolyte, while thinner and more porous cathodes are dominated by Ohmic/charge-transfer limitations, particularly at higher lower cutoff voltages. Crucially, these results allow us to identify the rate-limiting mechanisms in different cathode configurations, offering clear insights into how cathode design can be optimized for improved performance. Understanding these mechanisms is essential for designing next-generation batteries with enhanced rate performance, which is critical for applications such as electric vehicles and renewable energy storage systems.

Brischetto, Martin (ORCID:0000000339865813)↗
DOE OSTI2019

Advancing Lithium- and Manganese-Rich Cathodes through a Combined Electrolyte Additive/Surface Treatment Strategy

Lithium- and manganese-rich (LMR) materials provide cost and environmental advantages to other competing cathodes based on nickel or cobalt chemistries. Within the LMR family, layered-layered-spinel (LLS) cathodes have unique properties, detailed herein, that address several of the challenges faced in large-scale implementation of LMR cathodes. This paper details how a LLS//graphite system was considerably improved by combining optimization strategies. First, a cathode surface-treatment process was optimized. Interestingly, cathodes surface-treated at a low temperature (similar to 100 degrees C) exhibited the best results. The optimized LLS cathode was tested vs. graphite using small amounts of lithium difluoro(oxalate)borate electrolyte additive. The combined approach improved various aspects of the electrochemical performance (e.g., impedance, cycle life, and coulombic efficiency) more than each strategy used alone by mitigating Mn dissolution from the cathode and the ensuing deposition on the anode. The report describes a unique method to improve the performance of practically relevant LMR//graphite cells.

25 ENERGY STORAGE↗
DOE OSTI2016

In Situ X-ray Absorption Spectroscopy Studies of Discharge Reactions in a Thick Cathode of a Lithium Sulfur Battery

Lithium sulfur (Li-S) batteries are well known for their high theoretical specific capacities, but are plagued with scientific obstacles that make practical implementation of the technology impossible. The success of Li-S batteries will likely necessitate the use of thick sulfur cathodes that enable high specific energy densities. However, little is known about the fundamental reaction mechanisms and chemical processes that take place in thick cathodes, as most research has focused on studying thinner cathodes that enable high performance. In this study, in situ X-ray absorption spectroscopy at the sulfur K-edge is used to examine the back of a 115 μm thick Li-S cathode during discharge. Our results show that in such systems, where electrochemical reactions between sulfur and lithium are likely to proceed preferentially toward the front of the cathode, lithium polysulfide dianions formed in this region diffuse to the back of the cathode during discharge. We show that high conversion of elemental sulfur is achieved by chemical reactions between elemental sulfur and polysulfide dianions of intermediate chain length (Li 2 S x , 4 ≤ x ≤ 6). Our work suggests that controlling the formation and diffusion of intermediate chain length polysulfide dianions is crucial for insuring full utilization of thick sulfur cathodes.

25 ENERGY STORAGE↗
DOE OSTI2018

Fluidized Bed Production of Surface Functionalized Powders for Solid Oxide Fuel Cell Cathodes

Fuel cells offer tremendous potential for highly efficient conversion of fossil fuels to useable electrical power. Solid oxide fuel cells (SOFC) are particularly attractive, due to their high efficiency and capability to utilize either hydrogen or hydrocarbon fuels. Presently, there is considerable incentive to develop medium temperature (600 C to 800 C) SOFC's, in order to reduce the material compatibility issues and the engineering challenges associated with higher operating temperatures. Developing cathode materials with viable performance at intermediate temperatures is presently one of the key challenges in commercialization of solid oxide fuel cells. Recent works have shown the advantages of using surface functionalized cathode materials to improve SOFC performance at intermediate temperatures. However, present techniques for surface functionalization are expensive and difficult to implement in commercial SOFC production. In this SBIR Program, Structured Materials Industries, Inc. (SMI), along with partners FuelCell Energy, Inc. (FCE) and the University of Connecticut (UConn), demonstrated a simple and economical process to produce surface functionalized cathode materials, based on fluidized bed technology. SMI has developed a variation on this technology, known as Fluidized Bed Chemical Vapor Deposition (FBCVD), and is presently implementing and commercializing FBCVD as an economical and scalable process to deposit coatings on powder materials. In Phase I of this Project, the SBIR team demonstrated technical feasibility of this approach for producing high performance SOFC cathode materials. In this Phase II Project, the SBIR team refined and optimized the FBCVD process and the surface functionalized cathode materials. Surface functionalized powders of various composition and morphology were produced at SMI using the FBCVD process. Electrochemical characterization of the powders was done at FCE under actual SOFC operating conditions. The results demonstrated the potential for significant improvement in SOFC performance. Long term testing at FCE showed the performance enhancement to be stable with time. Advanced materials characterization at UConn identified the composition and morphology of the materials. SMI's FBCVD processed materials represent a "drop in" replacement for present cathode materials, and should have minimal impact on SOFC production costs. SMI has designed a scaled up FBCVD system for high volume production of SOFC cathode materials, and is well positioned for future implementation and commercialization of the technology developed in this SBIR.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Structure–Property Relationships of Recycled Lithium-Ion Battery Cathodes: Microstructure Optimization Using Virtual Materials Testing

The increasing demand for sustainable battery technologies requires effective recycling strategies for end-of-life lithium-ion battery cathodes. In this study, virtual materials testing, a well-established framework for modeling conventionally manufactured NMC-based cathodes, is applied to partially recycled cathodes. To this end, virtual cathodes consisting of mixtures of pristine and recycled NMC particles are utilized to systematically analyze structure–property relationships depending on mixing ratios and different spatial arrangement strategies. For this purpose, a stochastic 3D model is developed that is capable of generating virtual cathodes with arbitrary volume fractions of active materials and mixing ratios of pristine and recycled NMC particles. Particularly, the stochastic 3D model can mimic the different size distributions of pristine and recycled particles that are observed in image data. Additionally, the model allows the structuring of pristine and recycled NMC either uniformly mixed or layer-wise arranged, mimicking single- and dual-layer cathodes. Subsequently, a systematic computational analysis is conducted to assess the influence of increasing active material ratios of recycled particles, ranging from 0 % to 100 %, while maintaining a constant overall active material volume fraction. The impact of particle mixing on cathode performance is evaluated by examining transport-relevant geometrical descriptors and effective properties, such as geodesic tortuosity, specific surface area, and tortuosity factor.

25 ENERGY STORAGE↗
NASA NTRS1973

Mercury vapor hollow cathode component studies

An experimental study of starting and operating characteristics of conventional hollow cathodes and of hollow cathodes without alkaline earth emissive materials demonstrated that the emissive mix is essential to obtain the desired cathode operation. Loss of the emissive mix by evaporation and chemical reaction was measured. New insert designs consisting of emissive mix supported on nickel and of barium impregnated porous tungsten were studied. Cathodes with a modified orifice geometry operated in a low voltage, 'spot' mode over a broad range of discharge current. Thermal degradation tests on cathode heaters showed the flame sprayed SERT II type to be the most durable at high temperatures. Thermal shock was observed to be a significant factor in limiting cathode heater life. A cathode having a barium impregnated porous tungsten tip and a heater which is potted in sintered alumina was found to have favorable operating characteristics.

Zuccaro, D. E.↗
NASA NTRS1973

High speed electrostatic photomultiplier tube for the 1.06 micrometer wavelength. Cup and slat dynode chain combined with flat cathode and coax output produces 0.25 nsec rise time

The Varian cup and slat dynode chain was modified to have a flat cathode. These modifications were incorporated in an all-electrostatic photomultiplier tube having a rise time of 0.25 n sec. The tube delivered under the contract had a flat S-20 opaque cathode with a useful diameter of 5 mm. The design of the tube is such that a III to V cathode support is mounted in place of the existing cathode substrate. This cathode support is designed to accept a transferred III to V cathode and maintain the cathode surface in the same position as the S-20 photocathode.

Sparks, S. D.↗
NASA NTRS1976

On the emission mechanism in high current hollow cathode arcs

Large hollow cathodes have been operated in a magnetoplasmadynamic arc over wide ranges of current and mass flow, with orifice current densities and mass fluxes encompassing those encountered in low current steady state hollow cathode arcs. Detailed cathode interior measurements of current and potential distributions show that maximum current penetration into the cathode is about one diameter axially upstream from the tip, with peak inner surface current attachment up to one cathode diameter upstream of the tip. The spontaneous attachment of peak current upstream of the cathode tip is suggested as a criterion for characteristic hollow cathode operation. This empirical criterion was verified by experiment.

Krishnan, M.↗
NASA NTRS1980

Hydrogen hollow cathode ion source

A source of hydrogen ions is disclosed and includes a chamber having at one end a cathode which provides electrons and through which hydrogen gas flows into the chamber. Screen and accelerator grids are provided at the other end of the chamber. A baffle plate is disposed between the cathode and the grids and a cylindrical baffle is disposed coaxially with the cathode at the one end of the chamber. The cylindrical baffle is of greater diameter than the baffle plate to provide discharge impedance and also to protect the cathode from ion flux. An anode electrode draws the electrons away from the cathode. The hollow cathode includes a tubular insert of tungsten impregnated with a low work function material to provide ample electrons. A heater is provided around the hollow cathode to initiate electron emission from the low work function material.

Mirtich, M. J., Jr.↗
NASA NTRS1983

Evaluation of the emission capabilities of Spindt-type field emitting cathodes

The electron emitting capabilities of Spindt-type field emitting cathodes (FEC) are being studied at the Lewis Research Center, NASA. These cathodes, having 5000 emitting points in a 1 mm diameter, have been shown to be capable of emission current densities of 10 A/sq cm and higher. The purposes of this study are to (1) demonstrate that the cathodes can be processed and used in a tube-type configuration, (2) determine whether, at a sufficiently high current density, the cathode can operate in the space charge mode, and (3) evaluate failure mechanisms in this unique type of electron emitter. FEC's have been tested in a diode configuration, by the use of pulse techniques, up to current densities of 6 A/sq cm and anode potentials of 3000 V. Space charge effects have been observed in the range of 5 A/sq cm as an apparent linear increase of cathode current with anode voltage for a constant emitter-gate potential. Failed cathodes were studied by means of scanning electron microscopy and the major failure modes encountered are attributed to gas evolution, followed by arcing, which destroys either individual emitters or a large segment of the cathode area.

Forman, R.↗
NASA NTRS1993

Evaluation of externally heated pulsed MPD thruster cathodes

Recent interest in solar electric orbit transfer vehicles (SEOTV's) has prompted a reevaluation of pulsed magnetoplasmadynamic (MPD) thruster systems due to their ease of power scaling and reduced test facility requirements. In this work the use of externally heated cathodes was examined in order to extend the lifetime of these thrusters to the 1000 to 3000 hours required for SEOTV missions. A pulsed MPD thruster test facility was assembled, including a pulse-forming network (PFN), ignitor supply and propellant feed system. Results of cold cathode tests used to validate the facility, PFN, and propellant feed system design are presented, as well as a preliminary evaluation of externally heated impregnated tungsten cathodes. The cold cathode thruster was operated on both argon and nitrogen propellants at peak discharge power levels up to 300 kW. The results confirmed proper operation of the pulsed thruster test facility, and indicated that large amounts of gas were evolved from the BaO-CaO-Al2O3 cathodes during activation. Comparison of the expected space charge limited current with the measured vacuum current when using the heated cathode indicate that either that a large temperature difference existed between the heater and the cathode or that the surface work function was higher than expected.

Myers, Roger M.↗
NASA NTRS1994

Life test of a xenon hollow cathode for a space plasma contractor

A plasma contacting device using a hollow cathode for plasma production has been baselined for use on the Space Station. This application will require reliable, continuous operation of the cathode at electron emission currents of between 0.75 and 10 A for two years (17,500 hours). In order to validate life-time capability, a hollow cathode, operated in a diode configuration, has been tested for more than 8600 hours of stable discharge operation as of March 30, 1994. This cathode is operated at a steady-state emission current of 12.0 and a fixed xenon flow rate of 4.5 sccm. Discharge voltage and cathode temperature have remained relatively stable at approximately 12.9 V and 1260 C during the test. The test has experienced 7 shutdowns to date. In all instances, the cathode was reignited at about 42 V and resumed stable operation. This test represents the longest demonstration of stable operation of high current (greater than 1A) xenon hollow cathodes reported to date.

Sarver-Verhey, Timothy R.↗