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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Modulating the Lattice Stability in Sodium-Layered Oxide Cathodes through Inductive Effect

Stability and safety of sodium layered oxide cathodes relative to lithium analogs remain a critical concern, yet its fundamental origin remains poorly understood. Here, we examine the role of sodium – oxygen bond ionicity in governing outgassing by introducing 5% lithium (Li), potassium (K), or both into layered NaNiO 2 (NNO), yielding Na 0.95 Li 0.05 NiO 2 , Na 0.95 K 0.05 NiO 2 , and Na 0.90 Li 0.05 K 0.05 NiO 2 . Online electrochemical mass spectrometry at 4.3 V reveals that K substitution increases gas evolution with similar charge capacity, whereas Li substitution reduces gas evolution by nearly 80% with only a 16% capacity decrease. Capacity-controlled experiments show that NNO must be charged to only 3.8 V (144 mA h g -1 ) to achieve gas evolution comparable to Na 0.95 Li 0.05 NiO 2 charged to 4.3 V (175 mA h g -1 ). These results demonstrate that tuning alkali-metal–oxygen bond ionicity through the inductive effect regulates Ni–O covalency, lattice oxygen stability, and interfacial reactivity, providing design guidance for safer sodium layered oxide cathodes.

25 ENERGY STORAGE↗
DOE OSTI2022

High-Entropy and Superstructure-Stabilized Layered Oxide Cathodes for Sodium-Ion Batteries

Layered transition metal oxides are appealing cathodes for sodium-ion batteries due to their overall advantages in energy density and cost. But their stabilities are usually compromised by the complicated phase transition and the oxygen redox, particularly when operating at high voltages, leading to poor structural stability and substantial capacity loss. Here, in this study, an integrated strategy combing the high-entropy design with the superlattice-stabilization to extend the cycle life and enhance the rate capability of layered cathodes is reported. It is shown that the as-prepared high-entropy Na 2/3 Li 1/6 Fe 1/6 Co 1/6 Ni 1/6 Mn 1/3 O 2 cathode enables a superlattice structure with Li/transition metal ordering and delivers excellent electrochemical performance that is not affected by the presence of phase transition and oxygen redox. It achieves a high reversible capacity (171.2 mAh g –1 at 0.1 C), a high energy density (531 Wh kg –1 ), extended cycling stability (89.3% capacity retention at 1 C for 90 cycles and 63.7% capacity retention at 5 C after 300 cycles), and excellent fast-charging capability (78 mAh g –1 at 10 C). This strategy would inspire more rational designs that can be leveraged to improve the reliability of layered cathodes for secondary-ion batteries.

25 ENERGY STORAGE↗
NASA NTRS2009

Subcooling Cryogenic Propellants for Long Duration Space Exploration

The use of cryogenic propellants such as hydrogen and oxygen is crucial for exploration of the solar system because of their superior specific impulse capability. Future missions may require vehicles with the flexibility to remain in orbit or travel in space for months, necessitating long-term storage of these cryogens. One powerful technique for easing the challenge of cryogenic fluid storage is to remove energy from tlie cryogenic propellant by isobaricly subcooling them below their normal boiling point prior to launch. The isobaric subcooling of the cryogenic propellant will be performed by using a cold pressurant to maintain the tank pressure while the cryogen's temperature is simultaneously reduced. After launch, even with the use of the best insulation systems, heat will leak into the cold cryogenic propellant tank. However, the large heat capacity available in highly subcooled cryogenic propellants allows them to absorb the energy that leaks into the tank until the cryogen reaches its operational thermodynamic condition. During this period of heating of the subcooled cryogen there will be no loss of the propellant due to venting for pressure control. This simple technique can extend the operational life of a spacecraft or an orbital cryogenic depot many months with minimal mass penalty. Subcooling technologies for cryogenic propellants would thus provide the Exploration Systems Mission Directorate with an enhanced level of mission flexibility. However, there are a few challenges associated with subcooling cryogenic propellants since compact subcooling ground support equipment has not been demonstrated. This paper explores the beneficial impact of subcooling cryogenic propellants on the launch pad for long-term cryogenic propellant storage in space and proposes a novel method for implementing subcooling of cryogenic propellants for spacecraft such as the Ares V Earth Departure Stage (EDS). Analysis indicates that with a careful strategy to handle the subcooled cryogen it would be possible to store cryogenic propellants in space for many months without venting. A concept for subcooling the cryogenic propellant relatively quickly and inexpensively on the launch pad - the thermodynamic cryogen subcooler (TCS) - will be presented. Important components of the TCS and an associated subcooled cryogen tank (SCT) will be discussed in this paper. Results from a preliminary thermodynamic model of the performance of a TCS for an EDS sized hydrogen tank will also be presented.

Mustafi, Shuvo↗
DOE OSTI2022

Improving the oxygen redox reversibility of Li-rich battery cathode materials via Coulombic repulsive interactions strategy

The oxygen redox reaction in lithium-rich layered oxide battery cathode materials generates extra capacity at high cell voltages (i.e., >4.5 V). However, the irreversible oxygen release causes transition metal (TM) dissolution, migration and cell voltage decay. To circumvent these issues, we introduce a strategy for tuning the Coulombic interactions in a model Li-rich positive electrode active material, i.e., Li 1.2 Mn 0.6 Ni 0.2 O 2 . In particular, we tune the Coulombic repulsive interactions to obtain an adaptable crystal structure that enables the reversible distortion of TMO 6 octahedron and mitigates TM dissolution and migration. Moreover, this strategy hinders the irreversible release of oxygen and other parasitic reactions (e.g., electrolyte decomposition) commonly occurring at high voltages. When tested in non-aqueous coin cell configuration, the modified Li-rich cathode material, combined with a Li metal anode, enables a stable cell discharge capacity of about 240 mAh g -1 for 120 cycles at 50 mA g -1 and a slower voltage decay compared to the unmodified Li 1.2 Mn 0.6 Ni 0.2 O 2 .

25 ENERGY STORAGE↗
DOE OSTI2021

Al Substitution for Mn during Co-Precipitation Boosts the Electrochemical Performance of LiNi 0.8 Mn 0.1 Co 0.1 O 2

We report nickel-rich layered oxides, such as LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC 811), are considered as one of the most promising candidates for the next-generation cathode because of their high energy densities and relatively low cost. However, the poor first Coulombic efficiency of NMC 811 leads to around a 15% capacity loss in the first cycle at a cut-off voltage of 4.4 V. Moreover, the structure degradation during cycling results in capacity fading and safety concerns, due to potential oxygen loss after charging. Here, with aluminum substitution for manganese through a developed continuous co-precipitation approach, the electrochemical performance of NMC 811 cathodes has been greatly enhanced. Among different Al% substituted samples, LiNi 0.8 Mn 0.06 Co 0.1 Al 0.04 O 2 cathodes reduced by 50% the first capacity loss of pristine NMC 811(18.0 vs 35.9 mAh g -1 ) and improved the capacity retention from 81.4 to 96.4% after 60 cycles at 0.5C in the voltage range of 2.8–4.4 V.

25 ENERGY STORAGE↗
DOE OSTI2023

Structure and lithium insertion in oxides of molybdenum

Oxides of molybdenum, MoO x , have a rich structural chemistry arising from the accommodation of oxygen deficiency as MoO 3 is reduced and varied redox behavior arising from the ability of Mo to take on several different oxidation states. We review MoO 3 , MoO 2 , and all the reduced Mo oxides with intermediate compositions for their performance as Li-ion battery electrode materials. These reduced oxides are perhaps the most structurally diverse in the field of energy storage materials, taking on structures ranging from ones with crystallographic shear to bronze-like structures and distorted rutile. The crystal structure can have a significant impact on the performance of battery materials, which makes the reduced Mo oxides a promising domain of study. Electrochemical studies of these oxides from as early as 1971 to as recently as 2022 are compiled, and characteristics of capacity, capacity retention, and rate performance are compared. We find that certain oxides indeed display promising and highly reversible capacities for Li + storage. Typical redox voltages for Mo oxides lie in a regime that hinders maximizing energy density when they are paired with higher-voltage cathodes or lower-voltage anodes. The possibility of decreasing the redox voltage in the future will expand the promise of these materials while offering an alternative to more critical elements such as Nb.

25 ENERGY STORAGE↗
DOE OSTI2021

A universal method to fabricating porous carbon for Li-O 2 battery

The main bottleneck in the application of biomass-based carbon material in energy field is the development of an economical, nanoscale controllable and universal fabrication method. Herein, we demonstrate that a biomass-derived carbon consisting of loose carbon nanosphere clusters could serve as an ideal cathode material for high performance Li-O 2 batteries. The carbon nanomaterial can be prepared from both biomass derivatives and crude biomass by a low cost, facile and nanoscale controllable method. The open slit-shaped hierarchical pore structure endows the electrode sufficient active surface sites and mass transport channels that are not easily asphyxiated by the discharge products. The concentration of oxygenic groups and structure defects on the surface of obtained carbon materials is very low, which minimizes the side reactions associated with carbon decomposition. Finally, the unique pore structure and surface properties of the carbon electrode give rise to a superhigh specific capacity of 20,300 mA h g -1 and an extremely long cycle life which a cyclic capacity retention of 100% is maintained for 543 cycles with current density of 0.2 mA cm -2 at controlled discharge-charge depths of 500 mA h g -1 .

25 ENERGY STORAGE↗
DOE OSTI2023

Towards commercialization of fluorinated cation-disordered rock-salt Li-ion cathodes

Cation-disordered rock-salt cathodes (DRX) are promising materials that could deliver high capacities (>250 mAh g −1 ) with Earth abundant elements and materials. However, their electrochemical performances, other than the capacity, should be improved to be competitive cathodes, and many strategies have been introduced to enhance DRXs. Fluorination has been shown to inhibit oxygen loss and increase power density. Nevertheless, fluorinated cation-disordered rock-salts still suffer from rapid material deterioration and low scalability which limit their practical applications. This mini-review highlights the key challenges for the commercialization of fluorinated cation-disordered rock-salts, discusses the underlying reasons behind material failure and proposes future development directions.

25 ENERGY STORAGE↗
NASA NTRSDate not supplied

Ultrahigh Mass Loading Batteries with Holey Graphene-Enabled Dry-Pressed Cathode Architectures

Holey graphene is a structural derivative of graphene with arrays of nanometer-sized, through-thickness holes across the lateral surface of the atomically thin nanosheet. It has been widely acknowledged that the presence of holes improves ion transport through the graphene planes, making holey graphene an ideal electrode material for electrochemical energy storage. We recently discovered another unique attribute of holey graphene in that it can be directly compressed from powder into electrode in a single step without the use of solvent or binder. In addition to neat holey graphene electrodes, composite electrodes with holey graphene as an ultralightweight scaffold host filled with various active materials can also be readily prepared in a similar solvent-free and binder-free fashion. The active materials can be metal-containing catalysts for lithium-oxygen batteries, lithium-ion battery electrode materials, or high energy density components such as sulfur. Compared to the conventional slurry-based process, the dry-press method is comparably much more suitable toward the facile and scalable preparation of ultrahigh mass loading electrodes with ultrahigh areal capacities.

holey graphene, cathode scaffold, lithium metal, h↗
DOE OSTI2023

Regulating Anionic Redox via Mg Substitution in Mn-Rich Layered Oxide Cathodes Enabling High Electrochemical Stability for Sodium-Ion Batteries

Here, with the limited resources and high cost of lithium-ion batteries (LIBs) and the ever-increasing market demands, sodium-ion batteries (SIBs) gain much interest due to their economical sustainability, and similar chemistry and manufacturing processes to LIBs. As cathodes play a vital role in determining the energy density of SIBs, Mn-based layered oxides are promising cathodes due to their low cost, environmental friendliness, and high theoretical capacity. However, the main challenge is structural instability upon cycling at high voltage. Herein, Mg is introduced into the P2-type Na 0.62 Ni 0.25 Mn 0.75 O 2 cathode to enhance electrochemical stability. By combining electrochemical testing and material characterizations, it is found that substituting 10 mol% Mg can effectively alleviate the P2–O2 phase transition, Jahn-Teller distortion, and irreversible oxygen redox. Moreover, structural integrity is greatly improved. These lead to enhanced electrochemical performances. With the optimized sample, a remarkable capacity retention of 92% in the half cell after 100 cycles and 95% in the full cell after 170 cycles can be achieved. Altogether, this work provides an alternative way to stabilize P2-type Mn-based layer oxide cathodes, which in turn, put forward the development of this material for the next-generation SIBs.

25 ENERGY STORAGE↗
DOE OSTI2022

Microporous water with high gas solubilities

Liquids with permanent microporosity can absorb larger quantities of gas molecules than conventional solvents , providing new opportunities for liquid-phase gas storage, transport, and reactivity. Current approaches to designing porous liquids rely on sterically bulky solvent molecules or surface ligands and thus are not amenable to many important solvents, including water. Here, we report a generalizable thermodynamic strategy to preserve permanent microporosity and impart high gas solubilities to liquid water. Specifically, we show how the external and internal surface chemistry of microporous zeolite and metal–organic framework nanocrystals can be tailored to promote the formation of stable dispersions in water while maintaining dry networks of micropores that are accessible to gas molecules. As a result of their permanent microporosity, these aqueous fluids can concentrate gases, including oxygen (O 2 ) and carbon dioxide (CO 2 ), to much higher densities than are found in typical aqueous environments. Furthermore, when these fluids are oxygenated, record-high capacities of O 2 can be delivered to hypoxic red blood cells, highlighting one potential application of this new class of microporous liquids for physiological gas transport.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Densification of Cathode/Electrolyte Interphase to Enhance Reversibility of LiCoO 2 at 4.65 V

For LiCoO 2 (LCO) operated beyond 4.55 V (vs Li/Li + ), it usually suffers from severe surface degradation. Constructing a robust cathode/electrolyte interphase (CEI) is effective to alleviate the above issues, however, the correlated mechanisms still remain vague. Herein, a progressively reinforced CEI is realized via constructing Zr-O deposits (ZrO 2 and Li 2 ZrO 3 ) on LCO surface (i.e., Z-LCO). Upon cycle, these Zr-O deposits can promote the decomposition of LiPF6, and progressively convert to the highly dispersed Zr-O-F species. In particular, the chemical reaction between LiF and Zr-O-F species further leads to the densification of CEI, which greatly reinforces its toughness and conductivity. Further, combining the robust CEI and thin surface rock-salt layer of Z-LCO, several benefits are achieved, including stabilizing the surface lattice oxygen, facilitating the interface Li + transport kinetics, and enhancing the reversibility of O3/H1-3 phase transition, etc. As a result, the Z-LCO||Li cells exhibit a high capacity retention of 84.2% after 1000 cycles in 3–4.65 V, 80.9% after 1500 cycles in 3–4.6 V, and a high rate capacity of 160 mAh g -1 at 16 C (1 C = 200 mA g -1 ). This work provides a new insight for developing advanced LCO cathodes.

25 ENERGY STORAGE↗
DOE OSTI2020

Highly reversible oxygen redox in layered compounds enabled by surface polyanions

Oxygen-anion redox in lithium-rich layered oxides can boost the capacity of lithium-ion battery cathodes. However, the over-oxidation of oxygen at highly charged states aggravates irreversible structure changes and deteriorates cycle performance. Here, we investigate the mechanism of surface degradation caused by oxygen oxidation and the kinetics of surface reconstruction. Considering Li 2 MnO 3 , we show through density functional theory calculations that a high energy orbital (lO 2p’ ) at under-coordinated surface oxygen prefers over-oxidation over bulk oxygen, and that surface oxygen release is then kinetically favored during charging. We use a simple strategy of turning under-coordinated surface oxygen into polyanionic (SO 4 ) 2- , and show that these groups stabilize the surface of Li 2 MnO 3 by depressing gas release and side reactions with the electrolyte. Experimental validation on Li 1.2 Ni 0.2 Mn 0.6 O 2 shows that sulfur deposition enhances stability of the cathode with 99.0% capacity remaining (194 mA h g -1 ) after 100 cycles at 1 C. Our work reveals a promising surface treatment to address the instability of highly charged layered cathode materials.

25 ENERGY STORAGE↗
DOE OSTI2022

Real-space measurement of orbital electron populations for Li 1-x CoO 2

The operation of lithium-ion batteries involves electron removal from and filling into the redox orbitals of cathode materials, experimentally probing the orbital electron population thus is highly desirable to resolve the redox processes and charge compensation mechanism. Here, we combine quantitative convergent-beam electron diffraction with high-energy synchrotron powder X-ray diffraction to quantify the orbital populations of Co and O in the archetypal cathode material LiCoO 2 . The results indicate that removing Li ions from LiCoO 2 decreases Co t 2g orbital population, and the intensified covalency of Co–O bond upon delithiation enables charge transfer from O 2p orbital to Co e g orbital, leading to increased Co e g orbital population and oxygen oxidation. Theoretical calculations verify these experimental findings, which not only provide an intuitive picture of the redox reaction process in real space, but also offer a guidance for designing high-capacity electrodes by mediating the covalency of the TM–O interactions.

25 ENERGY STORAGE↗
DOE OSTI2026

Chemical factors controlling the behaviour of oxide cathodes in batteries

Oxide cathodes enable high-energy lithium-ion and sodium-ion batteries, with their performances fundamentally governed by three interrelated chemical factors: electronic configuration, chemical bonding, and chemical reactivity. Here, we illustrate how these factors dictate the redox energy, structural stability, ionic and electronic transport, and interfacial behavior in both layered oxide and polyanion oxide cathodes. We discuss how crystal-field effects and octahedral-site stabilization energies influence cation migration, and how inductive effects tune bond covalency and operating voltages. We also explain how chemical bonding governs thermal stability, gas evolution, and first-cycle capacity loss, and how alignment of transition-metal redox band with the oxygen 2p band determines electrolyte reactivity. Comparison between lithium and sodium layered oxides further reveals how differences in Li-O and Na-O bond ionicity affect chemical reactivity. Finally, we outline strategies including compositional tuning, surface doping, and electrolyte optimization, and emphasize how high-throughput, data-driven approaches in guiding the design of next-generation oxide cathodes.

25 ENERGY STORAGE↗
DOE OSTI2020

Scalable synthesis of nanoporous silicon microparticles for highly cyclable lithium-ion batteries

Nanoporous silicon is a promising anode material for high energy density batteries due to its high cycling stability and high tap density compared to other nanostructured anode materials. However, the high cost of synthesis and low yield of nanoporous silicon limit its practical application. Here, we develop a scalable, low-cost top-down process of controlled oxidation of Mg 2 Si in the air, followed by HCl removal of MgO to generate nanoporous silicon without the use of HF. By controlling the synthesis conditions, the oxygen content, grain size and yield of the porous silicon are simultaneously optimized from commercial standpoints. In situ environmental transmission electron microscopy reveals the reaction mechanism; the Mg 2 Si microparticle reacts with O 2 to form MgO and Si, while preventing SiO 2 formation. Owing to the low oxygen content and microscale secondary structure, the nanoporous silicon delivers a higher initial reversible capacity and initial Coulombic efficiency compared to commercial Si nanoparticles (3,033 mAh/g vs. 2,418 mAh/g, 84.3% vs. 73.1%). Synthesis is highly scalable, and a yield of 90.4% is achieved for the porous Si nanostructure with the capability to make an excess of 10 g per batch. Our synthetic nanoporous silicon is promising for practical applications in next generation lithium-ion batteries.

25 ENERGY STORAGE↗
NASA NTRS2010

Subcooling for Long Duration In-Space Cryogenic Propellant Storage

Cryogenic propellants such as hydrogen and oxygen are crucial for exploration of the solar system because of their superior specific impulse capability. Future missions may require vehicles to remain in space for months, necessitating long-term storage of these cryogens. A Thermodynamic Cryogen Subcooler (TCS) can ease the challenge of cryogenic fluid storage by removing energy from the cryogenic propellant through isobaric subcooling of the cryogen below its normal boiling point prior to launch. The isobaric subcooling of the cryogenic propellant will be performed by using a cold pressurant to maintain the tank pressure while the cryogen's temperature is simultaneously reduced using the TCS. The TCS hardware will be integrated into the launch infrastructure and there will be no significant addition to the launched dry mass. Heat leaks into all cryogenic propellant tanks, despite the use of the best insulation systems. However, the large heat capacity available in the subcooled cryogenic propellants allows the energy that leaks into the tank to be absorbed until the cryogen reaches its operational thermodynamic condition. During this period of heating of the subcooled cryogen there will be minimal loss of the propellant due to venting for pressure control. This simple technique can extend the operational life of a spacecraft or an orbital cryogenic depot for months with minimal mass penalty. In fact isobaric subcooling can more than double the in-space hold time of liquid hydrogen compared to normal boiling point hydrogen. A TCS for cryogenic propellants would thus provide an enhanced level of mission flexibility. Advances in the important components of the TCS will be discussed in this paper.

Mustafi, Shuvo↗