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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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All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Phase Stability and Electrochemical Performance of La-Site-Doped Li6La3Zr0.5Nb0.5Ta0.5Hf0.5O12 High-Entropy Garnets

We investigate La-site substitution in the high-entropy garnet Li6La3Zr0.5Nb0.5Ta0.5Hf0.5O12 (LLZNTH) using Ba2+, Sr2+, and Sm3+ to elucidate how dopant governs phase stability, Li-site distribution, and electrochemical behavior. X-ray diffraction shows that Sr2+ is incorporated homogeneously into the garnet lattice, whereas the larger Ba2+ and smaller Sm3+ ions partially exceed the structural tolerance, generating secondary phases. Nevertheless, the Sm-doped composition (x = 0.05) exhibits the highest room-temperature ionic conductivity (2.7 × 10–4 S cm–1). Neutron powder diffraction reveals that Sm substitution drives a redistribution of Li+ from the tetrahedral 24 d sites into the higher-mobility 96 h positions, enhancing the connectivity of the three-dimensional Li-ion migration network. A Sm-doping series (x = 0.01–0.05) further shows that only sufficiently high Sm levels induce this redistribution, whereas lower concentrations retain Li arrangements similar to the undoped garnet. Critical current density measurements demonstrate that La-site dopants also influence interfacial stability against Li metal, underscoring a trade-off between bulk transport enhancement and mechanical robustness. Collectively, these findings reveal that in high-entropy garnets improved ionic conductivity can originate not only from phase-pure structures but also from targeted modification of the Li sublattice, even when accompanied by secondary phases, offering a compositional design principle for garnet electrolytes.

Li, Chang [Mechanical Engineering, School of Scien↗
DOE OSTI2026

How Silica Surface Chemistry Modulates Interfacial Water: Insights from Machine Learning Molecular Dynamics

Controlling water structure and dynamics at silica interfaces are central to a wide range of technologies, including protective oxide layers for solar water splitting and nanoporous membranes. In this work, we develop a machine learning interatomic potential, trained via active learning, to achieve ab initio accuracy for water confined between hydroxylated silica surfaces over a range of silanol coverages and slit widths. We find that partially hydroxylated surfaces (50 and 75% OH) support stronger water−surface hydrogen bonding and more extended interfacial density profiles than fully hydroxylated (100% OH) surfaces, indicating that increasing OH coverage does not necessarily strengthen interfacial hydrogenbond networks. Translational diffusion decreases approximately linearly with slit width and OH coverage, whereas rotational dynamics respond nonlinearly. In particular, at the smallest slit width of 5 Å, 75% OH coverage produces an enhanced local tetrahedral ordered interfacial network that strongly suppresses reorientation, while 100% coverage yields a crowded, disordered interfacial layer that also hinders rotation. In contrast, the 50% OH coverage is sufficiently sparse that it does not markedly alter water structure or dynamics under confinement. These results show that coupled control of pore size and surface chemistry enables nonlinear tuning of interfacial water structure and transport, providing a design strategy for optimizing porous silica for either enhanced interfacial stability and controlled reactivity or rapid and selective transport.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

New Cost-Effective Halide Solid Electrolytes for All-Solid-State Batteries: Mechanochemically Prepared Fe 3+ -Substituted Li 2 ZrCl 6

Owing to the combined advantages of sulfide and oxide solid electrolytes (SEs), that is, mechanical sinterability and excellent (electro)chemical stability, recently emerging halide SEs such as Li 3 YCl 6 are considered to be a game changer for the development of all-solid-state batteries. However, the use of expensive central metals hinders their practical applicability. In this study, a new halide superionic conductors are reported that are free of rare-earth metals: hexagonal close-packed (hcp) Li 2 ZrCl 6 and Fe 3+ -substituted Li 2 ZrCl 6 , derived via a mechanochemical method. Conventional heat treatment yields cubic close-packed monoclinic Li 2 ZrCl 6 with a low Li + conductivity of 5.7 × 10 –6 S cm –1 at 30 °C. In contrast, hcp Li 2 ZrCl 6 with a high Li + conductivity of 4.0 × 10 –4 S cm –1 is derived via ball-milling. More importantly, the aliovalent substitution of Li 2 ZrCl 6 with Fe 3+ , which is probed by complementary analyses using X-ray diffraction, pair distribution function, X-ray absorption spectroscopy, and Raman spectroscopy measurements, drastically enhances the Li + conductivity up to ≈1 mS cm –1 for Li 2.25 Zr 0.75 Fe 0.25 Cl 6 . The superior interfacial stability when using Li 2+ x Zr 1– x Fe x Cl 6 , as compared to that when using conventional Li 6 PS 5 Cl, is proved. Furthermore, an excellent electrochemical performance of the all-solid-state batteries is achieved via the combination of Li 2 ZrCl 6 and single-crystalline LiNi 0.88 Co 0.11 Al 0.01 O 2 .

25 ENERGY STORAGE↗
DOE OSTI2020

Tuning the Anode–Electrolyte Interface Chemistry for Garnet-Based Solid-State Li Metal Batteries

Lithium (Li) metal anode is a promising candidate for high energy density solid-state batteries. However, the interface issues, including large interfacial resistance and Li dendrite generation, have always frustrated the attempt to commercialize solid-state Li metal batteries (SSLBs). Here, we report that infusing the garnet-type solid electrolytes (GSEs) with air-stable electrolyte Li 3 PO 4 (LPO) dramatically reduces the interfacial resistance to ~1 Ω cm 2 and achieves a high critical current density of 2.2 mA cm -2 under ambient condition due to enhanced interfacial stability to Li metal anode. The coated and infused LPO electrolytes not only improve the mechanical strength and Li-ion conductivity of grain boundaries, but also form a stable Li-ion conductive but electron-insulating LPO-derived solid-electrolyte interphase between Li metal and GSEs, and consequently eliminates the Li dendrites growth and prevents the direct reduction of GSEs by Li metal over a long cycle life. This interface engineering approach together with grain-boundary modification on GSEs represents a promising strategy to revolutionize the anode-electrolyte interface chemistry for SSLBs and provides new design strategy for other-types of solid-state batteries.

25 ENERGY STORAGE↗
DOE OSTI2025

Orientation Control in Epitaxial PdO Thin Films Grown on MgO (001) – Role of Oxygen Chemical Potential

Control of crystal orientations in thin films of functional materials allowsedictive tuning of their strain states, electronic properties, and surface chemical reactivity. Here, conditions for orientation control in epitaxial PdO films are investigated. Due to its tetragonal structure, PdO can form two orientational relationships with the MgO (001). It is shown that, under an oxygen-rich environment provided by oxygen-plasma-assisted molecular beam epitaxy, both (00l)- and (100)-oriented PdO domains form on MgO (001). Subsequent thermal annealing in a vacuum promotes film restructuring to a predominantly (100)-oriented PdO with improved crystallinity. Ab initio calculations reveal that the (001) orientation has lower strain energy but weaker interfacial interactions and serves as an oxygen vacancy sink, whereas the (100) orientation benefits from significantly stronger MgO─PdO bonding. Consequently (100)-oriented domains become favored under oxygen-poor conditions. A mechanism is proposed whereby vacuum annealing drives orientation transformation by generating oxygen vacancies that destabilize the (001) domains and promote (100) ordering. These findings deepen the understanding of how oxygen content impacts interfacial stability and reorganization, thereby offering a route to tune domain orientations in oxide thin films.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Stabilizing Zinc Anode Reactions by Polyethylene Oxide Polymer in Mild Aqueous Electrolytes

Abstract Zn dendrites growth and poor cycling stability are significant challenges for rechargeable aqueous Zn batteries. Zn metal deposition‐dissolution in aqueous electrolytes is typically determined by Zn anode–electrolyte interfaces. In this work, the role of a long‐chain polyethylene oxide (PEO) polymer as a multifunctional electrolyte additive in stabilizing Zn metal anodes is reported. PEO molecules suppress Zn 2+ ion transfer kinetics and regulate Zn 2+ ion concentration in the vicinity of Zn anodes through interactions between ether groups of PEO and Zn 2+ ions. The suppressed Zn 2+ ion transfer kinetics and homogeneous Zn 2+ ion distribution at the interface promotes dendrite‐free homogeneous Zn deposition. In addition, electrochemically inert PEO molecules adsorbed onto Zn anodes can protect the anode surfaces from H 2 generation and, thereby, enhance their electrochemical stability. Stable cycling over 3000 h and high reversibility (Coulombic efficiency > 99.5%) of Zn anodes is demonstrated in 1 m ZnSO 4 electrolyte with 0.5 wt% PEO. This finding provides helpful insights into the mechanism of Zn metal anodes stabilization by low‐cost multifunctional polymer electrolyte additives that stabilize interfacial reactions.

Jin, Yan↗
DOE OSTI2025

Hybrid Doping Strategy with High‐Entropy Cu/Fe Surface Modification and Zr Bulk Incorporation for Ni‐Rich Cathodes

A hybrid doping strategy combining Zr 4+ bulk doping with high-entropy Cu 2+ /Fe 3+ surface doping is developed to enhance the structural and interfacial stability of Ni-rich layered oxide cathodes. Cu and Fe are selectively introduced at the particle surface via a surface-selective ion-exchange process, forming a ≈15 nm Fe-rich layer while preserving the layered framework. Compared to the pristine cathode, the hybrid sample exhibits significantly improved electrochemical performance in both half-cell and full-cell configurations. In half-cells, the hybrid retains 88.5% and 90.2% after 100 cycles at 1C under 4.6 and 4.5 V, respectively. During high-voltage full-cell cycling, the hybrid cathode maintains over 80% capacity retention, whereas the pristine counterpart retains less than 10% under identical conditions over the same cycling period. XPS, EELS, and DEMS analyses confirm improved oxygen retention, suppressed gas evolution, and stable surface chemistry, while DFT calculations indicate enhanced Me–O bonding in the selected Fe 0.75 Cu 0.25 (Mn 1/16 Co 2/16 Ni 13/16 )O 2 surface composition, which is identified through DFT-calculated mixing energy reaching a minimum at this ratio, indicating the most thermodynamically favorable configuration. In conclusion, these results demonstrate the effectiveness of this hybrid doping strategy in mitigating coupled degradation pathways in Ni-rich cathodes.

15 GEOTHERMAL ENERGY↗
DOE OSTI2023

Tuned Reactivity at the Lithium Metal–Argyrodite Solid State Electrolyte Interphase

Thin intermetallic Li 2 Te–LiTe 3 bilayer (0.75 µm) derived from 2D tellurene stabilizes the solid electrolyte interphase (SEI) of lithium metal and argyrodite (LPSCl, Li 6 PS 5 Cl) solid-state electrolyte (SSE). Tellurene is loaded onto a standard battery separator and reacted with lithium through single-pass mechanical rolling or transferred directly to SSE surface by pressing. State-of-the-art electrochemical performance is achieved, e.g., symmetric cell stable for 300 cycles (1800 h) at 1 mA cm -2 and 3 mAh cm -2 (25% DOD, 60 µm foil). Cryo-stage focused ion beam (Cryo-FIB) sectioning and Raman mapping demonstrate that the Li 2 Te–LiTe 3 bilayer impedes SSE decomposition. The unmodified Li–LPSCl interphase is electrochemically unstable with a geometrically heterogeneous reduction decomposition reaction front that extends deep into the SSE. Decomposition drives voiding in Li metal due to its high flux to the reaction front, as well as voiding in the SSE due to the associated volume changes. Analysis of cycled SSE found no evidence for pristine (unreacted) lithium metal filaments/dendrites, implying failure driven by decomposition phases with sufficient electrical conductivity that span electrolyte thickness. In conclusion, DFT calculations clarify thermodynamic stability, interfacial adhesion, and electronic transport properties of interphases, while mesoscale modeling examines interrelations between reaction front heterogeneity (SEI heterogeneity), current distribution, and localized chemo-mechanical stresses.

25 ENERGY STORAGE↗
DOE OSTI2025

Flux Upcycling of Degraded Layered Cathodes to LiNi x Mn y Co z O 2 (NMCs) with Gradient Transition Metal Distribution

The rising demand for lithium-ion batteries (LIBs) has intensified the need for efficient recycling methods to address both supply chain constraints and environmental impacts. Direct upcycling, distinguished by its ability to achieve both the structural and compositional integrity of cathode materials, has gained prominence as a sustainable alternative to conventional pyrometallurgical and hydrometallurgical processes. However, the current direct upcycling methods are typically limited by incorporating Li and/or Ni, significantly constraining the adaptability across diverse LiNi x Mn y Co z O 2 (NMCs). Here, in this study, a versatile molten salt approach is reported that expands the scope of direct upcycling by enabling simultaneous incorporation of Li, Ni, and Mn. This methodology facilitates flexible conversion among diverse NMC compositions, including non-stoichiometric Co/Mn systems such as upcycling degraded LiCoO 2 (D-LCO), LiNi 1/3 Mn 1/3 Co 1/3 O 2 (D-NMC111), LiNi 0.8 Mn 0.1 Co 0.1 O 2 (D-NMC811) to surface Mn enriched NMC111, LiNi 0.5 Mn 0.3 Co 0.2 O 2 (NMC532), and NMC811, respectively. The gradient transition metal distribution in upcycled products, characterized by Mn-enriched outer layers and Co/Ni-enriched cores enhances the interfacial stability of NMC cathodes, addressing critical challenges in long-term performance and structural integrity. These results highlight the potential of flux methods for advancing the upcycling of spent cathodes and producing high-performance materials for next-generation LIBs applications.

lithium -ion batteries↗
DOE OSTI2023

Promoting reversibility of layered potassium cathode through interstitial doping

With the increasing needs for large-scale and low-cost energy storage devices, Mn-based layered oxide cathodes have achieved considerable researching interests for potassium-ion batteries owing to their high energy density, abundant resource and low toxicity. However, their developments are challenged by the absence of suitable cathode materials to tolerate large-sized K-ion insertion/extraction and the presence of Jahn-Teller distortion of Mn 3+ . To address this issue, here we present a strategy of embedding boron into interstitial tetrahedral sites to obtain a P3-K 0.5 Mn 0.8 Co 0.2 B 0.1 O 2 cathode. Strong B-O covalent bonds facilitate the construction of robust orthorhombic framework and alleviate the undesired elongation of Mn-O bonds, contributing to excellent electrochemical performance. In addition, boron ions are verified to promote the formation of a homogeneous cathode electrolyte interphase layer, improving interfacial stability and realizing highly reversible cycling in a wide voltage range (1.4-4.3 V). This strategy provides a new pathway towards the development of high-performance cathode materials for potassium-ion batteries.

25 ENERGY STORAGE↗
DOE OSTI2024

Ameliorating the sodium storage performance of hard carbon anode through rational modulation of binder

Hard carbon anodes have emerged as promising candidates for sodium-ion batteries due to their inherent advantages. Nevertheless, the surface imperfections in these materials often culminate in irreversible electrolyte consumption, fostering the development of a heterogeneous and fragile solid electrolyte interface (SEI), thereby compromising the initial Coulombic efficiency (ICE). Here, drawing inspiration from the catalytic potential of C=O (carbonyl) bonds in directing preferential salt reduction, we introduce a novel strategy that leverages the modulation of the binder, a long-term overlooked pivotal components in the electrode process. Specifically, Polymethyl methacrylate (PMMA), abundant in C=O groups, is partially substituted for PVDF, ensuring robust adhesion of the electrode material to the current collector while preserving superior mechanical properties. The accurate combination of two binders with delightful compatibility in the state-of-art electrode process, can promote a uniform formation of the SEI on the hard carbon surface enriched in inorganic components, which can ensure long-term interfacial stability and suppresses excessive solvent decomposition and facilitates Na + transfer at the interface. Consequently, the initial Coulombic efficiency of the hard carbon anode with 70 %PMMA binder achieves 86 %, with prominent cycling stability (88 % capacity retention over 500 cycles) at a high current density of 1.2 A g −1 . When paired with high loading cathodes to assemble the pouch cell, it also demonstrates stable operational scenarios.

25 ENERGY STORAGE↗
DOE OSTI2020

Degradation of solid oxide electrolysis cells: Phenomena, mechanisms, and emerging mitigation strategies—A review

Solid oxide electrolysis cell (SOEC) is a promising electrochemical device with high efficiency for energy storage and conversion. However, the degradation of SOEC is a significant barrier to commercial viability. In this review article, the typical degradation phenomena of SOEC are summarized, with great attention into the anodes/oxygen electrodes, including the commonly used and newly developed anode materials. Meanwhile, mechanistic investigations on the electrode/electrolyte interfaces are provided to unveil how the intrinsic factor, oxygen partial pressure , and the electrochemical operation conditions, affect the interfacial stability of SOEC. At last, this paper also presents some emerging mitigation strategies to circumvent long-term degradation, which include novel infiltration method, development of new anode materials and engineering of the microstructure.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Stable all-solid-state sodium-sulfur batteries for low-temperature operation enabled by sodium alloy anode and confined sulfur cathode

All-solid-state sodium-sulfur (Na-S) batteries are promising for stationary energy storage devices because of their low operating temperatures (less than 100 °C), improved safety, and low-cost fabrication. Using Na alloy instead of Na metal as an anode in Na-S batteries can prevent dendrite growth and improve interfacial stability between the anode and solid electrolytes to achieve long-cycling stability. A high-sulfur content cathode possessing high sulfur utilization is also important to enable an energy-dense Na-S battery. In this work, we studied Na-Sb and Na- Sn alloy anodes and demonstrated the superiority of Na 3 Sb alloy undergoing a stable Na alloying/dealloying process at 0.04 mA cm -2 for over 500 hours. Combining the optimized Na3Sb alloy anode with sulfur-carbon composites prepared by the vapor deposition approach, the full cell shows a high sulfur specific capacity and improved rate performance. Moreover, the all-solid-state Na alloy-S battery can deliver a high initial discharge specific capacity of 1377 mAh g -1 and maintain good capacity retention of 70 % after 180 cycles at 60 °C. Further, post-cycle characterizations show that both the anode and cathode perform a reversible discharge/charge process after the 1st cycle, and the cathode undergoes significantly rearranged distributions of carbon and solid-state electrolytes after 180 cycles due to severe volume change induced by repeated sodiation/desodiation process.

25 ENERGY STORAGE↗
DOE OSTI2020

Polymer–Ceramic Composite Electrolytes for Lithium Batteries: A Comparison between the Single-Ion-Conducting Polymer Matrix and Its Counterpart

Single-ion-conducting polymer electrolytes are attractive to use in lithium batteries as the transference number of the lithium cation approaches unity. This helps prevent concentration gradients across the electrolyte, which can result in dendrite formation. The addition of ceramic particles to polymer electrolytes at high loadings can increase the mechanical strength of the polymer, which can also help suppress dendrite formation. Here, a single-ion-conducting polymer electrolyte is blended with lithium-conducting oxide ceramic particles to make a composite electrolyte. This electrolyte is studied in comparison to a composite electrolyte containing freely dissolved lithium salt. It is found that the addition of ceramic particles to the single-ion-conducting polymer can result in increased cation dissociation and consequent increased ionic conductivity. The electrolytes are cycled in lithium symmetrical cells, and it is found that the ceramic-containing electrolytes show increased interfacial stability with the lithium metal compared to the pristine polymer electrolytes. Our findings shed light on how to optimize the polymer host chemistry to form composite electrolytes that can meet the challenging requirements to stabilize the lithium metal anode.

25 ENERGY STORAGE↗
DOE OSTI2023

Tuning Bulk Redox and Altering Interfacial Reactivity in Highly Fluorinated Cation-Disordered Rocksalt Cathodes

Lithium-excess, cation-disordered rocksalt (DRX) materials have been subject to intense scrutiny and development in recent years as potential cathode materials for Li-ion batteries. Despite their compositional flexibility and high initial capacity, they suffer from poorly understood parasitic degradation reactions at the cathode-electrolyte interface. These interfacial degradation reactions deteriorate both the DRX material and electrolyte, ultimately leading to capacity fade and voltage hysteresis during cycling. In this work, differential electrochemical mass spectrometry (DEMS) and titration mass spectrometry are combined to quantify the extent of bulk redox and surface degradation reactions for a set of Mn 2+/4+ -based DRX oxyfluorides during initial cycling with a high-voltage charging cutoff (4.8 V vs Li/Li + ). Increasing the fluorine content from 7.5 to 33.75% is shown to diminish oxygen redox and suppresses high-voltage O 2 evolution from the DRX surface. Additionally, electrolyte degradation processes resulting in the formation of both gaseous species and electrolyte-soluble protic species are observed. Subsequently, DEMS is paired with a fluoride-scavenging additive to demonstrate that increasing fluorine content leads to increased dissolution of fluorine from the DRX material into the electrolyte. Finally, a suite of ex situ spectroscopy techniques (X-ray photoelectron spectroscopy, inductively coupled plasma optical emission spectroscopy, and solid-state nuclear magnetic resonance spectroscopy) are employed to study the change in DRX composition during charging, revealing the dissolution of manganese and fluorine from the DRX material at high voltages. Here this work provides insight into the degradation processes occurring at the DRX-electrolyte interface and points toward potential routes of interfacial stabilization.

25 ENERGY STORAGE↗
DOE OSTI2023

Laser-Induced Trapping of Metastable Amorphous AlO x /C (2.5 < x ≤ 3.5) Nanocomposites: Implications for Use as Solid Phase Gas Generators

The synthesis of kinetically "frozen" metastable nanostructures remains elusive. This limitation has severely restricted the current paradigms in materials discovery. We overcame this challenge by phase-stabilizing unusually hyperoxidized and metastable amorphous aluminum oxide (a-AlO x ; 2.5 < x ≤ 3.5) nanostructures. Specifically, we employed laser ablation synthesis in solution (LASiS) as a one-pot nonequilibrium technique to achieve this pivotal advancement. Structural and compositional characterizations of the as-synthesized material reveal highly disordered a-AlO x nanoparticles that are remarkably stabilized by interfacial monolayers of ordered carbon atoms. Both structure and chemical composition were confirmed with disparate characterization methods at different length scales. The nanoparticles of sizes less than10 nm were stable even at elevated temperatures. Only at temperatures higher than 750 °C do the a-AlO x structures undergo a solid-solid phase transition that culminates in the formation of stable α-Al 2 O 3 while releasing excess trapped gases. In conclusion, such disruptive materials can find applications in emerging technologies seeking metastable phase-change materials for solid phase gas generators, batteries, neuromorphic computing, and energetic additives.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Practical Considerations for Testing Polymer Electrolytes for High-Energy Solid-State Batteries

Polymer electrolytes are an important class of materials in enabling solid-state batteries, which have the potential to exceed 400 Wh/kg energy density. Despite significant advancements in their lithium-ion transport and mechanical properties over the last two decades, the integration and testing of these novel electrolyte materials into functioning cells with the electrode loadings and dimensions required to meet the cell-level energy density goals have been limited. Here, through multiple representative examples, we demonstrate the need of testing in close to practical cell conditions for a faster and more reliable evaluation of polymeric electrolytes. In particular, the need for testing with thin lithium anodes and practical cycling capacities is demonstrated for evaluation of their lithium-metal interfacial stability and dendritic resistance, respectively, and a testing protocol is suggested. The guidelines presented here will also apply to testing of other solid electrolytes for solid-state batteries.

25 ENERGY STORAGE↗
DOE OSTI2026

Pressure Heterogeneity and Material Utilization in Thin-Film Solid-State Cathodes

Intimate interfacial contact between the solid electrolyte and the cathode active material is critical for maximizing cathode utilization in solid-state batteries. However, volume changes during electrochemical cycling induce internal stresses that drive interfacial degradation, particularly under nonuniform stack pressure. In this study, we employ in situ energy-dispersive X-ray diffraction tomography to visualize and quantify reaction heterogeneities across a 3 mm-diameter solid-state cathode with a well-defined interface. Our results reveal that regions under a lower stack pressure exhibit reduced material utilization and reversibility, which negatively affect the high-pressure regions. Interfacial degradation further impedes lithium-ion transport and amplifies microscale reaction heterogeneity. These findings highlight the critical role of stack pressure distribution in governing interfacial stability and electrochemical performance, offering important design insights into practical solid-state battery systems.

36 MATERIALS SCIENCE↗