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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 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Solid electrolyte for solid-state batteries: Have lithium-ion batteries reached their technical limit?

With increasing demand for electrical power on a distribution grid lacking storage capabilities, utilities and project developers must stabilize what is currently still intermittent energy production. In fact, over half of utility executives say “the most important emerging energy technology” is energy storage. Advanced, low-cost battery designs are providing promising stationary storage solutions that can ensure reliable, high-quality power for customers, but research challenges and questions lefts. Have lithium-ion batteries (LIBs) reached their technical limit? The industry demands are including high costs, inadequate energy densities, long recharge times, short cycle-life times and safety must be continually addressed. Safety is still the main problem on developing the lithium ion battery.The safety issue must be considered from several aspects, since it would become serious problems, such as an explosion in a Japan Airlines 787 Dreamliner’s cargo hold, due to the battery problem. The combustion is mainly due to the leakage or shortcut of the electrodes, caused by the liquid electrolyte and polymer separator. For this reason, the research on solid electrolyte for replacing the existing liquid electrolyte is very important. The materials used in existing lithium ion battery, such as a separator and liquid electrolyte must be replaced to new solid electrolytes, solid materials that exhibits high ionic conductivity. Due to these reasons, research on solid state ionics materials have been vastly growing worldwide, with the main aim not only to search new solid electrolyte to replace the liquid one, but also looking for low cost materials and environmentally friendly. A revolutionary paradigm is also required to design new stable anode and cathode materials that provide electrochemical cells with high energy, high power, long lifetime and adequate safety at competitive manufacturing costs. Lithium superionic conductors, which can be used as solid electrolytes, promise the potential to replace organic liquid electrolytes and thereby improve the safety of next-generation high-energy batteries. Li{sub 3}PO{sub 4} has been proved to be a good candidate for solid electrolyte, due to its easy in preparation, low cost, high melting temperature and good compatibility with the electrode materials. In the present work, Li{sub 3}PO{sub 4} has been prepared by wet chemical reaction, a simple method with the advantage of recycling a waste product H{sub 3}PO{sub 4}. The crystal structure has been characterized by both neutron and x-ray diffraction. The use of neutron scattering plays important role on observing the light atoms such as lithium ion. The x-ray diffraction results showed the crystal structure of orthorhombic phase P m n 21 (31), that belongs to the β-Li{sub 3}PO{sub 4}, with the lattice parameters are a = 6.123872, b = 5.250211, c = 4.876378. The conductivity of β-Li{sub 3}PO{sub 4} was around 10{sup −8} S/cm. Furthermore, the future application of the solid electrolyte layer in lithium ion battery will also be considered. It is concluded that the used of local resources on producing the solid electrolyte Li{sub 3}PO{sub 4} for lithium ion battery will give more added values to the researches and national industry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Synthesis of Fluorine-Doped Lithium Argyrodite Solid Electrolytes for Solid-State Lithium Metal Batteries

Solid-state lithium metal batteries (SSLMBs) that utilize novel solid electrolytes (SEs) have garnered much attention because of their potential to yield safe and high-energy-density batteries. Sulfide-based argyrodite-class SEs are an attractive option because of their impressive ionic conductivity. Recent studies have shown that LiF at the interface between Li and SE enhances electrochemical stability. However, the synthesis of F-doped argyrodites has remained challenging because of the high temperatures used in the state-of-the-art solid-state synthesis methods. In this work, for the f irst time, we report F-doped Li 5+y PS 5 F y argyrodites with a tunable doping content and dual dopants (F-/Cl- and F-/Br-) that were synthesized through a solvent-based approach. Among all compositions, Li 6 PS 5 F 0.5 C l0.5 exhibits the highest Li-ion conductivity of 3.5 x 10 -4 S cm -1 at room temperature (RT). Furthermore, Li symmetric cells using Li 6 PS 5 F 0.5 Cl 0.5 show the best cycling performance among the tested cells. X-ray photoelectron spectroscopy and ab initio molecular dynamics simulations revealed that the enhanced interfacial stability of Li 6 PS 5 F 0.5 C l0.5 SE against Li metal can be attributed to the formation of a stable solid electrolyte interphase (SEI)-containing conductive species (Li 3 P), alongside LiCl and LiF. These findings open new opportunities to develop high-performance SSLMBs using a novel class of F-doped argyrodite electrolytes.

25 ENERGY STORAGE↗
DOE OSTI2019

High-conduction GE substituted LiAsS4 solid electrolyte

A solid electrolyte for a lithium battery includes Li3+xGexAs1-xS4 where x=0 to 0.50. The value of x can be a range of any high value and any lower value from 0 to 0.50. For example, x can be 0.25 to 0.50, and x can be 0.3 to 0.4, among many other possible ranges. In one embodiment x=0.33 such that the solid electrolyte is Li3.334Ge0.334As0.666S4. A solid electrolyte for a lithium battery can include LiAsS4 wherein ½ to ⅔ of the As is substituted with Ge. A lithium battery and a method for making a lithium battery are also disclosed.

25 ENERGY STORAGE↗
DOE OSTI2023

Imaging solid–electrolyte interphase dynamics using operando reflection interference microscopy

The quality of the solid–electrolyte interphase is crucial for the performance of most battery chemistries, but its formation dynamics during operation are not well understood due to a lack of reliable operando characterization techniques. Herein, we report a dynamic, non-invasive, operando reflection interference microscope to enable the real-time imaging of the solid–electrolyte interphase during its formation and evolution processes with high sensitivity. The stratified structure of the solid–electrolyte interphase formed during four distinct steps includes the emergence of a permanent inner inorganic layer enriched in LiF, a transient assembly of an interfacial electrified double layer and a consequent emergence of a temporary outer organic-rich layer whose presence is reversible with electrochemical cycling. Reflection interference microscope imaging reveals an inverse correlation between the thicknesses of two interphasial subcomponents, implying that the permanent inorganic-rich inner layer dictates the organic-rich outer layer formation and lithium nucleation. In conclusion, the real-time visualization of solid–electrolyte interphase dynamics provides a powerful tool for the rational design of battery interphases.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2026

Distinct Melt Infusion Architectures of Antiperovskite Solid Electrolytes

Antiperovskite solid electrolytes are an emerging class of lithium‐ion conductors distinguished by their unusually low melting points, enabling scalable, low‐temperature processing routes not accessible to most solid electrolytes. In this work, we synthesize phase‐pure chloride (Cl), bromide (Br), and mixed halide (ClBr) variants of antiperovskites and investigate their ionic conductivities in both powder and hot‐pressed forms. Hot pressing significantly enhances conductivity across all compositions, while energy‐dispersive X‐ray spectroscopy (EDS) of the mixed halide system reveals halide surface migration during densification. We further investigate the melt‐infiltration behavior of these electrolytes into substrates relevant to solid‐state battery architectures, including Al and Cu current collectors, conventional NMC and LFP cathodes, and a foamed NMC cathode with a highly porous architecture. The foamed cathode enables deep and uniform electrolyte penetration, highlighting the role of electrode architecture in facilitating melt infiltration. Across all substrates, electrolyte halide chemistry strongly influences wetting behavior, penetration depth, and resulting microstructural morphology. Together, these results establish clear processing–structure relationships for melt‐infiltrated antiperovskite solid electrolytes and demonstrate how electrolyte chemistry and electrode architecture govern interfacial morphology during integration, providing practical guidelines for processing and structural design in solid‐state battery systems.

antiperovskite↗
DOE OSTI2020

In Situ Investigation of Chemomechanical Effects in Thiophosphate Solid Electrolytes

Solid-state batteries can suffer from catastrophic failure at high current densities due to solid electrolyte fracture, interface decomposition, or lithium filament growth. Failure is linked to chemomechanical material transformations that can manifest during electrochemical cycling. We systematically investigate how solid electrolyte microstructure and interfacial decomposition (e.g., interphase) affect failure mechanisms in lithium thiophosphates (Li3PS4, LPS) electrolytes. Kinetically metastable interphases are engineered with iodine doping, and microstructural control is achieved using milling and annealing processing techniques. In situ transmission electron microscopy reveals iodine diffusion to the interphase, and upon electrochemical cycling, pores are formed in the interphase region. In situ synchrotron tomography reveals that interphase pore formation drives edge fracture events, which are the origin of through-plane fracture failure. Fractures in thiophosphate electrolytes actively grow toward regions of higher porosity and are affected by heterogeneity in microstructure (e.g., porosity factor). This report provides fundamental design guidelines for high-performance solid-state batteries.

25 ENERGY STORAGE↗
DOE OSTI2019

Incorporating Solvate and Solid Electrolytes for All‐Solid‐State Li 2 S Batteries with High Capacity and Long Cycle Life

Abstract The development of all‐solid‐state lithium–sulfur batteries is hindered by the poor interfacial properties at solid electrolyte (SE)/electrode interfaces. The interface is modified by employing the highly concentrated solvate electrolyte, (MeCN) 2 −LiTFSI:TTE, as an interlayer material at the electrolyte/electrode interfaces. The incorporation of an interlayer significantly improves the cycling performance of solid‐state Li 2 S batteries compared to the bare counterpart, exhibiting a specific capacity of 760 mAh g −1 at cycle 100 (330 mAh g −1 for the bare cell). Electrochemical impedance spectroscopy shows that the interfacial resistance of the interlayer‐modified cell gradually decreases as a function of cycle number, while the impedance of the bare cell remains almost constant. Cross‐section scanning electron microscopy (SEM)/ energy dispersive X‐ray spectroscopy (EDS) measurements on the interlayer‐modified cell confirm the permeation of solvate into the cathode and the SE with electrochemical cycling, which is related to the decrease in cell impedance. In order to mimic the full permeation of the solvate across the entire cell, the solvate is directly mixed with the SE to form a “solvSEM” electrolyte. The hybrid Li 2 S cell using a solvSEM electrolyte exhibits superior cycling performance compared to the solid‐state cells, in terms of Li 2 S loading, Li 2 S utilization, and cycling stability. The improved performance is due to the favorable ionic contact at the battery interfaces.

Shin, Minjeong↗
DOE OSTI2026

Dissecting Disorder: Defect-Driven Structural Complexity in Layered Li3InCl6 Solid Electrolyte

Halide solid electrolytes have emerged as promising candidates for solid-state batteries owing to their high oxidative stability and ionic conductivity. Among them, Li3InCl6 (LIC) has attracted significant attention. However, diffraction patterns of LIC synthesized via different methods exhibit distinct differences particularly at low-angle reflectionsindicative of underlying structural disorder. These variations are attributed to deviations from ideal crystallographic order, especially stacking faults, whose impact on structure and ion transport remains poorly understood. Here, we identify and quantify stacking faults in LIC samples prepared under different synthetic conditions. Using X-ray diffraction and time-of-flight neutron diffraction, we construct and refine stacking fault models that accurately reproduce the experimental diffraction features. LIC samples with higher degrees of stacking faults exhibit only negligible differences in ionic conductivities and activation energies. This indicates that stacking faults have a limited impact on altering the Li+ diffusion pathway along the c-axis, likely due to the high concentration of vacancies in the In layers, while Li+ diffusion remains nearly unchanged in the ab-plane. Our results account for the observed differences in diffraction patterns across samples and provide a quantitative assessment of faulting probabilities and stacking sequences. The insights gained from this study are expected to be broadly applicable to other layered halide solid electrolytes and contribute to a deeper understanding of the role of structural disorder in ion transport.

Liu, Jue [ORNL] (ORCID:000000024453910X)↗
DOE OSTI2018

Anomalous Self-Assembly and Ion Transport in Nanostructured Organic–Inorganic Solid Electrolytes

Nanostructured solid electrolytes containing ion-conducting domains and rigid non-conducting domains are obtained by block copolymer self-assembly. In this work, we report on the synthesis and characteristics of mixtures of a hybrid diblock copolymer with an organic and inorganic block: poly(ethylene oxide)-b-poly(acryloisobutyl polyhedral oligomeric silsesquioxane) (PEO-POSS) and a lithium salt. In the neat state, PEO-POSS exhibits a classical order-to-disorder transition upon heating.Dilute electrolytes exhibit a dramatic reversal; a disorder-to-order transition upon heating is obtained, indicating that the addition of salt fundamentally changes interactions between the organic and inorganic chains. At higher salt concentrations, the electrolytes primarily form a lamellar phase. Coexisting lamellae and cylinders are found at intermediate salt concentrations and high temperatures. The conductivity and shear modulus of PEO-POSS are significantly higher than that of an all organic block copolymer electrolyte with similar molecular weight and morphology, demonstrating that organic-inorganic block copolymers provide a promising route for developing the next generation of solid electrolytes for lithium batteries.

25 ENERGY STORAGE↗
DOE OSTI2023

Interfacial Issues and Modification of Solid Electrolyte Interphase for Li Metal Anode in Liquid and Solid Electrolytes

Abstract The high energy density required for the next generation of lithium batteries will likely be enabled by a shift toward lithium metal anode from the conventional intercalation‐based anode such as graphite. However, several critical challenges for Li metal originate from its highly reactive nature and the hostless reaction of deposition and stripping impede the practical use of Li metal as an anode. The role of the solid electrolyte interphase (SEI) is very important for the Li metal anode where the SEI must protect the dynamically changing surface of the Li metal. Since the SEI‐generating reaction mechanisms for the two different electrolyte systems, liquid and solid, are considerably different, the SEI layers formed between the Li metal and the electrolytes in the two electrolyte systems have substantially different properties, causing different interfacial issues. Inhibition of the interfacial problems requires different strategies to reinforce the SEI layer for each of the electrolyte systems. However, the differences in the two electrolyte systems have not been clearly compared in the prior literature. In this report, the interfacial issues for the two different electrolyte systems are compared and different strategies for SEI modification are provided to overcome the issues.

25 ENERGY STORAGE↗
DOE OSTI2020

Encapsulated sulfide glass solid electrolytes and solid-state laminate electrode assemblies

Nanofilm-encapsulated sulfide glass solid electrolyte structures and methods for making the encapsulated glass structures involve a lithium ion conducting sulfide glass sheet encapsulated on its opposing major surfaces by a continuous and conformal nanofilm made by atomic layer deposition (ALD). During manufacture, the reactive surfaces of the sulfide glass sheet are protected from deleterious reaction with ambient moisture, and the nanofilm can be configured to provide additional performance advantages, including enhanced mechanical strength and improved chemical resistance.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Encapsulated sulfide glass solid electrolytes and solid-state laminate electrode assemblies

Nanofilm-encapsulated sulfide glass solid electrolyte structures and methods for making the encapsulated glass structures involve a lithium ion conducting sulfide glass sheet encapsulated on its opposing major surfaces by a continuous and conformal nanofilm made by atomic layer deposition (ALD). During manufacture, the reactive surfaces of the sulfide glass sheet are protected from deleterious reaction with ambient moisture, and the nanofilm can be configured to provide additional performance advantages, including enhanced mechanical strength and improved chemical resistance.

Visco, Steven J.↗
DOE OSTI2022

Encapsulated sulfide glass solid electrolytes and solid-state laminate electrode assemblies

Nanofilm-encapsulated sulfide glass solid electrolyte structures and methods for making the encapsulated glass structures involve a lithium ion conducting sulfide glass sheet encapsulated on its opposing major surfaces by a continuous and conformal nanofilm made by atomic layer deposition (ALD). During manufacture, the reactive surfaces of the sulfide glass sheet are protected from deleterious reaction with ambient moisture, and the nanofilm can be configured to provide additional performance advantages, including enhanced mechanical strength and improved chemical resistance.

Visco, Steven J.↗
DOE OSTI2023

Boosting the interfacial superionic conduction of halide solid electrolytes for all-solid-state batteries

Designing highly conductive and (electro)chemical stable inorganic solid electrolytes using cost-effective materials is crucial for developing all-solid-state batteries. Here, we report halide nanocomposite solid electrolytes (HNSEs) ZrO 2 (-ACl)-A 2 ZrCl 6 (A = Li or Na) that demonstrate improved ionic conductivities at 30 °C, from 0.40 to 1.3 mS cm -1 and from 0.011 to 0.11 mS cm -1 for Li + and Na + , respectively, compared to A 2 ZrCl 6 , and improved compatibility with sulfide solid electrolytes. The mechanochemical method employing Li 2 O for the HNSEs synthesis enables the formation of nanostructured networks that promote interfacial superionic conduction. Via density functional theory calculations combined with synchrotron X-ray and 6 Li nuclear magnetic resonance measurements and analyses, we demonstrate that interfacial oxygen-substituted compounds are responsible for the boosted interfacial conduction mechanism. Compared to state-of-the-art Li 2 ZrCl 6 , the fluorinated ZrO 2 -2Li 2 ZrCl 5 F HNSE shows improved high-voltage stability and interfacial compatibility with Li 6 PS 5 Cl and layered lithium transition metal oxide-based positive electrodes without detrimentally affecting Li + conductivity. We also report the assembly and testing of a Li-In||LiNi 0.88 Co 0.11 Mn 0.01 O 2 all-solid-state lab-scale cell operating at 30 °C and 70 MPa and capable of delivering a specific discharge of 115 mAh g -1 after almost 2000 cycles at 400 mA g -1 .

36 MATERIALS SCIENCE↗
DOE OSTI2020

NASICON Li 1.2 Mg 0.1 Zr 1.9 (PO 4 ) 3 Solid Electrolyte for an All‐Solid‐State Li‐Metal Battery

Abstract A thin solid electrolyte with a high Li + conductivity is used to separate the metallic lithium anode and the cathode in an all‐solid‐state Li‐metal battery. However, most solid Li‐ion electrolytes have a small electrochemical stability window, large interfacial resistance, and cannot block lithium‐dendrite growth when lithium is plated on charging of the cell. Mg 2+ stabilizes a rhombohedral NASICON‐structured solid electrolyte of the formula Li 1.2 Mg 0.1 Zr 1.9 (PO 4 ) 3 (LMZP). This solid electrolyte has Li‐ion conductivity two orders of magnitude higher at 25 °C than that of the triclinic LiZr 2 (PO 4 ) 3 . 7 Li and 6 Li NMR confirm the Li‐ions in two different crystallographic sites of the NASICON framework with 85% of the Li‐ions having a relatively higher mobility than the other 15%. The anode–electrolyte interface is further investigated with symmetric Li/LMZP/Li cell testing, while the cathode–electrolyte interface is explored with an all‐solid‐state Li/LMZP/LiFePO 4 cell. The enhanced performance of these cells enabled by the Li 1.2 Mg 0.1 Zr 1.9 (PO 4 ) 3 solid electrolyte is stable upon repeated charge/discharge cycling.

Zhou, Qiongyu↗