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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 253 records · Page 14
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Signal Origin of Electrochemical Strain Microscopy and Link to Local Chemical Distribution in Solid State Electrolytes

Electrochemical strain microscopy (ESM) is a distinguished method to characterize Li-ion mobility in energy materials with extremely high spatial resolution. The exact origin of the cantilever deflection when the technique is applied on solid state electrolytes (SSEs) is currently discussed in the literature. Under-standing local properties and influences on ion mobility in SSEs is of utmost importance to improve such materials for next generation batteries. Here, the exact signal formation process of ESM when applied on sodium super ionic conductor (NASICON)-type SSE containing Na- and Li-ions is investigated. Changes in the dielectric properties, which are linked to the local chemical composition, are found to be responsible for the observed contrast in the deflection of the cantilever instead of a physical volume change as a result of Vegard´s Law. The cantilever response is strongly reduced in areas of high sodium content which is attributed to a reduction of the tip-sample capacitance in comparison to areas with high lithium content. This is the first time a direct link between electrostatic forces in contact mode and local chemical information is demonstrated on SSEs. Furthermore, the results open up new possibilities in information gain since dielectric proper-ties are sensitive to subtle changes in local chemical composition.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Co-intercalation-free ether electrolytes for graphitic anodes in lithium-ion batteries

Carbonate-based electrolytes are widely used in Li-ion batteries but are limited by a small operating temperature window and poor cycling with silicon-containing graphitic anodes. The lack of non-carbonate electrolyte alternatives such as ether-based electrolytes is due to undesired solvent co-intercalation that occurs with graphitic anodes. Here, we show that fluoroethers are the first class of ether solvents to intrinsically support reversible lithium-ion intercalation into graphite without solvent co-intercalation at conventional salt concentrations. In full cells using a graphite anode, they enable 10-fold higher energy densities compared to conventional ethers, and better thermal stability over carbonate electrolytes (operation up to 60 °C) by producing a robust solvent-derived solid electrolyte interphase (SEI). As single-solvent–single-salt electrolytes, they remarkably outperform carbonate electrolytes with fluoroethylene carbonate (FEC) and vinylene carbonate (VC) additives when cycled with graphite–silicon composite anodes. In conclusion, our molecular design strategy opens a new class of electrolytes that can enable next generation Li-ion batteries with higher energy density and a wider working temperature window.

25 ENERGY STORAGE↗
DOE OSTI2026

Interface-induced fast Li+ transport in mixed ionic–electronic conductors

Interfacial instability between lithium metal and solid-state electrolytes limits the performance of all-solid-state lithium metal batteries (ASSLBs), leading to parasitic reactions, non-uniform Li+ flux, and dendrite growth. Here, we develop a composite interlayer composed of the anti-perovskite Li2OHCl0.75Br0.25 (AP) and carbon nanotubes (CNTs) to enhance both interfacial stability and ionic transport. The AP–CNT interlayer exhibits enhanced Li+ conductivity arising from interfacial electron transfer from AP to CNTs, which generates a built-in electric field that facilitates Li+ migration. Lithium symmetric cells incorporating this interlayer achieve a high critical current density of 2.4 mA cm−2 at 55 °C. This design integrates chemical robustness with coupled ion–electron transport, offering a generalizable strategy for safe, dendrite-free, and high-performance ASSLBs.

He, Chenche↗
DOE OSTI2020

Temperature-induced changes in the synthesis gas composition in a high-temperature H 2 O and CO 2 co-electrolysis system

Solid oxide electrolysis cell (SOEC) is an attractive renewable technology capable of producing synthesis gas (H 2 + CO) from H 2 O and CO 2 . An SOEC consists of a solid oxide electrolyte and two ceramic or metal-ceramic electrodes. H 2 O and CO 2 are electrolyzed at the cathode producing H 2 and CO, releasing O 2- ions, which travel through the electrolyte to the anode side and recombine to produce pure oxygen gas as the byproduct. In the present study, a La 0.7 Sr 0.2 Ni 0.2 Fe 0.8 O 3 cathode was used to co-electrolyze H 2 O and CO 2 at three different operating temperatures- 700 °C, 750 °C and 800 °C. Synthesis gas was produced at all three operating temperatures with 100% Faradaic efficiency. The composition of the syngas, however, was found to be a function of the operating temperature. In general, the H 2 /CO ratio in the syngas decreased with increased temperature. This was partially due to CO 2 electrolysis becoming more favorable compared to H 2 O electrolysis at higher temperatures.

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

Aliovalent Anion Incorporation in Halide Na-ion Conductors for Enhanced Ionic Conductivity

Halide-based solid electrolytes (SEs), particularly zirconium (Zr)-centered halides, are attractive from a material cost perspective. Nevertheless, Zr-centered halide SEs are hindered by their low ionic conductivity. Here, in this study, we report on the cubic Na 3 ZrCl 5 S superionic conductor through strategic sulfur anion incorporation, achieving 10 times higher ionic conductivity than that of Na 2 ZrCl 6 . With the optimal composition, the highest ionic conductivity of 0.753 mS cm –1 is obtained for the 0.6Na 2 S–1.4NaCl–ZrCl 4 compound. When paired with a NaCrO 2 cathode, the assembled all-solid-state batteries (ASSBs) achieve a specific discharge capacity of 110 mA h g –1 at 0.1C and exhibit long-term cycling stability at 0.3C at room temperature over 1000 cycles (with 83% capacity retention). Moreover, in situ electrochemical impedance spectroscopy combined with distribution of relaxation times analysis reveal the dynamically interfacial stability between Na halide with electrodes. In conclusion, this work highlights the design and synthesis of advanced halide electrolytes through anion incorporation, paving the way for the development of next-generation ASSBs.

Guo, Xiaolin [Univ. of Louisville, KY (United Stat↗
DOE OSTI2022

Operating High-Energy Lithium-Metal Pouch Cells with Reduced Stack Pressure Through a Rational Lithium-Host Design

Transitioning from a liquid electrolyte to an inorganic solid electrolyte offers a potential pathway to enable highly reversible lithium-metal anodes. However, the solid-electrolyte-protected lithium-metal anode suffers from poor interfacial ionic contacts and requires an impractically high stack pressure (>1.0 MPa) to maintain the interfacial contacts. It is demonstrated here that combining a hollow silver/carbon fiber scaffold and an inorganic/organic composite electrolyte enables a highly reversible lithium-metal anode. Since the high surface area of the electrode provides intimate contact and the hollow structure of the electrode relieves the lithium plating-induced stress, the electrode/electrolyte interface remains stable during cycling even under mild stack pressure. This unconventional structural design is validated in practical pouch cells assembled with the 3D lithium host containing a onefold excess of lithium and a high-nickel cathode. At a mild stack pressure of 320 kPa, the pouch cell displays 83% capacity retention for 200 cycles. This work illustrates that combining a hollow electrode architecture and a robust solid electrolyte offers a practical pathway toward rechargeable lithium-metal anodes.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Electrospinning of PVdF-HFP: novel composite polymer electrolytes (CPES) with enhanced ionic conductivities for lithium-sulfur batteries

The invention relates to lithium ion batteries and, more particularly, to lithium ion conducting composite polymer electrolyte separators. The separators include a nanofiber mat composed of electrospun nanofibers. The nanofibers include a polymer having one or more polar halogen groups, a lithium-containing solid or liquid electrolyte and nanoparticle filler. The polymer, electrolyte and filler are combined to form a solution that is subjected to the electro-spinning process to produce electrospun nanofibers in the form of the mat.

Kumta, Prashant N.↗
DOE OSTI2023

Composite Cathode Architectures Made By Freeze-Casting for All Solid State Lithium Batteries (CRADA Final Report)

As part of a Battery 500 seedling project, MBRDNA partnered with LBNL and Montana State University (MSU) to develop solid-state batteries based on an Al-substituted LLZO (Li 7 La 3 Zr 2 O 12 ) ceramic ion-conductor. All solid-state lithium batteries are attractive contenders for use as power sources for electric vehicles because of their potential for better safety and higher energy density than state-of-the-art lithium-ion batteries, although they are still at early stages of development. Al-substituted LLZO is one of the most promising solid electrolytes for battery applications based on high ionic conductivity, a wide operating voltage window, and apparent stability vs. reduction by lithium. However, difficulties with processing thin (< 20 $\textit{um}$ and dense LLZO membranes have hampered development of devices based on this material. It is non-compressible and must be sintered at high temperatures to densify components. It is also difficult to maintain contact between the active cathode material and LLZO in the composite cathodes, which is critical for successful operation. This research project aimed to use novel processing methods to overcome these issues. The end result was the first ever-reported truly all solid-state battery based on LLZO operating at room temperature without application of exogenous pressure. During the course of the project, we also identified a number of issues that need to be addressed to improve the technology readiness level of this battery.

25 ENERGY STORAGE↗
DOE OSTI2020

Exploiting the Spinel Structure for Li-ion Battery Applications: A Tribute to John B. Goodenough

This review provides a personal account of career-long efforts, interwoven with the contributions of others, to exploit the [B 2 ]O 4 framework of an A[B 2 ]O 4 spinel structure for lithium-ion battery applications, where A = Li, and B is one or more metal cations. The narrative begins at the Council for Scientific and Industrial Research (CSIR) in South Africa in the mid-1970s when, in response to the Middle East oil crisis, worldwide efforts were turned to develop high-temperature sodium and lithium batteries to power electric vehicles. In 1981, results in CSIR's program on a high-temperature lithium battery led to a collaborative project on room-temperature lithium cells with Prof. John B. Goodenough at Oxford University, where studies of Fe 3 O 4 , Mn 3 O 4 , and LiMn 2 O 4 cathodes led to the recognition of the broad utility of the [B2]O4 spinel framework as an anode, cathode, or solid electrolyte for rechargeable lithium cells. This finding has had a profound and lasting impact, influencing further ideas and discoveries at the CSIR, Argonne National Laboratory, and elsewhere. The narrative emphasizes the compositional versatility of the spinel structure and the opportunities to tailor the electrochemical potential and stability of a Li-ion cell.

25 ENERGY STORAGE↗
DOE OSTI2024

The Key Role of Grain Boundary Dynamics in Revolutionizing the Potential of Solid Electrolytes

Solid electrolytes (SEs) have the potential to enhance the safety and performance of Li-metal batteries. However, the existence of grain boundaries in polycrystalline SEs presents a significant challenge for both ionic and electronic migration, promoting the propagation of detrimental lithium dendrites. This study compares the roles of grain boundaries in electrical properties of three distinct SEs including garnet-type Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 (LLZO), argyrodite-type Li 6 PS 5 Cl (LPSC), and NASICON-type Li 1+x+y Al x (Ti,Ge) 2-x Si y P 3-y O 12 (LATP). Results demonstrate that the electronic and ionic conductivities of solid-state electrolytes are affected differently by grain boundaries, depending on the specific type of electrolyte. For instance, LLZO and LATP experience dielectric breakdown at 3.7 and 5.3 V, respectively, while LPSC does not exhibit such behavior. Here, a new chemical modification is proposed that simultaneously alters the composition of both the surface and grain boundaries of SEs, ultimately reducing electronic conductivity for the LLZO SEs. Consequently, the proposed LLZO exhibits unprecedented dendrite-free cycling stability, achieving a remarkable 12 000-h lifetime at room temperature, surpassing conventional strategies such as surface coatings in dendrite mitigation. This study highlights the significance of modifying grain boundaries to design safe and durable Li-metal batteries. It provides new insights for developing SEs that are highly resistant to dendrite formation.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Design principles for NASICON super-ionic conductors

Na Super Ionic Conductor (NASICON) materials are an important class of solid-state electrolytes owing to their high ionic conductivity and superior chemical and electrochemical stability. In this paper, we combine first-principles calculations, experimental synthesis and testing, and natural language-driven text-mined historical data on NASICON ionic conductivity to achieve clear insights into how chemical composition influences the Na-ion conductivity. These insights, together with a high-throughput first-principles analysis of the compositional space over which NASICONs are expected to be stable, lead to the successful synthesis and electrochemical investigation of several new NASICONs solid-state conductors. Among these, a high ionic conductivity of 1.2 mS cm ₋1 could be achieved at 25 °C. We find that the ionic conductivity increases with average metal size up to a certain value and that the substitution of PO 4 polyanions by SiO 4 also enhances the ionic conductivity. While optimal ionic conductivity is found near a Na content of 3 per formula unit, the exact optimum depends on other compositional variables. Surprisingly, the Na content enhances the ionic conductivity mostly through its effect on the activation barrier, rather than through the carrier concentration. These deconvoluted design criteria may provide guidelines for the design of optimized NASICON conductors.

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

Lithiophilic CoF 2 @C hollow spheres towards spatial lithium deposition for stable lithium metal batteries

Lithium metal (LM) is a promising anode for next-generation batteries due to its high theoretical capacity and low electrode potential. Nonetheless, side reactions, volume change, and unwanted lithium dendrite growth seriously limit the practical application of LM. Herein, with the aid of a hard template approach, a novel lithiophilic CoF 2 -carbon hollow sphere (CoF 2 @C-HS) composite material is successfully prepared via a facile in-situ fluorination and etching strategy. The lithiophilic CoF 2 acts as nucleation sites to reduce nucleation overpotential as well as induces the spatial Li deposition and the formation of LiF-rich solid electrolyte interphase (SEI), and the hollow carbon matrix can enhance the electrical conductivity and offer free space for LM deposition. Theoretical simulations reveal that the synergistic effect of lithiophilic CoF 2 and hollow carbon matrix homogenizes the electric field distribution and Li + flux. Benefiting from these advantages, the CoF 2 @C-HS-modified copper substrate electrode delivers an enhanced Coulombic efficiency (CE) of 93.7% for 280 cycles at 1 mA cm –2 and 1 mA h cm –2 . The symmetrical cell using CoF 2 @C-HS can stably cycle more than 1800 h with a low voltage hysteresis of 11 mV at a current density of 0.5 mA cm –2 and an areal capacity of 0.5 mA h cm –2 . Moreover, the Li@CoF 2 @C-HS composite anode enables more than 300 stable cycles at 1 C with a capacity retention of 95% in LiFePO 4 -based full cell and 110 stable cycles at 1 C in LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811)-based high-voltage full cell. Finally, this work might shed a new light on designing lithiophilic hosts to spatially confine LM deposition, realizing dendrite-free LM anodes and the practical applications of LM batteries.

25 ENERGY STORAGE↗
DOE OSTI2020

Elastic NaxMoS2-carbon-BASE triple interface direct robust solid-solid interface for all-solid-state Na-S batteries

The promises of all-solid-state (ASS) sodium batteries for the next generation energy storage are widely recognized but their developments have been severely constrained by the difficulties to design favorable solid-solid interfaces for unhindered Na-ion transport. Using the most promising ß?-Al2O3 solid state electrolyte (BASE) as a platform, we demonstrate here a triple nanojunction strategy that provides simultaneous strong Na adhesion and continuous Na-ions diffusion at solid-solid interface. Such triple junctions (NaxMoS2-carbon-BASE) were constructed by adhering ternary composite Na anodes containing dispersed 3 wt% MoS2 and 3 wt% carbon on BASE, and provide nearly complete adhesion of Na on BASE with a much smaller contact angle (~ 45o vs. 120o of pristine Na). The composite Na anodes exhibited ~ 3 times improved elastic property and the synergy of NaxMoS2 and carbon provides the required ionic and electronic diffusion channels at solid-solid interface, which significantly improve Na utilization and resist premature failure due to loss of solid-solid contact as Na shrink during high capacity stripping. As a result, Na metal at the triple junction exhibited more than five time reduced charge transfer resistance and at least 200 hours stable battery cycling at practical current densities. The novel anode architecture also enabled high capacity cycling of prototype ASS sodium sulfur batteries when coupled with advanced sulfur cathodes containing intrinsic Na-ions diffusion channels and redox catalytic mediators, leading to stable cycling with specific capacity of 1110 mAh g-1.

ß”-Al2O3 solid electrolyte, solid state batteries,↗
DOE OSTI2020

High-Energy All-Solid-State Organic–Lithium Batteries Based on Ceramic Electrolytes

Recent studies have identified unique properties of organic battery electrode materials such as moderate redox potentials and mechanical softness which are uniquely beneficial for all-solid-state batteries based on ceramic electrolytes. Here, we further explore the promise of organic materials and demonstrate a sulfide electrolyte- based organic-lithium battery with a specific energy of 828 Wh kg –1 , rivaling the state-of- the-art of all-solid-state batteries. Two innovation steps are responsible for the accomplishment. First, the combination of lithium anode and the high-capacity cathode material pyrene-4,5,9,10-tetraone ensures a high theoretical specific energy. Second, the microstructure of the organic cathode is optimized with the introduction of cryomilling, a technique common to processing soft materials but not familiar to electrode fabrication. The cathode material utilization increases to 99.5% as a result, up from the 55–89% previously reported for ceramic electrolyte-based solid-state organic batteries. In conclusion, the improvement highlights the special requirements of solid-state organic electrodes for microstructural engineering while preserving the chemical integrity of components.

25 ENERGY STORAGE↗
DOE OSTI2021

Highly Ordered Hierarchical Anodes for Extreme Fast Charging Batteries (Final Report)

The goal of this project is to enable extreme fast charging (XFC) of Li-ion batteries, which was accomplished through a combination of 1) rational design and manufacturing of hierarchically structured anode architectures; 2) blending graphite/hard carbon into a bulk hybrid anode; 3) engineering artificial solid-electrolyte interphase (SEI) coatings with reduced interphase impedance; 4) computational modeling of coupled transport, kinetic, and electrochemical phenomena; and 5) improved fundamental understanding of lithium plating through operando analysis. This work integrated structural, compositional, and surface modification of graphite anodes, multi-physics modeling of ion transport, electrochemical activity, and heat transfer, advanced strategies to detect Li plating, and semi-automated roll-to-roll cell assembly. The unique facilities at the University of Michigan (UM) and Sandia National Laboratories (SNL) were leveraged to manufacture, prototype, and characterize commercially relevant >2Ah and >180 Wh/kg cells with a target of <20% capacity fade over 500 XFC cycles.

25 ENERGY STORAGE↗
DOE OSTI2022

Ammonia eurefstics: Electrolytes for liquid energy storage and conversion at room temperature and ambient pressure

Herein we report the transformation of gaseous ammonia to a liquid at room temperature and ambient pressure through mixing with simple solid ammonium salts. The resulting liquids, named eurefstics, are potentially advantageous for the storage and electrochemical conversion of ammonia and the realization of a green ammonia energy economy. Physical properties of these eurefstics, including the temperature-dependent composition and composition-dependent densities, are reported to glean initial insight into the formation and behavior of this intriguing liquid. Preliminary electrochemical investigations of the eurefstics were also performed. We have found that these eurefstics formed are conductive and can be used directly as electrolytes for ammonia electrolysis reactions to produce hydrogen on demand. Open-circuit potential measurements were also made to determine the formal potential of the hydrogen evolution and corresponding overpotentials. Finally, safety concerns of the eurefstics are discussed in comparison with other liquid phase energy carriers.

25 ENERGY STORAGE↗
DOE OSTI2023

Low Impedance Cathode/Electrolyte Interfaces for High Energy Density Solid-State Batteries

All-solid-state batteries (ASSBs) using a ceramic fast Li-ion conductor as a solid-state electrolyte (SSE) have been proposed as a promising strategy to significantly increase the energy density of lithium batteries. Due to their high ion conductivity and excellent stability, Li-stuffed garnets exhibit the most promising physical and chemical properties for SSEs. However, the typical microstructure, thick (>100 μm) bulk electrolyte and simple planar electrode/electrolyte interfaces, combined with poor electrode wetting of the garnet result in excessively high area specific resistances (ASRs) that severely limit achievable current density and cell energy density. In this project, the team is building on their demonstrated expertise with garnet electrolytes and ASSBs to accomplish the following: (1) engineer interfaces to overcome high NMC/LLZ interfacial impedance and interfacial degradation; (2) develop processing and fabrication techniques to achieve high loading NMC/LLZ composite cathodes with low resistance and high cyclability; and (3) integrate the NMC/LLZ cathodes into all-solid-state Li-metal/LLZ cells to achieve high-energy-density batteries.

25 ENERGY STORAGE↗