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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 181 records · Page 10
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

A quantitative imaging framework for lithium morphology: Linking deposition uniformity to cycle stability in lithium metal batteries

Characterizing the morphology of lithium (Li) is crucial for developing long-lasting lithium metal batteries. It is well established that more uniform Li deposition correlates with better cell performance. Li morphology is often characterized through qualitative analysis of scanning electron microscopy (SEM) images; however, there are no widely accepted metrics to quantitatively describe deposition uniformity. Here, we propose a framework to quantify uniformity through SEM image analysis via the index of dispersion (ID) metric, which is defined and presented in the context of Li metal batteries. We also explore experimental impacts of sampling protocols onIDmeasurements. Our results demonstrate that theIDmetric is highly sensitive to variations in deposition uniformity, including the coexistence and uniformity of multiple morphologies, uniformity within a single morphology, and particle size distribution uniformity. Furthermore, it is demonstrated that uniformity, as measured by theID, can be related to the average potential of Li||Li symmetric cells over cycling. Higher capacity cycling leads to more pronounced changes in bothIDand average cell potential. Local minima/maxima are found consistently in bothIDand average cell potential immediately before cells short-circuit, which we suggest may indicate a collapse of the microstructure prior to failure. We put forward this framework as a more robust approach to quantify Li deposition uniformity, advancing the development of Li metal batteries that are safer and longer lasting.

Science & Technology - Other Topics↗
DOE OSTI2023

High-entropy electrolytes for practical lithium metal batteries

Electrolyte engineering is crucial for improving battery performance, particularly for lithium metal batteries. Recent advances in electrolytes have greatly improved cyclability by enhancing electrochemical stability at the electrode interfaces, but concurrently achieving high ionic conductivity has remained challenging. Here we report an electrolyte design strategy for enhanced lithium metal batteries by increasing the molecular diversity in electrolytes, which essentially leads to high entropy electrolytes (HEEs). We find that in weakly solvating electrolytes, the entropy effect reduces ion clustering while preserving the characteristic anion-rich solvation structures, which is characterized by synchrotron-based X-ray scattering and molecular dynamics simulations. Electrolytes with smaller- sized clusters exhibit a 2-fold improvement in ionic conductivity compared to conventional weakly- solvating electrolytes, enabling stable cycling at high current densities up to 2C (6.2 mA cm -2 ) in anode- free LiNi 0.6 Mn 0.2 Co 0.2 (NMC622)||Cu pouch cells. In conclusion, the efficacy of the design strategy is verified by performance improvements in three disparate weakly solvating electrolyte systems.

25 ENERGY STORAGE↗
DOE OSTI2023

Evaluation of Lithium Metal Anode Volumetric Expansion through Laser Plasma Focused Ion Beam Cross-Sectional Imaging

Lithium metal is an ideal anode for high energy density batteries, however the implementation of lithium metal anodes remains challenging. Beyond the development of highly efficient electrolytes, degradation processes restrict cycle life and reduce practical energy density. Herein lithium volumetric expansion and degradation pathways are studied in half cells through coupling electrochemical analysis with cross-sectional imaging of the intact electrode stack using a cryogenic laser plasma focused ion beam and scanning electron microscope. Here, we find that the volumetric capacity is compromised as early as the first cycle, at best reaching values only half the theoretical capacity (1033 vs 2045 mAh cm -3 ). By the 101st electrodeposition, the practical volumetric capacity decreases to values ranging from 143 to 343 mAh cm -3 .

25 ENERGY STORAGE↗
DOE OSTI2022

A Fiber-Based 3D Lithium Host for Lean Electrolyte Lithium Metal Batteries

3D hosts are promising to extend the cycle life of lithium metal anodes but have rarely been implemented with lean electrolytes thus impacting the practical cell energy density. To overcome this challenge, a 3D host that is lightweight and easy to fabricate with optimum pore size that enables full utilization of its pore volume, essential for lean electrolyte operations, is reported. The host is fabricated by casting a VGCF (vapor-grown carbon fiber)-based slurry loaded with a sparingly soluble rubidium nitrate salt as an additive. The network of fibers generates uniform pores of ≈3 µm in diameter with a porosity of 80%, while the nitrate additive enhances lithiophilicity. This 3D host delivers an average coulombic efficiency of 99.36% at 1 mA cm -2 and 1 mAh cm -2 for over 860 cycles in half-cell tests. Full cells containing an anode with 1.35-fold excess lithium paired with LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cathodes exhibit capacity retention of 80% over 176 cycles at C/2 under a lean electrolyte condition of 3 g Ah -1 . This work provides a facile and scalable method to advance 3D lithium hosts closer to practical lithium-metal batteries.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Polymers in Lithium‐Ion and Lithium Metal Batteries

Abstract Lithium‐ion batteries play a significant role in modern electronics and electric vehicles. However, current Li‐ion battery chemistries are unable to satisfy the increasingly heightened expectations regarding energy demand and reliability. To boost the overall energy density while ensuring the safety of Li batteries, researchers have focused on alternative battery materials, such as silicon, sulfur, and Li metal. These represent promising avenues, although numerous obstacles (e.g., Si cracking, polysulfide shuttling, Li dendrites, etc.) must be tackled before batteries based on these materials can enter mass production and penetrate the mainstream market. Polymers are a class of materials that are widely used in current battery systems; however, many novel polymer chemistries may offer better performance and reliability than the current ones, and even overcome the issues of the above‐mentioned new battery materials. In this review, selected polymeric materials for solving these issues are categorized into four parts: polymer electrolytes, polymer artificial solid‐electrolyte interphases, binders, and separators. Both the current progress and the characterization methods are included. Potential future directions of energy materials research are pointed out as well.

Li, Junheng↗
DOE OSTI2025

Dimolybdenum Paddlewheel Complexes with Cation Binding Sites as Electrolyte Additives to Manipulate the Solid-Electrolyte Interphase at Lithium Metal Anodes

The use of electrolyte additives at millimolar loadings to control the surface chemistry of lithium metal anodes (LMAs) is a leading strategy to improve lithium metal batteries and promote electrosynthetic reactions. Whereas previous studies employed either inorganic or organic additives, in this study, we report the first organometallic additive, Mo 2 (mea) 4 [1, mea = 2-(2-methoxyethoxy)acetate], a dimolybdenum paddlewheel complex that is stable under Li plating conditions and features cation binding sites in the second coordination sphere that promote reversible Li + coordination. Binding of Li + ions to 1 induces immobilization of cationically charged aggregates (or products thereof) into the solid electrolyte interphase (SEI), imparting multiple beneficial functions. The modified SEI was found to protect the LMA against parasitic side reactions, produce modest but measurable improvements to Li plating properties (e.g., overpotential, surface structure, and Coulombic efficiency), and improve interfacial charge transport properties. Furthermore, the most notable benefit to battery cycling performance appears in calendar aging tests, which show that the presence of the additive protects the LMA from parasitic side reactions that would otherwise decrease overall cell cycling efficiency over time. Collectively, these data disclose a tactic for designing electrolyte additives using principles of organometallic synthesis.

Additives↗
DOE OSTI2020

A Quantitative Failure Analysis on Capacity Fade in Rechargeable Lithium Metal Cells

Rechargeable lithium battery (RLB) technology is transforming portable devices, vehicle electrification, and grid modernization. To make RLB durable, reliable and safe, conducting failure mode and effect analysis (FMEA) to identify failure mechanism under the operating conditions is very desirable. However, this ability is often overlooked or even lacking. The failure analysis (FA) is often conducted by laboratory testing and postmortem analysis, and the knowledge typically empirical. Here we present a quantitative approach for FMEA that can reveal how failure modes and effects reduce the capacity of a RLB. This approach is based on the state of the battery for FMEA, contrary to the conventional approach based on operating or testing conditions. The key aspect of this FMEA method is to convert the experimental results to a state-of-charge (SOC)-based analytic methodology. Such a conversion can separate the thermodynamic and kinetic attributes of capacity fade based on compositional correspondence in the electrode, so the loss and the decreased utilization of the active materials can be determined respectively.

25 ENERGY STORAGE↗
DOE OSTI2021

Lithium metal synthesis

System and methods for producing lithium metal from an anodic half-cell and a cathodic half-cell with a lithium permeable membrane therebetween.

Hryn, John N.↗
DOE OSTI2021

Enabling High-Performance NASICON-Based Solid-State Lithium Metal Batteries Towards Practical Conditions

Solid-state lithium metal batteries (SSLMBs) are promising next-generation high-energy rechargeable batteries. However, the practical energy densities of the reported SSLMBs have been significantly overstated due to the use of thick solid-state electrolytes, thick lithium (Li) anodes, and thin cathodes. Here, a high-performance NASICON-based SSLMB using a thin (60 µm) Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP) electrolyte, ultrathin (36 µm) Li metal, and high-loading (8 mg cm -2 ) LiFePO 4 (LFP) cathode is reported. The thin and dense LAGP electrolyte prepared by hot-pressing exhibits a high Li ionic conductivity of 1 × 10 -3 S cm -1 at 80 °C. The assembled SSLMB can thus deliver an increased areal capacity of ≈1 mAh cm -2 at C/5 with a high capacity retention of ≈96% after 50 cycles under 80 °C. Furthermore, it is revealed by synchrotron X-ray absorption spectroscopy and in situ high-energy X-ray diffraction that the side reactions between LAGP electrolyte and LFP cathode are significantly suppressed, while rational surface protection is required for Ni-rich layered cathodes. This study provides valuable insights and guidelines for the development of high-energy SSLMBs towards practical conditions.

25 ENERGY STORAGE↗
DOE OSTI2023

Silver-carbon interlayers in anode-free solid-state lithium metal batteries: Current development, interfacial issues, and instability challenges

As an interlayer between the anode and the electrolyte of the all-solid-state lithium metal batteries (ASSLMBs), the silver-carbon (Ag-C) nanocomposite has been reported to significantly increase the energy density and cycle rate of solid-state lithium metal batteries. Ag-C interlayers serve as mixed ionic-electronic conductor that conducts both Li+ ions and electrons and lithium storage capacity. Unfortunately, it was unclear how the Ag-C interlayer regulated lithium plating and stripping. Moreover, the structural and chemical instabilities between the interlayer and the electrolyte, within the interlayer, or beneath the interlayer on lithium substrate are likely to cause cell failure. In this review, we discuss interfacial issues and summarize recent progress in solution strategies for ASSLMBs, with a specific focus on the use of a silver-carbon (Ag-C) nanocomposite interlayer in anode-free setups. Based on the Li transport kinetics among the Ag-C interlayers, the interfacial configurations of Ag-C interlayers are classified as either exterior or internal. Furthermore, the review concludes with a discussion of the perspectives and future prospects, allowing for the improvement of interlayer techniques for solid-state batteries.

25 ENERGY STORAGE↗
NASA NTRS2021

Local Ultrasonic Resonance Spectroscopy of Lithium Metal Batteries for Aerospace Applications

As next-generation aircraft and vehicles continue to develop, so do their associated energy demands. Lithium metal batteries are a leading candidate to fulfill this energy requirement, but these batteries are prone to internal dendrite defects that can lead to catastrophic thermal runaway events. Current battery management systems are capable of mitigating such risks, but are unable to detect such defects until thermal runaway has already begun. Various nondestructive evaluation (NDE) techniques, particularly ultrasonic NDE, can directly monitor internal battery parameters giving them the potential to detect critical defects prior to catastrophic failure. However, most of the current battery NDE research has focused on improved battery state-of-charge (SOC) and stateof- health (SOH) monitoring with little emphasis on critical defect detection. Thus, a measurement technique sensitive to subtle battery defects is needed. In addition, the complex mechanics of ultrasound in porous, thin, multilayered batteries prompt the use of physics-based simulation to guide inspections. In this work, an ultrasonic NDE technique has been developed utilizing frequency domain analysis of local battery resonances to detect the presence of battery defects. This technique is a practical extension of local ultrasonic resonance spectroscopy (LURS) – which previously required non-contact laser ultrasonics – to measurements with piezoelectric contact and immersion scan transducers. To extend the technique to work with piezoelectric transducers, ultrasonic battery measurements were compared to a sans-battery calibration measurement. Then, a linear systems deconvolution was used to eliminate the transfer functions of extraneous factors such as the transducer and electronics, leaving only the frequency-dependent battery reflection coefficient. The LURS technique was first validated on stainless steel and aluminum plates, producing reflection coefficients in line with analytical and numerical finite element modeling (FEM) results. Functioning Li-metal pouch cells were then seeded with lithium chip defects prior to LURS measurements. The presence of these defects is shown to cause a measurable shift in the battery’s through-thickness local resonances. 2D, frequency-domain poroelastic models of ultrasonic propagation in a single-cell lithium metal pouch battery were created and corroborated these findings. Thus, this work has both extended and proven the feasibility of the LURS technique in the detection of local battery defects.

Ultrasound↗
DOE OSTI2021

Identification of LiH and nanocrystalline LiF in the solid–electrolyte interphase of lithium metal anodes

A comprehensive understanding of the solid–electrolyte interphase (SEI) composition is crucial to developing high-energy batteries based on lithium metal anodes. A particularly contentious issue concerns the presence of LiH in the SEI. In this work, we report on the use of synchrotron-based X-ray diffraction and pair distribution function analysis to identify and differentiate two elusive components, LiH and LiF, in the SEI of lithium metal anodes. LiH is identified as a component of the SEI in high abundance, and the possibility of its misidentification as LiF in the literature is discussed. LiF in the SEI is found to have different structural features from LiF in the bulk phase, including a larger lattice parameter and a smaller grain size (<3 nm). These characteristics favour Li + transport and explain why an ionic insulator, like LiF, has been found to be a favoured component for the SEI. Finally, pair distribution function analysis reveals key amorphous components in the SEI.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Lattice engineering of high-entropy olivine-type lithium metal phosphate as high-voltage cathodes

Engineering of high-entropy cathode materials for lithium-ion batteries has been actively pursued owing to the outstanding conductivity of high-entropy materials benefited from the maximum entropy and unique antisite disordering structure. Olivine lithium metal phosphates such as LiMnPO 4 and LiNiPO 4 feature high working voltages but low capacities due to their insulation nature. Here in this work, the synthesis of the high-entropy lithium metal phosphate materials (HELMPs) is realized by combining mechanochemistry with a calcination method. By regulating lattice of HELMPs, the high-entropy Li(Mn 0.35 Fe 0.35 Co0.1Mg 0.1 Ca 0.1 )PO 4 reveals three typical high-voltage plateaus in charge–discharge curves corresponding to the redox of Fe, Mn, and Co in the voltage range of 2.0–4.9 V vs Li + /Li, and a much higher initial capacity than LiMnPO 4 (104 vs 15 mAh g -1 ).

25 ENERGY STORAGE↗
DOE OSTI2024

Molecular Engineering Enabled Stable Deep Eutectic Amide-Based Electrolyte for High-Temperature Lithium–Metal Batteries

The development of advanced lithium-metal batteries (LMBs), such as high-temperature LMBs and high-energy-density LMBs, has critical requirements for electrolytes. However, conventional electrolytes suffer from thermal instability and insufficient electrolyte/Li interfacial compatibility, severely limiting their utilization in high-temperature LMBs. Herein, we design a high-temperature N-methylacetamide (NMAc)-based deep eutectic electrolyte (DEE) by molecular engineering on a solvation structure via a sacrificial additive of vinyl ethylene carbonate (VEC). Specifically, VEC interacts with the Li prior to NMAc, facilitating the formation of a solid electrolyte interphase to inhibit the reaction between Li and NMAc. The stable VEC-DEE effectively suppresses the growth of lithium dendrites and ensures the battery a cycling stability of 550 cycles at 80 °C. Additionally, we also demonstrate the application of VEC-DEE in high-energy-density LMBs with a high mass loading of 2.5 mAh/cm 2 . In conclusion, this research opens a new avenue for the rational design of advanced high-temperature electrolytes.

25 ENERGY STORAGE↗
DOE OSTI2022

Performance Improvement of Lithium Metal Batteries Enabled By LiBF 3 CN as a New Electrolyte Additive

A newly synthesized electrolyte additive, lithium trifluoro(cyano) borate (LiBF 3 CN), has been investigated for electrochemical performance improvement of lithium metal batteries. The LiBF 3 CN has a structure where one fluorine atom of BF 4 – is substituted with a cyano group (–CN) prepared by the reaction of boron trifluoride etherate with lithium cyanide. The electrochemical performance in symmetric Li/Li cells and NCM523/Li cells is significantly improved upon the incorporation of LiBF 3 CN as an electrolyte additive into a carbonate-based electrolyte. Extensive characterization of the deposited lithium metal reveals that a thin (≈20 nm) and robust SEI composed of LiN x O y , Li 3 N and Li 2 O is formed by the reductive decomposition of the LiBF 3 CN additive, which plays an important role in decreasing the resistance and stabilizing lithium deposition/stripping. The insight into the substitution effect of a functional group obtained from this work provides guidance for the design of new electrolyte additives.

25 ENERGY STORAGE↗
DOE OSTI2021

Evolution of Protrusions on Lithium Metal Anodes Stabilized by a Solid Block Copolymer Electrolyte Studied Using Time-Resolved X-ray Tomography

The growing demand for rechargeable batteries with higher energy densities has motivated research focused on enabling the lithium metal anode. A prominent failure mechanism in such batteries is short circuiting due to the uncontrolled propagation of lithium protrusions that often have a dendritic morphology. In this paper, the electrodeposition of metallic lithium through a rigid polystyrene- b -poly(ethylene oxide) (PS- b -PEO or SEO) block copolymer electrolyte was studied using hard X-ray microtomography. In this system, protrusions were approximately ellipsoidal globules: we take advantage of this simple geometry to quantify their growth as a function of polarization time and electrolyte salt concentration. The growth of 47 different globules was tracked with time to obtain average velocities of globule growth into the electrolyte. The globule diameter was a linear function of globule height in the electrolyte with a slope of about 6, independent of time and electrolyte salt concentration.

25 ENERGY STORAGE↗