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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 OSTI2023

Direct in situ measurements of electrical properties of solid–electrolyte interphase on lithium metal anodes

The solid–electrolyte interphase (SEI) critically governs the performance of rechargeable batteries. An ideal SEI is expected to be electrically insulative to prevent persistently parasitic reactions between the electrode and the electrolyte and ionically conductive to facilitate Faradaic reactions of the electrode. However, the true nature of the electrical properties of the SEI remains hitherto unclear due to the lack of a direct characterization method. Here we use in situ bias transmission electron microscopy to directly measure the electrical properties of SEIs formed on copper and lithium substrates. We reveal that SEIs show a voltage-dependent differential conductance. A higher rate of differential conductance induces a thicker SEI with an intricate topographic feature, leading to an inferior Coulombic efficiency and cycling stability in Li||Cu and Li||LiNi 0.8 Mn 0.1 Co 0.1 O 2 cells. Further, our work provides insight into the targeted design of the SEI with desired characteristics towards better battery performance.

25 ENERGY STORAGE↗
DOE OSTI2023

Prospective Application, Mechanism, and Deficiency of Lithium Bis(oxalate)Borate as the Electrolyte Additive for Lithium-Batteries

Lithium bis(oxalate)borate (LiBOB) is one of the most common film-forming electrolyte additives used in lithium ion batteries (LIBs), since it can form a dense boron-containing polymer as a solid electrolyte interlayer (or cathode electrolyte interlayer) in order to isolate the electrode material from the electrolyte and prevent side reactions. LiBOB can serve as HF scavenger to maintain the structural integrity of electrodes via avoiding the transition metal dissolution caused by HF attack. Additionally, LiBOB also can react with LiPF 6 to generate lithium difluoro (oxalate)borate (LiDFOB) that can be further used as a clean-up agent for reactive oxygen radicals. This article lists the application of LiBOB in high capacity and high voltage cathode materials, and also reviews the working mechanisms of LiBOB used in these materials to improve the performance of LIBs. Finally, it presents the current shortcomings of LiBOB and strategies to overcome these. This article is expected to provide useful insights for employing LiBOB as a feasible method of dealing with the difficulty of running high capacity LIBs stably under high voltage.

25 ENERGY STORAGE↗
NASA NTRS2010

A Study on Advanced Lithium-Based Battery Cell Chemistries to Enhance Lunar Exploration Missions

NASAs Exploration Technology Development Program (ETDP) Energy Storage Project conducted an advanced lithium-based battery chemistry feasibility study to determine the best advanced chemistry to develop for the Altair Lunar Lander and the Extravehicular Activities (EVA) advanced Lunar surface spacesuit. These customers require safe, reliable batteries with extremely high specific energy as compared to state-of-the-art. The specific energy goals for the development project are 220 watt-hours per kilogram (Wh/kg) delivered at the battery-level at 0 degrees Celsius ( C) at a C/10 discharge rate. Continuous discharge rates between C/5 and C/2, operation between 0 and 30 C and 200 cycles are targeted. Electrode materials that were considered include layered metal oxides, spinel oxides, and olivine-type cathode materials, and lithium metal, lithium alloy, and silicon-based composite anode materials. Advanced cell chemistry options were evaluated with respect to multiple quantitative and qualitative attributes while considering their projected performance at the end of the available development timeframe. Following a rigorous ranking process, a chemistry that combines a lithiated nickel manganese cobalt oxide Li(LiNMC)O2 cathode with a silicon-based composite anode was selected as the technology that can potentially offer the best combination of safety, specific energy, energy density, and likelihood of success.

Reid, Concha M.↗
DOE OSTI2020

In Situ Formation of Li 3 P Layer Enables Fast Li + Conduction across Li/Solid Polymer Electrolyte Interface

Abstract Solid‐state polymer electrolytes provide better flexibility and electrode contact than their ceramic counterparts, making them a worthwhile pursuit for all‐solid‐state lithium‐metal batteries. However, their large Li/solid state electrolyte interfacial resistance, small critical current density, and rapid lithium dendrite growth during cycling still limit their viability. Owing to these restrictions, all‐solid‐state cells with solid polymer electrolytes must be cycled above room‐temperature and with a small current density. These problems can be mitigated with an in situ formed artificial solid electrolyte interphase that rapidly conducts Li + ions. Herein, a Li 3 P layer formed in situ at the Li‐metal/solid polymer electrolyte interphase is reported that significantly reduces the electrode/electrolyte interfacial resistance. Additionally, this layer increases the wettability of the solid polymer by the metallic lithium anode, allowing for the critical current density of lithium symmetric cells to be doubled by homogenizing the current density at the interface. All‐solid‐state Li/Li symmetric cells and Li/LiFePO 4 cells with the Li 3 P layer show improved cycling performance with a high current density.

Wu, Nan↗
DOE OSTI2020

Review on organosulfur materials for rechargeable lithium batteries

Organic electrode materials have been considered as promising candidates for the next generation rechargeable battery systems due to their high theoretical capacity, versatility, and environmentally friendly nature. Among them, organosulfur compounds have been receiving more attention in conjunction with the development of lithium-sulfur batteries. Usually, organosulfide electrodes can deliver relatively high theoretical capacity based on reversible breakage and formation of disulfide (S-S) bonds. Here, we provide an overview of organosulfur materials for rechargeable lithium batteries, including their molecular structural design, structure related electrochemical performance study as well as electrochemical performance optimization. In addition, recent progress of advanced characterization techniques for investigation of the structure and lithium storage mechanism of organosulfur electrodes are elaborated. To further understand the perspective application, additive effect of organosulfur compounds for lithium metal anodes, sulfur cathodes as well as high voltage inorganic cathode materials are reviewed with typical examples. Finally, some remaining challenges and perspective of the organosulfur compounds as lithium batteries components are also discussed. This review is intended to serve as a general guidance for researcher to facilitate the development of organosulfur compounds.

25 ENERGY STORAGE↗
DOE OSTI2020

High energy, long cycle life electrode for lithium-ion batteries

Anodes for electrochemical cells and batteries are described herein. In particular, and anode comprises silicon oxide particles on a transition metal current collector (e.g., copper, nickel, copper alloy, and the like), wherein the particles comprise nanocrystalline domains of silicon dispersed within a silicon oxide matrix. The particles do not include a metal oxide coating, and are produced by heating a silicon monoxide powder at a temperature in the range of about 400 to about 1100° C. under an inert atmosphere for about 2 to about 20 hours. In some embodiments, the particles are free from a metal oxide coating and have an average diameter of about 20 to 10000 nm; the nanocrystalline domains of silicon comprise about 10 to about 90 mole percent of the particles; and the nanocrystalline domains have dimensions of about 0.2 to about 50 nm in average diameter.

25 ENERGY STORAGE↗
DOE OSTI2022

Overcoming Anode Instability in Solid‐State Batteries through Control of the Lithium Metal Microstructure

Abstract Enabling the lithium metal anode (LMA) in solid‐state batteries (SSBs) is the key to developing high energy density battery technologies. However, maintaining a stable electrode–electrolyte interface presents a critical challenge to high cycling rate and prolonged cycle life. One such issue is the interfacial pore formation in LMA during stripping. To overcome this, either higher stack pressure or binary lithium alloy anodes are used. Herein, it is shown that fine‐grained ( d = 20 µm) polycrystalline LMA can avoid pore formation by exploiting the microstructural dependence of the creep rates. In a symmetric cell set‐up, i.e., LiǀLi 6.25 Al 0.25 La 3 Zr 2 O 12 (LLZO)ǀLi, fine‐grained LMA achieves > 11.0 mAh cm −2 compared to ≈ 3.6 mAh cm −2 for coarse‐grained LMA ( d = 295 µm) at 0.1 mA cm −2 and at moderate stress of 2.0 MPa. Smaller diffusion lengths (≈ 20 µm) and higher diffusivity pathway along dislocations ( D d ≈ 10 −7 cm 2 s −1 ), generated during cell fabrication, result in enhanced viscoplastic deformation in fine‐grained polycrystalline LMA. The electrochemical performances corroborate well with estimated creep rates. Thus, microstructural control of LMA can significantly reduce the required stack pressure during stripping. These results are particularly relevant for “anode‐free” SSBs wherein both the microstructure and the mechanical state of the lithium are critical parameters.

25 ENERGY STORAGE↗
DOE OSTI2022

Long–Cycling Sulfide–Based All–Solid–State Batteries Enabled by Electrochemo–Mechanically Stable Electrodes

Anode significantly determines the energy density of all-solid-state Lithium batteries (ASLBs). Silicon (Si) and Lithium (Li) metal are two of the most attractive anodes because of their ultrahigh theoretical capacities. However, most investigations focus on Li metal; the great potential of Si is underrated. This study investigates Si anode's stability, processability, and cost in ASLBs and compares them with Li metal. Moreover, the single-crystal LiNi 0.8 Co 0.1 Mn 0.1 O 2 is stabilized with a lithium silicate (Li 2 SiO x ) through a scalable sol-gel method. ASLBs with a cell-level energy density of 285 Wh kg -1 are obtained through sandwiching Si anode, thin sulfide solid-state electrolyte membrane, and interface stabilized LiNi 0.8 Co 0.1 Mn 0.1 O 2 . The full cell delivered a high capacity of 145 mAh g -1 at C/3 and maintained stability for 1000 cycles. This work inspires commercializing the ASLBs on a large scale with exciting manufacturing lines for large-scale, safe, and economical energy storage.

25 ENERGY STORAGE↗
DOE OSTI2021

Advanced strategies for the development of porous carbon as a Li host/current collector for lithium metal batteries

Lithium metal is considered a promising anode material for high-energy-density rechargeable batteries because of its high specific theoretical capacity (3860 mAh g -1 , low mass density (0.534 g cm -3 ), and low electrochemical redox potential (-3.04 V vs. the standard hydrogen electrode). However, the high reactivity of Li with the electrolyte leads to the formation of an unstable solid electrolyte interphase (SEI) and continuous side reactions. Also, the non-uniform lithium-ion flux and infinite volume expansion of Li metal cause the growth of Li dendrites. These pose significant safety challenges and cause rapid capacity fading of the lithium metal batteries (LiMBs). To resolve these issues, a low-cost, easily processed, lightweight, high-performance carbon-based porous matrix is considered promising to host Li metal deposition. The three-dimensional (3D) porous nano/microstructured carbon provides sufficient space for Li accommodation during Li plating, buffers the volume changes during Li plating/stripping, and lowers the effective current density contributing to dendrite-free Li deposition. Besides, the outstanding electrochemical and mechanical stability, flexibility and the high electronic conductivity enable the nano/microstructured carbon to serve as both Li host and current collector. The development of 3D carbon/Li composite by mechanical roll-press techniques not only eliminates the complex and risky procedure of making carbon/Li composite based on Li plating or molten Li infusion but also stabilizes the capacity at higher Li plating/stripping rates. Recently, there is an advancement in the lithiophilic decorations of 3D structure to introduce sufficient nucleation sites and the development of artificial SEI on top of the 3D matrix to suppress Li dendrite formation. Such 3D structural modifications create a uniform electric field, lower the Li nucleation overpotential, provide strong mechanical and chemical stability, and stabilize the interface thereby inhibiting the degradation of lithium and the electrolyte. Here we summarize the research progress on porous carbon/Li composites in terms of materials type, structure, fabrication technique, their electrochemical battery performance, and identify the critical challenges that need to be addressed for high-energy-density practical LiMBs.

25 ENERGY STORAGE↗
NASA NTRS1992

Symposium on High Power, Ambient Temperature Lithium Batteries, 180th Meeting of the Electrochemical Society, Phoenix, AZ, Oct. 13-17, 1991, Proceedings

Papers presented in these proceedings are on the state of the art in high-power lithium batteries, a design analysis of high-power Li-TiS2 battery, the performance and safety features of spiral wound lithium/thionyl chloride cells, the feasibility of a superhigh energy density battery of the Li/BrF3 electrochemical system, and an enhanced redox process of disulfide compounds and their application in high energy storage. Attention is also given to the structure and charge-discharge characteristics of mesophase-pitch based carbons, a study of carbons and graphites as anodes for lithium rechargeable cells, Li metal-free rechargeable Li(1+x)Mn2O4/carbon cells, and rechargeable lithium batteries using V6O13/V5O5 as the positive electrode material. Other papers discuss the electrochemical stability of organic electrolytes in contact with solid inorganic cathode materials, the electrochemical behavior of methyl formate solutions, and the interface between a solid polymer electrolyte and lithium anode.

Clark, W. D. K.↗
NASA NTRS1998

The 1997 NASA Aerospace Battery Workshop

This document contains the proceedings of the 30th annual NASA Aerospace Battery Workshop, hosted by the Marshall Space Flight Center on November 18-20, 1997. The workshop was attended by scientists and engineers from various agencies of the U.S. Government, aerospace contractors, and battery manufacturers, as well as international participation in like kind from a number of countries around the world. The subjects covered included nickel-cadmium, nickel-hydrogen, nickel-metal hydride, lithium, lithium-ion, and silver-zinc technologies, as well as various aspects of nickel electrode design.

Brewer, Jeffrey C.↗
DOE OSTI2022

An Investigation of Chemo-Mechanical Phenomena and Li Metal Penetration in All-Solid-State Lithium Metal Batteries Using In Situ Optical Curvature Measurements

Solid-electrolytes (SEs) can provide a pathway to increase energy-density in lithium metal batteries. However, lithium metal penetration through garnet based LLZO solid electrolytes has been identified as a critical failure process. This phenomenon is related to chemo-mechanical processes which are difficult to probe. In particular, characterizing the dynamic mechanical deformations that occur in electrode-SE structures is very challenging. Here study reports in situ curvature measurements that are thus designed to probe chemo-mechanical phenomena that occur during lithium plating. The novel experimental cell configuration created for this work shows that pressure builds up in the Li metal during plating, up until the point where short circuits occur. The resulting data are analyzed with a detailed finite element model (FEM) to quantitatively evaluate stress evolution. The results show that Li metal plating within a surface flaw can produce stress build-up prior to short-circuiting. The combined results from both the experiments and the FEM suggest that it is critical to minimize surface defects and flaws during the manufacturing processes.

25 ENERGY STORAGE↗
DOE OSTI2020

In situ Diagnostics of Coupled Electrochemical-Mechanical Properties of Solid Electrolyte Interphases on Lithium Metal Rechargeable Batteries (Final Technical Report)

The fundamental understanding of the coupled mechanical/chemical degradation of the SEI layer during lithium cycling will enable the project to identify the desirable mechanical properties on SEI/lithium as a system and the specific transport properties that enable the homogenous lithium stripping/plating while avoiding the mossy structure. Furthermore, it will allow the project to develop a highly impactful strategy to protect lithium metal and achieve dendrite free high cycle efficiency, which can dramatically increase the energy density of lithium batteries for EV applications. During past three years, four coherent steps have been taken to solve the coupled mechanical and electrochemical degradation: (1) Developed a comprehensive set of in-situ diagnostic techniques to investigate the coupled mechanical/chemical properties of SEI layer and its impact on lithium striping/plating. (2) Identified failure mechanisms of SEI/Li as a whole electrode system using in-situ electrochemical tools. (3) Established a design strategy of protective coatings on Li metal to extend the cycle life Li meal electrode. (4) Developed novel surface coatings as the artificial SEI layer to protect Li metal and significantly extend cycle life. During past 3-year budget period, we have published over 16 peer-reviewed paper, filed 7 patents, and given over 30 invited talks. 5 graduated students and 2 postdocs were supported by this project.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Detecting onset of lithium plating during fast charging of Li-ion batteries using operando electrochemical impedance spectroscopy

Electrochemical plating of Li metal on the graphite electrode is the key limitation behind slow charging times of Li-ion batteries (LIBs) in electric vehicles (EVs). Currently, electrochemical methods to detect the onset of Li plating while a battery is fast charging are sparse. In this study, we use operando electrochemical impedance spectroscopy to reliably detect the onset of Li plating on graphite electrodes in three-electrode LIBs. An increase in the graphite solid-electrolyte interface (SEI) resistance indicates that Li plating has occurred. By cross-validating with a highly sensitive ex situ chemical titration, we determine that this technique can detect very small amounts of plated Li (<0.6% of the graphite electrode's capacity). We also offer physical explanations for the observed impedance behavior. Finally, we show that this technique can be applied to standard two-electrode LIB systems, making the method an important step toward safely implementing fast charging protocols for LIBs in EVs.

25 ENERGY STORAGE↗
NASA NTRSDate not supplied

Molten Salt Electrolytes: Computational Analysis of Transport, Electrochemical Properties and Designing New Mixtures

Electric aircraft propulsion has gained a traction over the last decade due to possible high-energy density electrochemistries with reasonable cycle life and identification of non-flammable chemistries that can guarantee much better safety. Commercial Li-ion batteries cannot reach such high capacities because of weight limitations that arise from the widely used intercalation electrodes. Also, use of organic electrolytes make them highly susceptible to fire on exposure to air and humidity. Currently, use of Lithium metal anode along with conversion electrochemistries such as Li-O2 and Li-S are being pursued to achieve such high energy densities. Safer inorganic solid-state electrolytes, recently discovered Water-in-Salt electrolytes, molten salt electrolytes are some of the alternatives being pursued for a safer/non-flammable battery. Of these safer alternatives, molten-salt electrolytes offer some attractive properties: liquid at operating temperatures resulting in better electrode-wetting, stable interface with Li-metal anodes and good ionic conductivity; their only drawback being high operating temperatures. In this talk, we will discuss some of the computational studies, driven via atomistic simulations, of the properties of molten-salt electrolytes including transport mechanism and interface stability. We will also discuss predicting electrochemical properties of these high-temperature electrolytes. Further, we will discuss a thermodynamic approach to predicting new molten-salt eutectics with lower melting points.

Molten Salt Electrolytes↗
DOE OSTI2020

Electrochemical cells for direct oxide reduction, and related methods

A method of direct oxide reduction includes forming a molten salt electrolyte in an electrochemical cell, disposing at least one metal oxide in the electrochemical cell, disposing a counter electrode comprising a material selected from the group consisting of osmium, ruthenium, rhodium, iridium, palladium, platinum, silver, gold, lithium iridate, lithium ruthenate, a lithium rhodate, a lithium tin oxygen compound, a lithium manganese compound, strontium ruthenium ternary compounds, calcium iridate, strontium iridate, calcium platinate, strontium platinate, magnesium ruthenate, magnesium iridate, sodium ruthenate, sodium iridate, potassium iridate, and potassium ruthenate in the electrochemical cell, and applying a current between the counter electrode and the at least one metal oxide to reduce the at least one metal oxide. Related methods of direct oxide reduction and related electrochemical cells are also disclosed.

Tripathy, Prabhat K.↗
NASA NTRS1989

A survey of advanced battery systems for space applications

The results of a survey on advanced secondary battery systems for space applications are presented. The objectives were: to identify advanced battery systems capable of meeting the requirements of various types of space missions, with significant advantages over currently available batteries, to obtain an accurate estimate of the anticipated improvements of these advanced systems, and to obtain a consensus for the selection of systems most likely to yield the desired improvements. Few advanced systems are likely to exceed a specific energy of 150 Wh/kg and meet the additional requirements of safety and reliability within the next 15 years. The few that have this potential are: (1) regenerative fuel cells, both alkaline and solid polymer electrolyte (SPE) types for large power systems; (2) lithium-intercalatable cathodes, particularly the metal ozides intercalatable cathodes (MnO2 or CoO2), with applications limited to small spacecrafts requiring limited cycle life and low power levels; (3) lithium molten salt systems (e.g., LiAl-FeS2); and (4) Na/beta Alumina/Sulfur or metal chlorides cells. Likely technological advances that would enhance the performance of all the above systems are also identified, in particular: improved bifunctional oxygen electrodes; improved manufacturing technology for thin film lithium electrodes in combination with polymeric electrolytes; improved seals for the lithium molten salt cells; and improved ceramics for sodium/solid electrolyte cells.

Attia, Alan I.↗
DOE OSTI2020

Significantly Improved Cyclability of Conversion-Type Transition Metal Oxyfluoride Cathodes by Homologous Passivation Layer Reconstruction

Electrode stabilization by surface passivation has been explored as the most crucial step to develop long-cycle lithium-ion batteries (LIBs). In this work, functionally graded materials consisting of “conversion-type” iron-doped nickel oxyfluoride (NiFeOF) cathode covered with a homologous passivation layer (HPL) are rationally designed for long-cycle LIBs. The compact and fluorine-rich HPL plays dual roles in suppressing the volume change of NiFeOF porous cathode and minimizing the dissolution of transition metals during LIBs cycling by forming a structure/composition gradient. The structure and composition of HPL reconstructs during lithiation/delithiation, buffering the volume change and trapping the dissolved transition metals. As a result, a high capacity of 175 mAh g -1 (equal to an outstanding volumetric capacity of 936 Ah L -1 ) with a greatly reduced capacity decay rate of 0.012% per cycle for 1000 cycles is achieved, which is superior to the NiFeOF porous film without HPL and commercially available NiF 2 -FeF 3 powders. Finally, the proposed chemical and structure reconstruction mechanism of HPL opens a new avenue for the novel materials development for long-cycle LIBs.

25 ENERGY STORAGE↗