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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 OSTI2024

Low-Temperature Molten Salt Electrochemical CO 2 Upcycling for Advanced Energy Materials

One strategy for addressing the climate crisis caused by CO 2 emissions is to efficiently convert CO 2 to advanced materials suited for green and clean energy technology applications. Porous carbon is widely used as an advanced energy storage material because of its enhanced energy storage capabilities as an anode. Herein, we report electrochemical CO 2 upcycling to solid carbon with a controlled microstructure and porosity in a ternary molten carbonate melt at 450 °C. Controlling the electrochemical parameters (voltage, temperature, cathode material) enabled the conversion of CO 2 to porous carbon with a tunable morphology and porosity for the first time at such a low temperature. Additionally, a well-controlled morphology and porosity are beneficial for reversible energy storage. In fact, these carbon materials delivered high specific capacity, stable cycling performances, and exceptional rate capability even under extremely fast charging conditions when integrated as an anode in lithium-ion batteries (LIBs). In conclusion, the present approach not only demonstrated efficient upcycling of CO 2 into porous carbon suitable for enhanced energy storage but can also contribute to a clean and green energy technology that can reduce carbon emissions to achieve sustainable energy goals.

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

Feasibility of Prelithiation in LiFePO 4

Lithium iron phosphate (LiFePO 4 ) is widely applied as the cathode material for the energy storage Li-ion batteries due to its low cost and high cycling stability. However, the low theoretical specific capacity of LiFePO 4 makes its initial capacity loss more concerning. Therefore, lithium compensation by way of prelithiation and applications of sacrificial Li-rich additives in LiFePO 4 is imminent in elevating the energy density and/or prolonging the lifetime of the LiFePO 4 -based Li-ion batteries (LIBs). Prelithiation in LiFePO 4 is herein carried out by electrochemical and chemical methods and its feasibility is proved on the basis of the electrochemical evaluations such as the initial charge capacity and the cycling stability. In addition, the site of the pre-intercalated Li-ions is found via comprehensive physical characterizations and the density functional theory (DFT) calculations. Furthermore, these findings open a new avenue for elevating the energy density and/or prolonging the lifetime of the high-energy-density batteries.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Designing Electrolytes With Controlled Solvation Structure for Fast‐Charging Lithium‐Ion Batteries

Recharging battery-powered electric vehicles (EVs) in a similar timeframe as those used for refueling gas-powered internal combustion vehicles is highly desirable for rapid penetration of the EV market. It is well known that the electrolyte in a battery plays a critical role in fast-charging capability of the battery because it determines the rate of ion transport together with its derived electrode/electrolyte interphases on both cathode and anode of the battery. In this study, the effects of contents of salt, coordinating solvent, and noncoordinating diluent on salt dissociation degree and electrolyte ionic conductivity are investigated, and a controlled solvation structure electrolyte is developed to improve the lithium ion mobility and conductivity in the electrolyte and to enhance the kinetics and stability of the electrode/electrolyte interphases in the battery. This electrolyte enables fast-charging capability of high energy density lithium-ion batteries (LIBs) at up to 5 C rate (12-min charging), which significantly outperforms the state-of-the-art electrolyte. The controlled solvation structure sheds light on the future electrolyte design for fast-charging LIBs.

25 ENERGY STORAGE↗
DOE OSTI2022

Polyanionic insertion hosts for aqueous rechargeable batteries

Safety concerns and costs of present-day lithium-ion batteries (LIBs) are prompting the development of alternate battery technologies with different types of electrolyte ( e.g. , solid-state, gel-polymer, aqueous, etc. ); notably, systems based on aqueous electrolytes have emerged as a promising alternative, especially for grid storage applications. The last decade has witnessed a considerable spike in the research carried out on aqueous batteries. However, the narrow operating voltage window of aqueous electrolytes and the structural instability of materials in aqueous media demand proper selection of cathode materials to achieve desirable energy density. Polyanionic materials can be an ideal choice as they are structurally more stable and exhibit tunable redox potentials. This class of materials is considered as a storehouse in which many materials can be realized by substituting different polyanionic subunits. Here, this review highlights some of the recent advances made in the polyanionic class of cathode materials for rechargeable aqueous batteries (Li-, Na- and Zn-ion batteries). The challenges facing the field, possible remedies to overcome them and future perspectives are also presented.

25 ENERGY STORAGE↗
DOE OSTI2017

Stretchable Lithium-Ion Batteries Enabled by Device-Scaled Wavy Structure and Elastic-Sticky Separator

Fast developments and substantial achievements have been shaping the field of wearable electronic devices, resulting in the persistent requirement for stretchable lithium-ion batteries (LIBs). Despite recent progress in stretchable electrodes, stretching full batteries, including electrodes, separator, and sealing material, remains a great challenge. Here, a simple design concept for stretchable LIBs via a wavy structure at the full battery device scale is reported. All components including the package are capable of being reversibly stretched by folding the entire pouch cell into a wavy shape with polydimethylsiloxane filled in each valley region. In addition, the stretchable, sticky, and porous polyurethane/poly(vinylidene fluoride) membrane is adopted as a separator for the first time, which can maintain intimate contact between electrodes and separator to continuously secure ion pathway under dynamic state. Commercial cathode, anode, and package can be utilized in this rationally designed wavy battery to enable stretchability. The results indicate good electrochemical performances and long-term stability at repeatable release–stretch cycles. A high areal capacity of 3.6 mA h cm -2 and energy density of up to 172 W h L -1 can be achieved for the wavy battery. The promising results of the cost-effective wavy battery with high stretchability shed light on the development of stretchable energy storages.

25 ENERGY STORAGE↗
DOE OSTI2019

Synergy of Epoxy Chemical Tethers and Defect‐Free Graphene in Enabling Stable Lithium Cycling of Silicon Nanoparticles

Abstract We report a new approach for nanosilicon–graphene hybrids with uniquely stable solid electrolyte interphase. Expanded graphite is gently exfoliated creating “defect‐free” graphene that is non‐catalytic towards electrolyte decomposition, simultaneously introducing high mass loading (48 wt. %) Si nanoparticles. Silane surface treatment creates epoxy chemical tethers, mechanically binding nano‐Si to CMC binder through epoxy ring‐opening reaction while stabilizing the Si surface chemistry. Epoxy‐tethered silicon pristine–graphene hybrid “E‐Si‐pG” exhibits state‐of‐the‐art performance in full battery opposing commercial mass loading (12 mg cm −2 ) LiCoO 2 (LCO) cathode. At 0.4 C, with areal capacity of 1.62 mAh cm −2 and energy of 437 Wh kg −1 , achieving 1.32 mAh cm −2 , 340.4 Wh kg −1 at 1 C. After 150 cycles, it retains 1.25 mAh cm −2 , 306.5 Wh kg −1 . Sputter‐down XPS demonstrates survival of surface C‐Si‐O‐Si groups in E‐Si‐pG after repeated cycling. The discovered synergy between support defects, chemical‐mechanical stabilization of Si surfaces, and SEI‐related failure may become key LIB anode design rule.

Liu, Wei↗
DOE OSTI2022

Battery aging mode identification across NMC compositions and designs using machine learning

A comprehensive understanding of lithium-ion battery (LiB) lifespan is the key to designing durable batteries and optimizing use protocols. Although battery lifetime prediction methods are flourishing, diagnosis of the root causes of aging and degradation have not yet been well developed nor studied for a broad mixture of designs and use cases. Here, we create a machine-learning (ML)-based framework that distinguishes aging modes using multiple electrochemical signatures recorded cycle-by-cycle. The predominant aging behaviors include a combination of loss of active materials in cathode (LAMPE) and a loss of Li inventory (LLI) in Li plating or solid electrolyte interphase (SEI) formation, manifested from 44 batteries representing two cathode chemistries, two electrode loadings, and five charging rates. Here, the aging mode classification accuracy is 86% using features within the first 50 cycles and increases to 88% beyond 225 cycles. The same features can quantify the percentage of end-of-life LAMPE with only 4.3% of error.

25 ENERGY STORAGE↗
DOE OSTI2017

Mitigating thermal runaway of lithium-ion battery through electrolyte displacement

Alkanes are investigated as thermal-runaway retardants (TRR) for lithium-ion battery (LIB). TRR is a chemical that can rapidly terminate exothermic reactions in LIB. Under normal working conditions, TRR is sealed in separate packages in the LIB cell, and upon mechanical abuse, it is released to suppress heat generation. The alkanes under investigation include octane, pentadecane, and icosane, among which pentadecane has the highest thermal-runaway mitigation (TRM) efficiency. In nail penetration test on coin cells, ∼4 wt. % pentadecane reduced the maximum temperature by ∼60%; in impact test on pouch cells, ∼5 wt. % pentadecane reduced the maximum temperature by ∼90%. The high TRM efficiency of pentadecane is attributed to its high wettability to separator and its immiscibility with electrolyte. By forming a physical barrier between the cathode and anode, pentadecane interrupts lithium ion (Li+) transport and increases the charge transfer resistance by nearly two orders of magnitude. The diffusion rate of pentadecane in the electrode layer stack was measured to be ∼580 μm/s.

Shi, Yang↗
DOE OSTI2022

Resolving Graphite‐Electrolyte Interphase of Lithium‐Ion Batteries using Air‐Tight Ambient Mass Spectrometry

Abstract The formation of a stable solid electrolyte interphase (SEI) at graphite electrode is necessary for lithium‐ion batteries (LIB) to prevent excessive degradation of electrolytes. Until now, the exact organic composition of SEI has not been decisively determined with lithium ethylene mono‐carbonate (LEMC) being one of the debated components. An air‐tight ambient mass spectrometry (MS) platform is developed to directly characterize the air‐sensitive organic components present in SEI. Ionization occurs via a solvent‐free field‐induced process at atmospheric pressure. Our experimental data, based on tandem MS analysis, revealed LEMC to be the major organic component in SEI. This result resolves a long‐standing mystery surrounding the composition of native SEI in LIB, where no trace of the other debated compound, lithium ethylene dicarbonate, was detected. The energetics of fragmentation of LEMC and the corresponding stabilities of various ionic species detected during the air‐tight ambient MS analysis were calculated using density functional theory (DFT). Our findings confirmed favorable protonation energies and suggested the molecular structures for many of the detected species. Solvent (i. e., ethylene carbonate)‐induced stabilization effects observed during the ionization process were also confirmed by DFT. The reported study encourages the routine use of ambient mass spectrometry to characterize both anodic and cathodic electrodes of all battery types as well as to study other air‐sensitive materials in their native state.

25 ENERGY STORAGE↗
DOE OSTI2022

Wet chemical synthesis and properties of argyrodite sulfide solid electrolytes for solid state lithium batteries

The commercialization of the lithium-ion battery (LIB) in 1991 was responsible for the explosion in portable electronic technologies that has been seen over the past 30 years. With the advent of electric vehicles and other high-powered technologies, there is tremendous demand for LIBs with higher energy density and high safety. To achieve this, new electrode materials must be explored. The obvious choice of anode material would be pure metal lithium, which has a theoretical specific capacity of 3860 mAh g-1 . Unfortunately, metal lithium anodes have not been widely commercialized due to their tendency to react violently with the flammable liquid electrolytes used in today’s batteries. Battery safety can best be achieved by adopting solid electrolytes in place of liquid electrolytes. Solid electrolytes are nonvolatile and nonflammable, safely allowing for the combination of high-capacity cathode materials with a Li metal anode. Argyrodite sulfide solid electrolytes such as halogen-doped Li6PS5X (X = Cl, Br, I) are noted for their high ionic conductivity. But before sulfides can be commercially adopted, they possess several disadvantages which must be addressed, including time- and energy-consuming synthesis processes, poor electrochemical stability, and intrinsically poor air stability. This dissertation seeks to address each of these challenges through materials design an synthesis strategies. In this work, we pioneer a solvent-based approach for the synthesis of argyrodite solid electrolytes Li7PS6 and Li6PS5Xinstead of a stringent solid-state synthesis. Nontoxic ethanol is employed as the solvent, enabling a rapid synthetic approach to produce argyrodite solid electrolytes with high phase purity and compositional flexibility. Compared with Li7PS6, halogen doping (i.e. X = F, Cl, Br, I) not only increases the ionic conductivity, but also enhances the electrochemical stability at the interface towards Li metal. Specifically, F-doped argyrodites produce a robust SEI layer containing LiF, contributing to enhanced interfacial stability. Finally, to address the air instability challenge, argyrodite-incorporated composite solid electrolytes (CSEs) are designed and prepared to produce stable and flexible membranes that are demonstrated in solid-state Li metal batteries. These advances push argyrodite sulfide solid electrolyte research further and pave the way for the proliferation of next generation lithium metal batteries.

25 ENERGY STORAGE↗
DOE OSTI2020

Oxygen-Based Anion Redox for Lithium Batteries

The importance of current Li-ion batteries (LIBs) in modern society cannot be overstated. While the energy demands of devices increase, the corresponding enhancements in energy density of battery technologies are highly sought after. Currently, many different battery concepts, such as Li-S and metal-air among many others, have been investigated. However, their practical implementation has mostly been restricted to the prototyping stage. In fact, most of these technologies require rework of existing Li-ion battery manufacturing facilities and will naturally incur resistance to change from industry. For this reason, one specifically attractive technology, anionic redox in transition metal oxides, has gained much attention in the recent years. Its ability to be directly used in already established processes and higher energy density with similar electrolyte formulation make it a key materials research direction for next generation Li-ion batteries. In regular LIBs, the redox active centers are the transition metal cation. In anion redox, both the anion (typically O) and the transition metal cation are utilized as redox centers with enormous implications for increasing energy density. This new material can be highly competitive for replacing the current LIB technologies. However, much is still unknown about its cyding mechanism. Upon activating the O redox couples, most cationic and anionic redox active materials will either evolve O 2 or undergo irreversible structural degradation with associated severe decreases in electrochemical performance. By understanding the transition from full anion redox to partial cationic and anionic redo; we hope readers can gain a deeper understanding of the topic. This Account will focus mainly on the work that was conducted by our group at Argonne National Laboratory. Herein, the phenomenon of cationic and anionic redox in a lithium-ion battery cathode will first be discussed. Our work in resonant inelastic X-ray scattering to investigate the spectroscopic features of O after delithiation has found potential "fingerprint" signals that could likely be used to identify and confirm reversible O redox if corroborated with other techniques. To follow, we will examine our work on Li-O 2 batteries. While our group and the research community have had many significant contributions and improvements to the field of Li-O 2 (such as decreasing overpotential and achieving cyclability in air environment), its practical application is still far from realization. Perhaps our most important contribution to this area is the discovery that Ir deposited on reduced graphene oxide can be used to halt the reduction of O 2 at the LiO 2 oxidation state. This not only significantly decreases the charge overpotential but also presents the important concept of oxidation-state controlled discharge. Subsequently, we will focus on our oxidation state-controlled redox-based charging of oxygen in a pure oxygen redox Li-ion battery. Future implications of this technology will be emphasized.

25 ENERGY STORAGE↗
DOE OSTI2026

The Influence of Mesoscale Particle Structure on the Electrode Degradation and Resultant Electrochemistry of Lithium Ion Cells With Nickel Rich Lithium Nickel Manganese Cobalt Oxide Positive Electrodes

Nickel-rich lithium nickel manganese cobalt oxide, NMC (LiNi x Mn y Co z O 2 ), materials are desirable positive electrodes in lithium ion batteries, providing high capacity and energy density. The mesoscale structure of NMC materials is commonly a polycrystalline aggregate, providing opportunity for short lithium ion transport distance of the small primary particles, yet facile material handling due to the larger secondary particles. On (de)lithiation the NMC unit cell changes volume, where the anisotropic strain can result in secondary particle fracture. This secondary particle fracture process during cycling has been associated with several degradation modes of NMC materials in LIBs. In this work, a milling process was determined whereby the secondary particles could be pre-fractured with retention of the parent primary particle crystallographic structure, crystallite size, and morphology, providing the ability to unambiguously determine the influence of NMC secondary particle size and mesostructure on resultant functional behavior. The bulk and interfacial properties and electrochemistry of as-received commercially obtained polycrystal NMC811 (LiNi 0.8 Mn 0.1 Co 0.1 O 2 , PC NMC) and its milled MPC NMC counterpart were compared. The smaller secondary particle size, higher surface area MPC NMC was found to result in 1) greater cathode tortuosity, 2) reduced surface Ni on the cycled MPC cathodes consistent with surface reconstruction, and 3) increased Ni deposition on the anodes from cathode-anode crosstalk. These factors manifested in unfavorable electrochemical behavior of MPC with lower functional capacity at both 1C and C/10 rates and higher impedance over extended moderate voltage (dis)charge cycling.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Graphene foam integrated with lithium titanate as anode of Li ion batteries

Graphical abstract: Integrated graphene foam supported LTO electrodes are synthesized via a hydrothermal method and exhibit a noticeable electrochemical performance as cathode of Li ion batteries. - Highlights: • Integrated graphene foam supported LTO electrodes are synthesized. • Self-supported GF/LTO electrodes show high electrochemical performance. • Integrated porous architecture is favorable for capacity enhancement. - Abstract: In this work, we construct a binder-free electrode by integrating Li{sub 4}Ti{sub 5}O{sub 12} (LTO) nanoparticles onto free-standing graphene foam (GF) via hydrothermal method. The CVD-grown GF is used as the backbone for the deposition of LTO nanoparticles of 20–50 nm. Enhanced reaction kinetics including fast ion/electron transfer is achieved with the help of conductive GF matrix. The electrochemical performance of the VG/LTO as the anode of Li ion batteries (LIBs) are studied and demonstrated with a capacity of 171 mAh g{sup −1} at 1 C, and good cycles with a capacity retention of 77%. High-rate capability is also verified with a capacity of 108 mAh g{sup −1} at 10 C. The designed porous integrated architecture is favorable for the diffusion of ion/electrons, and good contact with the electrolyte. Our results provide a new way for developing high-performance anode of LIBs.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Final Report - Advanced High Energy Li-Ion Cell for PHEV and EV Applications

Lithium Ion Battery (LIB) technology’s potential to enable a commercially viable high energy density is the key to a lower $/Wh, thereby a low cost battery. The design of a LIB with high energy, high power, safety and long life is a challenge that requires cell design from the ground up and synergy between all components. 3M Company (3M), the Recipient, led by its Principal Investigator, Jagat Singh, pursued this challenging task of a LIB by ‘teaming’ key commercial businesses [General Motors (GM), Umicore and Iontensity] and labs [Army Research Laboratory (ARL) and Lawrence Berkley National Laboratory (LBNL)]. The technology from each team member was complimentary and a close working relationship spanning the value chain drove productivity.The completion of this project is a significant step towards more energy efficient and environmentally friendly vehicles, making America less dependent on imported oil.

25 ENERGY STORAGE↗
DOE OSTI2023

A Materials Perspective on Direct Recycling of Lithium-Ion Batteries: Principles, Challenges and Opportunities

As the dominant means of energy storage technology today, the widespread deployment of lithium-ion batteries (LIBs) would inevitably generate countless spent batteries at their end of life. From the perspectives of environmental protection and resource sustainability, recycling is a necessary strategy to manage end-of-life LIBs. Compared with traditional hydrometallurgical and pyrometallurgical recycling methods, the emerging direct recycling technology, rejuvenating spent electrode materials via a non-destructive way, has attracted rising attention due to its energy efficient processes along with increased economic return and reduced CO 2 footprint. This review investigates the state-of-the-art direct recycling technologies based on effective relithiation through solid-state, aqueous, eutectic solution and ionic liquid mediums and thoroughly discusses the underlying regeneration mechanism of each method regarding different battery chemistries. It is concluded that direct regeneration can be a more energy-efficient, cost-effective, and sustainable way to recycle spent LIBs compared with traditional approaches. Additionally, it is also identified that the direct recycling technology is still in its infancy with several fundamental and technological hurdles such as efficient separation, binder removal and electrolyte recovery. Finally, in addressing these remaining challenges, this review proposes an outlook on potential technical avenues to accelerate the development of direct recycling toward industrial applications.

25 ENERGY STORAGE↗
DOE OSTI2022

Tailored Solvation and Interface Structures by Tetrahydrofuran-Derived Electrolyte Facilitates Ultralow Temperature Lithium Metal Battery Operations

Ineffectiveness of Li-ion batteries (LIBs) in cold climates hinders electronics to work in various conditions including frigid environments, despite high demands. Given that intrinsic properties of LIB materials cause this problem, optimized cell chemistries ultimately are required for low-temperature usage. In this study, Li-metal batteries (LMBs) composed of a Li-metal anode (LMA) stabilized by a localized high-concentration electrolyte (LHCE) are found to significantly enhance low-temperature performance. The LHCE allows the LMA to have compact and regular deposition and excellent plating/stripping efficiency at sub-zero temperatures. The LHCE produces an inorganic-rich solid-electrolyte interphase with larger amounts of Li 2 O/LiF interfaces, dominance of ion aggregates in Li + solvation, and enhanced Li + transport, which can greatly improve the LMA stability. LMB full cells based on LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathodes with the tailored electrolyte show high retentions of 75 and 64 % at -20 and -40 °C, respectively. Furthermore, the LMB configuration retains its charge-discharge capability even at -60 °C.

25 ENERGY STORAGE↗
DOE OSTI2024

Research Progress and Perspectives on Pre‐Sodiation Strategies for Sodium‐Ion Batteries

Sodium‐ion batteries (SIBs) with abundant elements have garnered significant attention from researches as a promise compensation to lithium‐ion batteries (LIBs). However, the large‐scale commercial application of SIBs is partially hindered by the limited initial coulombic efficiency (ICE) due to the irreversible formation of solid electrolyte interphase (SEI) and intercalation into the defects in the anode. Similar to pre‐lithiation techniques, pre‐sodiation approaches are considered to be one of the most direct and effective way to compensate for the loss of active sodium at the anode side of SIBs during the initial cycle. In this context, additional sodium ions are pre‐injected to the cathode/anode material by chemical/electrochemical methods, aiming to improve battery span life and energy density. Here, this review delves into the necessity and impact of pre‐sodiation techniques, compiling the latest research progress, for instance, self‐sacrificing cathode additives, over‐sodiated cathode materials, direct contact and solution chemical pre‐sodiation. Notably, the research mechanisms underlying solution chemical pre‐sodiation are highlighted. This comprehensive overview aims to foster a deeper understanding of the pre‐sodiation techniques and expects to provide guidance for realizing the commercial application of high energy density sodium‐ion batteries.

25 ENERGY STORAGE↗