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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 361 records · Page 20
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Simultaneous Heat and Electricity Storage in a Flow Battery System

This study investigates the dual-storage capability of a redox flow battery (RFB) system, enabling simultaneous storage of heat and electricity within a single platform. Through electrochemical and thermal experiments, we evaluated how heat storage affects battery performance and vice versa using a counterflow heat exchanger integrated in a conventional RFB configuration. The results show that incorporating heat storage had a minimal impact on the electrochemical charging and discharging processes. Further, the heat discharge operated independently of electrochemical storage, confirming that both functions can coexist without interference. The combined system also enhanced overall energy conversion efficiency, demonstrating its potential as an efficient solution for supplying both thermal and electrical energythe two most widely used energy forms.

Electrical energy↗
DOE OSTI2020

Structural Distortion Induced by Manganese Activation in a Lithium-Rich Layered Cathode

The search for batteries with high energy density has highlighted lithium-rich manganese-based layered oxides due to their exceptionally high capacity. Although it is clear that both cationic and anionic redox are present in the charge compensation mechanism, the microstructural evolution of the Li 2 MnO 3 -like phase during anionic redox and its role in battery performance and structural stability are still not fully understood. Here, we systematically probe microstructural evolution using spatially resolved synchrotron X-ray measurements and reveal an underlying interaction between the Li 2 MnO 3 -like domains and bulk rhombohedral structure. Mn ion activation and a previously unobserved structural distortion are discovered at high voltages, and can be related to structural strain present in the Li 2 MnO 3 -like phase upon substantial lithium ion extraction. Moreover, we elucidate a correlation between this structural distortion and irreversible phase transitions by thermally perturbing delithiated samples. These insights highlight a pathway toward achieving high capacity cathode materials required for future commercial applications.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Formation of Surface Impurities on Lithium–Nickel–Manganese–Cobalt Oxides in the Presence of CO 2 and H 2 O

Surface impurities involving parasitic reactions and gas evolution contribute to the degradation of high Ni content LiNi x Mn y Co z O 2 (NMC) cathode materials. The transient kinetic technique of Temporal Analysis of Products (TAP), density functional theory, and infrared spectroscopy have been used to study the formation of surface impurities on varying nickel content NMC materials (NMC811, NMC622, NMC532, NMC433, NMC111) in the presence of CO 2 and H 2 O. CO 2 reactivity on a clean surface as characterized by CO 2 conversion rate in the TAP reactor follows the order: NMC811 > NMC622 > NMC532 > NMC433 > NMC111. The capacity of CO 2 uptake follows a different order: NMC532 > NMC433 > NMC622 > NMC811 > NMC111. Moisture pretreatment slows down the direct CO 2 adsorption process and creates additional active sites for CO 2 adsorption. Electronic structure calculations predict that the (012) surface is more reactive than the ($10\bar{1}4$) surface for CO 2 and H 2 O adsorption. CO 2 adsorption leading to carbonate formation is exothermic with formation of ion pairs. The average CO 2 binding energies on the different materials follow the CO 2 reactivity order. Water hydroxylates the (012) surface and surface OH groups favor bicarbonate formation. Water creates more active sites for CO 2 adsorption on the ($10\bar{1}4$) surface due to hydrogen bonding. The composition of surface impurities formed in ambient air exposure is dependent on water concentration and the percentage of different crystal planes. Different surface reactivities suggest that battery performance degradation due to surface impurities can be mitigated by precise control of the dominant surfaces in NMC materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Elucidating Gas Reduction Effects of Organosilicon Additives in Lithium-Ion Batteries

Lithium-ion batteries (LIBs) with nonaqueous liquid electrolytes are prone to gas generation at elevated voltages and temperatures, degrading battery performance and posing serious safety risks. Organosilicon (OS) additives are an emerging candidate solution for gassing problems in LIBs, but a detailed understanding of their functional mechanisms remains elusive. In this work, we present a combined computational and experimental study to elucidate the gasreducing effects of OS additives. Cell volume measurements and gas chromatography–mass spectrometry reveal that OS additives can substantially reduce gas evolution in LIBs, particularly CO 2 regardless of source. Through density functional theory calculations, we identify multiple plausible pathways for CO 2 evolution, including (1) nucleophile-induced ring-opening of ethylene carbonate (EC) and the subsequent electro-oxidation and (2) direct electro-oxidation of lithium carbonate (Li 2 CO 3 ). Correspondingly, we find that OS additives function via two primary mechanisms: (1) scavenging of nucleophiles such as superoxide (O 2 •– ), peroxide (O 2 2– ), and carbonate ion (CO 3 2– ); (2) oligomerization with ethylene carbonate oxide ion and ethylene dicarbonate ion. Moreover, we discover that OS additives possess strong lithium coordination affinity, which helps further reduce the nucleophilic reaction energies and hence increases their nucleophile-scavenging efficiency. Finally, we provide a mechanistic interpretation for the enhanced gasreduction effects observed with fluorinated OS compounds, corroborated by surface analysis results from X-ray photoelectron spectroscopy. Our study offers the first molecular-level insights into how OS additives contribute to reduced gas formation in LIBs, paving the way for improved safety and performance of LIBs.

25 ENERGY STORAGE↗
DOE OSTI2023

Enabling selective zinc-ion intercalation by a eutectic electrolyte for practical anodeless zinc batteries

Abstract Two major challenges hinder the advance of aqueous zinc metal batteries for sustainable stationary storage: (1) achieving predominant Zn-ion (de)intercalation at the oxide cathode by suppressing adventitious proton co-intercalation and dissolution, and (2) simultaneously overcoming Zn dendrite growth at the anode that triggers parasitic electrolyte reactions. Here, we reveal the competition between Zn 2+ vs proton intercalation chemistry of a typical oxide cathode using ex-situ/ operando techniques, and alleviate side reactions by developing a cost-effective and non-flammable hybrid eutectic electrolyte. A fully hydrated Zn 2+ solvation structure facilitates fast charge transfer at the solid/electrolyte interface, enabling dendrite-free Zn plating/stripping with a remarkably high average coulombic efficiency of 99.8% at commercially relevant areal capacities of 4 mAh cm −2 and function up to 1600 h at 8 mAh cm −2 . By concurrently stabilizing Zn redox at both electrodes, we achieve a new benchmark in Zn-ion battery performance of 4 mAh cm −2 anode-free cells that retain 85% capacity over 100 cycles at 25 °C. Using this eutectic-design electrolyte, Zn | |Iodine full cells are further realized with 86% capacity retention over 2500 cycles. The approach represents a new avenue for long-duration energy storage.

25 ENERGY STORAGE↗
DOE OSTI2019

Three-dimensional phase evolution and stress-induced non-uniform Li intercalation behavior in lithium iron phosphate

A lithium iron phosphate (LiFePO 4 ) olivine cathode displays rich phase transition behavior during charging/discharging. Despite extensive studies, the evolution of the LiFePO 4 /FePO 4 two-phase coexistence structure and the underlying mechanism are still a point of debate due to the intricate and often disparate phase morphologies observed. Here we apply phase-field simulations to provide detailed insights into the three-dimensional phase evolution process in LiFePO 4 upon delithiation under a large driving force. The simulation reveals that the coherency stress arising from the LiFePO 4 /FePO 4 lattice mismatch destabilizes the initially flat delithiation front and induces filamentary growth of the FePO 4 phase along [010], which is in excellent agreement with a recent operando X-ray imaging study. The combined simulation and experimental results provide the first illustration of the phenomenon of stress-induced instability of the lithium (de)intercalation front in battery electrode compounds. We show that this phenomenon is facilitated by the surface mode of coherent spinodal decomposition in LiFePO 4 and influenced by the anisotropies of misfit strain, elasticity and lithium diffusion. It is detrimental to battery performance and life by causing stress concentration and reducing the lithium (de)intercalation kinetics and thus should be mitigated.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2020

Solvent oligomerization pathways facilitated by electrolyte additives during solid-electrolyte interphase formation

The solid–electrolyte interphase (SEI) layer formation is known to play an important role in determining the lifetime of lithium-ion batteries. A thin, stable SEI layer is linked to overall improved battery performance and longevity, however, the factors and mechanisms that lead to optimal SEI morphology and composition are not well understood. Inclusion of electrolyte additives (fluoroethylene carbonate, FEC; and vinylene carbonate, VC) is often necessary for improving SEI characteristics. To understand how these electrolyte additives impact SEI formation, we employed molecular dynamics (MD) and density functional theory (DFT) simulations to study the reaction networks and oligomerization pathways, respectively, for three systems containing ethylene carbonate (EC), a lithium ion, and FEC or VC. MD simulations suggest radical oligomerization pathways analogous to traditional oligomerization with nucleophilic alkoxide species via SN1 reaction mechanisms. Both S N 1 and S N 2 mechanisms were studied for all three systems using DFT. Oligomerization reactions were studied with both a standard alkoxide species and a ring-opened EC radical as the nucleophiles and EC, FEC, and VC as the electrophiles. For all cases, FEC and VC exhibited lower free energy barriers and more stable adducts when compared with EC. We conclude that one of the role of additives is to modify the oligomerization process of EC by introducing branching points (FEC) or termination points (VC).

25 ENERGY STORAGE↗
DOE OSTI2024

Correlating concerted cations with oxygen redox in rechargeable batteries

Rechargeable batteries currently power much of our world, but with the increased demand for electric vehicles (EVs) capable of traveling hundreds of miles on a single charge, new paradigms are necessary for overcoming the limits of energy density, particularly in rechargeable batteries. The emergence of reversible anionic redox reactions presents a promising direction toward achieving this goal; however this process has both positive and negative effects on battery performance. While it often leads to higher capacity, anionic redox also causes several unfavorable effects such as voltage fade, voltage hysteresis, sluggish kinetics, and oxygen loss. However, the introduction of cations with topological chemistry tendencies has created an efficient pathway for achieving long-term oxygen redox with improved kinetics. The cations serve as pillars in the crystal structure and meanwhile can interact with oxygen in ways that affect the oxygen redox process through their impact on the electronic structure. This review delves into a detailed examination of the fundamental physical and chemical characteristics of oxygen redox and elucidates the crucial role that cations play in this process at the atomic and electronic scales. Furthermore, here we present a systematic summary of polycationic systems, with an emphasis on their electrochemical performance, in order to provide perspectives on the development of next-generation cathode materials.

25 ENERGY STORAGE↗
DOE OSTI2020

Insights on the cycling behavior of a highly-prelithiated silicon–graphite electrode in lithium-ion cells

Nanosized silicon materials are being developed for use in the anodes of high-energy lithium-ion batteries. However, the high surface areas of these materials increase the rate of parasitic reactions in the electrode, which consume cyclable Li + and degrade battery performance. Prelithiation offers a realistic strategy to compensate for this reactivity, by injecting additional charge into the cell to counterbalance the Li + loss. Interestingly, the benefits offered by prelithiation extend beyond its more obvious purpose. Here, by using a reference electrode in NMC532//Si–Gr cells, we show how prelithiation alters the cycling potentials experienced by the Si-containing anode and how that translates into gains in cycle life. The rate of consumption of the prelithiated charge is lower than that expected from the behavior of non-prelithiated cells. Curiously, the Si particles become partially unresponsive during the C/3 cycling apparently because of kinetic constraints. Electrochemical studies on harvested electrodes in half-cells show that capacities are intact after the long-term cycling and that most of the lithium reservoir is still present in the anode. We conclude that the high capacity retention displayed by the prelithiated cells mainly results from a higher participation of graphite particles during the extended electrochemical cycling.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Image registration for accurate electrode deformation analysis in operando microscopy of battery materials

Operando imaging techniques have become increasingly valuable in both battery research and manufacturing. However, the reliability of these methods can be compromised by instabilities in the imaging setup and operando cells, particularly when utilizing high-resolution imaging systems. The acquired imaging data often include features arising from both undesirable system vibrations and drift, as well as the scientifically relevant deformations occurring in the battery sample during cell operation. For meaningful analysis, it is crucial to distinguish and separately evaluate these two factors. To address these challenges, we employ a suite of advanced image-processing techniques. These include fast Fourier transform analysis in the frequency domain, power spectrum-based assessments for image quality, as well as rigid and non-rigid image-registration methods. These techniques allow us to identify and exclude blurred images, correct for displacements caused by motor vibrations and sample holder drift and, thus, prevent unwanted image artifacts from affecting subsequent analyses and interpretations. Additionally, we apply optical flow analysis to track the dynamic deformation of battery electrode materials during electrochemical cycling. This enables us to observe and quantify the evolving mechanical responses of the electrodes, offering deeper insights into battery degradation. Together, these methods ensure more accurate image analysis and enhance our understanding of the chemomechanical interplay in battery performance and longevity.

Sun, Tianxiao↗
DOE OSTI2026

Observation of N-rich solid-electrolyte interphase by ToF-SIMS.

Formation of a stable solid electrolyte interphase (SEI) between lithium electrodes and electrolyte upon multiple charge/discharge cycles is crucial to a long-term lithium-ion battery performance. Addition of LiNO3 to lithium bis (fluorosulfonyl) imide/poly(ethylene oxide) (LiFSI/PEO) electrolyte leads to a durable SEI that is electrically insulating yet highly conductive to Li ions, chemically and electrochemically stable, physically uniform, and mechanically robust. ToF-SIMS was used here in combination with sputtering by a gaseous cluster ion beam (GCIB) to examine how the addition of a small proportion of LiNO3 to the LiFSI/PEO electrolyte affects the SEI composition. Negative ion ToF-SIMS spectra of the cycled samples display an intense m/z 26 peak associated with the SEI. Exact mass assignments and isotopic ratios indicate that this peak should be assigned as (CN-)-C-12, with little to no negative secondary ion signal arising from (LiF-)-Li-7. This CN- signal appears to arise from an N-rich portion of the SEI adjacent to the Li electrode that is depleted in LiF relative to the bulk electrolyte. The dearth of LiF- (and LiF+ from the positive ion spectra) is unexpected because LiF has been identified in the SEI in similar samples. Finally, GCIB sputtering indicates that the SEI adheres more strongly to the Li electrode than to the LiFSI/PEO electrolyte.

Shavandi, Seyedeh Reyhaneh↗
DOE OSTI2023

Progressive and instantaneous nature of lithium nucleation discovered by dynamic and operando imaging

The understanding of lithium (Li) nucleation and growth is important to design better electrodes for high-performance batteries. However, the study of Li nucleation process is still limited because of the lack of imaging tools that can provide information of the entire dynamic process. We developed and used an operando reflection interference microscope (RIM) that enables real-time imaging and tracking the Li nucleation dynamics at a single nanoparticle level. This dynamic and operando imaging platform provides us with critical capabilities to continuously monitor and study the Li nucleation process. We find that the formation of initial Li nuclei is not at the exact same time point, and Li nucleation process shows the properties of both progressive and instantaneous nucleation. In addition, the RIM allows us to track the individual Li nucleus’s growth and extract spatially resolved overpotential map. The nonuniform overpotential map indicates that the localized electrochemical environments substantially influence the Li nucleation.

25 ENERGY STORAGE↗
DOE OSTI2022

Capturing the swelling of solid-electrolyte interphase in lithium metal batteries

Although liquid-solid interfaces are foundational in broad areas of science, characterizing this delicate interface remains inherently difficult because of shortcomings in existing tools to access liquid and solid phases simultaneously at the nanoscale. This leads to substantial gaps in our understanding of the structure and chemistry of key interfaces in battery systems. We adopt and modify a thin film vitrification method to preserve the sensitive yet critical interfaces in batteries at native liquid electrolyte environments to enable cryo–electron microscopy and spectroscopy. We report substantial swelling of the solid-electrolyte interphase (SEI) on lithium metal anode in various electrolytes. Here, the swelling behavior is dependent on electrolyte chemistry and is highly correlated to battery performance. Higher degrees of SEI swelling tend to exhibit poor electrochemical cycling.

25 ENERGY STORAGE↗
DOE OSTI2022

Tuning Fluorination of Linear Carbonate for Lithium-Ion Batteries

Liquid electrolyte engineering plays a critical role in modern lithium-ion batteries. However, the existing electrolytes fall short when used with some trending battery chemistries such as high-voltage and high-energy-density electrodes. Fluorination of electrolyte solvents has been identified as an effective approach for improved cyclability, but few works systematically studied the effects of fluorination extent of carbonate solvents on battery performance. Here we design and synthesize a family of fluorinated ethyl methyl carbonates. Different numbers of F atoms are finely tuned to yield monofluoroethyl methyl carbonate (F1EMC), difluoroethyl methyl carbonate (F2EMC) and trifluoroethyl methyl carbonate (F3EMC). The cycling behavior of several types of lithium-ion pouch cells, including graphite (Gr)/single-crystalline LiNi 0.8 Mn 0.1 Co 0.1 O 2 (SC-NMC811), Gr-SiO x /LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC622), high-voltage Gr/LiNi 0.5 Mn 1.5 O 4 (LNMO), Gr/layered Li-rich Mn-based oxide (LLMO) and fast-charging Gr/NMC622, were systematically investigated to understand the impact of fluorination degree. Compared to the commercially available F3EMC, we found that the partially-fluorinated F1EMC and F2EMC in some cases showed improved cycling stability, which we attribute to their locally-polar –CH 2 F and –CHF 2 groups and thus fast ion conduction than –CF 3 . This work suggests that highly or fully fluorinated solvents are not necessarily desirable; instead, fluorination degree needs to be rationally and finely tuned for optimized lithium-ion cell performance.

25 ENERGY STORAGE↗
DOE OSTI2026

Binder-Stabilized Carbon Fiber Hosts for High-Utilization Sodium–Polysulfide Flow Catholytes

Sodium-sulfur (Na-S) batteries hold promise as high-energy-density batteries for long-duration energy storage due to their high open circuit voltage and Earth-abundant active materials. However, low utilization of the sulfur active material limits the achievable specific capacity, especially when a liquid polysulfide catholyte is utilized. High-surface-area carbon materials demonstrate promise to increase sulfur utilization in a Na-S battery. To make the carbon host material applicable for a flow battery application, a binder is required to bind the carbon materials together and to a porous substrate. Here, we utilize a composite carbon paper electrode coated by polymer,carbon nanofibers (CNFs) and carbon black (CB). By varying the mass ratios of CNF to CB, we found that a 70/20/10 mass ratio of CNF/CB/binder provided the highest capacity (260 mAh g −1 compared to the baseline of 156 mAh g −1 ) and stable battery performance over 100 cycles. Analysis of the composite electrode and full cells reveals that the amount of CB in the composite electrode influences binder distribution, cell resistance, and full cell performance.

Lehmann, Michelle L. [Oak Ridge National Laborator↗
DOE OSTI2020

High-dimensional and high-resolution x-ray tomography for energy materials science

At the forefront of developments in synchrotron x-ray microscopy, we report nanoscale-resolution high-dimensional spectrotomography under controlled sample environments has been demonstrated. Such cutting-edge experimental capability has been broadly applied to scientific studies in the field of energy materials science, where the dynamically evolving structural and chemical defects play a vital role in the functionality. In this article, we review novel developments of this technique from both experimental and data/information mining perspectives. Using studies on lithium-ion battery electrode materials as examples, we highlight the rich information in the high-dimensional and high-resolution x-ray tomographic data, which can be used to interpret the complicated thermal-electro-chemo-mechanical interplay that occurs under the operating conditions and collectively determines battery performance. We also discuss the frontier challenges in this field and our perspectives of the future directions in the context of projected major developments in the landscape of largescale x-ray facilities across the globe.

36 MATERIALS SCIENCE↗