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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 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Rationalizing nitrogen-doped secondary carbon particles for practical lithium-sulfur batteries

Nanostructured carbon host materials are widely used to improve both sulfur utilization rate and reaction kinetics in lithium-sulfur (Li-S) batteries. However, high complexity/cost of materials synthesis and difficulty in processing nano-materials into high-mass-loading electrodes are still significant barriers to the development of low-cost and high-energy Li-S batteries. In this study, we reported a generic and scalable synthesis approach to prepare nitrogen-doped secondary carbon particles. By using nitrogen-containing precursor as an integration reagent, the nanosized Ketjen Black particles were integrated into micron-size secondary ones and nitrogen-doped (NKB) simultaneously through a one-step heat treatment. With NKB as an example material, the effects of particle integration degree on the secondary particles’ structures, pore volume and connectivity, sulfur loading capability, and cell performance were studied and discussed. At an optimal integration condition, the NKB particles had significantly improved particle dimensions with well-maintained high specific surface area and pore volume. Here, contributed by the micron size and high pore volume, the NKB/S were successfully used for high-sulfur-loading cathodes (4–7 mg s /cm -2 ) and were able to deliver a specific capacity of ~1100 mAh g -1 at a low-porosity (50%) and lean-electrolyte conditions (E/S =4 µL/mg -1 ). Feasibility of the materials for practical use was validated through scaling up synthesis (40 g/batch), large-area electrode coating, and practical pouch cell (1.6 Ah) assembly and test.

25 ENERGY STORAGE↗
DOE OSTI2018

Rational Design of a Dual-Function Hybrid Cathode Substrate for Lithium-Sulfur Batteries

Here, a unique 3D hybrid sponge with chemically coupled nickel disulfide–reduced graphene oxide (NiS 2 –RGO) framework is rationally developed as an effective polysulfide reservoir through a biomolecule–assisted self–assembly synthesis. An optimized amount of NiS 2 (≈18 wt%) with porous nanoflower–like morphology is uniformly in situ grown on the RGO substrate, providing abundant active sites to adsorb and localize polysulfides. The improved polysulfide adsorptivity from sulfiphilic NiS 2 is confirmed by experimental data and first–principle calculations. Moreover, due to the chemical coupling between NiS 2 and RGO formed during the in situ synthesis, the conductive RGO substrate offers a 3D electron pathway to facilitate charge transfer toward the NiS 2 –polysulfide adsorption interface, triggering a fast redox kinetics of polysulfide conversion and excellent rate performance (C/20–4C). Therefore, the self–assembled hybrid structure simultaneously promotes static polysulfide–trapping capability and dynamic polysulfide–conversion reversibility. As a result, the 3D porous sponge enables a high sulfur content (75 wt%) and a remarkably high sulfur loading (up to 21 mg cm –2 ) and areal capacity (up to 16 mAh cm –2 ), exceeding most of the reported values in the literature involving either RGO or metal sulfides/other metal compounds (sulfur content of <60 wt% and sulfur loading of <3 mg cm –2 ).

25 ENERGY STORAGE↗
DOE OSTI2025

Catalytic Electrolyte Additive for High-Loading and Lean Electrolyte Li–S Batteries

The cycle life of high-energy Li–S cells is largely constrained by the quick electrolyte depletion. LiNO 3 has been a well-established additive known for protecting the Li metal anode and stabilizing the battery from polysulfide “shuttling”. However, it can be depleted prematurely and can pose safety risks when exposed to carbon, sulfur, or Li metal under harsh conditions. Here, in this study, LiPO 2 F 2 was explored as a safe and durable alternative additive in ether-based electrolytes. LiPO 2 F 2 demonstrates superior performance in Li/S batteries, especially under high sulfur loading (∼4 mg/cm 2 ) and lean electrolyte conditions (E/S = 4), achieving a long-term cycling stability of 40%, compared to 14.7% with LiNO 3 . This additive facilitates the disproportionation of polysulfides, reducing their dissolution and mitigating the shuttle effect. Additionally, LiPO 2 F 2 promotes the formation of a stable solid-electrolyte interphase (SEI) composed of inorganic anion-derived species, improving the battery’s overall stability and functionality. These findings blaze a trail in the design of safer and more durable electrolytes for Li–S batteries.

Li-S batteries↗
DOE OSTI2023

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

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

25 ENERGY STORAGE↗
DOE OSTI2022

Extreme fast charge aging: Correlation between electrode scale and heterogeneous degradation in Ni-rich layered cathodes

Extreme fast charging (XFC) is a key requirement for the adoption of battery-based electric vehicles by the transportation sector. However, XFC has been shown to accelerate degradation, causing the capacity, life, and safety of batteries to deteriorate. There are no systematic studies in the open literature regarding aging modes in Ni-rich Li y Ni 0.a Mn 0.b Co 0.c O 2 (NMCabc) cathodes caused by fast charging. Herein, we report the effects of cathode composition and electrode loading in pouch cells containing NMC532, 622 and 811 paired with graphite and cycled under XFC conditions. The relative anisotropic volume change in the unit cell increases with Ni content in low-loading cells, while it levels up for all three NMC cathodes in high-loading cells because of substantial Li plating. The amounts of lithium plating and heterogeneity on the anode, determined by crystallographic phase quantification, were found to be correlated with electrode loading and cathode heterogeneity. The concentrations of the transition metals deposited on the anodes depend on NMCabc composition in a complex way. More particle cracking and surface degradation was found in NMC811. Here, the findings in this work provide a new understanding of the failure mechanisms and their practical implications for compositional tuning of future high-Ni NMCabc cathode materials during fast charging.

25 ENERGY STORAGE↗
DOE OSTI2017

Gel based sulfur cathodes with a high sulfur content and large mass loading for high-performance lithium–sulfur batteries

A significantly improved conductive matrix design for the sulfur electrode is essential to solve several problems related to sulfur electrochemistry toward the development of practical lithium–sulfur batteries (LSBs). Great progress has been made by using a variety of carbon-based nanostructures for physically and chemically confining soluble polysulfides as well as providing conductive paths. However, most of these electrode designs have a low sulfur content or a low sulfur loading, leading to a low specific capacity or low areal capacity at the electrode level. Herein, intrinsically N- and O-doped carbon nanoribbon (CNR) aerogels, obtained by pyrolysis of bacterial cellulose (BC) aerogels, were employed to form gel-based sulfur cathodes, simultaneously achieving both a high sulfur content and a high sulfur loading. With a sulfur loading of 6.4 mg cm−2 and a sulfur content of 90% at the whole electrode (including the current collector) level, a capacity as high as 943 mA h g−1 was achieved, which corresponds to an areal capacity of 5.9 mA h cm−2. The outstanding cell performance is attributed to the gel based cathode structure, which can strongly hold a large amount of the catholyte and relieve the shuttle effect of lithium polysulfides.

Li, Shiqi↗
DOE OSTI2021

Efficient diffusion of superdense lithium via atomic channels for dendrite-free lithium–metal batteries

The non-uniform aggregation of fast-diffused Li on an anode surface would aggravate its tip-effect-induced nucleation/growth, leading to the notorious dendrite growth in Li metal batteries (LMBs). Tuning the Li diffusion on the anode surface has been regarded previously as a mainstream method to induce its uniform deposition, while the diffusion of Li in the anode bulk is usually ignored. In this study, conceptually different from the classic surface modification, we propose a molecular tunnelling strategy to construct atomic channels in graphite bulk, which enables the fast diffusion of superdense Li. Density functional theory calculations and ab initio molecular dynamics simulations prove that the bulk diffusion through atomic channels could become a new and dominating path. Its reversible and efficient diffusion has been further visualized by in situ transmission electron microscopy. As a result, when coupled with high-loading LiFePO 4 cathodes (20 mg cm –2 ), a high areal capacity and 100% capacity retention are achieved over 370 cycles. Through this work a new strategy is developed based on the bulk-diffusion of superdense Li for dendrite-free LMBs, which can be pervasive in other high-performance energy storage systems.

25 ENERGY STORAGE↗
DOE OSTI2016

A core–shell electrode for dynamically and statically stable Li–S battery chemistry

Sulfur is an appealing cathode material for establishing advanced lithium batteries as it offers a high theoretical capacity of 1675 mA h g -1 at low material and operating costs. However, the lithium–sulfur (Li–S) electrochemical cells face several formidable challenges arising from both the materials chemistry (e.g., low electrochemical utilization of sulfur and severe polysulfide diffusion) and battery chemistry (e.g., dynamic and static instability and low sulfur loadings). Here in this study, we present the design of a core–shell cathode with a pure sulfur core shielded within a conductive shell-shaped electrode. The new electrode configuration allows Li–S cells to load with a high amount of sulfur (sulfur loadings of up to 30 mg cm -2 and sulfur content approaching 70 wt%). The core–shell cathodes demonstrate a superior dynamic and static electrochemical stability in Li–S cells. The high-loading cathodes exhibit (i) a high sulfur utilization of up to 97% at C/20–C/2 rates and (ii) a low self-discharge during long-term cell storage for a three-month rest period and at different cell-storage conditions. Finally, a polysulfide-trap cell configuration is designed to evidence the eliminations of polysulfide diffusion and to investigate the relationship between the electrode configuration and electrochemical characteristics. Finally, the comprehensive analytical results based on the high-loading cathodes suggest that (i) the core–shell cathode is a promising solution for designing highly reversible Li–S cells and (ii) the polysulfide-trap cell configuration is a viable approach to qualitatively evaluating the presence or absence of polysulfide diffusion.

25 ENERGY STORAGE↗
DOE OSTI2019

Pathways for practical high-energy long-cycling lithium metal batteries

Lithium (Li)-ion batteries play a critical role in modern day technologies, but their specific energy (Wh kg-1) and energy density (Wh L-1) are approaching the maximum practically achievable values based on existing manufacturing processes with the conventional cathode and anode materials. Developing the next generation rechargeable batteries with a specific energy higher than 300 Wh kg-1, up to 500 Wh kg-1, is a significant challenge. This paper discusses the pathways to build the next generation 500 Wh kg-1 rechargeable Li battery based on Li metal anode and a high nickel-content lithium nickel-manganese-cobalt oxide (high-Ni NMC) cathode. The fundamental requirements and practical technical approaches will be explored to hopefully address this grand challenge. In particular, we discuss the detailed cell level requirements and parameters to achieve high energy density, as well as the significant scientific challenges and potential solutions, including but not limited to enable the direct utilization of Li metal anode with high efficiency and long-term cycling stability, dendrite-free Li metal deposition, high utilization of the cathode materials with high mass loading and reasonable electrode thickness along with minimum parasitic weight in the cathode side. The cell level understanding and validation of the materials properties for high performance and control of interfacial reactions across the whole cell will be explored. New concepts in emerging multifunctional materials and electrolytes/additives and their implications will also be discussed.

lithium metal anode, lithium nickel manganese coba↗
DOE OSTI2017

Rational Design of Statically and Dynamically Stable Lithium-Sulfur Batteries with High Sulfur Loading and Low Electrolyte/Sulfur Ratio

Here, the primary challenge with lithium–sulfur battery research is the design of sulfur cathodes that exhibit high electrochemical efficiency and stability while keeping the sulfur content and loading high and the electrolyte/sulfur ratio low. With a systematic investigation, a novel graphene/cotton–carbon cathode is presented here that enables sulfur loading and content as high as 46 mg cm –2 and 70 wt% with an electrolyte/sulfur ratio of as low as only 5. The graphene/cotton–carbon cathodes deliver peak capacities of 926 and 765 mA h g –1 , respectively, at C/10 and C/5 rates, which translate into high areal, gravimetric, and volumetric capacities of, respectively, 43 and 35 mA h cm –2 , 648 and 536 mA h g –1 , and 1067 and 881 mA h cm –3 with a stable cyclability. They also exhibit superior cell–storage capability with 95% capacity–retention, a low self–discharge constant of just 0.0012 per day, and stable poststorage cyclability after storing over a long period of six months. Here, this work demonstrates a viable approach to develop lithium–sulfur batteries with practical energy densities exceeding that of lithium–ion batteries.

25 ENERGY STORAGE↗
DOE OSTI2017

Burning lithium in CS 2 for high-performing compact Li 2 S–graphene nanocapsules for Li–S–batteries

Here, tremendous efforts have been made to design the cathode of Li–S batteries to improve their energy density and cycling life. However, challenges remain in achieving fast electronic and ionic transport while accommodating the significant cathode volumetric change, especially for the cathode with a high practical mass loading. Here we report a cathode architecture, which is constructed by burning lithium foils in a CS 2 vapour. The obtained structure features crystalline Li 2 S nanoparticles wrapped by few-layer graphene (Li 2 S@graphene nanocapsules). Because of the improvement on the volumetric efficiency for accommodating sulfur active species and electrical properties, the cathode design enables promising electrochemical performance. More notably, at a loading of 10 mg Li 2 S cm –2 , the electrode exhibits a high reversible capacity of 1,160 mAh g –1 s, namely, an area capacity of 8.1 mAh cm –2 . Li 2 S@graphene cathode demonstrates a great potential for Li-ion batteries, where the Li 2 S@graphene-cathode//graphite-anode cell displays a high capacity of 730 mAh g –1 s as well as stable cycle performance.

25 ENERGY STORAGE↗
DOE OSTI2016

A Carbon-Cotton Cathode with Ultrahigh-Loading Capability for Statically and Dynamically Stable Lithium–Sulfur Batteries

Sulfur exhibits a high theoretical capacity of 1675 mA h g -1 via a distinct conversion reaction, which is different from the insertion reactions in commercial lithium-ion batteries. In consideration of its conversion reaction battery chemistry, a custom design for electrode materials could establish the way for attaining high-loading capability while simultaneously maintaining high electrochemical utilization and stability. In this study, this process is undertaken by introducing carbon cotton as an attractive electrode-containment material for enhancing the dynamic and static stabilities of lithium-sulfur (Li-S) batteries. The carbon cotton possessing a hierarchical macro-/microporous architecture exhibits a high surface area of 805 m 2 g -1 and high microporosity with a micropore area of 557 m 2 g -1 . The macroporous channels allow the carbon cotton to load and stabilize a high amount of active material. The abundant microporous reaction sites spread throughout the carbon cotton facilitate the redox chemistry of the high-loading/content Li-S system. As a result, the high-loading carbon-cotton cathode exhibits (i) enhanced cycle stability with a good dynamic capacity retention of 70% after 100 cycles and (ii) improved cellstorage stability with a high static capacity retention of above 93% and a low time-dependent self-discharge rate of 0.12% per day after storing for a long period of 60 days. In conclusion, these carbon-cotton cathodes with the remarkably highest values reported so far of both sulfur loading (61.4 mg cm -2 ) and sulfur content (80 wt %) demonstrate enhanced electrochemical utilization with the highest areal, volumetric, and gravimetric capacities simultaneously.

25 ENERGY STORAGE↗
DOE OSTI2022

Polyimide as a durable cathode for all-solid-state Li(Na)–organic batteries with boosted cell-level energy density

The integration of organic electrode materials (OEMs) with solid-state electrolytes (SSEs) is expected to build an all-solid-state battery (ASSB) with long-term sustainability, high safety, and high energy density. Despite this great promise, the cell-level energy density is still far from practically applicable, which stems from the ultrathick SSE layer and thin cathode layer used in a pellet-type ASSB design. Here, a cost-effective polyimide (PI) material was first exploited as an organic cathode for sulfide-based ASSBs. A capacity of ~190 mAh g -1 was delivered with almost no capacity decay over 300 cycles. Moreover, for the first time, a dry-film approach was introduced to manufacture a sheet-type Li–organic ASSB with an ultrathin SSE layer and a high-areal-loading PI cathode. Notably, PI is a perfect candidate for dry-film technology due to its high thermal stability and extraordinary chemical inertness toward sulfide SSEs. Remarkably, the free-standing SSE membrane was merely 46 μm thick, and an ultralow areal resistance of 3.3 Ω cm 2 was achieved, more than tenfold lower than that of reported SSE pellets. One order of magnitude boost in the cell-level energy density was achieved. This work presents a significant leap in transferring organic ASSB technology from laboratory research to factory manufacturing.

25 ENERGY STORAGE↗
DOE OSTI2017

A Fluorinated Ether Electrolyte Enabled High Performance Prelithiated Graphite/Sulfur Batteries

Lithium/sulfur (Li/S) batteries have attracted great attention as a promising energy storage technology, but so far their practical applications are greatly hindered by issues of polysulfide shuttling and unstable lithium/electrolyte interface. To address these issues, a feasible strategy is to construct a rechargeable prelithiated graphite/sulfur batteries. In this study, a fluorinated ether of bis(2,2,2-trifluoroethyl) ether (BTFE) was reported to blend with 1,3-dioxolane (DOL) for making a multifunctional electrolyte of 1.0 M LiTFSI DOL/BTFE (1:1, v/v) to enable high performance prelithiated graphite/S batteries. First, the electrolyte significantly reduces polysulfide solubility to suppress the deleterious polysulfide shuttling and thus improves capacity retention of sulfur cathodes. Second, thanks to the low viscosity and good wettability, the fluorinated electrolyte dramatically enhances the reaction kinetics and sulfur utilization of high-areal-loading sulfur cathodes. More importantly, this electrolyte forms a stable solid-electrolyte interphase (SEI) layer on graphite surface and thus enables remarkable cyclability of graphite anodes. Lastly, by coupling prelithiated graphite anodes with sulfur cathodes with high areal capacity of ~3 mAh cm -2 , we demonstrate prelithiated graphite/sulfur batteries that show high sulfur-specific capacity of ~1000 mAh g -1 and an excellent capacity retention of >65% after 450 cycles at C/10.

25 ENERGY STORAGE↗
DOE OSTI2020

Dry-pressed lithium nickel cobalt manganese oxide (NCM) cathodes enabled by holey graphene host

There is an increasing demand for electric vehicle batteries with higher energy densities that can be manufactured with low cost utilizing environmentally friendly processes. Lithium nickel cobalt manganese oxides (NCM), such as LiNi(0.5)Co(0.2)Mr(0.3)O(2) (NCM523), are commonly used in commercial lithium ion batteries for electric vehicle applications. These cathodes are typically fabricated using environmentally hazardous, energy intensive, and time-consuming solvent-based slurry casting processes. Polymeric binders, also required for cathode preparation, add weight and can undergo parasitic reactions during battery cycling. Here we report a facile, solvent-free, binder-free, and rapid cold-press electrode fabrication process to prepare high mass loading NCM cathodes within minutes. This process is enabled by the use of holey graphene, a unique lightweight, compressible carbon nanomaterial that serves as both a binder and an electrically conductive matrix. NCM cathodes fabricated by this method are stable and exhibit good active material utilization. A significant advantage for the dry-press process is that the electrode mass loadings can be readily increased simply by adding more composite powder to the compression molding die, resulting in improved areal capacities that are attractive for applications requiring high energy per unit footprint. (C) 2020 Elsevier Ltd. All rights reserved.

25 ENERGY STORAGE↗
DOE OSTI2025

Locally Confined Polysulfide-Reactive Electrolytes for Shuttle-Free Sodium–Sulfur Batteries

Sodium-sulfur batteries promise high-energy-density and sustainable electrochemical energy storage but suffer from uncontrolled polysulfides dissolution and high sodium reactivity. These challenges fundamentally originate from poor electrolyte-electrode compatibility. Current electrolyte research inadequately addresses the trade-off between minimal polysulfides solvation and stabilizing sodium interfaces. Here, we present a locally-confined polysulfide-reactive electrolyte strategy that mediates the polysulfide dissolution dynamics and sodium stability by leveraging an electrophilic solvating species with a localized high-concentration electrolyte. This design enables shuttle-free cell operation by synergistically restricting the global solvating power of the electrolyte through intermolecular interactions and locally scavenging sparingly dissolved polysulfides via electrolyte electrophilicity. The precisely confined surface reaction facilitates a protective cathode-electrolyte interface, realizing a quasi-solid-state sulfur conversion in our liquid ether-based electrolyte, which crucially avoids crossover-induced catastrophic sodium-metal degradation. The proposed electrolyte demonstrates long-term cycling of high-mass-loading sulfur cathodes (> 3 mg S cm −2 with commercial carbon host and 70 wt% sulfur content), which afford 710 mA h g −1 over 400 cycles in coin cells and steady pouch cell operation over 180 cycles. Furthermore, this work establishes a scalable electrolyte design protocol that regulates the reaction chemistry of highly reactive electrodes, offering a pathway toward sustainable renewable energy storage.

25 ENERGY STORAGE↗
DOE OSTI2024

Optimizing high energy density sulfur cathodes: A multivariate approach to electrode formulation and processing

Lithium-sulfur (Li-S) batteries involve complex solid-liquid-solid phase transformations during both discharging and charging processes, where cathode materials, formulation, and structure play a crucial role. Here, a design of experiments (DoE) methodology and an empirical model are developed to systematically explore the interactions and trade-offs among cathode factors and process variables, and to obtain generalizable effects estimates for the multivariate system. Compared to the conventional one-factor-at-a-time (OFAT) approach, this work demonstrates advantages in both efficiency and accuracy by allowing the data to guide future research and decisions. Further, an optimized cathode formulation and processing parameters are predicted and validated experimentally, achieving over 1000 mAh g -1 in discharge capacity and improved cycling under practical lean electrolyte (4 µL mg -1 S) and high S-loading cathodes (>4 mg cm -2 ) conditions. The optimized cathode was scaled up and assembled into Li-S pouch cells, achieving 316 Wh kg -1 in cell-level energy, proving that the comprehensive and rigorous framework for optimizing complex systems with DoE leads to improved performance in a practical pouch cell system.

25 ENERGY STORAGE↗