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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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Several of NASA's future Planetary Exploration (specifically Mars) missions will require rechargeable batteries of high specific energy and energy density and more importantly of good low temperature performance.
Electric vehicles are pivotal in the global shift toward decarbonizing road transport, with lithium-ion batteries at the heart of this technological evolution. However, the pursuit of batteries capable of extremely fast charging that also satisfy high energy and safety criteria, poses a significant challenge to current lithium-ion batteries technologies. Additionally, the increasing demand for aluminum (Al) and copper (Cu) in electrification, solar energy technologies, and vehicle light-eighting is driving these metals toward near-critical status in the medium term. This study introduces metalized polythylene terephthalate (mPET) polymer films by depositing an Al or Cu thin layer onto two sides of a polyethylene terephthalate film—named mPET/Al and mPET/Cu, as lightweight, cost-effective alternatives to traditional metal current collectors in lithium-ion batteries. We have fabricated current collectors that significantly reduce weight (by 73%), thickness (by 33%), and cost (by 85%) compared with traditional metal foil counterparts. These advancements have the potential to enhance energy density to 280 Wh kg -1 at the electrode level under 10-min charging at 6 C. Through testing, including a novel extremely fast charging protocol across various C-rates and long-term cycling (up to 1000 cycles) in different cell configurations, the superior performance of these metalized polymer films has been demonstrated. Notably, mPET/Cu and mPET/Al films exhibited comparable capacities to conventional cells under extremely fast charging, with the mPET cells showing a 27% improvement in energy density at 6 C and maintaining significant energy density after 1000 cycles. This study underscores the potential of mPET films to revolutionize the roll-to-roll battery manufacturing process and significantly advance the performance metrics of lithium-ion batteries in electric vehicles applications.
Abstract Lithium metal solid‐state batteries (LMSSBs) have demonstrated their high energy density and cycling performance at high current densities in an anode‐free architecture, featuring a thin Ag/C composite buffer layer (BL) between the current collector (CC) and the solid electrolyte (SE). This study explains the microscopic mechanism of the Ag/C BL by using first‐principles atomistic and continuum modeling. It is shown that Ag effectively acts as a homogeneous solid‐solution beyond AgLi 2.32 and maintains a positive potential even at AgLi 25 during lithiation. Key factors underlying the working of the Ag/C BL include lower interfacial resistance at the BL/CC interface than at the BL/SE interface, leading to predominant Li deposition on BL/CC, and substantial Ag–Li volume expansion during lithiation. This, combined with stronger BL/SE adhesion, causes BL/SE separation and Ag–Li extrusion toward the CC side. During delithiation, Ag re‐precipitates as nanoparticles uniformly on the CC, with its positive lithiation potential homogenizing Li currents in subsequent cycles. Other metals are less effective due to their relatively large overpotential, premature lithiation termination, and limited volume expansions hindering movement toward the CC. The study aids the BL design, focusing on metal choice and optimization material and microstructural properties, such as the Li‐ion conductivity and interfacial resistance.
The anode-free lithium (Li) batteries (AFLBs) have great potential to provide higher energy density than most other batteries. However, the performance of AFLBs is very sensitive to pressure and other operating parameters, especially for coin cells widely used in AFLB investigations. Therefore, optimizing cell assembly parameters and test protocol is critical to get reliable and comparable results in this field. In this work, the operating voltage range of AFLBs using a localized high concentration electrolyte has been optimized. The morphology of the deposited Li in AFLBs is much more indicting to the pressure than other type of batteries due to the absence of anode active material (i.e. Li) as a pressure cushion layer in the as prepared cells. With an optimized cycling protocol, a thin layer of uniform nucleation sites can be formed in the initial cycle which will facilitate smooth Li desposition/stripping in the subsequent cycles of AFLBs. The solid electrolyte interphase layer formed under optimized pressure and uniform pressure distribution exhibits a good mechanical stability even after long-term cycling. In conclusion, with an optimized cell configuration, the internal pressure in the coin cells has been optimized to improve the cycling performance of AFLBs (Cu||NMC811) with 72% of capacity retention in 100 cycles.
Lithium extraction from clay deposits is typically hampered by low lithium grades and the high capital and energy demands of conventional processing. We report an ambient temperature electrochemical leaching method that bypasses high-temperature roasting and concentrated-acid leaching, directly liberating 93% of lithium from low-grade hectorite in 24 h at 1 V, with 77% Faradaic efficiency, an energy intensity of 3.91 MWh/t lithium carbonate equivalent (LCE). Utilizing a carbon-mineral composite slurry electrode strategy we achieve electron-driven lattice deconstruction through iron oxidation coupled with proton uptake to drive lithium deintercalation, offering a new strategy for low-temperature critical-metal recovery. A preliminary cost analysis highlights pathways to achieving cost intensities below $3000/t LCE. Challenges remain in improving current density, extraction kinetics, and demonstrating process scalability, however, this work establishes a foundation for effective electrochemical lithium extraction from abundant but previously uneconomical clay deposits.
All-solid-state lithium ion batteries (ASSLBs) are considered next-generation devices for energy storage due to their advantages in safety and potentially high energy density. As the key component in ASSLBs, solid-state electrolytes (SSEs) with non-flammability and good adaptability to lithium metal anodes have attracted extensive attention in recent years. Among the current SSEs, composite solid-state electrolytes (CSSEs) with multiple phases have greater flexibility to customize and combine the advantages of single-phase electrolytes, which have been widely investigated recently and regarded as promising candidates for commercial ASSLBs. Based on existing investigations, herein, we present a comprehensive overview of the recent developments in CSSEs. Initially, we introduce the historical development from solid-state ionic conductors to CSSEs, and then summarize the fundamentals including mechanisms of lithium ion transport, key evaluation parameters, design principles, and key materials. Finally, four main types of advanced structures for CSSEs are classified and highlighted according to the recent progress. Moreover, advanced characterization and computational simulation techniques including machine learning are reviewed for the first time, and the main challenges and perspectives of CSSEs are also provided for their future development.
With the increasing use of Li batteries for storage, their safety issues and energy densities are attracting considerable attention. Recently, replacing liquid organic electrolytes with solid-state electrolytes (SSE) has been hailed as the key to developing safe and high-energy-density Li batteries. In particular, Li 1+ x Al x Ti 2- x (PO4) 3 (LATP) has been identified as a very attractive SSE for Li batteries due to its excellent electrochemical stability, low production costs, and good chemical compatibility. However, interfacial reactions with electrodes and poor thermal stability at high temperatures severely restrict the practical use of LATP in solid-state batteries (SSB). Herein, a systematic review of recent advances in LATP for SSBs is provided. Here, this review starts with a brief introduction to the development history of LATP and then summarizes its structure, ion transport mechanism, and synthesis methods. Challenges (e.g., intrinsic brittleness, interfacial resistance, and compatibility) and corresponding solutions (ionic substitution, additives, protective layers, composite electrolytes, etc.) that are critical for practical applications are then discussed. Last, an outlook on the future research direction of LATP-based SSB is provided.
The lithium metal battery is one of today's most promising high-energy-density storage devices. Its full-scale implementation depends on solving operational and safety issues intrinsic to the Li metal high reactivity leading to uncontrolled electrolyte decomposition and uneven Li deposition. In this work, we study the spontaneous formation of the solid electrolyte interphase (SEI) upon contact of Li metal with the electrolyte and describe the heterogeneous SEI morphological features. Multiple electrolyte formulations based on lithium bis(fluorosulfonyl)imide (LiFSI), dimethoxyethane (DME), dimethyl carbonate (DMC), 1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE) and bis(2,2,2-trifluoroethyl) ether (BTFE) are used. Findings include the description of the SEI evolution from dispersed LiO, LiS, LiN, and LiF clusters to a continuous and compact inorganic phase in which the LiO and LiF content depend on the presence of fluorine diluents. Further, the role of the DME ether solvent helping the growth of a “wet-SEI” is compared to that of the highly unstable carbonate DMC, which decomposes into complex radical oligomers that might contribute to further electrolyte decomposition. The impact of the electrolyte-to-anode ratio on LiFSI decomposition is highlighted. Finally, we suggest the existence of a critical LiFSI concentration and electrolyte-to-anode ratio that could potentially balance the rate of electrolyte depletion and lithium consumption.
The widespread adoption of electric vehicles necessitates higher-energy-density and longer-life cathode materials for Li-ion batteries. LiNiO 2 offers a higher energy density at a lower cost than other high-Ni-content cathodes containing additional transition-metal ions. However, detrimental phase transformations and impedance growth, resulting from structural defects formed during synthesis, lead to poor cyclability and limit the practical viability of LiNiO 2 . Herein, we demonstrate a considerably improved cycle life for LiNiO 2 by synthesizing it under a pressurized oxygen environment. The capacity retention in pouch-type full cells with a graphite anode after 1000 cycles is increased from 59 to 76% by applying a mere 1.7 atm of oxygen pressure during the synthesis of LiNiO 2 . With iodometric titration and inductively coupled plasma optical emission spectroscopy analysis, we provide clear evidence that oxygen pressure during synthesis reduces the occurrence of lattice oxygen vacancies and increases the content of Ni 3+ in LiNiO 2 , improving its structural integrity and cyclability. Post-mortem analysis of the cycled cathodes provides insights into the sources of degradation occurring during long-term cycling. Here, this work demonstrates a practically viable, synthetic approach combined with doping and coating to achieve improved performance with high-Ni layered oxide materials. Furthermore, this work represents the first report of extended cycling of LiNiO 2 in pouch full cells with graphite anode and will, therefore, serves as an important benchmark for future research on LiNiO 2 .
Superconductivity is a fascinating phenomenon that involves an attractive interaction by which electrons are paired and can move without electrical resistance below a critical temperature T c . A paradigm for understanding superconductive pairing, the successful “BCS” theory, developed more than 65 years ago, is challenged by certain classes of materials for which parameters (e.g. the value of T c , the density of electrons, etc.) fall outside the range for which BCS theory is applicable. The study of such materials is important because new physics may be revealed and because superconductivity has many potential applications in sensing and electronics. Superconductivity at very low carrier density is a rare and fascinating phenomenon that is of considerable importance and interest in condensed matter physics. The conditions of high density of states and effective screening of Coulomb repulsion, both key ingredients of stable Cooper pairing in the BCS theory, may not be met at low carrier density. Thus, such systems may also harbor unconventional electron pairing (e.g. non-phononic) or pairing without phase coherence as a precursor to Bose-Einstein condensation. An intriguing route toward extreme low-density (and possibly unconventional) superconductivity may be found in quasi-one-dimensional metals for which density-wave instabilities compete for the ground state and can lead to gapping of substantial portions of the Fermi surface (FS), leaving a residual (reconstructed) FS comprising a very small carrier density. Our work highlights a novel material in this unusual category: Li 0.9 Mo 6 O 17 (T c =2 K) (also known as "lithium purple bronze" or "LiPB"). We present both electrical and thermoelectric magnetotransport measurements that reveal superconductivity to occur at carrier density 2 x10 17 cm -3 , among the lowest known for any superconductor, and four orders of magnitude lower than is expected from its chemical valence and band structure. With its exceptionally large ratio of superconducting to Fermi temperature, T c /TF ≳ 0.1, LiPB is properly placed at the top of a very small group of superconductors (including cuprates, heavy-fermion and Fe-based superconductors) for which this ratio falls in the BCS-BEC crossover regime and for which pairing is believed to be spin mediated.
Fluorine substitution is a critical enabler for improving the cycle life and energy density of disordered rocksalt (DRX) Li-ion battery cathode materials which offer prospects for high energy density cathodes, without the reliance on limited mineral resources. Due to the strong Li–F interaction, fluorine also is expected to modify the short-range cation order in these materials which is critical for Li-ion transport. In this work, density functional theory and Monte Carlo simulations are combined to investigate the impact of Li–F short-range ordering on the formation of Li percolation and diffusion in DRX materials. Additionally, the modeling reveals that F substitution is always beneficial at sufficiently high concentrations and can, surprisingly, even facilitate percolation in compounds without Li excess, giving them the ability to incorporate more transition metal redox capacity and thereby higher energy density. It is found that for F levels below 15%, its effect can be beneficial or disadvantageous depending on the intrinsic short-range order in the unfluorinated oxide, while for high fluorination levels the effects are always beneficial. Using extensive simulations, a map is also presented showing the trade-off between transition-metal capacity, Li-transport, and synthetic accessibility, and two of the more extreme predictions are experimentally confirmed.
The lithium–sulfur (Li–S) battery is an attractive high-energy-density technology for future flexible and wearable electronics, but it is a challenge to simultaneously realize adequate flexibility, stability, and energy density. Recent studies show that fibrous materials are promising to achieve flexible batteries with high energy density, by taking advantages of their intrinsic flexibility, lightweight, large surface area, and cost-effectiveness. With a good tunability of the structure and function, fibrous materials can be suitable to construct various components of a working battery, including current collectors, buffer layers, interlayers, and solid-state electrolytes. In this review, we summarize the recent development of fibrous materials for flexible Li–S batteries, with an emphasis on the discussion of the synthesis and preparation of materials, design of fibrous structures and functionalities, and layout of battery cells for achieving high Coulombic efficiency, long cycle life, and good flexibility.
Abstract The development of solid‐state batteries (SSBs) with lithium Li metal anodes holds significant promise for enhancing the energy density and safety of next‐generation energy storage systems. However, their commercialization is hindered by challenges related to Li dendrite formation, which can lead to short circuits and battery failure. In this study, the role of Ag nanoparticles embedded within solid electrolytes (SE) is investigated in suppressing dendrite propagation. The results demonstrate that Ag nanoparticles effectively mitigate two key failure mechanisms: (1) dendrite growth within porous networks at low current densities and (2) stress intensification‐induced SE fracture at higher current densities (12 mA cm −2 ). Ex situ characterization using focused‐ion beam – scanning electron microscopy (FIB–SEM) and energy dispersive X‐ray spectroscopy (EDS,) reveals that Ag nanoparticles migrate alongside advancing Li dendrites, promoting homogeneous dendrite growth and reducing the likelihood of localized stress concentrations. Additionally, the incorporation of Ag nanoparticles is shown to facilitate a more uniform Li distribution toward the anode side, which can potentially enable the use of higher charging rates in SSBs. This study provides a new perspective on Li dendrite suppression and presents new opportunities for enhancing the performance and safety of SSBs.
Silicon is seen as one of the most promising anode candidates for next-generation lithium-ion batteries, due to its high theoretical capacity and energy density. However, many technical barriers remain to its implementation, due to its high chemical/electrochemical reactivities with standard electrolytes and incomplete passivation from large volume changes. Herein, we report an isosorbide dimethyl ether (IDE) based electrolyte, which exhibits greatly improved stability, as evidenced by long cycle life and calendar life. An analysis of the cycled silicon surface shows minimal decomposition of organic species from IDE solvent, confirming that the electrolyte maintains a limited chemical reactivity with nucleophilic lithiated silicon (Li x Si). Here, this research opens up new avenues for designing new electrolytes which could ultimately enable the practical application of silicon anodes.
Charging energy-dense lithium-ion batteries (LIBs) with thick graphite electrodes at high current densities are typically accompanied by poor performance and safety issues. The root cause is the onset of Li plating at the surface of graphite when lithiated to a high capacity within a short time period. Here, we investigated the behavior of graphite electrodes with various particle sizes under fast charge operations. Results from the electrochemical characterization on graphite electrodes exhibit the superiority of smaller particles over bigger particles in terms of suppressing the onset of Li plating and growth of plated Li particles. Observations from scanning electron microscopy also corroborate the presence of plated Li in electrodes with big graphite particles and its absence in graphite electrodes with small particles, when the cells were lithiated to 90% of the state of charge (SOC). Further, the improved performance of cells with the small particles might be associated with the low Li-ion concentration at the surface of graphite and thus reduced overpotential in graphite electrodes. The simulated results revealed that, compared to bigger particles, smaller particles have lower surface intercalation at any given cell SOC, which may significantly reduce the overpotential in the graphite electrodes and mitigate the onset of Li plating. This agrees well with experimental observations.
Interfacial instability between lithium metal and solid-state electrolytes limits the performance of all-solid-state lithium metal batteries (ASSLBs), leading to parasitic reactions, non-uniform Li+ flux, and dendrite growth. Here, we develop a composite interlayer composed of the anti-perovskite Li2OHCl0.75Br0.25 (AP) and carbon nanotubes (CNTs) to enhance both interfacial stability and ionic transport. The AP–CNT interlayer exhibits enhanced Li+ conductivity arising from interfacial electron transfer from AP to CNTs, which generates a built-in electric field that facilitates Li+ migration. Lithium symmetric cells incorporating this interlayer achieve a high critical current density of 2.4 mA cm−2 at 55 °C. This design integrates chemical robustness with coupled ion–electron transport, offering a generalizable strategy for safe, dendrite-free, and high-performance ASSLBs.
Currently produced electric vehicles (EVs) rely on the use of lithium ion battery technology due to its high energy and power density. However, a major barrier facing the adoption of electric vehicles is that currently utilized Li-ion batteries take significantly longer to recharge (~ 30 minutes) compared to the time necessary to refuel vehicles powered by internal combustion engines (< 10 minutes). Thus, the need to develop Li-ion batteries which can be charged in approximately 10 minutes (6 C rate) without sacrificing range, cost, or cycle life is critical for the widespread implementation of EVs.
Anode-free solid-state batteries (AFSSBs) are a promising route toward achieving high energy density. In these cells, the anode contains no pre-stored lithium (Li). Instead, all Li inventory originates from the cathode and is freshly deposited onto a bare current collector during charging. However, achieving uniform and defect-free Li plating on this bare current collector remains a major challenging, often resulting in low Li plating/stripping efficiency and rapid capacity decay. Here, for the first time, operando neutron imaging is employed to visualize Li plating/stripping behavior in an anode-free full cell with LiNi 0.82 Mn 0.07 Co 0.11 O 2 (NMC) as the cathode. Operando measurements reveal that complete stripping of Li leaves isolated Li residues on the current collector, which degrades interfacial contact between the current collector and solid-state electrolyte. To mitigate this interfacial issue and promote more uniform Li deposition, we implement a discharge cutoff voltage strategy that intentionally retains a thin residual Li layer after stripping. This thin Li layer, serving as an in situ–formed seed layer, not only enables more homogeneous subsequent Li plating but also improves interfacial contact. As a result, the anode-free cell with a controlled discharge voltage of 3.5 V exhibits excellent long-term cycling stability, maintaining a discharge capacity of 116 mAh g -1 with a retention rate of 83.4% and an average Coulombic efficiency of approximately 99.9% after 430 cycles at 0.25 C. In contrast, the cell with a conventional discharge cutoff voltage of 2.8 V exhibits rapid capacity decay, retaining only 59.7 mAh g -1 after 50 cycles with a capacity retention of 40.7%. This work offers a practical strategy to unlock the long-term viability of anode-free solid-state batteries.