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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 55 records · Page 3

Unravelling high-temperature stability of lithium-ion battery with lithium-rich oxide cathode in localized high-concentration electrolyte

Lithium (Li)-rich manganese (Mn)-rich oxide (LMR) cathode materials, despite of the high specific capacity up to 250 mAh g-1 suffer from instability of cathode/electrolyte interfacial layer at high working voltages, causing continuous voltage decay and capacity fading, especially at elevated temperatures. In various battery systems, localized high-concentration electrolytes (LHCEs) have been widely reported as a promising candidate to form effective electrode/electrolyte interphases. Here, an optimized LHCE is studied in graphite (Gr)-based full cells being cycled at 25, 45 and 60 °C with the reference of a conventional LiPF6-based electrolyte. It is revealed that the LHCE can effectively suppress continuous electrolyte decompositions and mitigate the dissolution of Mn ions due to the formation of more protective electrode/electrolyte interphases on both anode and cathode, which, in turn, lead to significantly improved cycling stability and enhanced rate capability under the selected temperatures. The mechanistic understanding on the failure of the conventional LiPF6-containing electrolyte and the function of the LHCE in Gr||LMR cells under high temperatures provides valuable perspectives of electrolyte development for practical application of LMR cathodes in high energy density batteries over a wide temperature range.

Localized high-concentration electrolyte, Lithium-↗

Failure Mechanism of Fast-Charged Lithium Metal Batteries in Liquid Electrolyte

In recent years, lithium anode has re-attracted broad interest because of the necessity of employing lithium metal in the next-generation battery technologies such as lithium sulfur (Li-S) and lithium oxygen (Li-O2) batteries. Fast capacity degradation and safety issue associated with rechargeable lithium metal batteries have been reported, although the fundamental understanding on the failure mechanism of lithium metal at high charge rate is still under debate due to the complicated interfacial chemistry between lithium metal and electrolyte. Herein, we demonstrate that, at high current density, the quick growth of porous solid electrolyte interphase towards bulk lithium, instead of towards the separator, dramatically builds up the cell impedance that directly leads to the cell failure. Understanding the lithium metal failure mechanism is very critical to gauge the various approaches used to address the stability and safety issues associated with lithium metal anode. Otherwise, all cells will fail quickly at high rates before the observation of any positive effects that might be brought from adopting the new strategies to protect lithium.

Environmental Molecular Sciences Laboratory↗

A lithium–oxygen battery with a long cycle life in an air-like atmosphere [Lithium-oxygen batteries with long cycle life in a realistic air atmosphere]

Lithium-air batteries are considered to be a potential alternative to lithium-ion batteries for transportation applications, owing to their high theoretical specific energy. So far, however, such systems have been largely restricted to pure oxygen environments (lithium oxygen batteries) and have a limited cycle life owing to side reactions involving the cathode, anode and electrolyte. In the presence of nitrogen, carbon dioxide and water vapour, these side reactions can become even more complex. Moreover, because of the need to store oxygen, the volumetric energy densities of lithium-oxygen systems may be too small for practical applications. Here we report a system comprising a lithium carbonate-based protected anode, a molybdenum disulfide cathode and an ionic liquid/di methyl sulfoxide electrolyte that operates as a lithium-air battery in a simulated air atmosphere with a long cycle life of up to 700 cycles. We perform computational studies to provide insight into the operation of the system in this environment. Furthermore this demonstration of a lithium-oxygen battery with a long cycle life in an air-like atmosphere is an important step towards the development of this field beyond lithium-ion technology, with a possibility to obtain much higher specific energy densities than for conventional lithium ion batteries.

25 ENERGY STORAGE↗

Investigation of the Decomposition Mechanism of Lithium Bis(oxalate)borate (LiBOB) Salt in the Electrolyte of an Aprotic Li-O 2 Battery

The stability of the lithium bis(oxalate) borate (LiBOB) salt against lithium peroxide (Li2O2) in an aprotic Li-O2 cell is investigated. From theoretical and experimental findings, we find that the chemical decomposition of LiBOB in electrolytes leads to the formation lithium oxalate during discharge of a Li-O2 cell. According to DFT calculations, the formation of lithium oxalate as the reaction product is exothermic, and therefore is thermodynamically feasible. This reaction seems to be independent of solvents used in the Li-O2 cell, and therefore LiBOB is probably not suitable to be used as the salt in Li-O2 cell electrolytes.

Lau, Kah Chun↗

Effects of Imide–Orthoborate Dual-Salt Mixtures in Organic Carbonate Electrolytes on the Stability of Lithium Metal Batteries

The effects of lithium imide and lithium orthoborate dual-salt electrolytes of different salt chemistries in carbonate solvents on the cycling stability of Li metal batteries were systematically and comparatively investigated. Two imide salts (LiTFSI and LiFSI) and two orthoborate salts (LiBOB and LiDFOB) were chosen for this study and compared with the conventional LiPF6 salt. The cycling stability of the Li metal cells with the electrolytes follows the order from good to poor as LiTFSI-LiBOB > LiTFSI-LiDFOB > LiPF6 > LiFSI-LiBOB > LiFSI-LiDFOB, indicating that LiTFSI behaves better than LiFSI and LiBOB over LiDFOB in these four dual-salt mixtures. The LiTFSI-LiBOB can effectively protect the Al substrate and form a more robust surface film on Li metal anode, while the LiFSI-LiBOB results in serious corrosion to the stainless steel cell case and a thicker and looser surface film on Li anode. Computational calculations indicate that the chemical and electrochemical stabilities also follow the order of LiTFSI-LiBOB > LiTFSI-LiDFOB > LiFSI-LiBOB > LiFSI-LiDFOB. The key findings of this work emphasize that the salt chemistry is critically important for enhancing the interfacial stability of Li metal anode and should be carefully manipulated in the development of high performance Li metal batteries.

Li metal batteries, dual-salt electrolyte, solid e↗

Lithium-Ion Batteries with Lithium Manganese Iron Phosphate Cathodes and Lithium Titanate Anodes: Linking Electrode Dynamics to Cell Performance

This study examines the electrochemical performance, impedance behavior, and aging mechanisms of lithium-ion cells pairing lithium manganese iron phosphate (LiMn 0.6 Fe 0.4 PO 4 , LMFP64) cathodes with lithium titanate (Li 4 Ti 5 O 12 , LTO) anodes. LMFP64 half-cells display distinct Fe and Mn redox plateaus at ∼3.5 and ∼4.1 V, respectively, and deliver excellent rate capability. Three-electrode measurements show that LMFP64 dominates cell impedance, which changes sharply across the Fe–Mn redox transition and decreases with increasing temperature (30 °C–50 °C). Voltage hysteresis arises mainly from the cathode, with higher C-rates shortening redox plateaus and broadening the transition region. Elevated temperature lowers impedance, especially near the Mn-redox and transition regions, but accelerates capacity fade. Post-cycling analyses of electrodes confirm structural stability of LMFP64 and indicate loss of lithium inventory (LLI) as the source of capacity fade. This LLI causes potential slippage between the LMFP64 and LTO electrodes, which decreases the Fe-redox plateau width. Long-term cycling highlights the critical role of electrode overhang: cathode overhang mitigates capacity fade by buffering lithium loss, whereas anode overhang cells experience faster capacity decline due to uncompensated lithium depletion. These results clarify LMFP64/LTO battery impedance evolution, thermal effects, and degradation pathways and provide insights for their applications in electric vehicles.

Area Specific Impedance↗

Long term stability of Li-S batteries using high concentration lithium nitrate electrolytes

The lithium-sulfur (Li-S) battery is a very promising candidate for the next generation of energy storage systems required for electrical vehicles and grid energy storage applications due to its very high theoretical specific energy (2500 W h kg(-1)). However, low Coulombic efficiency (CE) during repeated Li metal plating/stripping has severely limited the practical application of rechargeable Li-S batteries. In this work, a new electrolyte system based on a high concentration of LiNO3 in diglyme (G2) solvent is developed which enables an exceptionally high CE for Li metal plating/stripping and thus high stability of the Li anode in the sulfur-containing electrolyte. The tailoring of electrolyte properties for the Li anode has proven to be a highly successful strategy for improving the capacity retention and cycle life of Li-S batteries. This electrolyte provides a CE of greater than 99% for over 200 cycles of Li plating/stripping. In contrast, the Li anode cycles for less than 35 cycles (with a high CE) in the state-of-the-art 1 M LiTFSI + 0.3 M LiNO3 in 1,3-dioxolane: 1,2-dimethoxyethane (DOL:DME) electrolyte under the same conditions. The stable Li anode enabled by the new electrolyte may accelerate the applications of high energy density Li-S batteries in both electrical vehicles and large-scale grid energy storage markets.

Coulombic efficiency↗