The stability of high-energy-density lithium metal batteries (LMBs) heavily relies on the composition of the solid electrolyte interphase (SEI) formed on lithium metal anodes. In this study, the inorganic-rich SEI layer was achieved by incorporating bisalts additives into carbonate-based electrolytes. Within this SEI layer, the presence of LiF, polythionate, and LiN was observed, generated by combining 1.0 м lithium bis(trifluoromethanesulfonyl)imide in ethylene carbonate: ethyl methyl carbonate:dimethyl carbonate in a 1 : 1 : 1 volume ratio, with the addition of 2 wt% lithium difluorophosphate and 2 wt% lithium difluoro(oxalato)borate additives (EL-DO). Furthermore, this formulation effectively mitigated corrosion of aluminum current collectors. EL-DO exhibited outstanding performance, including an average coulombic efficiency of 98.2 % in Li||Cu cells and a stable discharge capacity of approximately 162 mAh g after 200 cycles in a Li||LiNiCoMnO (NCM811) configuration. Moreover, EL-DO displayed the potential to enhance the performance not only of LMBs but also of lithium-ion batteries. In the case of Gr||NCM811 cell using EL-DO, it consistently maintained high discharge capacities, even achieving around 135 mAh g after the 100 cycle, surpassing the performance of other electrolytes. This study underscores the synergistic impact of bisalts additives in elevating the performance of lithium batteries.
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http://dx.doi.org/10.1002/cssc.202400636 | DOI Listing |
Proc Natl Acad Sci U S A
January 2025
Department of Physics and Astronomy, University of California, Irvine, CA 92697.
Understanding topological defects-controlled structural degradation of layered oxides-a key cathode material for high-performance lithium-ion batteries-plays a critical role in developing next-generation cathode materials. Here, by constructing a nanobattery in an electron microscope enabling atomic-scale monitoring of electrochemcial reactions, we captured the electrochemically driven atomistic dynamics and evolution of dislocations-a most important topological defect in material. We deciphered how dislocations nucleate, move, and annihilate within layered cathodes at the atomic scale.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
January 2025
Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science & Engineering, Beijing Institute of Technology, Beijing 100081, China.
Lithium-ion batteries (LIBs) have become advanced energy storage technologies; however, specific capacity remains limited by the active materials in cathodes. Here, we report Li-LiNO batteries (LNBs) where LiNO in electrolyte serves as both active materials and ion conductor at room temperature. LNBs operate on a highly reversible redox between NO and NO, which results in an impressive areal capacity of 19 mAh cm at a plateau voltage of 1.
View Article and Find Full Text PDFDalton Trans
January 2025
State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, 210023, China.
Silicon-based anode materials experience significant volume changes and low conductivity during the lithiation process, which severely hinders their successful application in lithium-ion batteries. Reducing the size of silicon particles and effectively combining them with carbon-based materials are considered the main strategies to enhance the lithium-ion storage performance of silicon-based anodes. In this study, we employed a "bottom-up" strategy to synthesize Si@C anode materials by cross-linking octa-aminopropyl polyhedral oligomeric silsesquioxane (NH-POSS) with terephthalaldehyde and subsequent high-temperature treatment and low-temperature liquid reduction.
View Article and Find Full Text PDFChem Commun (Camb)
January 2025
School of Metallurgy and Environment, Central South University, Changsha 410083, Hunan, China.
CuF and LiBOB were co-introduced into polycarbonate-based polymer electrolytes (PVT-CB) to overcome the trade-offs between ionic conduction and interfacial stability, resulting in improved ionic conductivity (8.4 × 10 S cm) and enhanced electrochemical stability (5.04 V Li/Li).
View Article and Find Full Text PDFMacromol Rapid Commun
January 2025
Institut für Chemie, Technische Universität Chemnitz, Straße der Nationen 62, 09111, Chemnitz, Germany.
Aromatic diimides such as naphthalene diimide (NDI) and pyromellitic diimide (MDI) are important building blocks for organic electrode materials. They feature a two-electron redox mechanism that allows for energy storage. Due to the smaller size of MDI compared to NDI its theoretical capacity is higher.
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