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The most successful lithium-ion batteries (LIBs) based on ethylene carbonate electrolytes and graphite anodes still suffer from severe energy and power loss at temperatures below -20 °C, which is because of high viscosity or even solidification of electrolytes, sluggish de-solvation of Li at the electrode surface, and slow Li transportation in solid electrolyte interphase (SEI). Here, a coherent lithium phosphide (LiP) coating firmly bonding to the graphite surface to effectively address these challenges is engineered. The dense, continuous, and robust LiP interphase with high ionic conductivity enhances Li transportation across the SEI. Plus, it promotes Li de-solvation through an electron transfer mechanism, which simultaneously accelerates the charge transport kinetics and stands against the co-intercalation of low-melting-point solvent molecules, such as propylene carbonate (PC), 1,3-dioxolane, and 1,2-dimethoxyethane. Consequently, an unprecedented combination of high-capacity retention and fast-charging ability for LIBs at low temperatures is achieved. In full-cells encompassing the LiP-coated graphite anode and PC electrolytes, an impressive 70% of their room-temperature capacity is attained at -20 °C with a 4 C charging rate and a 65% capacity retention is achieved at -40 °C with a 0.05 C charging rate. This research pioneers a transformative trajectory in fortifying LIB performance in cryogenic environments.
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http://dx.doi.org/10.1002/adma.202308675 | DOI Listing |
Angew Chem Int Ed Engl
September 2025
College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, 518060, P.R. China.
Intrinsic structural instability and sluggish reaction kinetics at the electrode/electrolyte interface are two critical concerns that block the application of MnO cathode in high-performance aqueous zinc-ion batteries. This work proposes a theoretical screening principle to select the compatible guest cation for MnO host, not only to strengthen the structure but also customize high-efficiency cathode/electrolyte interphase (CEI). As identified, Sr is selected as the suitable intercalation ion that enable in situ forming the SrSO CEI after partial release upon charge process.
View Article and Find Full Text PDFJ Colloid Interface Sci
November 2025
Key Laboratory of Optoelectronic Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, 155 Yangqiao Road West, Fuzhou, Fujian 350002, PR China.
The resurgence of lithium metal batteries (LMBs) has opened new avenues for the advancement of high-energy density secondary batteries. However, the electrochemical performance of LMBs at extreme temperatures remains suboptimal. As a critical component, electrolytes significantly influence the wide-temperature performance of LMBs.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
July 2025
State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, China.
Lithium metal batteries (LMBs) operating at high cut-off voltages can achieve an energy density exceeding 500 Wh kg; however, they often suffer from severe capacity degradation due to electrolyte decomposition. Herein, propylene glycol monomethyl ether acetate (PMA) is introduced as a novel solvent for LMB electrolytes. The unique ether-oxygen functionality in PMA exhibits high steric hindrance, leading to weak lithium-ion coordination, which promotes the formation of contact ion pairs (CIPs) in the electrolyte solvation structure, especially in the presence of dual salts.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
June 2025
Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055, P.R. China.
Construction of robust solid electrolyte interphases (SEIs) has proved effective in mitigating dendrite growth and side reactions of zinc (Zn) anodes in aqueous electrolytes. Fluorinated SEIs, in particular, have garnered significant attention due to their exceptional electrochemical stability and high Zn conductivity. However, the formation of such SEIs typically relies on the use of fluorine (F)-containing precursors, which inadvertently raise environmental and biological concerns because they show high resistance to degradation in natural environments.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
May 2025
Hubei Key Laboratory of Electrochemical Power Sources, Hubei Key Lab on Organic and Polymeric Opto-Electronic Materials, College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, 430072, China.
Lithium (Li) metal exhibits great potential for achieving high-energy-density rechargeable batteries. However, the practical application of Li metal anodes is severely hindered by the uncontrollable growth of lithium dendrites as well as the instability of the spontaneously generated solid electrolyte interphase (SEI), causing safety concerns and lifespan issues. Herein, we customize a novel urea-linked covalent organic framework (COF-531) as an interfacial Li-ion guided channel.
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