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The commercial use of lithium metal batteries is greatly limited by dendrite formation and slow Li transport at the anode-electrolyte interface. Herein, the constructed high-modulus polymer interlayer suppressed the Li dendrite formation, leading to dense deposition and enhanced Li transport. Meanwhile, this formed robust organic solid-electrolyte interphase inhibited the side reactions occurring at the anode-electrolyte interface while promoting a high Li flux. By constructing the polymer interlayer, the Li@P3DDT||Li@P3DDT symmetric cells demonstrated an impressive stability lifespan of over 3400 h at 1 mA/cm and 1 mAh/cm. The LFP||Li@P3DDT full cells exhibit a remarkable capacity retention of 85.0% over 300 cycles at 4 C. Furthermore, the 50 μm Li@P3DDT||LiCoO pouch cell with 380 Wh kg maintained over 99.9% retention of capacity over 60 cycles at 0.5 C. The research paves the way for the advancement of stable lithium anodes.
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http://dx.doi.org/10.1021/acs.nanolett.5c01606 | DOI Listing |
Small
September 2025
Key Laboratory of Electrochemical Power Sources of Hubei Province, College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, 430072, China.
Hybrid artificial layer based on inorganic/polymer composite endows superior toughness and mechanical strength, which can achieve high stability of lithium metal anode. However, the large particle size and uneven distribution of inorganic fillers hinder the uniform flow of lithium ions across the membrane, making it difficult to achieve smooth lithium metal deposition/stripping. In this work, a chemical lithiation-induced defluorination strategy is proposed to engineer poly(vinylidene difluoride) (PVDF)-based artificial layers, enabling in situ incorporation of highly dispersed LiF nanofiller within the polymer matrix and precise control over the LiF content.
View Article and Find Full Text PDFSmall
September 2025
School of Materials Science and Engineering, State Key Laboratory of Silicon and Advanced Semiconductor Materials, Zhejiang University, Hangzhou, 310027, P. R. China.
High-concentration electrolytes (HCEs) face inherent challenges such as high viscosity and diminished ionic conductivity caused by the formation of three-dimensional (3D) anion networks, which limit their practical applications. In this study, it is demonstrated that encapsulating HCEs within metal-organic frameworks (MOFs) effectively disrupts these 3-D networks, resulting in significantly enhanced ionic conductivity. Raman spectroscopy, nuclear magnetic resonance (NMR), and molecular dynamics (MD) simulations reveal a significant reduction in aggregates (AGGs)-state anion within MOF-confined electrolytes, confirming the reconstruction of the solvation environment.
View Article and Find Full Text PDFNatl Sci Rev
September 2025
College of Chemistry, Huazhong Agricultural University, Wuhan 430070, China.
The stress distribution in Li metal strongly affects the interfacial Li-ion diffusion, thereby influencing the morphology of plated Li and the performance of the battery. Here, we report a mechano-electrochemical coupling strategy that utilizes an arched structured carbon aerogel to achieve stable Li-plating/stripping electrochemistry. The arch-structured carbon aerogel can actively regulate stress distributions in response to the compressive stresses induced by Li deposition, generating the transition of stress from compressive on the convex surface to tensile on the concave surface, which can effectively promote the Li-migration kinetics and thus suppress the non-uniform deposition of Li.
View Article and Find Full Text PDFNanoscale Horiz
September 2025
Department of Chemistry and Biochemistry, University of California, Los Angeles, California 90095, USA.
Nanostructuring, which shortens lithium-ion diffusion lengths, can help facilitate pseudocapacitive behavior in some battery materials. Here, nanostructured LiNiCoAlO (NCA), with porosity and decreased crystallite size compared to commercial bulk NCA, was synthesized using a colloidal polymer template. Small particles (∼150 nm) were obtained using rapid thermal annealing (RTA), while medium particles (∼300 nm) were obtained with conventional heating.
View Article and Find Full Text PDFACS Appl Mater Interfaces
September 2025
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Institute of New Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Fudan University, Shanghai 200433, China.
Li-metal batteries promise ultrahigh energy density, but their application is limited by Li-dendrite growth. Theoretically, fluorine-containing anions such as bis(fluorosulfonyl)imide (FSI) in electrolytes can be reduced to form LiF-rich solid-electrolyte interphases (SEIs) with high Young's modulus and ionic conductivity that can suppress dendrites. However, the anions migrate toward the cathode during the charging process, accompanied by a decrease in the concentration of interfacial anions near the anode surface.
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