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Composite polymer-ceramic electrolytes have shown considerable potential for high-energy-density Li-metal batteries as they combine the benefits of both polymers and ceramics. However, low ionic conductivity and poor contact with electrodes limit their practical usage. In this study, a highly conductive and stable composite electrolyte with a high ceramic loading is developed for high-energy-density Li-metal batteries. The electrolyte, produced through in situ polymerization and composed of a polymer called poly-1,3-dioxolane in a poly(vinylidene fluoride)/ceramic matrix, exhibits excellent room-temperature ionic conductivity of 1.2 mS cm and high stability with Li metal over 1500 h. When tested in a Li|electrolyte|LiFePO battery, the electrolyte delivers excellent cycling performance and rate capability at room temperature, with a discharge capacity of 137 mAh g over 500 cycles at 1 C. Furthermore, the electrolyte not only exhibits a high Li transference number of 0.76 but also significantly lowers contact resistance (from 157.8 to 2.1 Ω) relative to electrodes. When used in a battery with a high-voltage LiNi Mn Co O cathode, a discharge capacity of 140 mAh g is achieved. These results show the potential of composite polymer-ceramic electrolytes in room-temperature solid-state Li-metal batteries and provide a strategy for designing highly conductive polymer-in-ceramic electrolytes with electrode-compatible interfaces.
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http://dx.doi.org/10.1002/smll.202302691 | DOI Listing |
J Colloid Interface Sci
September 2025
Key Laboratory of Automobile Materials, Ministry of Education and School of Materials Science and Engineering, Jilin University, Changchun 130022, China. Electronic address:
Neither single electrolyte design nor solid electrolyte interface (SEI) engineering alone can effectively resolve the dual challenges of sluggish reaction kinetics and unstable interfaces in polymer-based lithium metal batteries (LMBs). Herein, a rational integrated design strategy is adopted to simultaneously fabricate poly(trifluoroethyl methacrylate-co-4-oxo-5,8,11-trioxa-3-azatridec-12-en-1-yl acrylate)-based gel polymer electrolyte (PTDA-GPE) and stable composite SEI during the thermal-induced in situ polymerization process. The resulting PTDA-GPE demonstrates superior Li transport kinetics (1.
View Article and Find Full Text PDFSmall
September 2025
Department of Mechanical and Industrial Engineering, Northeastern University, 360 Huntington Avenue, Boston, Massachusetts, 02115, USA.
Understanding the electrochemical extraction and deposition of lithium (Li) from cathode is crucial for advancing anode-free solid-state batteries (AFSSBs). Herein, cryo-transmission electron microscopy (cryo-TEM) and electrochemical studies are employed to investigate how current collector surface properties, current densities, and cathode loadings influence the morphology of fresh electrochemically deposited Li and the electrochemical performance in sulfide-based AFSSBs. Cryo-TEM reveals that Cu current collectors induce irregular, dendritic Li deposits due to their lithiophobic nature and reactivity with LiPSCl (LPSC), while Ni and Au facilitate more uniform, planar-like Li growth.
View Article and Find Full Text PDFJ Chem Phys
September 2025
Department of Chemical Engineering, National Taiwan University of Science and Technology, Taipei 106, Taiwan.
All-solid-state Li-metal batteries using solid polymer electrolytes (SPEs) in combination with high-voltage cathodes such as lithium nickel manganese cobalt oxide (NMC) promise enhanced battery safety, energy density, and flexibility. However, understanding the oxidative decomposition of SPEs on the cathode surfaces and characterizing the resulting cathode-electrolyte interphase (CEI) remain challenging both experimentally and computationally. This study introduces a new computational protocol based on ab initio molecular dynamics for simulating the decomposition of PEO:LiTFSI SPE on the NMC-811 cathode surface using a combined electron- and Li+-removal simulation approach.
View Article and Find Full Text PDFChemSusChem
September 2025
i-Lab & CAS Key Laboratory of Nanophotonic Materials and Devices, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou, 215123, China.
Solid-state lithium metal batteries (SSLMBs) are promising for realizing higher energy density. However, the poor interfacial Li transport kinetics and Li dendrite growth inhibit SSLMBs, leading to sluggish interfacial ion diffusion and depressive lifespan, which is attributed to high barriers blocked by anions or interface space in solid-state electrolytes. Herein, a flexible solid-state polymer skeleton employed with ionic liquid and metal-organic frameworks (PIM) electrolyte is proposed to strengthen interfacial Li ion exchange by improving the Li sieving effect and interfacial wettability.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2025
School of Materials and Chemistry, University of Shanghai for Science and Technology, Shanghai, 200093, China.
Nitride family compounds are among the earliest explored materials for solid electrolytes (SEs). The main challenge lies in effectively enhancing their electrochemical stability without compromising their excellent Li-ion conductivity and Li metal compatibility. Herein, a H -H comproportionation reaction between LiH and NHF is employed to synthesize a Li-N-H-F complex, consisting of Li NHF matrix and dispersed LiF nanoparticles.
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