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Garnet-type LiLaZrTaO (LLZTO) is a promising solid-state electrolyte (SSE) because of its fast ionic conduction and notable chemical/electrochemical stability toward the lithium (Li) metal. However, poor interface wettability and large interface resistance between LLZTO and Li anode greatly restrict its practical applications. In this work, we develop an in situ chemical conversion strategy to construct a highly conductive LiS@C layer on the surface of LLZTO, enabling improved interfacial wettability between LLZTO and the Li anode. The Li/LiS@C-LLZTO-LiS@C/Li symmetric cell has a low interface impedance of 78.5 Ω cm, much lower than the 970 Ω cm of a Li/LLZTO/Li cell. Moreover, the Li/LiS@C-LLZTO-LiS@C/Li cell exhibits a high critical current density of 1.4 mA cm and an ultralong stability of 3000 h at 0.1 mA cm. When used in a LiFePO battery, the Li/LiS@C-LLZTO/LiFePO battery exhibits a high initial discharge capacity of 150.8 mA h g at 0.2 C without lithium storage capacity attenuation during 200 cycles. This work provides a novel and feasible strategy to address interface issues of SSEs and achieve lithium-dendrite-free solid-state batteries.
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http://dx.doi.org/10.1021/acsami.3c19215 | DOI Listing |
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August 2025
S2e and Engineering, Jiangsu Key Laboratory of Advanced Metallic Materials Southeast University, Nanjing, 211189, P. R. China.
LiLaZrTaO (LLZTO) solid electrolyte, renowned for its high ionic conductivity and robust safety profile at room-temperature, holds tremendous promise for diverse applications. However, it faces significant challenges, including high interface impedance with lithium and a propensity for lithium dendrite formation. To address these issues, a novel Li(BH)I/2(d-BN) (LBHIbn) composite buffer layer - exhibiting high ionic conductivity and critical current density - is introduced at the LLZTO|Li interface.
View Article and Find Full Text PDFACS Appl Mater Interfaces
May 2025
State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, P. R. China.
With the rising demand for lithium metal, the electrochemical lithium extraction method utilizing solid oxide electrolytes has garnered significant attention. However, due to the inevitable Li/H exchange between the solid electrolyte and water, the lithium extraction rate is constrained by the electrochemical performance of the solid electrolyte. Furthermore, for the potential direct application of the extracted lithium in lithium metal batteries, the uniformity of the extracted anode material is crucial.
View Article and Find Full Text PDFChemSusChem
July 2025
School of Materials Science and Engineering, Southeast University, Nanjing, 211189, P. R. China.
Fluoropolymer-based solid-state electrolytes (SSEs) promise next-generation all-solid-state Li metal batteries but suffer poor stability against Li metal anodes and sluggish Li transport. Herein, a garnet-type LiLaZrTaO (LLZTO) is proposed as a bifunctional mediator to enable the in-situ grafting and compositing for poly(vinylidene fluoride-co-hexafluoropropylene) (PVH), aiming at electrochemically stable and superionic SSEs. The LLZTO not only induces the formation of CC bonds as active sites for effectively grafting methyl methacrylate (MMA) brush chains to PVH but also acts as an ion-conducting filler to enhance mechanical properties and ion transport.
View Article and Find Full Text PDFJ Colloid Interface Sci
July 2025
College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou 310014, China. Electronic address:
Non-flammable butanedinitrile (SN) is recognized as a highly prospective plasticizer for significantly reducing the operating temperature of polyethylene oxide (PEO)-based solid polymer electrolytes. However, the instability of the lithium anode interface severely hinders the practical application of PEO/SN-based solid polymer electrolytes in room-temperature solid-state lithium metal batteries. In this work, we propose fast-ion conductive LiLaZrTaO (LLZTO) nanoparticles as corrosion inhibitors to constructure a multifunctional buffer layer on the surface of PEO/SN-based solid electrolyte (PSE@LLZTO) to stabilize the interface structure of Li anode via a facile spin-coating transfer technique.
View Article and Find Full Text PDFACS Appl Mater Interfaces
February 2025
Department of Materials Science and Engineering, National Tsing Hua University, Hsinchu 30013, Taiwan.
As the demand for safer lithium batteries grows, the quality of solid electrolytes, a critical component for solid-state lithium batteries (SSLBs) construction, has become increasingly important. SSLBs typically underperform compared to conventional batteries with liquid electrolytes. In this study, two ceramic-based composite solid electrolytes (CSEs) with differing dispersion qualities were prepared, consisting of dispersion-treated and as-received LiLaZrTaO (LLZTO) particles within a poly(vinylidene fluoride--hexafluoropropylene) (PVDF-HFP) matrix.
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