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Garnet-type solid electrolytes (SEs) exhibit high ionic conductivity, a wide electrochemical window, and lithium stability, making them ideal for solid-state Li metal batteries. However, their air sensitivity leads to LiCO formation, causing poor Li wettability, high interfacial resistance, and dendrite growth. To address this, Mg(PO) is coated via a wet chemistry method, converting LiCO into a LiPO/MgO composite upon heating. This composite prevents reactions with moisture and CO, ensuring air stability while enhancing Li wettability and reducing interfacial resistance. The Li-conducting LiPO and insulating MgO in the composite interface enable rapid Li diffusion while effectively suppressing electron penetration, resulting in a high critical current density of 1.1 mA·cm, with stable cycling for over 1200 h at 0.4 mA·cm. Furthermore, the modified SEs demonstrate excellent cycling stability in Li metal batteries with LiFePO and LiCoO cathodes, confirming the practical feasibility of this solid electrolyte interface modification strategy.
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http://dx.doi.org/10.1021/acs.nanolett.5c01850 | DOI Listing |
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August 2025
Advanced Institute for Materials Research (WPI-AIMR), Tohoku University, Sendai, 980-8577, Japan.
Allsolidstate Li-metal batteries are emerging as a transformative energy storage technology, driven by the demand for higher energy density and enhanced safety in electric vehicles (EVs). Among myriad solid electrolytes, garnet-type LiLaZrO (LLZO) has attracted significant attention due to its high room-temperature (RT) Li-ion conductivity (>10 S cm) and chemical stability against metallic Li anodes. Nevertheless, achieving highly dense LLZO remains challenging, as conventional sintering methods, such as pressureless sintering or hot pressing (HP), require prolonged processing times, resulting in Li loss and low densification.
View Article and Find Full Text PDFACS Appl Mater Interfaces
September 2025
School of Mechanical Engineering, Yonsei University, 50 Yonsei-ro, Seodaemun-gu, Seoul 03722, Republic of Korea.
Exploring the vast chemical space of high-entropy (HE) solid-state electrolytes (SSEs) has become a highly active area of battery studies owing to the exceptional performance of all-solid-state batteries (ASSBs) with higher energy density and improved safety. The compositional complexity and extensive chemical space inherent to HE SSEs pose significant challenges for their investigation via conventional methodologies such as experimental approaches and density functional theory (DFT) calculations. In this study, we propose a novel material screening methodology aimed at accelerating the exploration of promising HE SSEs while maintaining reasonable computational costs and efficiency.
View Article and Find Full Text PDFRSC Adv
July 2025
Defense Materials and Energy Development Center, Agency for Defense Development Yuseong P.O. Box 35 Daejeon 34060 South Korea +82-42-821-3520 +82-42-821-2457.
The paradigm shift from conventional molten-salt electrolytes to solid-state garnet-type LiLaZrO (LLZO) electrolytes in thermal batteries represents a critical advancement in high-temperature energy-storage systems. This study evaluated Ta- and Ga-doped LLZO electrolytes for FeS/Li-Si thermal batteries, focusing on their structural stability and electrochemical performance at 500 °C. While Ga-doped LLZO exhibited superior ionic conductivity at 25 °C, Ta-doped LLZO demonstrated exceptional high-temperature stability.
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July 2025
Institute of New Energy for Vehicles, School of Materials Science and Engineering, Tongji University, Shanghai, 201804, China.
Pivoting toward high-safety solid-state batteries, garnet-type solid-state electrolytes (SEs) with 3D ion transport channels are highly promising candidates. Complex cation substitutions are proved efficacious in enhancing ionic conductivity, while the role of pre-exponential factor in Arrhenius equation receives insufficient attention compared to the activation energy term. Herein, multiple lattice site substitution is employed to elucidate the contribution of increased configurational entropy to phase formation and the predominance of local distortion on ionic conductivity.
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July 2025
Department of Materials Science and Engineering, National Yang Ming Chiao Tung University, 1001 University Road, Hsinchu, 30010, Taiwan.
Solid-state lithium batteries (SSLBs) with composite solid electrolytes (CSEs) offer enhanced energy density and high safety. However, their performance is hindered by large thickness and limited Li⁺ conductivity of CSEs, and large electrode/electrolyte interface resistance. This study develops an 18 µm-thick CSE using a polyethylene scaffold, which incorporates garnet-type LiLaZrGaO (LLZGO) oxide and an ionic liquid (IL) additive in a poly(vinylidene fluoride-co-hexafluoropropylene)/polypropylene carbonate matrix, achieving a high ionic conductivity of 8.
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