Abstract:The garnet-type electrolyte is one of the most promising solid-state electrolytes due to its high ionic conductivity and wide electrochemical window. However, such electrolytes generate Li2CO3 in the air, leading to an increase in impedance, which greatly limits their practical application.In turn, high-entropy ceramics can improve phase stability due to the high entropy effect. Herein, the high-entropy garnet (HEG) Li6.2La3(Zr0.2Hf0.2Ti0.2Nb0.2Ta0.2)2O12 (LL(ZrHfTiNbTa)O) solid-state J u s t A c c e p t e d h… Show more
“…The electronic conductivity of LLZTO was shortened from 1.4 × 10 −8 to 1.8 × 10 −10 S cm −1 after electron-blocking layer deposition. Figure 5b and Table S1 show the electronic conductivity comparison chart of our work with other literature reports 23 , 40 , 42 – 49 , which is the lowest value among reported publications. Fig.…”
Garnet oxide is one of the most promising solid electrolytes for solid-state lithium metal batteries. However, the traditional interface modification layers cannot completely block electron migrating from the current collector to the interior of the solid-state electrolyte, which promotes the penetration of lithium dendrites. In this work, a highly electron-blocking interlayer composed of potassium fluoride (KF) is deposited on garnet oxide Li6.4La3Zr1.4Ta0.6O12 (LLZTO). After reacting with melted lithium metal, KF in-situ transforms to KF/LiF interlayer, which can block the electron leakage and inhibit lithium dendrite growth. The Li symmetric cells using the interlayer show a long cycle life of ~3000 hours at 0.2 mA cm−2 and over 350 hours at 0.5 mA cm−2 respectively. Moreover, an ionic liquid of LiTFSI in C4mim-TFSI is screened to wet the LLZTO|LiNi0.8Co0.1Mn0.1O2 (NCM) positive electrode interfaces. The Li|KF-LLZTO | NCM cells present a specific capacity of 109.3 mAh g−1, long lifespan of 3500 cycles and capacity retention of 72.5% at 25 °C and 2 C (380 mA g−1) with an average coulombic efficiency of 99.99%. This work provides a simple and integrated strategy on high-performance quasi-solid-state lithium metal batteries.
“…The electronic conductivity of LLZTO was shortened from 1.4 × 10 −8 to 1.8 × 10 −10 S cm −1 after electron-blocking layer deposition. Figure 5b and Table S1 show the electronic conductivity comparison chart of our work with other literature reports 23 , 40 , 42 – 49 , which is the lowest value among reported publications. Fig.…”
Garnet oxide is one of the most promising solid electrolytes for solid-state lithium metal batteries. However, the traditional interface modification layers cannot completely block electron migrating from the current collector to the interior of the solid-state electrolyte, which promotes the penetration of lithium dendrites. In this work, a highly electron-blocking interlayer composed of potassium fluoride (KF) is deposited on garnet oxide Li6.4La3Zr1.4Ta0.6O12 (LLZTO). After reacting with melted lithium metal, KF in-situ transforms to KF/LiF interlayer, which can block the electron leakage and inhibit lithium dendrite growth. The Li symmetric cells using the interlayer show a long cycle life of ~3000 hours at 0.2 mA cm−2 and over 350 hours at 0.5 mA cm−2 respectively. Moreover, an ionic liquid of LiTFSI in C4mim-TFSI is screened to wet the LLZTO|LiNi0.8Co0.1Mn0.1O2 (NCM) positive electrode interfaces. The Li|KF-LLZTO | NCM cells present a specific capacity of 109.3 mAh g−1, long lifespan of 3500 cycles and capacity retention of 72.5% at 25 °C and 2 C (380 mA g−1) with an average coulombic efficiency of 99.99%. This work provides a simple and integrated strategy on high-performance quasi-solid-state lithium metal batteries.
“…The electronic conductivity of LLZTO was shortened from 1.4×10 − 8 S cm − 1 to 1.8×10 − 10 S cm − 1 after KF buffer layer deposition. Figure 5b and Table S1 showed the electronic conductivity comparation chart of our work with other literature reports 23,33,[35][36][37][38][39][40][41][42] , which is the lowest value among reported publications.…”
Garnet oxide is one of the most promising solid-state electrolytes for solid-state lithium metal batteries. However, the traditional interface modification layers cannot completely block electron migrating from the current collector to the interior of the solid-state electrolyte, which promotes the penetration of lithium dendrites. In this work, a highly electron-blocking interlayer composed of potassium fluorine (KF) is developed to inhibit lithium dendrite growth in garnet oxide Li6.4La3Zr1.4Ta0.6O12 (LLZTO). Thanks to the interlayer of stable KF with large band gap, the electronic conductivity of LLZTO reduces by two orders of magnitude. The Li symmetric cells using KF interlayer show an ultralong cycle life ~3000 hours at 0.2 mA cm-2 and over 350 hours at 0.5 mA cm-2 respectively. Moreover, an ionic liquid of LiTFSI in C4mim-TFSI is screened to wet the cathode interfaces. The solvent-free Li|LLZTO|LiNi0.8Co0.1Mn0.1O2 cells present a high specific capacity, and a long lifespan of 3500 cycles at 2C with an average coulombic efficiency of 99.99%. This work provides a simple and integrated strategy on high-performance solid-state lithium metal batteries.
“…The Ti doping improves the density, while the Hf doping prevents the Li + /H + exchange to enhance the air stability. The synergistic effect of multiple elements increases both air stability and ionic conductivity of high-entropy garnet [95]. Jung et al revealed that the high-entropy effects (e.g.…”
Section: Mechanism For High-entropy Electrolytesmentioning
confidence: 99%
“…In the LL(ZrHfTiNbTa)O electrolyte, Hf inhibits the Li + /H + from exchange, improving the air stability. Nb and Ta have the capability to enhance the ionic conductivity [95]. Additionally, Ti is able to prevent the Li dendrites [114].…”
Section: The Impacts Of Individual Components On the Electrochemical ...mentioning
Lithium-ion batteries (LIBs) has extensively utilized in electric vehicles and portable electronics due to their high energy density and prolonged lifespan. However, the current commercial LIBs are plagued by relatively low energy density. High-entropy materials with multiple components have emerged as an efficient strategic approach for developing novel materials that effectively improve the overall performance of LIBs. This article provides a comprehensive review the recent advancements in rational design of innovative high-entropy materials for LIBs, as well as the exceptional lithium ion storage mechanism for high-entropy electrodes and considerable ionic conductivity for high-entropy electrolytes. This review also analyses the prominent effects of individual components on the high-entropy materials’ exceptional capacity, considerable structural stability, rapid lithium ion diffusion, and excellent ionic conductivity. Furthermore, this review presents the synthesis methods and their influence on the morphology and properties of high-entropy materials. Ultimately, the remaining challenges and future research directions are outlined, aimed at developing more effective high-entropy materials and improving the overall electrochemical performance of LIBs.
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