Abstract
Garnet-type solid-state batteries (SSBs) are considered to be one of the most promising candidates to realize next-generation lithium metal batteries with high energy density and safety. However, the dendrite-induced short-circuit and the poor interfacial contact impeded the practical application. Herein, interface engineering to achieve low interfacial resistance without high temperature calcination was developed, which Li6.4La3Zr1.4Ta0.6O12 (LLZTO) was simply coated with complex hydride (Li4(BH4)3I (3L1L)) in various mass ratios n(Li4(BH4)3I)-(100−n)LLZTO (10 ≤ n ≤ 40). The interfacial conductivity increases by more than three orders of magnitude from 8.29 × 10−6 S·cm−1to 1.10 × 10−2 S·cm−1. Symmetric Li cells exhibit a high critical current density (CCD) of 4.0 mA·cm−2 and an excellent cycling stability for 200 h at 4.0 mA·cm−2. SSBs with polymeric sulfur-polyacrylonitrile (SPAN) cathode achieve a high discharge capacity of 1149 mAh·g−1 with a capacity retention of 91% after 100 cycles (0.2 C). This attempt guides a simple yet efficient strategy for obtaining a stable Li/LLZTO interface, which would promote the development of solid-state batteries.
Graphical abstract
摘要
本文设计了一种降低Li6.4La3Zr1.4Ta0.6O12(LLZTO)界面电阻的界面工程方法,整个过程无需长时间高温煅烧,在LLZTO表面制备了一系列具有不同质量比氢化物包覆的复合固态电解质n(Li4(BH4)3I)-(100‒n)LLZTO (10≤n≤40)。界面电导率从8.29×10−6 S·cm−1增加到1.10×10−2 S·cm−1,增加近4个数量级 临界电流密度高达4.0 mA·cm−2并且电池可以在4.0 mA·cm−2的电流密度中稳定循环超过200 h。组装的Li/SPAN 全固态电池在100次循环(0.2C)后维持1149 mAh·g−1的高放电容量,容量保持率为91%。这一尝试为获得稳定的Li/LLZTO界面提供了一种简单而有效的策略,这将有利于固态电池的发展。
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Acknowledgments
This study was financially supported by the National Natural Science Foundation of China (Nos. 52171180, 51802154, and 51971065), the National Science Fund for Distinguished Young Scholars (No. 51625102), the Innovation Program of Shanghai Municipal Education Commission (No. 2019-01-07-00-07-E00028), the Fundamental Research Funds for the Central Universities (No. NG2022005), the Open Fund for Graduate Innovation Base in Nanjing University of Aeronautics and Astronautics (No. xcxjh20210612), and partially supported by the Fundamental Research Funds for the Central Universities, NS2021043.
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Lv, YT., Zhang, TF., Hu, ZT. et al. High critical current density in Li6.4La3Zr1.4Ta0.6O12 electrolyte via interfacial engineering with complex hydride. Rare Met. 43, 692–701 (2024). https://doi.org/10.1007/s12598-023-02479-7
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DOI: https://doi.org/10.1007/s12598-023-02479-7