Garnet-based all-solid-state lithium batteries(ASSLBs)were considered as the most promising energy storage device due to their high energy density and good safety.However,interface problems caused by impurities such a...Garnet-based all-solid-state lithium batteries(ASSLBs)were considered as the most promising energy storage device due to their high energy density and good safety.However,interface problems caused by impurities such as Li_(2)CO_(3) on the surface still hinder the practical application of garnet-based ASSLBs.Here,we use a simple ultrasonic spraying method to coat SiO_(2) on the Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO)surface,and in-situ construct Li_(4)SiO_(4)/Li_(2) O/Li_(2)1 Si5 nano-multifunctional interlayer through the high-temperature conversion reaction of SiO_(2).Experiments and density functional theory(DFT)calculations demonstrate that the introduced Li_(4)SiO_(4)/Li_(2) O/Li_(2)1 Si_(5) nano-multifunctional interlayer at the LLZTO/Li interface can significantly improve the air stability and interface contact of LLZTO/Li.As a result,the interface impedance of Li/SiO_(2)@LLZTO/Li was reduced to 24.2Ωcm^(-2),and it can operate stably over 2400 and 1000 h at current densities of 0.05 and 0.2 mA cm^(−2),respectively.The full cell assembled with LiFePO_(4)(LFP)as cathode(Li/SiO_(2)@LLZTO/LFP)also exhibits excellent cycling performance(capacity retention rate of 95%after 50 cycles at 0.1 C)and rate performance(140 mAh g^(−1) at 0.1 C and 107 mAh g−1 at 1 C).This research provides a strategy to improve interface problems and achieve dendrite-free ASSLBs through in-situ transformation constructed nano-multifunctional interlayers.展开更多
基金The Key Research and Development Project of Hainan Province(No.ZDYF2022SHFZ093)sHainan Provincial Natural Science Foundation of China(No.120RC455)+1 种基金the Natural Science Foundation of China(No.61901142)the Program of Hainan Association for Science and Technology Plans to Youth R&D Innovation(No.QCXM202014)are acknowledged.
文摘Garnet-based all-solid-state lithium batteries(ASSLBs)were considered as the most promising energy storage device due to their high energy density and good safety.However,interface problems caused by impurities such as Li_(2)CO_(3) on the surface still hinder the practical application of garnet-based ASSLBs.Here,we use a simple ultrasonic spraying method to coat SiO_(2) on the Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO)surface,and in-situ construct Li_(4)SiO_(4)/Li_(2) O/Li_(2)1 Si5 nano-multifunctional interlayer through the high-temperature conversion reaction of SiO_(2).Experiments and density functional theory(DFT)calculations demonstrate that the introduced Li_(4)SiO_(4)/Li_(2) O/Li_(2)1 Si_(5) nano-multifunctional interlayer at the LLZTO/Li interface can significantly improve the air stability and interface contact of LLZTO/Li.As a result,the interface impedance of Li/SiO_(2)@LLZTO/Li was reduced to 24.2Ωcm^(-2),and it can operate stably over 2400 and 1000 h at current densities of 0.05 and 0.2 mA cm^(−2),respectively.The full cell assembled with LiFePO_(4)(LFP)as cathode(Li/SiO_(2)@LLZTO/LFP)also exhibits excellent cycling performance(capacity retention rate of 95%after 50 cycles at 0.1 C)and rate performance(140 mAh g^(−1) at 0.1 C and 107 mAh g−1 at 1 C).This research provides a strategy to improve interface problems and achieve dendrite-free ASSLBs through in-situ transformation constructed nano-multifunctional interlayers.
