Garnet-type Li_(7)La_(3)Zr_(2)O_(12)(LLZO)is one of the most promising solid-state electrolytes(SSEs).However,the application of LLZO is limited by structural instability,low ionic conductivity,and poor lithium stabil...Garnet-type Li_(7)La_(3)Zr_(2)O_(12)(LLZO)is one of the most promising solid-state electrolytes(SSEs).However,the application of LLZO is limited by structural instability,low ionic conductivity,and poor lithium stability.To obtain a garnet-type solid electrolyte with a stable structure and high ionic conductivity,a series of TaeCe co-doping cubic Li_(6.4)La_(3)Zr_(1.4-x)Ta_(0.6)Ce_(x)O_(12)(LLZTCO,x=,0.02,0.04,0.06,0.08,0.10,0.20,0.30)electrolytes were successfully synthesized through conventional solid-phase method.The Ta^(5+)doping can introduce more lithium vacancies and effectively maintain the stability of the cubic phase.The Ce^(4+)with a larger ionic radius is introduced into the lattice to widen the Lit migration bottleneck size,which significantly increased the ionic conductivity to 1.05×10^(-3)S/cm.It also shows excellent stability to lithium metal by the optimization of Lit transport channel.Li||LLZTCO||Li symmetric cells can cycle stably for more than 6000 h at a current density of 0.1 mA/cm^(2)without any surface modifications.The commercialization potential of LLZTCO samples in all solid-state lithium batteries(ASSLBs)is confirmed by the prepared LiFePO_(4)||LLZTCO||Li cells with a capacity retention rate of 98%after 100 cycles at 0.5C.This new co-doping method presents a practical solution for the realization of high-performance ASSLBs.展开更多
基金the National Natural Science Foundation of China(Grant No.52102123)Natural Science Foundation of Sichuan Province(Grant No.2022NSFSC2008,and Grant No.2023NSFSC0442)the China Postdoctoral Science Foundation(2022M710619).
文摘Garnet-type Li_(7)La_(3)Zr_(2)O_(12)(LLZO)is one of the most promising solid-state electrolytes(SSEs).However,the application of LLZO is limited by structural instability,low ionic conductivity,and poor lithium stability.To obtain a garnet-type solid electrolyte with a stable structure and high ionic conductivity,a series of TaeCe co-doping cubic Li_(6.4)La_(3)Zr_(1.4-x)Ta_(0.6)Ce_(x)O_(12)(LLZTCO,x=,0.02,0.04,0.06,0.08,0.10,0.20,0.30)electrolytes were successfully synthesized through conventional solid-phase method.The Ta^(5+)doping can introduce more lithium vacancies and effectively maintain the stability of the cubic phase.The Ce^(4+)with a larger ionic radius is introduced into the lattice to widen the Lit migration bottleneck size,which significantly increased the ionic conductivity to 1.05×10^(-3)S/cm.It also shows excellent stability to lithium metal by the optimization of Lit transport channel.Li||LLZTCO||Li symmetric cells can cycle stably for more than 6000 h at a current density of 0.1 mA/cm^(2)without any surface modifications.The commercialization potential of LLZTCO samples in all solid-state lithium batteries(ASSLBs)is confirmed by the prepared LiFePO_(4)||LLZTCO||Li cells with a capacity retention rate of 98%after 100 cycles at 0.5C.This new co-doping method presents a practical solution for the realization of high-performance ASSLBs.
