基于Cu-Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)复合层的3D多孔集流体用于构建稳定的锂金属负极  

Three-dimensional porous collector based on Cu-Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12) composite layer for the construction of stable lithium metal anode

作　　者：童志远 李子源 张可 TONG Zhiyuan;LI Ziyuan;ZHANG Ke(Aero Engine Research Center,School of Aerospace Engineering,Tsinghua University,Beijing 100084,China)

机构地区：[1]清华大学航天航空学院航空发动机中心,北京100084

出　　处：《无机化学学报》2025年第3期499-508,共10页Chinese Journal of Inorganic Chemistry

摘　　要：通过相转化共带浇筑法制备了一种基于Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO)固态电解质和3D多孔结构的铜复合层的集流体。LLZTO的加入为锂离子提供了丰富的离子传输通道与成核位点,而且具有3D多孔结构的铜为复合材料提供了丰富的比表面积,并可容纳大量的死锂等其他负极反应的副产物,同时相转化共带浇筑法操作简便,适合大面积商业化运用。制备的CuLLZTO@Li对称电池在4 mA·cm^(-2)的电流密度下实现了280 h的长循环寿命与25 mV的超低电压滞后,相较于铜箔和3D-Cu分别提升了4倍和3倍。得益于稳定的固态电解质(SEI)膜与无锂枝晶的生成,Cu-LLZTO@Li对称电池相较于Cu foil@Li和3D-Cu@Li对称电池表现出最低的欧姆电阻(2.749Ω·cm^(-2))和界面电阻(0.544Ω·cm^(-2))。Cu-LLZTO半电池在70圈循环中未产生软短路并保持了98.4%的库仑效率,循环中的充放电电压平台始终维持在0.15 V的较低水平。Here,we have prepared a kind of anode current collector based on Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO)solid electrolyte and copper composite layer with 3D porous structure by phase-transformation co-banding casting method,and the addition of LLZTO provides abundant ion transport channels and nucleation sites for lithium ions,while the copper with 3D porous structure provides enlarged specific surface area and can accommodate a large amount of dead lithium and other by-products generated in electrochemical process,and at the same time,the phasetransformation co-banding casting method is easy to operate and suitable for anode interface impedance increase.The prepared Cu-LLZTO@Li symmetric cell achieved a long cycle life of 280 h at a current density of 4 mA·cm^(-2)with an ultra-low voltage hysteresis of 25 mV,which was 4 times and 3 times higher than that of Cu foil and 3D-Cu,respectively.Thanks to the constructed stable solid electrolyte interphase(SEI)film and no lithium dendrite generation,the Cu-LLZTO@Li symmetric cell exhibited the lowest ohmic resistance(2.749Ω·cm^(-2))and interface resistance(0.544Ω·cm^(-2))compared to Cu foil@Li and [e-mail] the half-cell,Cu-LLZTO did not produce a soft short circuit and maintained 98.4%Coulombic efficiency over 70 cycles,and the charging and discharging voltage plateau was consistently maintained at a low level of 0.15 V during the cycle.

关 键 词：复合集流体 锂负极 固态电解质 界面接触 锂金属电池 

分 类 号：TM912[电气工程—电力电子与电力传动]