Dai Qiushi, Zhao Jun, Ye Hongjun, Chen Jingzhao, Su Yong, Yang Tingting, Liu Qiunan, Sun Haiming, Li Hui, Yao Jingming, Gao Zhiying, Fu Xingjie, Zhu Dingding, Yan Jitong, Li Mingyu, Qiu Hailong, Huang Qiao, Zhang Liqiang, Tang Yongfu, Guo Xiangxin, Huang Jianyu
Clean Nano Energy Center, State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao 066004, P. R. China.
School of Materials Science and Engineering, Xiangtan University, Xiangtan, Hunan 411105, P. R. China.
ACS Appl Mater Interfaces. 2021 Sep 15;13(36):42822-42831. doi: 10.1021/acsami.1c11613. Epub 2021 Sep 2.
High interfacial resistance and uncontrollable lithium (Li) dendrite are major challenges in solid-state Li-metal batteries (SSLMBs), as they lead to premature short-circuiting and failure of SSLMBs. Here, we report the synthesis of a composite anode comprising a three-dimensional LiCu nanowire network host infiltrated with Li (Li* anode) with low interfacial impedance and superior electrochemical performance. The Li* anode is fabricated by dissolving Cu foil into molten Li followed by solidification. The Li* anode exhibits good wettability with LiLaZrTaO (LLZTO) and high mechanical strength, rendering low Li*/LLZTO interfacial impedance, homogeneous deposition of Li, and suppression of Li dendrites. Consequently, the Li* anode-based symmetric cells and full cells with LiNiCoAlO (NCA), LiFePO (LFP), and FeF cathodes deliver remarkable electrochemical performance. Specifically, the Li*/LLZTO/Li* symmetrical cell achieves a remarkably long cycle lifetime of 10 000 h with 0.1 mA·cm; the Li*/LLZTO/NCA full cell maintains capacity retention of 73.4% after 500 cycles at 0.5C; and all-solid-state Li*/LLZTO/FeF full cell achieves a reversible capacity of 147 mAh·g after 500 cycles at 100 mA·g. This work demonstrates potential design tactics for an ultrastable Li*/garnet interface to enable high-performance SSLMBs.
高界面电阻和不可控的锂枝晶是固态锂金属电池（SSLMBs）面临的主要挑战，因为它们会导致SSLMBs过早短路和失效。在此，我们报道了一种复合阳极的合成，该阳极由三维锂铜纳米线网络主体组成，并渗透有锂（Li阳极），具有低界面阻抗和优异的电化学性能。Li阳极是通过将铜箔溶解在熔融锂中然后固化制成的。Li阳极与LiLaZrTaO（LLZTO）表现出良好的润湿性和高机械强度，使得Li/LLZTO界面阻抗低、锂均匀沉积并抑制锂枝晶。因此，基于Li阳极的对称电池以及与LiNiCoAlO（NCA）、LiFePO（LFP）和FeF阴极组成的全电池具有卓越的电化学性能。具体而言，Li/LLZTO/Li对称电池在0.1 mA·cm下实现了长达10000小时的显著循环寿命；Li/LLZTO/NCA全电池在0.5C下500次循环后容量保持率为73.4%；全固态Li*/LLZTO/FeF全电池在100 mA·g下500次循环后实现了147 mAh·g的可逆容量。这项工作展示了用于超稳定Li*/石榴石界面的潜在设计策略，以实现高性能的SSLMBs。
