Ultrastable Anode/Electrolyte Interface in Solid-State Lithium-Metal Batteries Using LiCu x Nanowire Network Host

Qiushi Dai; Jun Zhao; Hongjun Ye; Jingzhao Chen; Yong Su; Tingting Yang; Qiunan Liu; Haiming Sun; Hui Li; Jingming Yao; Zhiying Gao; Xingjie Fu; Dingding Zhu; Jitong Yan; Mingyu Li; Hailong Qiu; Qiao Huang; Liqiang Zhang; Yongfu Tang; Xiangxin Guo; Jianyu Huang

doi:10.1021/acsami.1c11613

Ultrastable Anode/Electrolyte Interface in Solid-State Lithium-Metal Batteries Using LiCu _x Nanowire Network Host

ACS Appl Mater Interfaces. 2021 Sep 15;13(36):42822-42831. doi: 10.1021/acsami.1c11613. Epub 2021 Sep 2.

Authors

Qiushi Dai¹, Jun Zhao¹, Hongjun Ye¹, Jingzhao Chen¹, Yong Su², Tingting Yang¹, Qiunan Liu¹, Haiming Sun¹, Hui Li¹, Jingming Yao¹, Zhiying Gao¹, Xingjie Fu³, Dingding Zhu², Jitong Yan⁴, Mingyu Li¹, Hailong Qiu¹, Qiao Huang², Liqiang Zhang¹, Yongfu Tang⁴, Xiangxin Guo⁵, Jianyu Huang^{1

2}

Affiliations

¹ Clean Nano Energy Center, State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao 066004, P. R. China.
² School of Materials Science and Engineering, Xiangtan University, Xiangtan, Hunan 411105, P. R. China.
³ Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Binhai New City, Fuzhou 350207, P. R. China.
⁴ Hebei Key Laboratory of Applied Chemistry, College of Environmental and Chemical Engineering, Yanshan University, Qinhuangdao 066004, P. R. China.
⁵ College of Physics, Qingdao University, Qingdao 266071, P. R. China.

PMID: 34473463
DOI: 10.1021/acsami.1c11613

Abstract

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_x 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 Li_6.4La₃Zr_1.4Ta_0.6O₁₂ (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 LiNi_0.88Co_0.1Al_0.02O₂ (NCA), LiFePO₄ (LFP), and FeF₂ 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^-2; the Li*/LLZTO/NCA full cell maintains capacity retention of 73.4% after 500 cycles at 0.5C; and all-solid-state Li*/LLZTO/FeF₂ full cell achieves a reversible capacity of 147 mAh·g^-1 after 500 cycles at 100 mA·g^-1. This work demonstrates potential design tactics for an ultrastable Li*/garnet interface to enable high-performance SSLMBs.

Keywords: LiCux NW; anode/electrolyte interface; garnet solid-state electrolyte; lithium anode; nanowire host.