Citation: Xuejie Gao, Xinyang Chen, Ming Jiang, Hanyan Wu, Wenfeng Ren, Xiaofei Yang, Runcang Sun. Long-lifespan thin Li anode achieved by dead Li rejuvenation and Li dendrite suppression for all-solid-state lithium batteries[J]. Chinese Chemical Letters, ;2024, 35(10): 109448. doi: 10.1016/j.cclet.2023.109448 shu

Long-lifespan thin Li anode achieved by dead Li rejuvenation and Li dendrite suppression for all-solid-state lithium batteries

Xuejie Gao ^{a, 1} ,
Xinyang Chen ^{a, 1} ,
Ming Jiang ^c ,
Hanyan Wu ^a ,
Wenfeng Ren ^a ,
Xiaofei Yang ^{b, *,} ,
Runcang Sun ^{a, *,}

a.
Center for Lignocellulosic Chemistry and Biomaterials, College of Light Industry and Chemical Engineering, Dalian Polytechnic University, Dalian 116034, China
b.
Division of Energy Storage, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
c.
Institute of Physical Science and Information Technology, Anhui University, Hefei 230601, China

yangxf@dicp.ac.cn

rcsun3@dlpu.edu.cn

Received Date: 9 November 2023
Revised Date: 7 December 2023
Accepted Date: 20 December 2023
Available Online: 22 December 2023

Figures(6)

Solid polymer electrolytes (SPEs) are considered to be one of the most promising systems applied in all-solid-state lithium metal batteries (ASSLMBs) on account of their chemical and electrochemical robustness, mechanical stability, cost-effective and scalable manufacturing techniques. Lately, significant endeavors have been directed towards mitigating the formation of the Li dendrite in SPE-based ASSLMBs, while research on the inactive lithium in the forms of the solid-electrolyte interface has been rarely reported. Herein, a bi-functional GaI₃ additive is developed for in-situ generating Li₃Ga alloy for suppressing Li dendrite growth, as well as I₃⁻ in recovering dead lithium. Relying on the density functional theory (DFT) results, the Li atom prefers to deposit on the Li₃Ga surface and then guide uniform Li deposition, while the I₃ species features a relatively lower lowest unoccupied molecular orbital (LUMO) energy level (-2.12 eV), meaning a higher electron affinity, which is beneficial for reviving inactive lithium to counterbalance the loss of lithium. As a result, in comparison to cells employing pure PEGDME-based electrolytes, the Li-Li symmetric cells utilizing GaI₃-containing solid-state electrolyte exhibited a cycling life nearly 30 times longer at a current density/capacity of 0.2 mA/cm², 0.2 mAh/cm². The full batteries of LFP//1%GaI₃-SPE//40 µm Li delivered a noteworthy capacity retention of 82% after 1300 cycles at a rate of 1 C.
- Synergistic effect,
- In-situ Li₃Ga alloy,
- Suppress Li dendrite,
- Dead lithium regeneration,
- All-solid-state lithium metal batteries
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